United States
Environmental Protection
Agency
EPA-90D-79-006 B
Applicability of Land
Treatment of
Wastewater in the Great
Lakes Area Basin
Effectiveness of Sandy
Soils at Muskegon County,
Michigan, for Renovating
Wastewater
                          MCD-55

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Preface

The U. S. Environmental Protection Agency was created because of in-
creasing public and governmental concern about the dangers of pollu-
tion to the health and welfare of the American people.  Noxious air,
foul water, and spoiled land are tragic testimony to the deterioration
of our natural environment.

The Great Lakes National Program Office (GLNPO) of the U.S. EPA was
established in Region V, Chicago, to provide specific focus on the
water quality concerns of the Great Lakes.  The Section 108(a)
Demonstration Grant Program of the Clean Water Act (PL92-500) is
specific to the Great Lakes drainage basin and thus is administered
by the Great Lakes National Program Office.

Land disposal of wastewater in the Great Lakes area is one alternative
for treatment that can provide tertiary quality effluent when properly
managed.  This report evaluates the effectiveness of sandy soils at
Muskegon County, Michigan, for renovating wastewater.

We hope the information and data contained herein will help planners and
managers of pollution control agencies to make better decisions
in carrying forward their pollution control responsibilities.
                                   Edith J. Tebo, Ph.D.
                                   Director
                                   Great Lakes National Program Office

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      APPLICABILITY OF LAND TREATMENT OF WASTEWATER
             IN THE GREAT LAKES AREA BASIN:


    EFFECTIVENESS OF SANDY SOILS AT NUSKEGON COUNTY,
           MICHIGAN, FOR RENOVATING WASTEWATER

                           by
B. G. Ellis, A. E. Erickson,  A.  R.  Wolcott,  B.  D.  Knezek,
               J. M. Tiedje and  J.  Butcher
    Departments:  Crop and Soil Sciences,  Entomology
                Michigan State University
              East Lansing, Michigan  48824
                           for
           Michigan Water Resources Commission
             Department of Natural Resources
                Lansing, Michigan  48926
                  EPA Grant No. G005104
                    Project Officers
              J. M. Walker and S.  Poloncsik
           Office of Research and Development
                 SECTION 108 (a)  PROGRAM
           GREAT LAKES NATIONAL PROGRAM OFFICE
     U.S. ENVIRONMENTAL PROTECTION AGENCY,  REGION V
                CHICAGO, ILLINOIS  60605

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                           EPA REVIEW NOTICE
This report has been reviewed by the Office of  Research  and Development
and the Great Lakes National Program Office of  Region V, U.S. EPA,
Chicago, and approved for publication.   Approval does not  signify  that
the contents necessarily reflect the views and  policies  of the Environmental
Protection Agency, nor does mention of  trade names  or commercial products
constitute endorsement or recommendation for use.
                                 ii

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                               FOREWORD

The Great Lakes are the world's largest fresh water resource.   It is
shared by the United States and Canada.  In the U.S., this lake system
serves important water needs of people and industries in eight states,
six of which comprise the area served by EPA Region V.   The usefulness
of the lakes, for many purposes, has been impaired by past misuses of
the lakes themselves and of land resources in contributing drainage
basins.  Management of the Great Lakes Area Basin to halt or reverse the
degradation of vital water resources is of great importance to both
countries.  Lake Michigan presents special concerns because of its
headwater relationship to the lower Great Lakes and because of the
intensity and variety of human activity that impacts upon it.   Responsi-
bilities for developing and enforcing ameliorative management  in the
Lake Michigan basin rest with the U.S. and the four states that share
the shoreline of the lake.

Land application of wastewater is one of the management options for
upgrading water after use.  From historical precedent and for  many
theoretical reasons, land application has the potential for effecting
full renovation of wastewater before release into the environment.
Whether this potential is realized will depend on many factors of soil,
climate and management which must be understood for each situation.
Performance must be assessed ultimately in terms of impact on  contiguous
aquatic systems.  The acquisition of background and early operational
data for a large land application system in Muskegon County, Michigan,
has been the objective of an intensive three-year study conducted for
EPA Region V by the Michigan Water Resources Commission, with  sub-
contracts to Michigan State University and the University of Michigan.
The three reports covering this work carry the general title,  "Applicability
of Land Treatment of Wastewater in the Great Lakes Area Basin," with
respective subtitles:

     The Muskegon County System—An Overview, Monitoring Considerations
     and Impacts on Receiving Waters.

     Effectiveness of Sandy Soils at Muskegon County, Michigan, for
     Renovating Wastewater.

     Impact of Wastewater Diversion, Spray Irrigation on Water Quality
     in Muskegon County, Michigan, Lakes.

In these volumes, data collected from 1972 through 1975 are evaluated in
relation to the applicability of land treatment for renovating municipal
and industrial wastewaters in Muskegon County.  Short-term and long-term
projections are made regarding management practices that can influence
the renovative effectiveness of soils and crops.  Observed and projected
effects of wastewater diversion and treatment on water quality and
ecosystem responses in lakes and streams that drain into Lake  Michigan
are described.
                                   iii

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                                   ABSTRACT

A key concept in design of the Muskegon Wastewater Management System is the
use of soils and crops as a "living filter."  Management to achieve a desired
degree of renovation at acceptable cost requires a knowledge of changes that
occur in water as it passes through the system, as well as a knowledge of
changes in soil that can be projected to estimate useful life of the system.

Four major soil types (Rubicon sand, AuGres sand, Roscommon sand and Granby
loamy sand) comprise a majority of the land area on the Muskegon wastewater
management site.  Analysis of soil profile samples representing each of the
four major soil types were conducted to determine the level of Kjeldahl N, N0_,
NH4, Ca, Mg, Na, K, P, Fe, Zn, Mn, Cu, Hg, Pb, total C and pH prior to appli-
cation of wastewater and after application of wastewater during 1974 and 1975.
Summaries of data are given in this report.  Some nitrate moved through the soil
profiles, apparently more the result of initiating the farming operation than
from applying wastewater.  Phosphorus was being adsorbed by the Rubicon sands
and Roscommon sands.  The AuGres sands did not appear to be adsorbing P, and
insufficient wastewater had been applied to the Granby loamy sands to make a
valid inference.  Soils which had received more than 300 cm of wastewater had
reached an equilibrium with respect to Na, Ca and Mg which allowed most of the
Na applied to pass through the soil profile.  Soil pH was increasing and should
approach the pH of the wastewater in a few years.  There was no apparent accumu-
lation of heavy metals in the soils due to a very low input of metals.

Soil physical properties were evaluated by measurement of infiltration rate,
hydraulic conductivity and bulk density.  The majority of these very sandy
soils will conduct water so fast that infiltration and hydraulic conductivity
should not be a problem.  However, a small percentage of the soils mapped as
Saugatuck or AuGres have been observed to have very slow hydraulic conductiv-
ities.

Electron-capturing organic chemical species were monitored in soils and waters,
using multi-column gas-liquid chromatography and thin layer.  Patterns of
encounter with 26 pesticide parameters in incoming wastewater are evidence
that chemicals from non-point sources can enter through feedwaters taken from
lakes and streams by industries that discharge into the system.  By inference,
chemicals that originate in extramural point-source discharges can enter also.
The potential problem from industrial trace organics originating within the
service area was addressed only superficially by analytical protocol employed
in this study.  Evidence was obtained for chronic entry, at substantial con-
centrations, of diethylhexylphthalate and three unreferenced electron-capturing
species.  Removals of trace organics from wastewater occurred in storage lagoons
and during passage through the soil mantle.  Chromatographic peaks observed in
incoming wastewater and peaks for pesticides used on site were found in extracts
of soils sampled after the system was placed in operation.  Intercepted chemicals
were found mainly in surface and shallow subsoil layers.  Organic chemicals
detected in drainage at outfalls were associated with heavy rains and with
                                       IV

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seasonally heavy applications of wastewater on restricted soil areas.
Frequency and concentration at outfalls for chronically input chemicals
declined from 1974 to 1975.  This suggests developmental changes in lagoons
and soils leading to increased effectiveness in removal of these chemicals
from wastewaters passing through the system.

This report was submitted in fulfillment of a subcontract by Michigan State
University to Michigan Water Resources Commission as part of their Grant
No. G005104 under the sponsorship of the U.S. Environmental Protection
Agency.  This report covers the period of April 1, 1972 to December 31, 1975,
and work was completed as of June 30, 1976.
                                      v

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                             CONTENTS
                                                                       Page

Forward	   ill
Abstract	   iv
List of Figures	   ix
List of Tables	    x
Abbreviations  	  xv
Acknowledgements	   xvi

Sections

     I  Summary and Conclusions  	    1

    II  Recommendations  	    7

   III  Introduction	    9

    IV  Chemical Analysis of Soil Profile Samples  	   16
        Introduction	   16
        Nitrogen	   18
             Effect of Soil Type on the Initial Nitrogen Content of
                  Soil Profiles	   18
             Effect of Drainage and Farming on Nitrogen in Soil
                  Profiles	   28
             Effect of Application of Wastewater on Nitrogen Distri-
                  bution in Soil Profiles	   30
        Calcium, Magnesium, Sodium, and Sodium Adsorption Ratio (SAR^   36
             Cation Exchange Capacity  	   38
             Background Levels of Exchangeable Bases	   38
             Changes in Exchangeable Bases with Application of
                  Wastewater	   39
        Phosphorus	   42
             Effect of Soil Type on the Initial Phosphorus Content of
                  Soil Profiles	   42
             Phosphorus Adsorption Maximum for the Major Soil Types  .   42
             The Relationship between Phosphorus and Agricultural
                  Production	   44
             Phosphorus Adsorption by Soils after Application of
                  Wastewater	   44
             Life of Site for Phosphate Removal	   48
         Soil pH	   51
             Background data	   51
             Changes Induced by Agronomic Development  	   52
             Changes Induced by Wastewater Application	   52

         Total  Carbon	   52

         Postassium	   53
             Background Data for Potassium	   53
             Changes Induced by Wastewater Application	   53

                                 vi

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                        CONTENTS (Continued)                       ^
                                                                   Page

        Total Soil Analysis	55

     V  Heavy Metals	57
        General Background and Summary	57
        Chelate Extractable Heavy Metals	67

    VI  Soil Physical Properties	68
        Study Sites	68
        Methods of Study	68
             Infiltration 	  68
             Mechanical Composition 	  69
             Hydraulic Conductivity and Soil Water Characteristic .  69
             Aeration and Redox	70
        Results and Discussion	70
             Mechanical Composition 	  70
             Soil Water Characteristics, Bulk Density and Hydraulic
                  Conductivity	70
             Infiltration 	  72
             Oxygen Diffusion Rates and Redox Potential 	  72
             Addendum	72

   VII  Microbial Studies 	  74

  VIII  Pesticides and Industrial Trace Organics	77
        Introduction	77
        Procedures	78
        Sampling and Extraction of Soils	78
        Sampling and Extraction of Water	79
        Cleanup of Extracts	79
             Detection and Quantitation of Organics 	  79
             Confirmation of Peak Identities	79
        Trace Organics in Waters	79
             Probable Sources and Modes of Entry	80
             Raw Influent and Discharges into Storage	84
             Pre-Chlorination Flows and Irrigation Water (1974) . .106
             Outfall Waters	106
             Frequencies of Occurrence and Ranges of Concentration
                  in Waters	110
             Particulate-Phase/Aqueous Phase Distributions	113
        Trace Organics in Soils	115
             Background Samples	115
             Post-Irrigation Samples	126
             Frequencies of Occurrence and Ranges of Detection. . .127
        Evaluation of Methods	134
        Summary—Trace Organics	137
        Recommendations	138
        Research Needs	139
        References	141

Appendix I—Methods of Analysis for Nutrients	145
Appendix II—Analytical Procedures for Trace Organics	150
Appendix III--Nutrient Content of Corn	164

                                vii

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                       CONTENTS (Continued)
Appendix IV--Availability of Data From U.S. EPA Storage
             and Retrieval Computer System "STORET"	165
                                Vlll

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                              FIGURES




Number                                                           Page




  1    Location of sampling sites for soils     and outfalls .  .  .15




  2    Major soil types at Muskegon Wastewater Treatment site.  .  .17
                              ix

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                              TABLES

Number                                                         Page

  1     List of Chemical Analyses Data Reported During Project
           Period	12

  2     Wastewater Application to Sampling Sites	13

  3.    Estimation of the Quantity of Nutrients Applied to Soils
           through Irrigation with Wastewater 	 14

  4     Sites Combined in Summarizing Each Soil Type	19

  5     Mean and Standard Deviations for Extractable and soluble
           Nutrient Content of Soils from Muskegon Spray Area-
           Baseline Data Rubicon Sand	20

  6     Mean and Standard Deviations for Extractable and Soluble
           Nutrient Content of Soils from Muskegon Spray Area-
           Baseline Data Roscommon Sand	21

  7     Mean and Standard Deviations for Extractable and Soluble
           Nutrient Content of Soils from Muskegon Spray area-
           Baseline Data Augres Sand	22

  8     Mean and Standard Deviations for Extractable and Soluble
           Nutrient Content of Soils from Muskegon Spray Area-
           Baseline Data Granby Sand	23

  9     Mean and Standard Deviation for total Nutrients of Soils
           from Muskegon Spray Area-Baseline Data Rubicon Sand. 24

 10     Mean and Standard Deviation for Total Nutrients of Soils
           from Muskegon Spray Area-Baseline Data Roscommon Sand 25

 11     Mean and Standard Deviation of Total Nutrients of Soils
           from Muskegon Spray Area-Baseline Data Augres Sand.  .26

 12     Mean and Standard Deviation of Total Nutrients of Soils
           from Muskegon Spray Area-Baseline Data Granby Sand.  .27

 13     Ammonium and Nitrate Contents of the Soil Profile at Site
           35  (Granby Sand)	29

 14     Mean and Standard Deviations for Extractable and Soluble
           Nutrient Content  of Soils from Muskegon Spray Area
           After Eight  Inches of Effluent Rubicon Sand	31

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                          TABLES (Continued)

Number                                                            Page

  15    Mean and Standard Deviations for Extractable and Soluble
          Nutrient Content of Soils from Muskegon Spray Area
          After Eight Inches of Effluent Roscommon Sand	32

  16    Mean and Standard Deviation for Extractable and Soluble
          Nutrient Content of Soils from Muskegon Spray Area
          After Eight Inches of Effluent AuGres Sand	33

  17    Mean and Standard Deviation for Extractable and Soluble
          Nutrient Content of Soils from Muskegon Spray Area
          After Eight Inches of Effluent Granby Sand	34

  18    Ammonium Content of Soil From Site 01.   (Circle 5)  as
          Compared to the Average of the Remaining Seven Rubicon
          Sites	35

  19    Average Content of Wastewater in the Lagoons at Muskegon
          waste Treatment Facility (Data from Demirjian, 1975,
          1976)	37

  20    Sodium, Calcium and Magnesium Concentrations in the Soil
          Profile of Site 01 (Circle 5) as a Function of Effluent
          Application	40

  21    Phosphorus Adsorption Capacity of Selected Samples  from
          Muskegon Wastewater Facility	43

  22    Increase in Extractable P after Application of 380  cm
          Wastewater to Site 02 (Circle 8)	46

  23     Change in Extractable P After Application of  380  cm
          Wastewater to Site 04 (Circle 24)	47

  24    Estimated Number of Years that P may be Removed from Waste-
          water Applied at 152 CM (60 Inches) per year	49

  25    Effect of Uneven Distribution of Water on the Effective
          Life of P Removal on Rubicon Sand	50

  26    Ammonium Acetate Extractable K at Various Sampling  Periods. 54

  27    Mean and Standard Deviation of Extractable Heavy Metals of
          Soils from Muskegon Spray Area-Baseline Data Rubicon
          Sand	58

  28    Mean and Standard Deviation of Extractable Heavy Metals of
          Soils from Muskegon Spray Area-Baseline Data Roscommon
          Sand	59

                                xi

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                        TABLES (Continued)

Number                                                            Page

29    Mean and Standard Deviation of Extractable Heavy Metals of
         Soils from Muskegon Spray Area-Baseline Data AuGres ...  60

30    Mean and Standard Deviation of Extractable Heavy Metals of
         Soils from Muskegon Spray Area-Baseline Data Granby Sand.  61

31    Mean and Standard Deviation of Total Heavy Metals of Soils
         from Muskegon Spray Area-Baseline Data Rubicon Sand ...  62

32    Mean and Standard Deviation of Total Heavy Metals of Soils
         from Muskegon Spray Area-Baseline Data Roscommon Sand . .  63

33    Mean and Standard Deviation of Total Heavy Metals of Soils
         from Muskegon Spray Area-Baseline Data AuGres Sand. ...  64

34    Mean and Standard Deviation of Total Heavy Metals of Soils
         from Muskegon Spray Area-Baseline Data Granby Sand....  65

35    Changes in Chelate Extractable Fe, Mn, Zn and Cu after Appli-
         cation of Wastewater	66

36    Summary of Averages of  Soil Physical Properties by Soil Series
         and Horizons	71

37    Summary of Infiltration Rates Determined During 1973-1975.  .  73

38    Change in Microbial Populations and Selected Chemical Parameters
         in Response to Initial Wastewater Irrigation on Three
         Soil Types	75

39    Trace Organics in Raw Influent, Muskegon, December 1973 to
         December 1974	85

40    Trace Organics in Raw Influent, Muskegon, Jan to Dec  1975.  .  86

41    Trace Organics in Discharges  into Storage Lagoons, Muskegon,
         April to Dec. 1974	87

42    Trace Organics in Discharges  into Storage Lagoons, Muskegon,
         Jan. to Dec.  1975	88

43    Trace Organics in Raw Influent and  in Discharge into  Storage
         Whitehall, Apr. to Dec.  1975	89

44    Trace Organics in Pre-Chlorination  Flows and Irrigation Water,
         Muskegon,  Jun. 74  to Dec.  74	90

45    Trace Organics in North Outfall Waters  (SW-05, Mosquito Creek),
         Muskegon;  Apr. 74  to Dec.  75	91

                                 xii

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                          TABLES (Continued)

Number                                                            Page

  46    Trace Organics in South Outfall Waters (SW-34, Black
           Creek), Muskegon, Apr. 74 to Dec. 75	   92

  47    Frequencies of Occurrence, Trace Organics in Waters, Muske-
           gon, Dec. 73 to Dec. 75	   93

  48    Detected Ranges of Concentration, Trace Organics in Water,
           Muskegon, Dec 73 to Dec. 75	   94

  49    Distribution of Trace organics Between Particulate and
           Aqueous Phases, Muskegon Wastewaters, Dec. 73 to Dec 75.114

  50    Trace Organics in Soils, Muskegon and Whitehall Systems,
           Background Samples Taken Summer 1972 or June 1973 (25
           Surface Samples, 14 Subsoil Samples) 	  116

  51    Trace Organics in Soils, Special Study Sites, Muskegon,
           Background Samples Taken June 197 3 and April 1974 (Sur-
           face Soils, 0-6")	119

  52    Trace Organics in Soils, Special Study Sites, Muskegon,
           Background Samples Taken June 1973 and April 1974 (Sub-
           Soils, 46-61 cm)	120

  53    Trace Organics in Soils, Special Study Sites, Muskegon,
           (November 1974 Sampling) 	  121

  54    Trace Organics in Soils, Special Study Sites, Muskegon
           (April 1975 Sampling)	122

  55    Trace Organics in Soils, Special Study Sites, Muskegon
           (October 1975 Sampling)	123

  56    Trace Organics in Soils, Special Study Sites, Whitehall,
           Background Samples Taken June 1973 and April 1974.  .  .  124

  57    Trace Organics in Soils, Special Study Sites, Whitehall,
           (Samplings of Nov. 1974, Apr. 1975 and Oct. 1975).  .  .  125

  58    Frequencies of Occurrence, Trace Organics in Soils, Muskegon,
           June 73 to October 75	128

  59    Frequencies of Occurrence, Trace Organics in Soils, Whitehall,
           June 73 to October 75	129

  60    Detected Ranges of Concentration.  Trace Organics in Soils,
           Muskegon, June 73 to Oct. 75	130

  61    Detected Ranges of Concentration, Trace Organics in Soils,
           Whitehall, June 73 to October 75	.131
                                 xiii

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                          TABLES (Continued)

Number                                                          Page

 II-l   Reference Chemicals (Purified Grade) and Sources .... 159

 II-2   Standard Solutions in (Benzene):   Retention Times (R )
           on Four GLC Columns and Typical Sensitivities and
           Detection Limits for the Quantitating Column	161

 II-3   Florisil Eluants:  Fractional Distributions and Total
           Recoveries for Reference Chemicals	163

III-l   Estimated Nutrient Content of Corn Grain (15.5% Moisture)164
                               xiv

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                     LIST OF ABBREVIATIONS AND SYMBOLS
ABBREVIATIONS

X
SD
ppm         —
ppb
me          —
ml          —
cm          —
8
kg/ha
ng/g
ng/1
GLC
TLC
GC-MS

BCD

SYMBOLS
mean
standard deviation
parts per million
parts per billion
milliequivalent
milliliter
centimeter
gram
kilogram/hectare
nanograms/gram (ppb)
nanograms/liter (parts per trillion)
gas-liquid chromatography
thin layer chromatography
mass spectrographic analysis of chemical species
isolated by preparative gas chromatography
electron capture detector
N
P
K
Ca
Mg
Na
Zn
Cu
Mn
Fe
Pb
Hg
Cr

NH4H
N03'
nitrogen
phosphorus
potassium
calcium
magnesium
sodium
zinc
copper
manganese
iron
lead
mercury
chromium
carbon
ammonium ion
nitrate ion
                                    xv

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                         ACKNOWLEDGMENTS

We gratefully acknowledge the cooperation and effort made by many
individuals in the development and operation of this project.  In
particular, Dr. Demirjian and his staff and the County of Muskegon
have been most cooperative and helpful in allowing us to collect
samples, collecting and retaining samples for us, and lending assis-
tance and equipment for on-the-spot use.  Their data has also been
made available whenever requested and has been absolutely necessary
for the interpretation of our data.

The Michigan Water Resources personnel have also contributed greatly
to the project in discussions and assembling and reproducing reports.

We would also gratefully acknowledge the cooperation and guidance
of Stephen Poloncsik and Dr. John M. Walker, Project Officers during
various phases of this project; Mr. Robert Bastian, EPA's special
representative at Muskegon; and to the Region Five personnel, Mr.
Ralph G. Christenson and Mr. Cliff Risley who worked closely with
the project.

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                                 SECTION I

                          SUMMARY AID CONCLUSIONS

GENERAL

Baseline data has been established for the major soil types at the Muskegon
land treatment system (Rubicon sand, Roscommon sand, AuGres sand, and Granby
loamy sand) for physical properties, chemical analysis, heavy metals, pesti-
cides, and certain industrial organics, microorganisms, and arthropods.
Establishment of the baseline levels and the soil variability within the soil
irrigation site allows for evaluation of the effectiveness of the land treat-
ment process in renovating wastewater.  Comparisons between baseline data and
soil analysis after one or two years of application of wastewater will allow
for predictions of the effectiveness of the system and possible management
changes that must be made to improve the effectiveness of the operation.
The soils were initially free of contamination from heavy metals.  Very low
levels of dieldrin and DDT species were indicated in most surface soils and
many subsoils, using chromatographic methods and electron capture for de-
tection.

CHEMICAL ANALYSIS

Both total and "available" nutrient analyses were determined for P, K, Ca,
Mg, and Na on profile samples from each of the major soil types.  Profile
samples were collected twice yearly from 15 cm (6 inch) layers to depths of
305 cm (10 feat).  Total C and N, distillable NH3, soluble N03, and pH were
also determined.  From the data the following conclusions were drawn:

1.  Available or extractable nutrients are much more sensitive to changes
produced by wastewater application for P, K, Ca, Mg, and Na than is total
analysis.  Changes in the available fraction were detected after as little
as 20 cm (8 inches) of wastewater application; whereas, few differences were
noted in total analysis after application of more than 380 cm (150 inches)
of wastewater.

2.  The NO^ content of Rubicon, Roscommon, and AuGres sands is low.  Further-
more, irrigation with the rather low N containing wastewater does not supply
adequate N for maximum growth of corn during the period of peak demand (i.e.,
during the months of July and August), but during the remainder of the year
some N as N03 is expected to be lost through the soil into the drainage water
because it is present in excess of crop needs.  In general, this quantity of
N moving in the soil profiles was under 5 ppm N as NO^, but occasional samples
were much higher.  The NO^ tended to move in bands in the soil profiles.  High
values for N03 were raore comnonly found in the Granby soils and appeared to

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originate from the oxidation of native organic matter in the surface layers
and not from wastewater application.

3.  Phosphorus was effectively removed from the wastewater applied to
Rubicon sand by adsorption in the surface layers.   The effective life of
the Rubicon sand for removal of P by  this mechanism should be more than 50
years at the present level of P input (less than 3 ppm P), average applica-
tions of 150 cm water per year, and with yields from 80 to 100 bushels of
corn per acre.  Initial data did not  show a gain of P in the AuGres and Gran-
by soils.  This may be partially attributed to lower application rates, par-
ticularly for the Granby soils, but adsorption isotherms also indicated that
these soils had lower adsorption capacities and that the AuGres soils may not
bind P as tightly as the other soil series.

4.  Uneven distribution of wastewater on the soil may adversely affect the
life of the system.  One site appeared to have received far less water in the
sampling area than was reported which suggests heavier application in other
parts of the circle.  This can lead to P leaking at an earlier than predicted
time.

5.  Two years of application of wastewater was adequate to allow for passage
of Na throughout the profile.  A land treatment system is not effective in
removing cations (Na, Ca, Mg and K),  but rather the process that functions
is one of cation exchange whereby adsorption of one base will result in re-
lease of another.  Some adsorption of Na does occur in the soils with release
of Ca, but an equilibrium is soon reached after which the water passing
through the soil will be very similar in bases to the wastewater being ap-
plied.  Our data would suggest that on all sites where greater than 305 cm
(120 inches) of wastewater have been applied, the Wa content of the tile
drainage water should be the same as the water being applied.  Where dis-
charge water levels of Na are lower than in the wastewater, dilution by
other drainage water has apparently occurred.  The level of exchangeable Na
at this equilibrium is not expected to cause appreciable change in  the physi-
cal properties of  these very sandy soils. High levels of Na in soils may lead
to dispersion of clay and organic matter and reduced infiltration of water.
Rubicon, Roscommon and AuGres sands are so low in clay and organic matter
content that they  are unlikely to be affected by the levels of Na in the
wastewater.  If any changes do occur, they should be expected on the Granby
soil which is considerably higher in organic matter.  Insufficient water has
been applied to the Granby soils at this time to ascertain  if there will be
any dispersion effects in the  soil resulting  in decreased ability of the soil
to accept water.

6.  Potassium is moving through  the soils and leaching  into the discharge
waters.  This occurs because the concentration of K  is much lower in the
water being applied than is the  concentration of Ca  and Mg  and does not com-
pete favorably with Ca and Mg  for exchange sites.  In addition to concentra-
tion, a major factor is that the monovalent K ion is not bonded as  strongly
to the exchange complex as are the divalent Ca and Mg ions.

7.  Total C content of Rubicon,  AuGres and Roscommon soils  is very  low.
Hence, these  soils are very effective  in eliminating BOD  from  the applied

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wastewater.  An increase in organic matter (C) would likely increase the
agricultural productivity of these soils.  This could be accomplished
through application of sludge.  Since the Granby soils are already high in
total C in the surface layers, low in P adsorption capacity, and release N
by decomposition of organic matter, an application of sludge would not be de-
sirable, but if well drained, the Granby soils will function well in reducing
BOD from wastewaters.

8.  Soil pH is increasing rapidly with the application of wastewater and
should stabilize within the next two years to a level near that of the in-
coming wastewater.  The soil adsorbs Ca, Mg and Na from the wastewater and
the H replaced is neutralized by the basic water.  This pH is slightly higher
than is desirable for agronomic purposes but should pose little problem.

9.  Low soil pH's resulted from draining and aerating the Granby soils prior
to application of wastewater.  This is usually a result of oxidation of S
that has accumulated in the subsoils.  As a result, Fe was mobilized and
moved into the drainage watar.  These soil pH values are increasing due to
movement of bases down in the profile after application of wastewater and to
soil chemical reactions.  Iron in the soil should soon stabilize as the pH
increases above 4 to 5.

PHYSICAL MEASUREMENTS

Initial clearing and beginning farming operation of these soils has left them
so variable in the surface layers that meaningful physical measurements are
difficult, and it is impossible to establish trends from the short period of
time that wastewater has been applied.  But the following conclusions may be
drawn:

1.  Infiltration rates are so high on all major soil types that it is diffi-
cult to imagine that this will ever become a limiting factor.  But some micro-
areas of Saugatuck sand may have limited infiltration.

2.  All aeration measurements have shown a high degree of aeration except
where there are definite drainage malfunctions.  Therefore, once drainage is
improved, aeration should be no problem.

HEAVY METALS

Selected total and chelate extractable micronutrient and heavy metal analyses
were conducted on soil profile samples.  The elements determined were Fe, Mn,
Zn, Cu, Pb, and Hg on samples taken at 15 cm  (6 inch) intervals down to a
depth of 305 cm (120 inches) in Rubicon sand, Roscommon sand, AuGres sand,
and Granby loamy sand which are the main soil types on the wastewater treat-
ment site.  From the data, the following conclusions were drawn:

1.  Total analyses indicate that none of the soil metals were increased sig-
nificantly by the addition of wastewater.  Lead and Hg, which are of parti-
cular concern, are still at levels below the detection limits of the methods
used.  Zinc which may have been added in amounts up to 0.2 ppm Zn in the
wastewater, did not show any total accumulation, even though 7.8 kg/ha of Zn

-------
per acre could have been added at sites receiving more than 380 cm (150 in-
ches) of wastewater.  Crop removal would account for less than 1 kg/ha of Zn.
Therefore, Zn should be detected in the surface samples in the next few years
if the level in the irrigation water is greater than 0.1 ppm Zn.

2.  Total Fe values fluctuated considerably throughout the soil profile, but
there was no obvious change in Fe content with profile depth. Total Cu and
Zn, and to a lesser extent Mn, were localized in the top 15 cm (6 inches) to
30 cm (12 inches) of soil.  The initial concentrations appeared to be asso-
ciated with the  organic matter in the surface layer of the soil.  After
plowing, the total Cu, Zn, and Mn were distributed to the depth of the plow
layer, but they did not move by leaching below that point over the duration
of the study.  The total quantity of heavy metals applied in wastewater  (380
cm) was very small compared to the total initially in the soil (less than 0.1
percent in all cases).  The localization of total Cu, Zn, and Mn in the sur-
face layers was most pronounced in the Rubicon sand.  By contrast, the total
Mn was relatively evenly distributed throughout the soil profile of the Gran-
by soil.  The other soils fell between these extremes.  The Mn in the lower
profile of the Granby sand can be explained by the relatively flooded (re-
ducing) conditions in the soil prior to drainage.  The flooded conditions
favored the formation of the relatively soluble manganous ion  (Mn"*~^) which
could move through the soil profile.  In contrast, conditions in the well-
aerated Rubicon sand favored the formation of the manganic ion  (Mn+^) which
forms relatively insoluble oxides that cannot move in the soil profile.  Also,
much of the Mn appeared to be associated with and bound to soil organic matter,
and Rubicon sand contained little organic matter below the soil surface.
Since solubility of Cu and Zn are not significantly influenced by soil oxida-
tion-reduction status, there were no pronounced changes in their soil profile
distributions as the result of aeration status.

3.  Chelate extractable soil micronutrients were determined  to estimate  the
magnitude of an "available" fraction which is potentially available for  plant
uptake and to movement through the soil profile with  irrigation water.   The
relative degree of extractability closely paralleled  the total amount of
micronutrient in the soil profile.  The relative magnitude of extractability
was as follows:  Fe>Mn>Zn>Cu.  Iron and Mn were the micronutrients most  in-
fluenced during the time frame of the investigation.  The changes which were
observed were due to changing the oxidation status of the soil with soil water
drainage and to disturbing the surface soil organic matter layer with the be-
ginning of cultivation practices.  Generally, the amount of  extractable  Fe
and Mn was high in  the surface layers of the soil initially  and decreased as
the organic fraction was broken up with cultivation practices.  Extractable
Fe in the surface layers decreased from a range of 50 to 200+  ppm Fe  ini-
tially to 10 to 40 ppm Fe by  the seventh sampling.  Initially  there were some
relatively high amounts of extractable Fe  (as much as 40 ppm Fe) in the  lower
levels of the soil profiles which had been flooded.   However,  as these  soils
were drained, the extractable Fe decreased to a background level below  10 ppm
Fe due to leaching of soluble Fe and formation of ferric hydroxide in the
well-aerated conditions.

Extractable Mn initially ranged from 1 to 40 ppm Mn in  the surface layers.
The extractable Mn  levels below the surface layers dropped to  about 1 ppm Mn

-------
and continued to decrease with time.  Most of the extractable fraction was
associated with the organic matter in the soil, and as the soil became well
aerated, less Mn was extractable due to the formation of more insoluble
manganese oxides.

Extractable Cu and Zn were less influenced by effects of management changes
on the soil.

TRACE ORGANICS

Local and regional hydrologic systems were described in some detail, with a
view to identifying probable sources and modes of entry for trace organics
into wastewater collection systems at Muskegon and Whitehall.  Electron-cap-
turing species were monitored in monthly composites of incoming wastewater
and outfall drainage over a two-year period.  The same analyses were per-
formed on extracts of soils sampled biennially, twice before and three times
after wastewater irrigation was initiated at the treatment sites.  Implica-
tions and limitations of the data are summarized here:

1.  Patterns of encounter with 26 pesticide parameters provide evidence that
chemicals from non-point sources can enter these systems through connected
discharges from industries that take their feedwaters from Muskegon Lake,
Mona Lake, White Lake or tributary streams.  By inference, chemicals origin-
ating at extramural point-sources can be expected also.

2.  A wide range of industrial chemicals which have become the focus of con-
cern in these systems was not addressed by analytical methods used in this
study.  Credible evidence for chronic entry of DEHP was obtained.  Peaks for
several unreferenced electron-capturing species were present frequently in
incoming wastewater but were not identified.

3.  In background soil samples, dieldrin and DDT species were indicated at
the very low concentrations that might be expected from global circulation,
with evidence at one sampling station for locally higher residues from earlier
use.

4.  Chromatographic peaks observed in incoming wastewaters and peaks for pes-
ticides used on site were found in extracts of soils after the systems were
placed in operation in 1974.  Both referenced and unreferenced species were
found mainly in surface  (0-15 cm) and shallow subsurface layers  (46-61 cm).
Encounters at 91-107 cm were infrequent or at levels approaching the limit
for quantitation.

5.  Outfalls were monitored only at the Muskegon site.  Detectable
amounts   observed for a number of chemicals  were associated with heavy
rains or with seasonally expedient modes of operation that resulted in un-
usually heavy applications of wastewater on limited soil areas.

6.  Data for successive flow points at Muskegon indicate that removals of
trace organics occurred both in storage lagoons and during passage through
the soil mantle.  Chemicals intercepted most effectively were those that are
strongly adsorbed by soils or sediments and those that are readily metabo-

-------
lized.  Chemicals responsible for unreferenced GLC/ECD peaks appeared to be
more recalcitrant or more mobile in soils than the referenced species.

7.  Chemicals observed frequently in incoming wastewater (lindane, heptachlor,
related species, DEHP) declined in frequency and concentration at outfalls
from 1974 to 1975.  This is hopeful evidence that the efficiency of the
system in removing exotic chemicals may improve over time.   Beneficial devel-
opmental changes may include the induction of adaptive enzymes in lagoons and
soils, increasing volume and adsorptive surface of sediments in lagoons, and
increased annual return of crop residues and exudates to support cometabolism
of recalcitrant compounds in soils and residual increases in adsorptive soil
organic matter.

MICROBIAL STUDIES

Limited microbial studies were made on three soil types representing  the ex-
tremes in the Muskegon land treatment site before and after wastewater appli-
cation.  The populations analyzed for were nitrifiers, denitrifiers,  aerobes,
and anaerobes.  The following conclusions were drawn:

1.  There was initially a very low number of nitrifiers on the Rubicon and
AuGres sands probably due to the very low soil pH.  This also related to
higher ammonium values on these soils.  As the pH increased with wastewater
application, the numbers of nitrifiers increased and ammonium disappeared.
The Granby initially had high soil pH's and a high nitrifier population.

2.  The denitrifier population relative to the total aerobes and anaerobes
was quite low in all soils, but there was a slight increase with irrigation,
particularly in the Rubicon soil.

3.  Irrigation with wastewater had no detrimental effect on the soil  micro-
bial community.

SOIL ARTHROPOD STUDY

Samples of soil arthropods were obtained and studied from each of the four
major soil types.  The soil animals were extracted and sorted into major
groups.  The soil faunal categories found to occur in the study area  were:
Diptera, Diptera  larvae, Coleoptera larvae, Hemiptera, Thysanoptera,
Enchytraeidae, Nematoda, Oribatid mites, predatory mites, and Collembola.
The major conclusion is that the site was and is very poor in both number
of species and in number of individuals.  If the soil organic fraction  in-
creased through application of sludge, the arthropod population would be
expected to increase.

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                                 SECTION II

                              RECOMMENDATIONS

GENERAL

Soil monitoring information indicates that the Muskegon County land treatment
site is generally operating in a satisfactory manner.  The initial years'
study indicates that certain areas should be monitored closely in the next
few months but that other areas are changing slowly and that a number of
years should elapse before reexamination of the latter areas.  The following
specific recommendations are divided into two general areas—management and
research needs:

Management

1.  The present balance between Na, Ca, and Mg in wastewater being applied
to the various coarse soils at Muskegon is satisfactory for crop growth and
soil structure, but the level of Na in this wastewater should not exceed
300 ppm.

2.  Differential water applications should be made, with Granby soils re-
ceiving substantially less water than Rubicon or Roscommon soils, because the
Granby soil has a lower P adsorption capacity, greater potential mineraliza-
tion of native N, and possible problems with dispersion of organic matter if
Na content becomes too high.

3.  Non-uniform application of wastewater should be avoided.  This practice
may materially shorten the period of time that the soil is able to remove P
from the wastewater.  Adsorption and degradation of organic chemicals requires
a period of time, and heavy application of wastewater may displace the or-
ganic chemicals before sufficient reaction time has occurred.

4.  From a crop management viewpoint:, available Mn and Zn both appear to be
at a low level where plant deficiencies could be a problem. Sufficient Zn to
prevent deficiencies may be added in the wastewater, but decreasing organic
matter in the soils and increasing soil pH as a result of added wastewater
may decrease the availability of Mn and Zn to plants.  Soil and plant Mn and
Zn levels should be monitored regularly to detect these possible deficiencies.

Research Needs

1.  A detailed study should be made of N stripping in the field by agronomic
crops to determine if both the period of effective NOo uptake by crops can
be extended and if the level of N03 leaching through to groundwater can be

-------
reduced.  Initial data indicates that NC>3 is leaching during periods when
the corn is not actively growing.

2.  Phosphorus adsorption in the AuGres soils should be examined in detail
because it does not appear to retain P.

3.  Soil physical measurements should be made again after approximately five
years of wastewater application to determine if long-term application will
affect the physical properties of very sandy soils.

4.  Areas of Saugutuck and a few areas of AuGres sands that are showing an
inability to remove water through the installed drainage should be studied
to suggest a management practice or improved drainage system that would
function in these areas.

5.  A close study of available heavy metals should be made in the next year.
The quantity of Zn, for example, that was supposed to have been added in the
wastewater should have been detectable in the soil but it was not found
during the first year after wastewater was applied.

6.  The monitoring of pesticides in soils at special study sites and of
waters at various stages of treatment should continue to confirm develop-
mental trends observed to date.  Additional flow points should be sampled to
increase the probability of detecting chemicals which enter sporadically.

7.  Routine monitoring for critical trace organics in waters at key flow
points within the collection and treatment systems is essential for rational
management.  This can best be done by personnel and facilities at the
Muskegon site.  Timely notification of anticipated critical discharges from
connected industries will be essential.

8.  An ordering of priorities among critical compounds considered for monitor-
ing is essential to allow for development of analytical capabilities and meth-
ods appropriate for different classes of compounds and realistic in relation
to available facilities, personnel and funds.  Methods for a given chemical
or group of chemicals should be  evaluated and quality control parameters es-
tablished before routine monitoring is undertaken.  Chromatographic entities,
when  first encountered, should be identified by definitive methods.

9.  Supporting research is needed to  identify mechanisms affecting the fate
of trace organics in  pretreatment basins, storage  lagoons and soil.  There
should be continuing  concern for the  possibility that specific  toxicants
might be transferred  from wastewaters  or sludges into animal feeds and human
food  channels.

10.   Computerization  will be required  to accumulate, retrieve and manipulate
the many kinds of information,  from many sources,  that are relevant  to the
management and regulation of these systems.  Modeling studies should continue
to this end.

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                                 SECTION III

                                INTRODUCTION

The methods of treating waste in the past have satisfactorily reduced BOD
but have not removed nutrients. Discharge of effluents after primary and/or
secondary treatment have often led to deterioration of rivers and lakes due
to inputs of nutrients as well as organic matter.  Federal and state regula-
tions now require that wastewaters be minimally polluting when they are dis-
charged into our waterways.  Land treatment of wastewater is one alternative
in removing polluting materials.  This method may be effective in the treat-
ment process, and it is also cost-effective in many cases;  but equally im-
portant, it offers a method of treatment that recycles a portion of the
nutrients directly back into the food chain, thereby offering conservation
of nutrients.

Soil types are of prime importance in considering various land treatment
alternatives.  Fine-textured soils offer considerable advantage in that they
are able to adsorb high quantities of P and other materials, but they have
a major disadvantage in that they are unable to receive high rates of water.
Oftentimes an application of just 2.5 cm of wastewater per week (1 inch), in
addition to the normal rainfall, may lead to reduced aeration and poor yields.
They would also require a considerable length of time after no water is ap-
plied before they could be farmed.

On the other end of the spectrum are the very sandy soils whose infiltration
rate and hydraulic conductivity are very high.  These soils can hydraulically
receive considerable quantities of wastewater without aeration problems, but
may not adequately remove P and other nutrients because of their low adsorp-
tion capacity, particularly at high rates of wastewater application.  Drainage
classification is another very important factor that must be considered in
selection of soil types for land disposal.  Since wastewater must move through
the soil for treatment, it is imperative that the drainage of the soil either
be good naturally or be developed into a good drainage system by the instal-
lation of tile drainage lines.

Some soils are poorly drained because of a very slowly permeable clay layer
somewhere in the subsoil.  Installation of tile lines above this layer may
easily remove the excess water if the hydraulic conductivity of the upper pro-
file is adequate.

Land treatment of wastewater is different from other more conventional methods.
The performance of a land treatment system may be much better for its first
few years of operation than thereafter because of the many sorptive and ex-
change reactions occurring in the soil which act as a buffer against rapid

-------
change.  Thus a system may appear satisfactory during the first few years of
operation but then suddenly begin to leak nutrients to the drainage water.
Early detection of the changes that occur in the soil after application of
effluent, therefore, becomes of major importance in estimating the life of
the system and in showing operational changes that must be made to prolong
the life or to produce a higher quality of effluent.

At the present time the Muskegon project is the largest land treatment sys-
tem in the United States.  It also has some unique features that make it
different from most other land treatment systems.  The site has very sandy,
level soils, approximately two-thirds of which are, or were in their natural
state, poorly drained due to the presence of a clay layer in the subsoils.
This clay layer varies in depth but, before drainage, effectively kept a high
water table under a large acreage on the treatment site.  These soils have
a very high hydraulic conductivity so that they remove water easily where a
satisfactory tile drainage system has been installed.  This site was marginal
from an agricultural viewpoint without the installation of a drainage system
and the application of water and nutrients during the growing season.  The
installation of drainage and irrigation systems necessary for treatment of
wastewater is converting this marginal land into productive agricultural  land.
Because of the necessity of increasing xvorld food production, simultaneous
renovation of wastewater and its use to produce food is an important feature
of the Muskegon system.

The wastewater being applied to the land at Muskegon is lower than average
in nutrient content due  to dilution by industrial wastewater from the S.  D.
Warren Paper Company.  Consequently, the M and P contents of the wastewater
after aeration and lagoon storage are about half that of an average effluent.
This has two important consequences:  1) the requirement for P removal will
not be as high, and the  low P adsorption capacity of the sandy soils at Mus-
kegon  is of less  importance than it might be for other wastewaters, and 2)
the N content of  the wastewater is sufficiently low that an agronomic crop
may be expected to be N  deficient during much of the growing season; thus,
management of this system must consider the application of N during the crit-
ical periods of growth.

To construct and  make the Muskegon land treatment system fully operational,
land was cleared  where the native vegetation was shrubs and trees, drainage
systems  installed (usually tile) where necessary, and the land surface was
tilled until it became suitable for growth of crops capable of removing nut-
rients from the wastewater.

During these clearing and construction phases, many changes may occur  in  the
soil properties,  both chemical and physical.  Drainage  and cultivation are
expected to produce better aeration of the soil and result in  decomposition
of soil  organic matter.  As a result, total soil C may  decrease.  With the
decomposition of  organic matter also comes the release  of N through ammonifi-
cation and  then oxidation of NH^ to NC^.  The results may be an increase  in
NCL  in the  drainage waters.

The  relative distribution of bases  (Ca, Mg, and Na) in  soil at various depths
to the groundwater  table is not expected  to change  greatly with the  initial

                                     10

-------
preparation of the site, but they will change rapidly with the addition of
wastewater.  Soil pH, a related chemical property, is expected to increase
with application of wastewater due to the replacement of H  with basic
cations.

Heavy metals may be associated with the organic matter in the soil.  Conse-
quently, oxidation of the organic matter may cause a redistribution of the
heavy metals.  Also, pH and oxidation changes within the soil profile would
be expected to exert major changes on the solubility of heavy metals and the
distribution between organic and precipitated phases.

A major goal of this study was to determine soil chemical and physical proper-
ties prior to and during preparation of the site; and, once having established
this baseline data, being able to clearly delineate changes brought about by
the application of wastewater to the land as separate from changes brought
about during preparation of the site.

The objectives of the study were to:

1.  Determine the quantity of N and C adsorbed or stabilized by other means
in the various soils.

2.  Determine the quantity of P, K, Ca, Mg, Zn, Cu, Mn, Fe, Pb, Hg, Cr, and
Na adsorbed by soils.

3.  Determine the changes in physical properties of the major soil series
receiving effluent.

4.  Monitor electron-capturing organic species in soils, in incoming waste-
waters, and in drainage at outfalls.

5.  Prepare soil samples for preservation as background and base level
samples for future measurements of other ions of interest.

To accomplish these objectives, a major portion of this study was devoted to
establishing the background for the site and the variability in the soils
that could be expected.

Detailed data have been reported in many quarterly reports over the past three
years.  In the case of mineral analyses and physical measurements, only sum-
mary data will be included in this final report.  Table 1 has been prepared
to show the location of previously reported data.  All data collected to date
for pesticides and other trace organics are reported here and should super-
sede previously reported data.

A knowledge of the water applied to each of the individual circles or sites
is important in interpretation of the data; consequently, a table has been
included from data furnished by the County of Muskegon indicating the quantity
of water that was applied by sampling periods (Table 2).  Total ion concen-
trations, together with sampling dates, are included in Table 3.  Specific
site locations are given in Figure 1.


                                      11

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Table 1.  LIST OF CHEMICAL ANALYSES DATA REPORTED DURING PROJECT PERIOD.
Parameter
Extractable
NH4, P, K, Ca
Mg, and Na
Soluble N03
PH







Total
N, C, P, K, Ca,
Mg, and Na




Extractable
Fe, Mn, Zn,
Cu, Pb, and Hg
Total
Fe, Mn, Zn,
Cu, Pb, and Hg

Table
No.

1

1

1
1
1
1

1
1

2


2
2
2

3

3

3
3
Sampling
Period

1

1

2
3
4
5

6
7

1


2
3
4, 5, 6, 7

1

2

3
4, 5, 6, 7
Sites
Reported

1-8, 10-12, 14-26
28-32
9, 13, 27, 33-37

1-37
1-37
1-37
1-6, 10-12, 14-15,
18-19, 21-23
1-37
1-37

1-5, 8, 10-21, 23-31

6, 7, 9, 22, 32-37
1-37
1-37
1-37

1-37

1-37

1-37
1-37
Report
Date

April 1973

April 1975

April 1974
June 1974
April 1975
Sept. 1975

April 1976
April 1976

Oct. 1973

April 1975
April 1975
April 1975
April 1976

April 1975

April 1975

April 1975
April 1976
                                     12

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        Table 2.  WASTEWATER APPLICATION TO SAMPLING SITES*.
c
Site
No

01
02
10
11
12
14
18
19
09
13
15
16
17
20
21
23
28
03
04
05
22
25
33
34
07
08
24
26
27
35
36
37
lircl
No

5
8
2
1
22
11
3
7
42
31
12
41
42
40
19
27
44
21
24
23
20
40
33
30
46
47
44
44
40
43
46
42
.e 1
Soil Type ]

Rubicon Sand
Rubicon Sand
Rubicon Sand
Rubicon Sand
Rubicon Sand
Rubicon Sand
Rubicon Sand
Rubicon Sand
Roscommon Sand
Roscommon Sand
Roscommon Sand
Roscommon Sand
Roscommon Sand
Roscommon Sand
Roscommon Sand
Roscommon Sand
Roscommon Sand
AuGres Sand
AuGres Sand
AuGres Sand
AuGres Sand
AuGres Sand
AuGres Sand
AuGres Sand
Granby Sand
Granby Sand
Granby Sand
Granby Sand
Granby Sand
Granby Sand
Granby Sand
Granby Sand
toy 74
to
Dec 74 .

216
214
212
149
196
200
196
232
55
53
193
75
55
48
139
172
36
144
181
171
173
58
64
32
71
41
36
36
48
51
71
55
Jan 75
to
Jun I,1 75

57
57
67
68
28
12
0
57
0
7
23
14
0
7
0
19
15
29
24
33
24
7
0
0
13
9
15
15
7
10
13
0
Jun 2
to
Sep 1,'7!

104
94
74
60
87
102
102
112
115
86
80
46
115
31
71
92
19
75
84
69
75
31
77
84
21
122
19
19
31
26
21
115
Sep 1
to
i Dec 33, '75

74
58
67
53
68
44
74
61
3
18
53
7
3
11
58
43
0
58
55
54
59
11
28
0.5
0.5
4
0
0
11
0
0.5
3.2
> Totals

451
423
420
330
379
358
372
462
173
164
349
142
173
97
268
326
70
306
344
327
331
97
169
116
105
176
70
70
97
87
105
173
* Data from Dr.  Demirjian, County of Muskegon
                            13

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Table 3.  ESTIMATION OF THE QUANTITY OF NUTRIENTS APPLIED TO
          SOILS THROUGH IRRIGATION WITH WASTEWATER.
Element
June
1974

N 9.1
P 2.3
K 13.9
Na 232
Ca 93
Mg 25.8
Zn 0.18
Mn 0.27
Fe 1.60
Sampling
Sept.
1974
V cr /Via
Kg/na
79.0
20,5
121
2,030
820
226
1.51
2.23
14.2
Date
June
1975
2
27.6
7.0
42.7
710
290
79.0
0.53
0.80
4.98

Sept.
1975

37.4
9.8
57.0
950
380
105
0.71
1.07
6.59

Total
Applied
V o /Via
Kg/ na
153
39.6
235
3,920
1,580
436
2.93
4.37
27.4
  Three background samples were collected in 1972 and 1973 prior to
  application of wastewater.  Sampling dates indicated are for sam-
  ples collected after application of wastewater.

  Quantity of each element applied in wastewater for the sampling
  period  terminating on the date indicated.  Data on water
  applied is based on circles 1, 2, 5 and 8 which received max-
  imum water application.  Data for nutrient content and water
  application rates from Dr. Demirjian, County of Muskegon.
                            14

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                                                          Number
                                                    Circle Number,
                   STORAGE LAGOONS
                   AppleAve. (M-46)
            I 1 m',\C
Figure 1.  Location of  sampling  sites for soils (• ) and outfalls  ( (g) )
                                15

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                            SECTION IV

             CHEMICAL ANALYSIS OF SOIL PROFILE SAMPLES

This section gives data and interpretation of the chemical analyses
which were performed on each of the major soil types to establish
background levels of N, P, K, Ca, Mg, Na and C, and soil pH.   Changes
in these properties or quantities after application of wastewater
during the first two years of operation are reported and discussed.
The discussions are arranged in the following order:  introduction;
nitrogen; calcium; magnesium, sodium and sodium adsorption ratio (SAR);
phosphorus; soil pH; total carbon; potassium; and total soil analysis.

INTRODUCTION

Two types of chemical measurements may be made in soils to reflect
changes in different ions or elements that occur because of some treat-
ment—total elemental analysis and "extractable or available" fractions
of the total.  Total analysis may be very useful over a long period
of time (i.e. 10 to 50 years) but over short time periods the changes
may be too small compared with total amounts already present in soil
to really determine accurately.  For example, total soil K will range
from 5,000 to 25,000 ppm K, but the fraction that is changing rapidly
may be only 25 to 100 ppm K.  On the other hand, a total measurement
of heavy metal content may be adequate to detect even short-term changes.

For this study, methods have been adapted from prior soil science studies
to measure extractable and/or nutrients that are available to plants
and hence more active and more likely to move with soil water.  In
most cases, these methods are expected to reflect early changes in
the status of nutrients within the soil profile.  These changes, in
turn, will indicate how the system is functioning, both for agronomic
production and, more importantly, in nutrient removal.  Individual
procedures are attached as appendix I to this report.

The land treatment site contains four major soil types—Rubicon sand,
Roscommon sand, AuGres sand, and Granby sand  (Figure 2).  These four
soil types account for more than 90 percent of the area.  The Rubicon
sand is a very sandy well-drained soil with a thin organic layer on
the surface.  The clearing operation  (i.e., most of this was in forest
prior to development of the land treatment site) disrupted this or-
ganic layer and produced a somewhat heterogeneous surface.  Both the
Roscommon and AuGres sands had high water tables prior to draining.
They are very sandy but have well aerated conditions in the surface
soils.  The Granby soils have much higher organic matter contents and
have developed under high water tables.  A moderate portion of these
soils have been farmed in the past.

To establish baseline data for the land treatment site, eight sites
were selected from within each of the major soil types by use of a
soil survey map of che area and by on-site inspection.  After analysis

                                 16

-------
                                                       Circle  Number
                      STORAGE LAGOON'S
                      Apole Ave. ( M 46)
                              ^  Rubicon Sand
                              /"""N  AuGres  Sand
                                  Roscommon Sand
                                  Granby  Loamy Sand
                                  Other Soil Types
Figure 2.  Major soil types at Muskegon Wastewater Treatment site.
                                  17

-------
of data from the sites, one site mapped as AuGres appeared more like
Roscommon; consequently, the final selections had eight Rubicon sands,
nine Roscommon sands, seven AuGres sands, and eight Granby sands.
The distribution of these by site and circle number are shown in Table  4.

Each sampling site consisted of a permanently marked area no greater
than 15 meters in diameter.  A single profile sample was collected
twice yearly from each sampling site with a bucket auger until the
water table was reached.  After the water table was encountered, a
2.5 cm plastic tube was inserted to a 305 cm depth by application of
slight vacuum.  The tube with sample was withdrawn while under vacuum,
carefully placed in a sampling trough, and then separated into the
15 cm (6 inch) increments.

Samples were run in a field moist state for NO^.  The moisture content
was determined concurrently so that the values could be corrected back
to oven dry moisture.  All other determinations were run on air-dried
samples.

NITROGEN

Three fractions of nitrogen were measured in the soil profile samples—
soluble NO^, NH^+, and total Kjeldahl N  (which included NH^+ but not
NOT).  Background data was obtained by computing the mean and standard
deviation for each of the four major soil types over three sampling
periods.  The individual sites were combined for each soil type as
shown in Table 4 for summer 1972, spring 1973, and fall 1973 sampling
periods, all prior to application of any wastewater.  It should be
noted, however, that clearing operations and the installation of drain-
age systems during this period of sample collection did have some effect
on the N fractions.

Effect of Soil Type on the Initial Nitrogen Content of Soil Profiles

Considering first the soluble and exchangeable forms of N  (NOo and
NH^+) (Tables 5 to 8), the Rubicon sand  and the AuGres sand were similar
in N content.  The Roscommon sand had nearly double the content of
both forms of N, and Granby sand contained about 6 times more NH/
and 10 times more NOo than either Rubicon or AuGres sand.  This is
somewhat reflected in the values for total N  (Tables 9 to  12) in that
Rubicon was much lower than AuGres and Roscommon, all of which were
many times lower than Granby.  The N contents reflect the  soil develop-
ment.  Rubicon sand  is a well-drained sand developed under forest with
a deep water table—generally deeper than 7 meters.  This  led to de-
velopment of a soil  profile that was low in total N because the aer-
ation caused decomposition of much of the organic matter.  The organic
matter present was in a relatively thin  layer on the surface of the
soil.  Both AuGres and Roscommon were developed under a fluctuating
water table.  While  the AuGres soil was  well aerated during the summer
months, the water table may have come to within 60 cm of the surface
during early spring.  Roscommon sand is  similar, but the water  table
                                18

-------
Table 4.  SITES COMBINED IN SUMMARIZING EACH SOIL TYPE
      Rubicon   Roscommon     Augres      Granby
       Sand        Sand        Sand        Sand
       	  sites  	

        01          09          03          07

        02          13          04          08

        10          15          05          24

        11          16          22          26

        12          17          25          27

        14          20          33          35

        18          21          34          36

        19          23                      37

                    28
                    19

-------
       Table  5.  MEAN  AND  STANDARD DEVIATIONS FOR EXTRACTABLE AND SOLUBLE NUTRIENT CONTENT OF  SOILS
                          FROM MUSKEGON SPRAY AREA-BASELINE DATA RUBICON SAND.
NJ
O
                            NO 3
K
Ca
    *   Mean  of  8  sites  (see Table 2) and 3 sampling dates  (7/72,  6/73  and  9/73).

   **   Standard deviation.
PH
Depth

cm
0-15
15-30
30-46
46-61
61-76
76-91
91-107
107-122
122-137
137-152
152-168
168-183
183-198
198-213
213-229
229-244
244-259
259-274
274-290
290-305
X*


5.4
3.8
2.9
2.5
2.3
2.1
2.2
2.0
1.8
2.0
1.9
2.0
2.0
2.5
2.0
1.6
1.5
2.0
2.1
1.9
SD**


5.9
3.6
2.1
2.3
2.0
2.2
1.9
2.2
1.8
2.2
2.0
2.1
2.0
2.7
2.1
1.7
1.6
2.3
2.6
2.7
X


2.8
1.6
1.4
1.3
1.2
1.2
1.1
1.0
1.1
1.0
0.9
0.9
1.0
0.9
0.9
0.9
0.9
0.8
0.8
0.8
SD


4.4
1.9
1.3
1.3
1.4
1.2
0.9
0.8
0.8
0.7
0.5
0.5
0.5
0.3
0.4
0.6
0.4
0.3
0.3
0.3
X


26
24
25
31
32
27
21
20
18
16
16
15
13
12
13
12
12
12
10
11
SD


13
15
13
14
15
14
10
9
9
8
9
6
5
5
5
5
5
6
5
5
X


21
13
11
9
6
5
4
4
4
4
4
4
13
6
4
5
5
5
13
5
SD


14
9
5
6
4
3
2
1
1
2
1
2
43
8
1
2
2
2
40
2
X

-ppra —
82
47
35
25
17
15
14
15
16
14
17
19
26
24
31
25
26
35
52
73
SD


59
40
31
21
16
15
13
12
15
12
15
17
35
31
38
20
21
37
79
203
X


8
5
4
3
1
1
1
2
3
2
2
3
3
3
3
4
5
6
6
6
SD


5
3
3
2
1
1
0.9
3
7
3
3
3
4
4
4
5
6
8
7
7
X


10.9
8.7
8.2
8.5
8.5
9.5
7.3
6.9
7.0
7.7
7.5
8.6
9.4
8.6
8.0
8.6
9.0
8.3
9.4
8.8
SD


12.9
8.7
10.2
12.4
13.0
14.1
9.1
9.6
9.0
9.6
10.7
12.8
12.8
12.8
10.1
11.9
13.2
12.6
13.0
12.8
X


5.0
5.1
5.3
5.3
5.3
5.3
5.4
5.5
5.6
5.6
5.6
5.7
5.7
5.8
5.9
5.9
5.9
6.0
6.0
6.1
SD


0.4
0.4
0.4
0.4
0.4
0.4
0.4
0.4
0.6
0.5
0.5
0.5
0.7
0.7
0.6
0.7
0.6
0.7
0.8
0.8

-------
      Table 6.   MEAN AND STANDARD DEVIATIONS FOR EXTRACTABLE AND SOLUBLE NUTRIENT CONTENT OF SOILS
                         FROM MUSKEGON SPRAY AREA-BASELINE DATA ROSCOMMON SAND.

Depth

cm
0-15
15-30
30-46
46-61
61-76
76-91
91-107
107-122
122-137
137-152
152-168
168-183
183-198
198-213
213-229
229-244
244-259
259-274
274-290
290-305
Nl
X*


10.0
8.7
3.8
2.8
2.4
2.b
2.3
2.8
2.1
2.3
2.4
2.6
2.1
2.1
2.5
2.1
2.6
2.5
2.4
2.7
Ii»
SD**


23.3
17.9
4.4
2.3
2.1
2.4
2.0
3.2
2.2
2.2
1.9
2.4
2.0
1.9
2.4
2.0
2.2
2.3
2.5
2.9
t
X


6.0
6.9
3.1
2.3
1.5
1.3
1.4
1.4
1.0
1.2
1.0
1.0
1.0
0.9
1.0
0.9
0.9
0.9
0.9
0.9
10 3
SD


12.4
12.3
4.3
3.0
1.0
1.4
1.7
1.7
0.5
0.6
0.4
0.6
0.4
0.4
0.4
0.4
0.3
0.3
0.3
0.3
I
X


9.6
7.9
5.6
7.2
9.1
8.4
8.6
9.0
9.2
9.6
9.2
8.9
8.2
8.9
8.3
8.0
7.5
7.3
7.7
8.0
>
SD


5.8
5.6
3.9
7.0
7.7
6.8
7.3
8.2
7.9
9.0
7.8
7.1
6.0
7.4
6.7
5.7
5.4
5.9
6.3
6.2
F
X


33
17
9
7
7
7
7
7
7
7
7
7
6
7
6
7
6
6
6
6
r
SD


23
10
7
4
3
4
4
4
4
4
6
7
5
5
3
5
4
3
4
3
C
X


420
240
130
200
110
96
130
110
140
220
210
120
96
100
94
95
93
93
120
130
;a
SD


430
240
140
580
210
83
230
110
230
460
420
230
130
140
140
140
120
120
180
180
W
X


78
44
11
10
13
17
23
26
27
26
22
20
21
23
24
23
25
22
23
24
lg
SD


150
110
13
15
29
34
48
49
50
52
48
44
49
52
50
44
45
40
39
41
K
X


11.0
9.2
8.0
7.5
7.5
9.4
9.6
8.6
9.9
10.5
11.1
9.0
8.6
9.3
9.4
9.6
9.5
10.1
11.0
10.3
[a
SD


8.9
8.4
9.1
8.7
9.2
13.1
12.5
12.0
13.4
17.8
17.2
12.2
10.9
12.1
11.4
13.4
12.8
12.3
11.8
11.9
P
X


5.6
5.6
5.8
6.0
6.0
6.2
6.2
6.3
6.2
6.2
6.2
5.9
5.7
5.7
5.7
5.7
5.7
5.8
6.0
6.1
>H
SD


0.7
0.9
0.9
0.9
0.9
0.9
1.0
1.0
1.0
1.1
1.2
1.0
1.1
1.1
1.1
1.2
1.2
1.1
1.2
1.2
 *  Mean of 9 sites (see Table 2) and 3 sampling dates (7/72,  6/73 and 9/73).

**  Standard deviation.

-------
             Table  7.   MEAN AND  STANDARD DEVIATIONS FOR EXTRACTABLE AND SOLUBLE NUTRIENT CONTENT OF  SOILS
                                  FROM MUSKEGON SPRAY AREA-BASELINE DATA AUGRES SAND.
10
Depth
t*>Tn
CIu
0-15
15-30
30-46
46-61
61-76
76-91
91-107
107-122
122-137
137-152
152-168
168-183
183-198
198-213
213-229
229-244
244-259
259-274
274-290
290-305
NI
X*


4.8
2.5
2.1
2.0
2.4
1.7
1.5
1.6
2.0
1.7
1.9
2.0
1.7
1.8
2.0
1.7
1.9
2.0
1.9
1.9
i«f
SD**


8.7
3.0
2.1
2.0
4.1
2.0
1.5
1.8
2.5
2.2
1.8
2.3
2.3
2.4
2.9
2.6
2.7
3.1
2.8
3.4
1
X


3.6
2.2
1.9
1.7
1.4
1.5
1.2
1.1
1.0
1.0
1.0
1.0
1.1
1.2
1.0
1.0
1.0
1.0
1.1
1.1
SO 3
SD


5.8
2.4
2.9
2.6
1.4
2.0
1.0
0.9
0.7
0.7
0.7
0.8
0.9
1.0
0.7
0.7
0.8
0.9
1.2
1.2
I
X


11.5
7.1
5.5
7.1
9.1
11.0
10.7
11.2
10.8
11.0
12.9
10.6
10.1
10.4
10.1
10.0
10.0
9.5
9.1
8.6
3
SD


12.2
10.7
5.6
6.8
6.4
9.0
8.4
7.5
7.0
6.5
6.1
5.4
5.8
6.5
6.6
8.3
8.8
7.7
7.0
7.0
I
X


32
21
9
6
5
6
5
5
5
8
5
5
5
5
5
5
6
8
6
7
C
SD

— ppt
20
30
6
5
2
4
2
2
2
11
2
3
2
2
3
2
4
11
2
5
C
X


310
210
100
67
51
61
47
54
50
43
32
45
43
40
86
130
120
140
100
170
:a
SD


260
200
82
56
55
66
44
50
64
57
25
52
55
47
161
280
280
290
190
290
1
X


49
37
20
8
6
8
6
9
7
8
7
8
10
10
8
8
8
11
16
16

-------
            Table 8.   MEAN AND STANDARD  DEVIATIONS FOR EXTRACTABLE  AND SOLUBLE  NUTRIENT CONTENT OF SOILS
                                FROM MUSKEGON SPRAY AREA-BASELINE DATA GRANBY SAND.
NJ
Depth
n m
cm
0-15
15-30
30-46
46-61
61-76
76-91
91-107
107-122
122-137
137-152
152-168
168-183
183-198
198-213
213-229
229-244
244-259
259-274
274-290
290-305
NI
X*


39.2
10.6
3.9
2.5
2.5
1.6
1.9
1.3
1.6
1.6
1.2
1.1
1.0
1.0
1.1
1.0
1.5
1.3
1.3
1.4
I«*
SD**


80.7
19.8
6.3
2.5
4.8
1.6
2.0
1.3
2.3
2.0
1.2
1.4
1.1
1.1
1.3
1.1
2.5
2.0
2.1
2.6
NC
X


34.3
18.6
8.1
3.1
2.4
1.7
1.5
1.2
1.3
1.3
1.3
1.2
1.3
1.3
1.2
1.2
1.1
1.2
1.1
1.1
'3
SD


80.2
41.4
17.1
3.3
2.2
1.1
0.9
0.6
0.6
0.7
0.8
0.6
0.9
0.9
0.7
0.5
0.4
0.5
0.5
0.6
E
X


17.8
7.8
4.9
5.1
5.1
5.9
6.5
8.0
7.0
6.8
6.9
7.2
7.4
6.8
6.3
6.6
6.7
6.0
6.4
6.3
i
SD


16.9
6.9
4.2
5.2
4.2
4.3
4.4
5.4
4.4
4.3
3.6
3.8
3.8
3.7
3.9
4.2
4.9
4.5
4.5
4.5
X


84
37
17
13
10
10
9
7
8
7
7
6
6
5
5
6
5
6
6
6
K
SD

	 PF
69
31
12
11
4
7
4
3
4
3
3
3
3
2
2
4
3
3
4
2
Ca
X


1970
1920
1230
770
565
440
390
340
330
360
335
320
310
300
340
295
320
335
310
340
i
SD


1830
2650
1680
1100
880
680
680
660
700
700
640
655
616
600
590
560
580
540
530
590
V.
X


210
190
140
110
110
110
110
100
100
110
100
93
86
91
94
92
90
100
91
100
lg
SD


450
430
330
340
340
410
400
390
390
390
360
340
310
350
320
320
320
340
310
320
Na
X


21.3
21.4
15.7
12.5
10.9
9.2
7.6
7.1
7.1
7.1
7.8
7.2
7.7
6.8
7.6
6.4
7.4
7.2
7.4
6.9
L
SD


12.4
17.7
14.4
10.9
8.8
8.3
5.8
6.0
5.0
5.1
9.3
5.7
7.0
5.0
8.4
4.0
7.1
5.0
5.5
4.8
1
X


6.4
6.3
6.4
6.6
6.6
6.4
5.8
5.1
5.2
4.9
4.9
4.7
4.7
4.7
6.0
5.2
5.4
5.6
5.5
5.6
PH
SD


0.8
0.7
0.9
0.8
0.8
1.2
1.6
1.7
1.8
1.8-
1.3
1.8
1.9
1.9
2.1
2.0
1.8
1.8
1.8
1.8
     *  Mean of 8 sites (see Table 2)  and 3 sampling dates (7/72,  6/73 and 9/73)

    **  Standard deviation.

-------
                  Table 9.  MEAN AND STANDARD DEVIATION FOR TOTAL NUTRIENTS OF  SOILS  FROM
                              MUSKEGON SPRAY AREA-BASELINE DATA RUBICON  SAND.
                                                      K
Me
Na
NJ
-P-
Depth

0-15
15-30
30-46
46-61
61-76
76-91
91-107
107-122
122-137
137-152
152-168
168-183
183-198
198-213
213-229
229-244
244-259
259-274
274-290
290-305
X*

490
280
180
130
92
71
56
51
42
35
44
34
33
32
30
34
32
31
29
31
SD**

160
67
57
41
31
43
24
25
20
18
18
13
19
19
16
27
21
14
12
18
X

.93
.49
.39
.21
.15
.21
.15
.14
.16
.15
.14
.14
.12
.09
.16
.11
.11
.12
.11
.11
SD

.31
.26
.21
.13
.14
.19
.20
.14
.18
.16
.17
.15
.11
.10
.21
.13
.09
,11
.13
.12
X

280
240
220
200
160
140
130
130
110
110
160
110
91
97
98
110
100
100
99
93
SD

140
110
130
90
62
52
47
60
40
43
180
73
37
42
44
66
49
48
39
46
X

9700
9400
10200
10000
9200
9500
9700
9100
9300
13100
9800
8800
8500
18800
8600
8700
8700
9100
9000
8900
SD

3400
3300
3200
2900
2600
3000
2800
2500
2500
18100
1700
3100
2900
50600
2300
2100
2300
2700
2900
2500
X

1800
1800
1800
1700
2000
2100
1800
2100
2000
1900
2100
2200
1900
1900
2200
2200
2400
2600
3100
3300
SD

1000
1000
900
800
1100
1500
800
1400
1600
1300
1100
1400
1000
1100
1400
1300
1200
1700
1800
3300
X

870
870
990
850
900
860
1110
1030
860
810
960
910
810
750
870
970
860
1000
1000
1270
SD

420
410
630
330
340
520
1640
640
640
390
390
400
380
310
410
720
380
700
520
1530
X

3560
3730
3840
4220
4120
4130
4290
4830
4200
4780
5530
4710
4620
4850
4540
5270
5530
4710
4960
4460
SD

1690
1810
1920
1890
2020
1820
2550
2950
2020
2580
4780
2070
3060
3680
2200
3530
3130
2100
3420
1680
   *  Mean of 8 sites  (see Table 2) and 3 sampling dates  (7/72,  6/73  and  9/73).

  **  Standard deviation.

-------
             Table 10.  MEAN AND STANDARD DEVIATION FOR TOTAL NUTRIENTS OF SOILS FROM MUSKEGON
                                 SPRAY AREA-BASELINE DATA ROSCOMMON SAND.
N3
Ui

Depth
r*m
(~IH
0-15
15-30
30-46
46-61
61-76
76-91
91-107
107-122
122-137
137-152
152-168
168-183
183-198
198-213
213-229
229-244
244-259
259-274
274-290
290-305
t
X*


990
610
220
100
89
61
48
50
39
36
34
31
28
26
30
32
27
26
26
26
I
SD**


440
370
170
52
86
25
24
29
13
12
14
9
9
11
21
24
14
11
12
11
C
X


1.48
.97
.61
.37
.31
.29
.28
.30
.26
.24
.24
.20
.21
.20
.20
.18
.18
.19
.20
.22

SD


.46
.66
.69
.28
.19
.18
.17
.21
.21
.18
.20
.17
.16
.17
.16
.19
.14
.17
.18
.18
E
X


190
160
150
95
92
100
110
110
100
100
110
100
110
97
100
94
100
100
91
90
>
SD


120
110
150
35
26
43
57
70
53
50
79
48
46
42
51
40
57
59
41
41
K
X


8800
10100
10200
10700
10600
10800
10900
11000
12000
10300
9700
11100
10100
9800
11100
9900
9700
13100
9900
9700

SD

- ppm
2400
2400
2500
2900
2700
3100
3100
2800
4500
3000
3700
2600
2500
2000
2700
2700
3000
17300
3000
2400
Ca
X


2700
2500
2400
2700
2600
3300
3100
3600
3300
4100
3300
3000
2700
3100
3600
3400
3500
3900
3900
4200

SD


1700
2000
1300
1700
2400
3300
2800
3200
2300
3300
2300
1800
1700
2000
2700
2500
2400
3200
3800
4300
Mg
X


780
600
660
880
830
950
970
1130
1350
1490
1160
950
980
970
1110
1140
1280
1540
1400
1500
r
SD


590
386
326
830
750
1000
1080
1080
1780
1780
1100
820
920
790
990
1130
1140
1980
1400
1990
Na
X


3420
3690
4160
4050
4410
4890
3650
4560
4480
3880
4010
4320
3730
3880
4140
3940
3700
3860
3680
3680

SD


1720
1600
1790
1410
1620
3140
2550
2440
1830
1250
2550
1540
1270
1270
1330
1700
1470
1650
1130
1110
   *  Mean of  9  sites  (see Table 2) and 3 sampling  dates  (7/72,  6/73  and  9/73).


  **  Standard deviation.

-------
            Table 11.   MEAN AND STANDARD DEVIATION OF TOTAL NUTRIENTS OF SOILS FROM
                            MUSKEGON SPRAY AREA-BASELINE DATA AUGRES SAND.

Depth

cm
0-15
15-30
30-46
46-61
61-76
76-91
91-107
107-122
122-137
137-152
152-168
168-183
183-198
198-213
213-229
229-244
244-259
259-274
274-290
290-305
1
X*


850
540
280
150
120
75
66
57
52
43
42
34
33
29
30
28
27
27
28
27

-------
                   Table 12.  MEAN AND STANDARD DEVIATION OF TOTAL NUTRIENTS OF SOILS FROM
                              MUSKEGON SPRAY AREA-BASELINE DATA GRANBY SAND.
ISJ
-vj

Depth

Cm
0-15
15-30
30-46
46-61
61-76
76-91
91-107
107-122
122-137
137-152
152-168
168-183
183-198
198-213
213-229
229-244
244-259
259-274
274-290
290-305

X*


2800
2120
1260
670
330
140
100
90
64
49
51
47
36
32
33
37
36
39
32
30
N
SD**


1900
1930
1610
900
440
130
88
84
37
23
23
23
17
13
17
23
18
25
13
16
C
X


3.21
3.24
2.14
1.51
1.05
.37
.32
.32
.28
.28
.27
.26
.24
.22
.25
.25
.28
.28
.26
.26

SD


2.42
4.59
3.95
3.06
2.69
.31
.31
.30
.29
.25
.27
.24
.24
.25
.26
.26
.35
.36
.33
.32
I
X


310
320
160
130
120
110
130
130
120
110
120
100
100
100
110
100
150
130
98
110
>
SD


260
470
140
63
60
58
98
68
54
54
80
52
46
58
53
52
270
150
57
81
I
X


10100
11100
11500
11500
12100
11800
12600
12300
12100
11400
11500
11600
11900
11300
11700
11100
11700
11600
11100
11300
r
SD


3000
2900
3000
2800
2000
2200
3100
3700
3400
3400
3500
3200
2900
3400
3800
3900
3300
3200
3000
3500
C,
X


9200
13400
15900
11300
7700
3800
4300
4500
4500
5000
4900
4800
4500
5000
4500
4500
4400
4700
4400
5500
a
SD


11400
24700
32800
25700
15400
3000
3900
4000
4300
5000
4600
4300
4000
4500
3900
3800
3400
3900
4100
5300
Mg
X


1300
1300
1300
1600
1500
1100
1200
1400
1400
1400
1500
1500
1300
1200
1300
1400
1400
1500
1400
1600
r
SD


1000
900
1100
2000
1700
700
1200
1300
1300
1200
1500
1600
1100
1100
1100
1100
1100
1300
1400
1400
Na
X


4270
4510
5320
5540
4480
4720
4970
4940
4490
4120
4120
4310
4380
4250
4480
4050
4190
3940
4250
4240
i
SD


1600
1180
2740
4030
1510
1260
2300
1210
1040
790
890
1250
1060
1190
1420
1210
1130
1090
1310
1490
   *  Mean of 8 sites  (see Table 2) and 3 sampling dates  (7/72,  6/73 and 9/73).

  **  Standard deviation.

-------
will be somewhat closer to the surface during the winter and spring
months.  The Granby soil has had a high water table—at the surface
during many months of the year—unless artificial drainage has been
installed.  This has led to accumulation of organic matter in the
Granby soil with the result of high total N and, in many cases, also
high soluble forms of N.

Effect of Drainage and Farming on Nitrogen Distribution in Soil Profiles

Installation of tile drainage systems and farming these sandy soils
resulted in at least two independent effects.  First, draining these
areas removed free water and allowed the soil profiles to be leached
of soluble nutrients.  Most notable was NOT which moves with the water.
Individual site 15 (circle 12) is an example of this effect.  At the
first sampling the nitrate content of the 0-15 cm (0-6 inch) layer
was 9.4 ppm N as NC^, and the 15-30 cm (6-12 inch) layer was 19.5 ppm
N.  All other layers in this profile were less than 1 ppm N except
for the 107-122 cm (42-48 inch) and the 229-244 cm (90-96 inch) layer
(2.26 and 2.51 ppm N as NO,,, respectively).  By the second sampling
taken during the spring of the following year, the levels of NOT were
less than 1 ppm N at all depths in the soil profile, indicating that
the NOT had been removed from the profile by leaching.

The second effect is the increased production of NH,  and NOT by miner-
alization of organic matter due to increased aeration after drainage.
 The best example of this occurred at site 35 (circle 43) on a Granby
sand (Table 13) .  The NH^4" content was high in the 0-15 cm layer at
the time of the first sampling  (120 ppm N) with levels decreasing in
the 15-30 cm (18.5 ppm N) and 15-46 cm (13.1 ppm N) layers.  At greater
depths the quantities of NH/  were quite low.  Nitrate N was low through-
out the profile with a high value of 3.51 ppm N as NO^ in the 0-15
cm layer.  By the second sampling the following spring, the soil content
of both NH,  and N0o+ were very high in the surface layers  (see Table
13).  It appears that with the time between the first and second samp-
ling, ammonification had progressed to a great degree and some nitri-
fication had occurred.  The band of higher NH,+ and NOo at 61-76 cm
suggests that the movement downward of the N had not occurred at a
fast rate.

By the fall of 1973 the NH   values were lower than in the spring but
still quite high.  The samples collected in the spring of 1974 were
very low in NH,+ and not really very high, comparatively speaking,
in NO^.  Three possibilities exist for the removal of the large quan-
tities of NH,  and NOT.  First, plant uptake could account for a por-
tion of the removal but not between fall 1973 and spring 1974.  Second,
leaching of N0~ may have occurred.  This should have lead to higher
values of NO^ in the lower horizons of the soil profile.  This, in
fact, occurred in the spring 1974 sampling where values as high as
5.52 ppm N as NO^ occurred in the soil at 290-305 cm depth.  It should
be pointed out that this 5.52 ppm concentration is on a dry weight
basis in the soil and the solution concentration would be considerably

                                28

-------
Table 13.  AMMONIUM AND NITRATE CONTENTS OF THE SOIL PROFILE AT SITE 35
                           (GRANBY SAND).

Depth

cm
0-15
15-30
30-46
46-61
61-76
76-91
91-107
107-122
122-137
137-152
152-168
168-183
183-198
198-213
213-229
229-244
244-259
259-274
274-290
290-305
Summer
NH.
4


120.0
18.5
13.1
3.4
2.5
1.3
5.4
1.5
1.4
. 1.0
2.2
2.6
1.0
1.1
1.1
1.2
0.9
0.8
0.9
0.9
1972
N03


3.5
2.1
1.5
1.6
1.5
1.4
1.3
1.2
1.8
1.8
2.0
1.3
1.6
1.6
1.8
1.8
1.8
1.8
2.0
1.8
Spring
NH4


324
71
29
7.7
24
3.0
6.2
2.6
4.7
2.4
2.6
1.8
2.5
1.8
1.5
0.9
0.9
1.8
2 1
2.1
1973
N03
VI

96
|22
13
2.6
8.3
1.7
1.9
1.5
1.8
1.4
1.2
1.4
1.7
1.6
1.5
1.3
0.7
1.1
1.1
1.2
Fall
NH.
4


177
31
12
8
2.0
2.3
3.0
2.3
2.7
2.0
1.5
1.8
1.0
.5
.8
.8
.5
.8
1.5
1.5
1973
N03


59
13
3.0
1.6
1.0
0.9
0.8
0.6
0.6
0.6
0.6
0.6
0.6
0.6
0.5
0.5
0.5
0.7
0.5
0.5
Spring
NH.
4


0.6
*
1.2
*
1.8
0.6
1.2
*
0.6
1.8
1.2
*
2.4
1.2
1.8
*
0.3
1.8
0.6
1.2
1974
N03


14
12
4.9
4.1
2.9
3.4
1.8
2.1
1.6
1.8
1.7
2.0
2.1
2.6
1.8
1.3
1.3
1.6
4.6
5.5
                            29

-------
higher (probably greater than 20 ppm N as NOo in the ground water at
this depth).   The third possibility is that considerable denitrification
may have occurred within this profile.  This is suggested by the low
values of NOo throughout the lower layers of the profile.  This is
a reasonable reaction to expect in that the NHL  was being nitrified
in the surface layers, the Granby sand does contain considerable or-
ganic matter which may move to the lower layers and serve as an energy
source, and this soil has a high water table.  But the potential does
exist for movement of high quantities of NOo into the ground water
through this profile even without the addition of wastewater.  If C
diminishes in the saturated zone, the NO, may no longer be denitrified
and could lead to increased concentrations of NOo in the groundwater.

Effect of Application of Wastewater on Nitrogen Distribution in Soil
Profiles

During the initial year of operation of the system  (1974) the N content
of the wastewater being applied to the fields was about 2.5 ppm N as
NH,  and 2.5 ppm N as NO^ for water from the east storage lagoon and
about 1 ppm N as NH,  plus NOo for water from the west lagoon  (Demirjian,
1975).  Soil profiles were collected, inasmuch as possible, after 20
cm (8 inches) of this wastewater had been applied.  Mean values for
these nutrients are included as tables 14 to 17.  With one exception,
the NH,  and NO" contents of the Rubicon soil profiles were reduced
by the application of this water.  Site number 01, however, was very
high in NH, which is affecting the averages presented in table 14.
Table 18 has been included to compare site 01 with the average of the
other 7 sites.  It is felt that site 01 must have been in an area where
rapid ammonification was occurring due to incorporation of organic
matter when preparing the site for farming operation.  The application
of water then moved much of this NH,  into the soil profile.  Although
this would not be expected to happen in a soil with a large cation
exchange capacity, the Rubicon sand has a very low cation exchange
capacity which will allow for movement of cations in the profile.
The evidence of high NH^  was still present in the surface soil in
September of 1974 after the application of many inches of wastewater
but had virtually disappeared by the spring of 1975.  The NH,  and
NOo contents of the Roscommon and AuGres sands were low and more uni-
form with depth, but the Granby sand gave indications of some  increased
NH,  and NO1^ in the lower horizons after application of  20 cm  (8 inches)
of wastewater.

Means have not been calculated for the later samplings since the quan-
tity of water that was applied to individual circles varied  considerably.
Thus, an examination has been made of individual  sites and general
conclusions drawn from this data.

After the application of rather large quantities  of wastewater, the
three soil types  (Rubicon, AuGres, and Roscommon) appeared to  stabilize
and give rather uniformly low values  for NH, and  NOo.  Bands of NO^
were apparent in these soils at both  samplings  (spring and fall 1975),

                                 30

-------
       Table 14.   MEAN AND  STANDARD DEVIATIONS  FOR EXTRACTABLE AND SOLUBLE NUTRIENT CONTENT OF
             SOILS FROM MUSKEGON  SPRAY AREA AFTER EIGHT INCHES OF EFFLUENT RUBICON SAND.

Depth
r*Tn
Llll
0-15
15-30
30-46
46-61
61-76
76-91
91-107
107-122
122-137
137-152
152-168
168-183
183-198
198-213
213-229
229-244
244-259
259-274
274-290
290-305
NI
X*


6.3
4.4
1.2
5.6
.5
4.5
6.2
5.3
.4
.3
3.8
1.5
1.3
.4
1.8
.4
.6
4.8
5.3
1.7
^
SD**


13
10
1.7
14.1
.7
11.7
16.7
14.1
.3
.1
9.8
3.4
2.6
.4
4.1
.5
.5
12.6
14.0
3.3
NO'
X


3.5
1.6
1.2
1.0
.9
.8
.9
.8
.7
.7
.8
.7
.7
.7
.7
.6
.6
.7
1.1
1.4
3
SD


2.2
1.
.6
.4
.4
.4
.4
.4
.4
.4
.5
.4
.4
.4
.3
.2
.2
.2
.5
1.
P
X


28
22
17
25
39
29
22
19
18
17
16
14
14
11
11
11
10
11
12.05
15.7

SD


12
13
5
16
13
14
6
5
3
3
3
3
4
4
4
3
4
4
4
4

X


32
21
13
7
5
4
3
3
3
4
4
4
4
4
4
4
4
4
5
6
K
SD

pprn — •
24
28
9
3
2
1
1
1
1
2
1
1
2
1
3
1
1
1
1
2
C;
X


140
84
40
34
25
30
15
23
15
15
19
14
20
21
28
25
44
61
71
68
a
SD


70
80
21
35
35
44
16
42
13
12
15
12
18
15
26
18
42
52
102
88
MF
X


18
15
7
5
2
3
2
2
1
2
3
2
3
4
3
3
6
6
8
11
r
SD


8
18
8
5
3
4
1
3
1
2
2
2
4
5
4
3
8
7
9
15
Ns
X


19.9
10.6
8.2
7.2
4.8
4.0
3.4
3.7,
3.6
3.2
3.8
3.1
3.2
5.0
3.9
2.5
4.6
4.1
4.8
5.5
i
SD


11.3
6.4
5.1
4.9
3.4
2.4
2.1
1.8
2.3
1.7
2.3
1.8
1.5
6.5
2.6
1.4
3.3
3.6
3.0
3.9
pH
X


5.1
5.0
4.0
5.0
5.9
5.2
5.3
5.3
5.4
5.4
5.5
5.5
5.6
5.6
5.6
5.6
5.8
6.0
6.1
6.2

SD


.4
.4
.5
.5
.5
.5
.6
.6
.5
.5
.6
.5
.6
.6
.6
.5
.8
.9
.9
.7
 *  Mean of 8 sites (see Table 2)

**  Standard deviation.

-------
       Table 15.   MEAN AND STANDARD DEVIATIONS  FOR  EXTRACTABLE AND SOLUBLE NUTRIENT CONTENT OF SOILS
                  FROM MUSKEGON SPRAY AREA AFTER  EIGHT INCHES OF EFFLUENT ROSCOMMON SAND.
CO

Depth

cm
0-15
15-30
30-46
46-61
61-76
76-91
91-107
107-122
122-137
137-152
152-168
168-183
183-198
198-213
213-229
229-244
244-259
259-274
274-290
290-305
NI
X*


2.9
2.9
1.0
.9
1.2
1.3
.8
.7
.6
.5
.6
.6
.6
.7
.4
1.9
.5
.5
.5
.3
^
SD**


4.5
4.3
1.1
1.0
1.9
1.6
.8
.6
.5
.5
.4
.6
.8
.8
.4
3.8
.6
.5
.3
.3
N(
X


2.4
1.5
1.0
1.0
.9
1.3
.8
.8
.8
.8
.8
.6
.8
1.2
1.5
1.2
1.0
1.0
1.2
1.3
5 3
SD


1.5
.8
.3
.5
.5
1.6
.4
.4
.4
.4
.4
.2
.4
.8
1.3
.8
.9
.8
.9
1.0
I
X


15
10
9
10
13
15
10
11
11
11
10
10
10
8
7
8
8
8
7
7
•>
SD


15
8
6
10
13
15
9
5
5
5
5
6
6
5
6
6
6
5
5
5
I
X


25
19
9
8
8
6
5
6
6
6
7
6
6
6
7
7
8
8
8
8
C
SD


16
18
7
6
5
4
4
4
7
5
5
5
5
5
6
7
7
5
5
6
d
X

ppm
298
340
212
112
96
87
86
83
118
94
112
83
88
89
100
109
104
165
203
196
i
SD


197
279
88
129
81
60
121
114
222
142
146
129
119
112
139
150
138
251
330
371
M
X


45
43
28
20
14
12
12
13
19
14
22
18
20
21
24
26
26
22
23
26
R
SD


37
28
35
33
21
12
20
24
46
27
28
30
34
36
39
43
46
39
41
43
Ni
X


29.6
22.2
7.3
7.9
7.9
8.6
7.0
7.2
7.7
6.6
7.6
6.4
6.6
6.5
6.9
6.6
6.1
8.8
11.6
12.2
i
SD


20.0
20.4
3.0
6.6
7,0
8.0
7.1
7.2
11.4
8.8
8.9
7.3
7.9
5.4
8.0
6.6
5.8
9.3
14.2
12.7
P
X


6.3
6.2
6.3
6.3
6.4
6.3
6.2
6.1
5.9
6.2
6.3
6.3
6.2
6.1
6.0
6.1
6.1
6.3
6.6
6.8
H
SD


1.1
1.1
1.1
1.1
1.4
1.1
1.1
1.2
1.3
1.2
1.2
1.5
1.5
1.7
1.7
1.7
1.6
1.4
1.3
1.2
    *  Mean of 9 sites (see Table 2)

   **  Standard deviation.

-------
       Table 16.  MEAN AND STANDARD DEVIATION FOR EXTRACTABLE AND SOLUBLE NUTRIENT CONTENT OF  SOILS
                  FROM MUSKEGON SPRAY AREA AFTER EIGHT INCHES OF EFFLUENT AUGRES SAND.
                NH,
NO.
K
Ca
Mg
Na
PH
Lo
Depth
r*Tn
Cul
0-15
15-30
30-46
46-61
61-76
76-91
91-107
107-122
122-137
137-152
152-168
168-183
183-198
198-213
213-229
229-244
244-259
259-274
274-290
290-305
X*


3.8
2.6
1.3
.8
.6
.6
.3
.3
.5
.4
.5
.7
.2
.5
.4
.7
.3
.3
.3
.3
SD**


5.5
5.1
.7
.6
.5
.3
.4
.3
.5
.5
.3
.8
.2
.4
.4
.8
.3
.2
.3
.1
X


6.2
4.7
2.9
2.3
2.1
2.0
1.6
1.6
1.5
1.4
1.6
1.5
1.7
1.5
1.4
2.0
1.9
2.2
2.2
2.3
SD


4.4
3.7
2.2
1.3
2.0
1.9
1.3
1.4
1.2
1.2
1.4
1.2
1.5
1.1
1.2
1.5
1.4
1.6
1.4
1.5
X


17
9
10
10
12
10
10
12
12
15
13
13
18
14
14
13
13
12
12
11
SD


17
9
7
9
9
5
5
7
9
11
8
10
14
9
10
11
11
8
8
8
X


33
16
10
6
4
4
3
4
3
4
4
4
4
4
4
4
5
4
5
6
SD


15
8
7
4
3
2
1
1
2
2
2
2
2
3
2
2
3
3
3
2
X


410
230
160
140
66
53
41
31
33
44
38
33
25
25
29
30
35
47
240
280
SD


230
170
200
210
69
49
33
1 32
25
36
27
19
19
31
26
26
28
28
490
590
X


40
22
12
9
6
5
4
3
3
3
4
4
3
3
5
5
5
9
15
17
SD


23
20
10
9
6
6
3
3
3
3
3
4
3
3
8
7
8
9
14
17
X


37.1
14.1
6.6
4.6
3.8
3.9
4.0
5.8
3.7
6.4
6.8
6.8
5.1
5.4
5.6
5.0
5.6
5.2
5.5
7.6
SD


13.7
6.0
2.3
2.2
2.0
2.0
2.2
3.8
3.1
8.4
8.5
9.3
7.8
8.9
8.2
6.4
5.9
7.7
7.0
8.5
X


5.9
5.8
5.8
5.8
5.8
5.8
5.8
5.8
5.8
6.0
6.0
5.9
5.7
5.6
5.4
5.4
5.4
5.5
5.6
5.9
SD


0.5
0.8
0.8
0.7
0.7
0.7
0.7
0.7
0.6
0.6
0.7
0.9
0.9
0.9
1.0
1.1
1.1
1.3
1.4
1.1
    *  Mean of  7  sites  (see Table 2)

  **  Standard deviation.

-------
       Table 17.   MEAN AND STANDARD  DEVIATION  FOR EXTRACTABLE AND SOLUBLE NUTRIENT CONTENT OF
             SOILS FROM MUSKEGON  SPRAY AREA AFTER EIGHT INCHES OF EFFLUENT GRANBY SAND.
                           NO 3
K
Ca
Na
PH
Depth

cm
0-15
15-30
30-46
46-61
61-76
76-91
91-107
107-122
122-137
137-152
152-168
168-183
183-198
198-213
213-229
229-244
244-259
259-274
274-290
290-305
X*


3.4
2.0
1.1
1.1
1.1
1.1
1.0
2.4
4.1
1.4
1.1
.9
1.7
.9
1.1
.8
.9
1.4
.9
1.1
SD**


3.9
3.3
1.5
1.1
.9
.7
.8
4.3
9.1
1.2
.6
.7
2.0
.6
.8
.7
.8
1.4
1.0
1.1
X


7.6
10.7
6.7
5.0
3.5
3.2
2.1
2.1
2.0
1.8
1.8
1.6
1.9
1.7
2.1
2.1
1.5
1.6
1.7
1.7
SD


9.5
16.7
8.6
5.4
3.8
2.8
2.4
2.0
2.4
1.8
1.5
1.2
1.8
1.8
2.5
2.2
1.4
1.6
2.0
2.5
X


28
16
7
9
10
13
12
12
10
10
8
8
9
9
9
9
8
8
8
9
SD


28
22
7
8
9
14
13
12
9
9
8
8
8
8
8
8
7
6
6
6
X


57
37
26
13
11
9
8
9
8
8
8
9
9
8
8
7
9
8
9
8
SD

ppm
36
30
25
4
5
5
6
5
4
4
3
4
4
4
3
2
6
4
4
5
X


940
940
920
720
570
550
440
560
670
680
630
650
630
510
570
550
570
600
530
580
SD


810
880
670
730
720
690
580
640
660
640
640
700
680
640
650
590
620
620
550
580
X


130
130
91
85
65
45
26
26
17
23
28
37
37
14
37
38
45
45
45
47
SD


100
110
70
83
76
56
26
23
13
17
31
45
45
12
58
64
76
66
63
68
X


88.0
50.8
32.9
24.9
17.5
10.4
7.6
10.8
9.5
11.5
12.3
17.3
13.9
11.9
12.7
10.8
13.9
10.5
9.8
12.8
SD


45.8
23.2
37.6
32.1
18.6
7.3
6.9
7.1
6.6
6.5
6.8
17.0
8.8
8.0
7.9
7.1
12.9
6.1
7.4
8.8
X


6.5
6.1
1.6
6.6
6.6
6.6
6.1
6.7
6.8
7.0
7.2
7.0
7.0
6.9
6.6
6.7
6.6
6.7
6.7
6.7
SD


.7
.8
1.1
.9
1.2
1.4
2.7
1.7
1.7
1.4
1.1
1.3
1.4
1.5
1.6
1.8
2.0
1.9
2.0
1.9
 *  Mean of 8 sites (see Table 2).

**  Standard deviation.

-------
Table 18.  "AMMONIUM CONTENT OF SOIL FROM SITE 01.
     (CIRCLE 5) AS COMPARED TO THE AVERAGE
      OF THE REMAINING SEVEN RUBICON SITES

Depth
COT

0-15
15-30
30-46
46-61
61-76
76-91
91-107
107-122
122-137
137-152
152-168
168-183
183-198
198-213
213-229
229-244
244-259
259-274
274-290
290-305
Fourth
Mean for
Seven Sites
•

1.52
.75
.64
.61
.32
.24
.33
.27
.32
.32
.32
.30
.39
.21
.35
.24
.45
.35
.37
.49
Sampling
Site
01
ac WH. — —

40.3
30.1
5.3
40.5
2.1
33.5
47.6
40.3
1.1
.24
27.9
9.9
7.6
1.4
11.9
1.6
1.7
35.9
40.0
9.9
                 35

-------
but the concentrations in these bands were generally low.   Rubicon
and AuGres contained less than 1 ppm N as NO., generally, which,  if
converted to ppm in solution for 15% moisture in the profile,  would
be less than 6 ppm N in solution.  The Roscommon sand did  show bands
of N07 in the range of 3 to 5 ppm N in the soil (20 to 30  ppm  N in
solution at 15% moisture).   Site 16 had 56 ppm N as NOo between the
depths of 46 and 107 cm and about 45 ppm N as NOo between  213  and 244
cm in the spring 1975 samples.  This was an extremely high NO-j content
in solution.  Since this concentration exceeds the quantity of NO-j
reported in the wastewater, it suggests that the source is breakdown
of soil organic matter.

The Granby sites tended to be higher in NO^ content.  This may be
attributed to two factors:   1) the high organic matter content of the
surface soil is yielding NH,+ ions through ammonification  and  later
NOo by nitrification; 2) these sites generally have received lower
applications of wastewater so they have not come to equilibrium with
the NO^ being removed by leaching.

It must be noted here that the samplings for this study were made in
early June and late September, outside of the period during which
corn is actively and rapidly adsorbing N07 from the soil;  consequently,
higher levels of NOo were observed here than would be expected during
July or August.  Nonetheless, the concentration of NO^ of  the Roscommon
and Granby soil profiles would suggest some loss of NO^ at levels in
solution greater than would be desired.  The Rubicon and AuGres sites
have lower levels.  In view of the level of NOo in the wastewater being
applied (i.e., approximately 4.5 ppm N during the 1974 and 1975 season
except when supplemented by N during the peak portion of the growing
season), one must conclude that the source of the N07 in the profiles
from Roscommon and Granby is from the soil.  This should then reduce
in level as the system stabilizes.  It does also suggest that the system
as operated at the present time would be incapable of removing higher
levels of NOo if it were in the wastewater since the system was not
capable of removing NO^ generated by the soil.  Thus, one would need
to look for N removal in the lagoon system or a cropping system that
is capable of NO- removal during a greater portion of the growing season.

CALCIUM, MAGNESIUM, SODIUM, AND SODIUM ADSORPTION RATIO (SAR)

During the first two years of operation the content of the wastewater
with respect to bases was quite stable as shown in the following table.
                                  36

-------
Table 19.  AVERAGE CONTENT OF WASTEWATER IN THE LAGOONS AT MUSKEGON
          WASTE TREATMENT FACILITY (DATA FROM DEMIRJIAN, 1975, 1976),
Nutrient                        1974                           1975
Na
Ca
Mg
K
115*
62.5
16
9
- - HHIII ---------
145*
65
15
10
* The 1974 figure is an average of 85 ppm Na for the west lagoon and
  145 ppm for the east lagoon; the 1975 figure is an average of 125
  ppm Na for the west lagoon and 164 ppm Na for the east lagoon.
This wastewater was much higher in Na than would normally be en-
countered in soil solution.  When such wastewater is passed through
a soil, by the process of cation exchange the soil will come to a stable
equilibrium with respect to the exchangeable bases.  If the exchangeable
Na percentage becomes too high, the Na ion which is highly hydrated
dispenses soil clays and organic matter, and the soil structure may
deteriorate.  This leads to reduced infiltration rates, poor aeration,
and difficulty in management of the agronomic aspects of the system.

There have been a number of cation exchange equations used to estimate
the quantity of exchange that may occur under this type of situation
(see Fried and Broeshart, 1967).  No single equation has proved suitable
for all soil types.  Exchange constants for a given soil should be
determined experimentally.  Sodium adsorption ratios (SAR) have been
particularly useful in estimating the exchangeable Na under conditions
of irrigation.

The following is an example of the calculation of SAR for 1975:

            me/1)
SAR
DriA.
        p— _     / 1 i        / -i ^^
        |Ca me/1 + mg me/1  I
        L        2         -J
             145 mg Na/1
SAR 19?5      23 mg Na/me	            =4.46
            I" 65 mg Ca/1  + 15 mg Mg/1
              20 mg Ca/me   12 mg Mg/me
            L             2
The SAR value for the water in 1975 is 4.46 which may lead to exchange-
able Na percentages of 5.5 percent (USDA Handbook 60, 1954).  Again
it must be cautioned that the value of 5.5 is strictly an estimate

                                37

-------
and that evaluations for the particular soils in question could lead
to different values.  It is normally estimated that serious difficulties
will arise if exchangeable Na exceeds 15%, thus 5.5 is well below this
value and should give little trouble in these sandy soils.

The question may be posed, "How much Na could be allowed in the waste-
water at Muskegon before serious difficulty is encountered with the
agronomic aspects of the land treatment site?"  The conditions that
should be met for safe irrigation is an SAR less than 15  (and less than
7.5 is better) and the conductivity of the water should be less than
2,200 u mhos/cm.  Using the 1975 lagoon levels for Ca and Mg an SAR of
7.5 would be reached at 260 ppm Na in the water.  It is also estimated
that approximately 400 ppm Na would be required to give a conductivity
of the water equal to 2,200 u mhos.  Using these two values, it would
appear that the concentration of Na in the water could be safely in-
creased to 260 ppm Na or even 300 (as an average rounded number).  But
values exceeding this should be avoided.

Cation Exchange Capacity

Cation exchange sites in the sandy soils on the Muskegon  land treat-
ment facility are expected to arise from the small amount of clay in
the soils and from the organic matter in the surface layers.  The clay
content of these soils is extremely low; consequently, the total number
of exchange sites from clay will be very low (probably less than 2
me/100 g soil unless a clay lens  is encountered).  On the other hand,
the organic matter content of the surface soils can be quite high in
certain areas, particularly for the Granby soils.  Thus,  the surface
soil of the Rubicon may be expected to have up to 4 me/100 g soil of
exchange sites from organic matter, and the Granby soils  might have
as high as 14 me/100 g soil of exchange sites from organic matter.
Furthermore, the exchange sites from organic matter are expected to
be pH dependent; consequently, the rather acid conditions, particularly
for the Rubicon soil, would effectively reduce the cation exchange
capacity to even lower values since the carboxyl groups,  clay and or-
ganic matter, would be occupied with H"*" at pH values less than 4 to 5.

Clearing the areas and preparing the land for cultivation has led
to non-uniformity of organic matter content in the surface of the soil.
This may be expected to produce very heterogeneous cation exchange
systems in the surface layers.  The areas will become more homogeneous
with time due to mixing through cultivation and to incorporation of
organic residues into the surface soils.

Background Levels of Exchangeable Bases

The Na content of all soils was low and rather uniform throughout
the profile  (see tables 5 to 8).  Except  for the surface  soils,  the
content was about 0.04 me Na/100 g soil.  The only significant devi-
ation from this quantity was in the surface soils  from the Granby series

                                 38

-------
which contained about double or 0.09 me Na/100 g soil.

The Mg content of the Rubicon soils was extremely low (Table 5).   The
mean of 8 ppm Mg would not be adequate for corn production without
additional Mg.  This low content is related to the very acid pH of
the Rubicon sand which has developed because of coniferous forest and
a well-drained sand soil which has led to the removal of Mg by leach-
ing.  This is aided by the reduced cation exchange capacity due to
the acid conditions.

The Mg content of the AuGres sand soils (Table 7) is adequate for crop
growth on the average with only site 22 (circle 20) being deficient
in Mg.  Again this low value of Mg (less than 10 ppm Mg) was associ-
ated with acid conditions.

The Mg content of the Roscommon soils (Table 6) was similar to the
AuGres except for higher values in the lower layers.  In the AuGres
soils the average values were generally less than 10 ppm Mg below 45
cm  (18 inches), but the values were generally between 20 and 30 ppm
Mg in the Roscommon soils.

The Granby soils (Table 8) contained considerable Mg in the surface
layers; in fact, the average was above 100 ppm Mg for all layers down
to a depth of 152 cm.  These soils were higher because of higher cation
exchange capacities associated with higher organic matter contents
and higher soil pH's in the surface layers.  Furthermore, several of
the Granby sites gave evidence of having received applications of dolo-
mitic limestone in the past during a farming operation.

Changes in Exchangeable Bases with Application of Wastewater

The Na content of the soil profiles increased with increasing appli-
cation of wastewater.  This is illustrated in table 20 for site 01
(circle 5, Rubicon).  The Na extracted by ammonium acetate was below
10 ppm in all layers of the soil prior to application of wastewater.
After application of 20 cm (8 inches) of wastewater, the Na content
of the surface layer was more than 20 ppm, but after the application
of 380 cm (150 inches) of wastewater the Na extracted had increased
throughout the entire profile.  In general, water soluble Na will be
much lower than the exchangeable; however, for the sandy Muskegon soils
the low cation exchange capacity of the subsurface layers together
with the high water content (about 15 to 20 percent moisture) makes
it possible for a considerable portion of the Na to be in a water
soluble form and not exchangeable.

This system is rapidly expected to overload with Na during the appli-
cation of wastewater.  If we assume a uniform cation exchange capacity
of 2 me/100 g (perhaps high for all but the Granby soil) and a final
exchangeable Na percentage of 5 percent (just slightly higher than
predicted by SAR), we can predict that the profile would hold 900 kg
of Na per ha.
                                 39

-------
   Table 20.   SODIUM,  CALCIUM AND MAGNESIUM CONCENTRATIONS IN THE SOIL PROFILE OF
            SITE 01 (CIRCLE 5) AS A FUNCTION OF EFFLUENT APPLICATION.
Effluent Applied Cm *
Depth
cm
0-15
15-30
30-46
46-61
61-76
76-91
91-107
107-122
122-137
137-152
152-168
168-183
183-198
198-213
213-229
229-244
244-259
259-274
274-290
290-305
0


5.9
5.4
5.5
5.6
5.6
4.8
4.4
4.3
4.6
5.6
3.8
4.7
5.2
6.5
6.8
5.6
4.4
8.1
5.7
7.4
20


22
9.5
5.0
3.5
2.5
2.3
1.8
3.3
1.5
2.0
2.0
1.3
2.8
2.3
2.5
1.3
1.5
2.0
2.7
3.0
380


51
55
54
38
32
25
22
21
23
24
27
28
23
21
22
22
18
20
22
26
0


61
22
13
11
7
7
6
6
6
6
13
7
7
11
22
16
34
75
62
62
20

— ppm Cs. —
40
12
13
1.8
1.8
1.3
1.3
2.8
5.0
0.9
0.4
*
22
12
22
21
21
22
15
44
380


380
230
170
110
67
44
33
33
60
56
35
56
54
54
53
57
40
41
60
153
0


4.7
2.1
1.4
1.5
.5
.2
.1
.1
.4
.2
1.1
.6
.5
1.2
2.7
2.3
5.0
13
9.6
12
20

ppm Mg —
9.4
2.2
1.6
1.0
1.0
1.0
0.8
0.7
0.7
0.7
1.0
0.9
1.0
1.2
1.2
0.3
0.4
0.8
5.3
6.2
380


120
64
61
39
22
14
7.8
8.0
7.6
7.2
9.6
6.9
7.5
8.1
6.6
7.0
6.4
6.5
9.6
8.1
*  0, 8 and 150 inches,  respectively.

-------
Example of calculation:

2 me CEC/100 g (5% Na)xlO = 1 me Na/1000 g soil.
1 me Na/1000 g x 23 mg Na/me = 23 mg Na/kg soil.
1 ha = 10,000 sq meters = IxlO8 cm2.
1 ha to a depth of 300 cm = 3.0 xlO10 cm3.
Total weight of soil is 1.3 gm/cm3 x 3.0 xlO1^ =  3.9xl010 gm.
3.9xl010x lxlO~3kg/g x 23 mg Na/kg soil x 10~6 kg/mg = 900 kg  Na/ha.

This quantity of Na is furnished by 2.53 x 106 kg (5.58 million pounds)
of water containing 165 ppm sodium.  Consequently, an application of
60 cm (24 acre inches) would be expected to saturate the soil  with Na
and then to pass most of the Na directly to the drainage water.  This
conclusion is verified by the experimental data and suggests that much
of the Na being measured in the lower portion of  the profile is in
fact in solution.  The final consequences of this should not be serious
since Na is not a real hazard to most crops at the concentration in
the incoming water.  Also, Na is not apparently a real pollution hazard
in rivers and lakes at this concentration, but it must be emphasized
that these soils will reach a rapid equilibrium with the incoming level
of Na and any changes in this level will be transmitted to the drainage
water after as little as 50 cm (20 acre inches) of irrigation.

Exchangeable Ca (Table 20) increased considerably in the surface layers
after application of wastewater, but the relative portion of Ca to
other bases decreased considerably as shown by table 20.  Thus, before
application of wastewater, the 0 to 15 cm layer contained .3 me Ca/100
gram soil which represented 80 percent of the .38 me bases/100 g soil.
After application of approximately 380 cm (150 inches) of wastewater,
the quantity of Ca had increased to 1.87 me Ca/100 grams but now was
only 62 percent of the bases.  This occurred because of the increase
in soil pH from 5.1 to 6.6 during the application of wastewater which
resulted in an increase in cation exchange capacity, most probably
from dissociation of carboxyl groups associated with soil organic matter.
This increase in cation exchange capacity will allow the soil to hold
more exchangeable bases. As with Na, it must be concluded that after
application of no more than one year's wastewater, the soil will be
at equilibrium and the composition of the incoming wastewater will
be very similar to the composition of the water being discharged from
the drainage system.  Again there should be no hazard to either agro-
nomic crops or surface waters from this input of Ca.

The Mg content of the soils (Table 20) has rapidly increased from the
deficient levels on the Rubicon soil to levels that would be adequate
for crop growth as a result of wastewater application.  The fraction
of the exchangeable bases that was Mg increased during the application
of wastewater.  For example, site 01 contained 0.039 me Mg/100 grams
before application of wastewater which was 10 percent of the bases;
after application of 380 cm (150 inches) of wastewater, the magnesium
content increased to 1.0 me Mg/100 grams which was now 33 percent of
the bases.  Again this is expected to stabilize at a level controlled

                                41

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by the ratio of Mg to other bases in the applied wastewater and should
not be detrimental to agronomic crops or to surface waters.

PHOSPHORUS

Both total and Bray PI extractable P (an index of P available to crops)
have been measured in the profile samples.  The background data (tables
5 to 8 and 9 to 12) were obtained by the same combination of profile
samples as outlined under the N section.

Effect of Soil Type on the Initial Phosphorus Content of Soil Profiles

Rubicon sand profiles were initially moderately high in available
P.  This was true to a 122 cm (48 inch) depth indicating that the P
content of the parent material was relatively high.  The quantity of
25 ppm P in the surface soils should be adequate for agronomic crops
(particularly corn) in the initial years of the operation.

Both AuGres and Roscommon sands were much lower in P initially as
compared to the Rubicon profiles.  The mean values of 9.6 and 11.5
ppm P for Roscommon and AuGres, respectively, may be deficient for
maximum corn production during the initial years of operation.  Generally
speaking, wastewater should supply adequate P for growth of the agro-
nomic crop so that this low value should not be a problem, but the
wastewater being applied at Muskegon is relatively low in P and was
particularly low during the first year.  Consequently, it may take
a few years before these soils become totally adequate for maximum
crop production.  But the addition of P fertilizer would not appear
to be justified since that would result in shortening the number of
years that the site will effectively remove P.

The Granby sand profiles have a mean value of 17.8 ppm P, but they
have a much higher standard deviation.  It appeared that certain of
the Granby sites  (for example, 07 in circle 46 and 26 in circle 41)
had been previously farmed and fertilized.  The level of P fell to
low levels in these soils after the 30  cm  (12 inch) depth.  Certain
of the Granby sites were very low in P  initially, indicating that when
they had not been fertilized, their P level was equal to or lower than
AuGres or Roscommon sands.

Phosphorus Adsorption Maximum for the Major Soil Types

It was not within the scope of this project to determine or estimate
the P adsorption  capacity of these soils, but nevertheless, 8 samples
were selected from the first sampling period and the P adsorption capa-
city estimated by the Langmuir adsorption  isotherm  (Ellis, 1973).
This data is given in table 21.  These  sands have a moderately low
P adsorption capacity.  The Rubicon sand  is the highest, the AuGres
and Roscommon sands intermediate, and the Granby sand extremely low.
It should also be noted that the AuGres sand had a very low K value
 (bonding energy), the sigificance of which will be discussed in a

                                 42

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       Table 21.   PHOSPHORUS ADSORPTION CAPACITY OF SELECTED SAMPLES
                    FROM MUSKEGON WASTEWATER FACILITY.
Soil
Series Site

Rubicon (01)

AuGres (03)

Roscommon (23)

Granby (24)

, , . Soil Content of
Adsorption* _ ,, „ _ . „ .,
„ , ., . „.,., P @ 3 ppm P in Soil
Depth Maximum K** _ ,
Solution
cm
0-15
15-30
0-15
15-30
0-15
15-30
0-15
15-30
ppm
160
158
115
175
137
114
42
23
xlO l
5.6
25.0
1.3
0.3
5.0
14.6
7.3
4.3
ppm
134
151
64
40
113
106
37
19
 Quantity of  P  that  will  be  adsorbed  by the soil with maximum P in
 solution (as predicted by Langmuir Adsorption isotherm).


kit
 K is  a  constant  from the Langmuir that is related to bonding energy.
                                    43

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later section.  With this limited number of samples it cannot  be certain
if the Granby sample is representative or if the adsorption capacity
for P would increase in the lower horizons.  Prior experience  has shown
that horizons high in organic matter are generally low in P adsorption
capacity and that the adsorption capacity increases in the subsoil
layers.

The Relationship Between Phosphorus and Agricultural Production

The levels of P needed in soils for agronomic production depends upon
the yield goal or level expected.  For the Muskegon area the maximum
yield that should be expected is probably near 121 q/ha (150 bu/acre)
for corn.  This is due to very sandy, low productive soils and climate.
In the initial years of operation of the site a 80 q/ha (100 bu/acre)
yield goal may be more realistic.  Twenty to 30 ppm extractable P would
be adequate for 80 q/ha and 30 to 40 ppm P would be adequate for 121 q/ha.
As pointed out earlier, only the Rubicon soils are adequate at the
present time, with the exception of those soils that had a previous
history of fertilization.  It is expected that the P in the wastewater
will increase the soil level so that in a few years all soils  will
be adequate.

One of the major objectives of the land treatment system is to produce
clean water through nutrient removal by crops or by adsorption by land.
Phosphorus removal by land treatment is an example where both  methods
operate.  Phosphorus is first expected to be adsorbed by the soil par-
ticles, but much of this P is left in a state that is available for
plant growth.  Therefore, the soil may accumulate P during late fall
and early spring when no crop is growing and make it available to the
crop when needed.  Total removal of P by a corn crop is expected to
be from 16 to 25 pounds per acre (18 to 25 kg/ha) depending mostly
upon final yield (See Appendix III).  The quantity of wastewater neces-
sary to supply 16 pounds of P  (18 kg) will be 36 ha-cm  (35 acre-inches)
containing 2 ppm P; 23.7 ha-cm  (23 acre-inches) containing 3 ppm P;
or 17.5 ha-cm  (17 acre-inches) containing 4 ppm P.  Although the content
of the wastewater is at the lowest level at the present time,  it may
likely increase to between 3 and 4 ppm P in the futu."ۥ..  Consequently,
the needs of the crop will easily be met and exc.ess P will be supplied
to the soil.

Phosphorus Adsorption by Soils after Application of Wastewater

The soils may be roughly divided into three groups based on the quantity
of wastewater applied during the first two years—those receiving 50
to 178 cm  (20  to 70 inches), those receiving from 254 to 330 cm  (100
to 130 inches), and those receiving greater than 380 cm  (150 inches).
Assuming a P concentration of  2 ppm in the wastewater, the P added
with the wastewater would thus vary from a low of approximately 10
pounds per acre  (llkg/ha) to a high of nearly 80 pounds per acre  (90
kg/ha).  Due to the non-random nature of the location of the soil types,
the Rubicon sands all received nearly 80 pounds of P/acre  (90 kg/ha);
                                 44

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whereas, the Granby sites received approximately 20 pounds of P/acre
(22 kg/ha).  AuGres and Roscommon were intermediate, receiving averages
of 43 and 35 pounds of P per acre, respectively (43 and 39 kg/ha).
Therefore, it is difficult to compare the different soil types as to
removal of P.  A site-by-site comparison showed that 6 of the 8 Rubicon
sites had accumulated P in their surface layers; one site was too vari-
able to draw a meaningful conclusion; and one showed no accumulation.
Table 22 illustrates the type of data that were obtained for the Rubicon
sand profiles.

The quantity of P accumulated in the surface two layers may be estimated
by the following calculation:

(1) Weight of soil in a 15 cm layer of one hectare is equal to the
bulk density (1.3 gm/cm) times the volume of soil (1 x 10" sq cm/ha
x 15 cm depth) = I,950xl06 gm = 1.95xl06 kg soil/ha.

(2) P adsorbed in the 0-15 cm layer = 38-21 = 17 ppm P.
               17 kg P
(3) 17 ppm P = Ixlo6 kg soil  x l-95xlOb kg soil = 33.1 kg P.

By a similar calculation, the P adsorbed in the 15-30 cm layer is:

10 k|f f	_  x 1.95xl06 kg soil = 19.5 kg P.
Ixl0b kg soil
The total P adsorbed in the surface two layers would be approximately
53 kg P.

Considering that about 70 kg of P per ha were applied and that crop
removal during the two years could be expected to be no more than 22
kg P per ha (since the yield was very low the first year), this balance
is within experimental error and would suggest that only trivial amounts
would have passed through the Rubicon sands into the drainage water.

The exception to the Rubicon data was site 12 located in circle 22.
This site showed no accumulation of P.  In addition, examination of
the sodium data suggests that it did not receive as much wastewater
as indicated in records.  The reason for this is not known, but it
could possibly have occurred due to non-uniform application of the
wastewater on the field with higher application at locations other
than that sampled.  The potential effects on soil and drainage water
of non-uniform application of wastewater will be discussed at a later
time.

With the AuGres sites it is difficult to ascertain any accumulation
of P in the profiles.  Characteristically, they have increased levels
of P at lower depths in the profiles in the background samples.  This
zone of accumulation appeared to vary in depth over rather short dis-
tances as judged by the different samplings.  Table 23 gives a compari-
son of background P and the level after the application of approximately
380 cm (150 inches) of wastewater for site 04 (circle 24).  Site 04
                                 45

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Table 22.  INCREASE IN EXTRACTABLE P AFTER APPLICATION OF
 380 cm OF WASTEWATER TO RUBICON SAND, SITE 02  (CIRCLE 8).

Depth

0-15
15-30
30-46
46-61
61-76
76-91
91-107
107-122
Extractat
Background *

- ppm
21
16
20
30
38
24
20
21
>le P
Fall 1975

38
26
18
19
44
34
21
17
           * Mean of 1st, 2nd and 3rd Samplings
             from Summer 1972 through Fall 1973.
                       46

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Table 23.  CHANGE IN EXTRACTABLE P AFTER APPLICATION OF 380 cm OF
           WASTEWATER TO AUGRES SAND, SITE 04 (CIRCLE 24).
Extractable P
Depth
cm
0-15
15-30
30-46
46-61
61-76
76-91
91-107
107-122
122-137
137-152
152-168
168-183
183-198
198-213
Background*
	 Ppm
5.8
4.1
4.2
7.1
14.6
16.4
11.6
10.3
12.5
12.4
13.6
11.4
8.6
8.1
Fall 1975

	 —
11.3
4.4
6.8
10.8
5.2
5.6
14.2
22.3
15.3
13.2
10.2
7.6
7.0
5.6


ppm
5.5
.3
2.6
3.7
( 9.4)
(10.8)
2.6
12.0
2.8
.8
( 3.4)
( 3.8)
( 1.6)
( 2.5)
Net Change

Kg/ha-15cm **
10.7
.6
5.1
7.2
(18.3)
(21.1)
5.1
23.4
5.5
1.6
( 6.6)
( 7.4)
( 3.1)
( 4.9)
    * Mean of  1st,  2nd and  3rd  Samplings  from  Summer  1972  through Fall
     1973.
   ** Assuming a bulk density of  1.3 gm/cc.
                             47

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data, showing no P accumulation in the soil profile, is representative
of AuGres sandy soils measured at each of the four sites (03, 04, 05,
22) receiving greater than 320 cm of water.  The remaining three sites
(25, 33, 34) received less than 170 cm of water and showed no accumu-
lation of P in the soil profile.  Although there is a slight increase
in the P content of the surface layer, it is probably within the ex-
perimental error and in no way accounts for the approximately 50 pounds
per acre of excess P (56 kg/ha) applied to this site.  If the change
in P is accumulated through the 213 cm depth, there is no net change
suggesting that all changes are within experimental error.  This must
then suggest that P is moving through this profile.  This may, in fact,
agree with the data for the adsorption isotherms in that the bonding
energy for P adsorption in the AuGres soils was extremely low, giving
rise to movement at low levels of P in solution.

Life of Site for Phosphate Removal

The data is too preliminary at this time to accurately estimate the
life of the site for P removal from measuring profile data, but a
preliminary estimate has been made from the adsorption data.  There
are many management techniques that will affect the number of years
that this site will remove P.  The discussion below is given to stimu-
late consideration as to these management factors and not with the
idea that the estimates are necessarily accurate.  It was assumed in
these calculations that effective drainage is to 152 cm  (5 feet) in
all cases, that water is applied at a rate of 152 cm (60 inches) per
year, and that the adsorption capacity is that given in  table 21.
The two soils that represented the extremes in P adsorption capacity,
Rubicon and Granby, were selected for examples.  From table 24 it is
evident the Rubicon sand is a good soil for adsorbing P, whereas the
Granby adsorbs little P.  With the combination of a high yield and
low P input, the life of Rubicon sand in P adsorption is very long.
Increasing the level of P in the wastewater added to the soil decreases
the effective life of the system drastically because crop removal then
no longer represents a major portion of the P removal.

     One effective management practice is to increase the yield of
corn.  Thus, in the initial year's operation the corn was nitrogen
deficient and yielded little more than 24 q/ha  (30 bushels per acre),
but increasing the yield to 80 q/ha  (100 bushels per acre) through
good management would increase the period of time that the soil would
adsorb P by 25 or more percent for 2 to 3 ppm P in  the wastewater.
Increasing the yield to 121 q/ha  (150 bushels per acre)  would double
the length of time that the soil would adsorb P at  these levels of
P  input.   (See Appendix III for nutrient content of  corn).

The management technique of producing uneven application of wastewater
by allowing it to flow freely  through ends of spray  bar  downspouts
may lead to a much shorter effective life of the system.  This is illus-
trated  in  table 25 where calculations show the  effect of putting all
of the water on either 100, 50, or 25 percent of the soil surface.
                                 48

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     Table 24.  ESTIMATED NUMBER OF YEARS THAT P MAY BE REMOVED
      FROM WASTEWATER APPLIED AT 152 cm  (60 INCHES) PER YEAR.
Soil Type
Rubicon**



Granbyt



Yield*
q/ha
24
40
80
120
24
40
80
120
bu/acre
30
50
100
150
30
50
100
150
P
2ppm

115
132
216
371
12
14
23
38
Content of Wastewater
3ppm

71
77
100
137
7.5
8
11
14
4ppm

52
56
67
81
5.5
5.9
7.0
8.6
5ppm

41
43
49
56
4.3
4.5
5.2
6.0
 * P removed by the crop would be 7.3, 15 and 22 pounds per acre for
   50, 100 and 150 bushels yield, respectively.

** The adsorption capacity for Rubicon sand is estimated to be 2,600
   pounds P per acre five foot depth; after this quantity is adsorbed
   the level in the drainage well approached that added in the waste-
   water.

 t The adsorption capacity for Granby sand is estimated to be 274
   pounds P per acre five foot depth; after this quantity is adsorbed
   the level in the drainage well approached that added in the waste-
   water.

tt The number of years before sufficient P has been added beyond that
   removed by crops to equal the adsorption capacity.
                            49

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Table 25.   EFFECT OF UNEVEN DISTRIBUTION OF WATER ON THE EFFECTIVE
                      LIFE OF P REMOVAL ON RUBICON SAND.
Method of        Fraction of the land                P level
distribution       receiving water       2ppm     3ppm     4ppm     5ppm

Even
Uneven
Uneven
/o
100
50
25

216
67
28
	 yec
100
39
17

67
28
13

49
21
10
* The number of years is the time required to saturate that fraction
  of soil (100, 50, 24 25) with P.
                                  50

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Even on the Rubicon soil the effective life of the system could be
shortened to 17 to 28 years if this practice were followed.  The level
of P that would result in the drainage water would not be as high as
if the entire soil were saturated—i.e. for a 3 ppm P input level,
the drainage should contain 1.5 or .75 ppm P, respectively, for 25
and 50 percent soil coverage.  The result would be an increased level
of P in the drainage beyond a tolerable level in a much shorter num-
ber of years.

Considering the rather drastic differences in ability to adsorb P by
these soils, they should be followed rather closely by soil analyses
and consideration given to applying more water to the Rubicon sand
and the Roscommon sand than to the other two series.

SOIL pH

Since large volumes of wastewater will pass through the soils on the
treatment site, following the law of mass action, soil pH is expected
to be ultimately controlled by the pH of the wastewater applied (i.e.,
7.2 to 7.4); consequently, it is of minor importance to our discussion.
But the soil pH does affect certain of the chemical reactions and thus
should be considered.

Background data

Initially the Rubicon sites (Table 5) were acid throughout the profile
with average pH's in the surface 122 cm (4 feet) between 5.0 and 5.5,
and below this depth the pH ranged from 5.5 to 6.0.  The AuGres soils
(Table 7) were between 5.5 and 6.2 throughout the profile.  The Roscommon
sands (Table 6) were slightly less acid in the surface 168 cm (5.5 feet).
The Granby soils (Table 8) were much more variable, both in the surface
and in the subsurface layers.  First, the surface layers of some lo-
cations have evidence of a prior history of lime application.  For
example, site 37 (circle 42) had a pH of 7.3 in the initial sampling,
but site 27  (circle 40) had a pH of 5.3 in the initial sampling.  This
illustrates the variation due to prior liming.  A second phenomenon
occurred on 6 of the 8 Granby profiles.  When samples were removed
and air-dried, the pH of the subsurface layers (generally from 100
to 300 cm) became very acid with pH values from 2.9 to 4.0.  This is
not an unusual phenomenon in soils that have been waterlogged for an
extended period of time.  Under reducing conditions, SO/~ is reduced
to sulfide and may then accumulate if little leaching occurs.  Soil
pH will generally be between 6.0 and 7.0 in the anaerobic condition,
but as soon as the soil is aerated, the sulfide will oxidize to SO^
and generate t^SO^ which leads to very acid conditions.  This is ex-
pected to be a temporary condition for two reasons:  1) soils are not
stable at extremely acid conditions and Fe and Al oxides and hydroxides
will decompose by combining H ions with hydroxyls to form water; this
will generally lead to soil pH's between 4.0 and 5.0; 2) the addition
of wastewater with pH of 7.2 to 7.4 and high levels of Ca, Mg and Na
will rapidly lead to increased soil pH's as these cations replace H+.
                                51

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Changes Induced by Drainage

The greatest change induced by agronomic development was  the change
in aeration status that occurred with the installation of tile drainage.
The acid conditions encountered in the Granby soils had disappeared
from all sites except site 36 (circle 46) by the fall of  1975.  Much
of this change must be attributed to chemical changes in the soil that
occurred because of acid dissolution of minerals, leaching of bases
from surface horizons, and losses of acid materials from the subsoils
through leaching.

Changes Induced by Wastewater Application

The soil pH is increasing rapidly with the application of wastewater.
By fall of 1975 only six sites had pH values below 5.0 in the surface
compared to 11 initially.  Thirty sites had pH values greater than
6.0 by fall of 1975 compared to 9 sites initially.  All sites had shown
increases in soil pH except site 36 (circle 46), a Granby which had
received low water application.

It was anticipated (and observed in the field	personal communication
from Dr. Demirjian) that the installation of drainage in the Granby
soils would lead to loss of iron in the drainage water.  As previously
explained, aeration of a soil that was previously waterlogged many
times leads to the production of H^SO^.  This reduces the soil pH and
dissolves Fe oxides and hydroxides.  The water draining from such an
area will then contain Fe in either ferrous or ferric state of oxida-
tion.  Characteristically, the drainage water which is initially clear
will form a white to gray colloidal precipitate upon exposure to other
water with a higher pH and to the air.  This precipitate will turn
to yellow and then to red upon oxidation.  It is expected that this
effect is caused by drainage and not by application of wastewater.
Once the pH of the soil profile is increased, due either to the ap-
plication of wastewater or to chemical reactions within the profile,
this loss of Fe should be eliminated.

TOTAL CARBON

The total C content of the Rubicon sand profiles was quite  low initially,
the AuGres slightly higher, the Roscommon sands about fifty percent
higher, and the Granby sands were very high in organic C  (0.93, 1.14,
1.48, and 3.21% C, respectively, for Rubicon, AuGres, Roscommon, and
Granby).  The organic matter content of  the Rubicon sands decreased
rapidly with depth in the  15 to 30 cm depth  (6  to  12 inch), but the
other soil series did not  show such a dramatic decrease.  The variation
in total C content between samplings was very  large, which  is expected
because of the clearing and deep discing in the  initial establishing
of the farming operation.

There were no obvious changes  in the organic C  content after  application
of wastewater.   It would be anticipated  that the  Granby soils would

                                 52

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decrease in organic matter content during the first five or ten years'
operation mainly due to the increased aeration.   Since the surface
of the other soils was well aerated initially, they should not under-
go this change.  The organic matter content of the wastewater is suf-
ficiently low that it is not expected to affect the organic C content
of the soils.  Application of sludge could increase the organic matter
content of these soils.

Agriculturally, the Rubicon, Roscommon, and AuGres sands could benefit
from additional organic matter.  This suggests that applications of
sludge could be quite beneficial in crop production.

POTASSIUM

Although K is not normally of concern from a pollution viewpoint,
it is of importance in agronomic production and, therefore, indirectly
affects the ability of a land treatment system to remove nutrients
by the action of a biological filter.  Also, K does move in sandy soils
and, consequently, may be expected to be leached under a land treatment
system.

Background Data for Potassium

Data for ammonium acetate extractable (exchangeable) K are summarized
in tables 5 to 8.  Rubicon sand (Table 5) was initially very low in
K with only 21 ppm average in the surface soil and decreasing to less
than 5 ppm in many of the subsurface layers.  This level is not ex-
pected to be adequate for crop growth without supplemental K.  The
wastewater contains about 2.34 kg K per ha-cm (2.27 pounds/acre-inch)
of effluent; therefore, an application of 150 cm (60 inches) of waste-
water per year should be adequate for crop growth.  Although they would
still be considered low, the Roscommon and AuGres soils (Tables 6 and
7) contained about 50 percent more K in the surface than did Rubicon.
Both soils were still very low in the subsurface layers.  The Granby
soils (Table 8) averaged 84 ppm K in the surface layers, undoubtedly
reflecting a prior farming history.

Changes Induced by Wastewater Application

Table 26 summarizes changes in soil K with application of wastewater.
Essentially the Rubicon, Roscommon, and AuGres soils show no change
in K status after application of wastewater.  This would suggest that
the quantity being applied is approximately that being removed by crops
or that K is being leached through the soil profile.  Eighty quintal
per hectare (100 bu/acre) of corn would be expected to remove 21 kg/ha
(19 pounds/acre) of K (Ellis, et al. 1973).  But many of the sites
had received more than 140 kg (125 pounds) of K per year applied in
the wastewater.  Since it was not recovered in the soil, this would
suggest that it was being lost in the drainage water.  Data by Demirjian
(1975) shows 3 and 6 ppm K in the tile and discharge water, respectively,
confirming that considerable K is being discharged from the site.

                                 53

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         Table 26.  AMMONIUM ACETATE EXTRACTABLE K AT
                  VARIOUS SAMPLING PERIODS*.
Sampling Period
Soil Type
Rubicon


Rosconnnon


AuGres


Granby


Depth
cm
0-15
15-30
106-122
0-15
15-30
106-122
0-15
15-30
106-122
0-15
15-30
106-122
Bkg

21
13
7
33
17
7
32
21
5
84
37
7
1974

32
21
6
25
19
6
33
16
4
57
37
9
Spring 1975

31
18
7.8
25
16
7.8
30
24
5.7
46
30
10
Fall 1975

22
13
4.4
29
19
4.4
28
20
6.5
30
23
7
* Bkg is a average of the first three sampling periods prior to
  application of wastewater, 1974 is an average of locations within
  each soil type after 8 inches of application, and the remaining
  two sampling periods are an average of all sites for each soil
  type even though water distribution was not uniform.
                        54

-------
Loss of the monovalent ion K in the drainage water occurs because it
does not compete favorably with divalent ions,  particularly Ca,  for
exchange sites.  Thus, when wastewater is applied that contains  3.25
m.e./liter Ca but only 0.25 m.e./liter K, it is most likely that a
large percent of the K will be lost by leaching.

TOTAL SOIL ANALYSIS

Total soil chemical analysis showed little change during the period
of wastewater application except for changes in total N and C which
were previously discussed.  Thus, for the short-run time period  it
may be concluded that available and extractable soil chemical analyses
are much more sensitive to changes induced by wastewater application
than total analyses.  This would suggest that these are the analyses
that should be followed during the next one to three years.  Nonethe-
less, the total chemical analysis data are valuable in establishing
background levels which may be useful for long-term evaluation of the
land treatment system.  But it would appear that total analysis  made
on an every-five-year basis would be adequate to follow all changes
in total nutrients except N and C.
                                 55

-------
                            REFERENCES
Demirjian, Y. A., 1975.  Muskegon County Wastewater Management System,
   Land Treatment of Municipal Wastewater Effluents Design Seminars,
   U. S. EPA Technology Transfer.

Demirjian, Y. A., 1976.  Muskegon County Wastewater Management System.
   Report to EPA.

Ellis, B. G., 1973.  The soil as a chemical filter.  In:   Recycling
   Treated Municipal Wastewater and Sludge through Forest and Cropland,
   Sopper, W. E. and L. T. Kardos (Eds.).  Penn. State Press, Univ. Park,
   PA.  pp. 46-70.

Ellis, B. G., A. E. Erickson, B. D. Knezek, R. J. Kunze,  I. F. Schneider,
   E. P. Whiteside, A. R. Wolcott and R. L. Cook.  1973.   Land Treatment
   of Wastewater in Southeastern Michigan.  Detroit Dist. U.S. Army
   Corps of Engineers.

Fried, Maurice and Hans Broeshart.   1967.  The Soil-Plant System.
   Academic Press, New York.
                                56

-------
                            SECTION V

                          HEAVY  METALS

This section gives data and interpretation of the chemical analyses
which were performed on each of the major soil types to establish back-
ground levels of Fe, Mn, Zn, Cu, Pb, and Hg.  Changes in the soil's
content of these heavy metals after application of wastewater during
the first two years of operation of the land treatment section of the
Muskegon waste treatment system are reported and discussed.  The dis-
cussions are arranged in the following order:  general background and
summary; and chelate extractable heavy metals.

GENERAL BACKGROUND AND SUMMARY

Selected total and chelate extractable micronutrients and heavy metal
analyses were conducted on soil profile samples.  The elements deter-
mined were Fe, Mn, Zn, Cu, Pb, and Hg on samples taken at 15 cm (6
inch) intervals down to a depth of 305 cm (120 inches) in Rubicon,
Roscommon, AuGres, and Granby sands which are the main soil types on
the wastewater treatment site.  Samples were obtained at 8 sites on
the Rubicon sand, 9 sites on the Roscommon sand, 7 sites on the AuGres
sand, and 8 sites on the Granby sand (Figure 1 and Table 2).

Differences in total and chelate extractable Fe, Mn, Zn, and Cu in
the Rubicon, Roscommon, AuGres, and Granby sands varied widely from
sampling site to sampling site even within a soil type.  However, general
trends were evident, and the major differences in extractable metals
were between the surface layers and points deeper in the profile.
Also, major changes in extractable metal levels occurred between the
background samples (first three samplings) and the final sampling taken
in September 1975.  The background data for extractable heavy metals
is given in tables 27 to 30, and the background data for total heavy
metals is given in tables 31 to 34.  Table 35 has been prepared to
compare the changes in extractable heavy metals in the final sampling
with the baseline data at two depths, 0 to 15 era (0 to 6 inches) and
137 to 152 cm (4.5 to 5 feet).

In general, the only metal added to the soils in appreciable quantities
through the wastewater was Zn.  Zinc, which may have been added in
amounts up to 0.2 ppm Zn in the wastewater, did not show any total
accumulation, even though more than 6 kg per ha (7 pounds per acre)
of Zn could have been added to sites receiving more than 380 cm (150
inches) of wastewater.  Crop removal would account for less than 0.9
kg/ha (1 pound per acre) of Zn.  Therefore, Zn should be detected in
the surface samples in the next few years if the level in the irriga-
tion water is greater than 0.1 ppm Zn.
                                 57

-------
                Table  27.   MEAN AND  STANDARD DEVIATION OF  EXTRACTABLE HEAVY METALS OF SOILS
                           FROM MUSKEGON  SPRAY AREA-BASELINE DATA RUBICON SAND.
Ol
00

Depth

cm
0-15
15-30
30-46
46-61
61-76
76-91
91-107
107-122
122-137
137-152
152-168
168-183
183-198
198-213
213-229
229-244
244-259
259-274
274-290
290-305
F
X*


72
36
14
11
6.9
6.1
6.3
5.8
5.7
7
6.6
6.2
6.5
7.1
7.9
7.9
8.3
7.5
8.4
9.1
e
SD**


54
40
8.9
7.1
5.6
4.8
4.5
4.1
3.6
5.2
5.6
4.1
3.7
4.1
6.3
5.4
6.5
6.5
6.9
7.2

X


9
3.2
1.6
1.5
1.2
1.4
1.4
1.4
1.3
1.6
1.3
1.3
1.4
1.4
1.7
1.4
1.4
1.3
1.6
1.6
Mn
SD


11.0
4.4
1.2
1.6
1.4
1.5
1.5
1.4
1.4
2.0
1.3
1.4
1.3
1.4
2.0
1.3
1.3
1.3
1.6
1.7

X


1.70
.59
.60
.27
.23
.26
.24
.21
.23
.34
.20
.24
.25
.27
.43
.26
.25
.26
.23
.41
Zn
SD


1.58
.32
.85
.18
.16
.31
.18
.21
.21
.63
.16
.17
.21
.21
.70
.23
.24
.21
.17
.56

X


.30
.27
.22
.18
.19
.17
.23
.16
.16
.19
.24
.21
.15
.17
.17
.22
.23
.22
.20
.22
Cu
SD


.24
.26
.24
.23
.26
.19
.23
.16
.24
.21
.30
.21
.15
.19
.20
.24
.29
.31
.25
.23
P
X


.23
.14
.09
.07
.07
.07
.09
.07
.07
.06
.07
.09
.06
.06
.05
.06
.07
.07
.08
.09
b
SD


.36
.29
.17
.10
.10
.10
.14
.11
.10
.09
.10
.12
.10
.09
.08
.09
.10
.10
.12
.12

X


.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
«g
SD


.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
     *   Mean of  8  sites (see  Table  2) and  3  sampling  dates  (7/72,  6/73 and 9/73).

    **   Standard deviation.

-------
             Table 28.  MEAN AND STANDARD DEVIATION OF EXTRACTABLE HEAVY METALS OF SOIL FROM
                             MUSKEGON SPRAY AREA-BASELINE DATA ROSCOMMON SAND.
                     Fe
Mn
Zn
Cu
Pb
Kg
Ul
VO
Depth
f*rn
V^IU
0-15
15-30
30-46
46-61
61-76
76-91
91-107
107-122
122-137
137-152
152-168
168-183
183-198
198-213
213-229
229-244
244-259
259-274
274-290
290-305
X*


107
73
32
21
23
13
14
14
16
18
18
21
20
19
18
14
18
15
14
14
SD**


60
48
24
14
29
7
12
9.6
12
16
13
15
17
18
15
10
12
9.6
10
14
X


2.9
1.7
1.1
.9
.7
.7
.9
.8
.9
1.1
.9
.9
1.0
1.2
.9
.9
1.1
1.0
1.0
1.2
SD


2.3
1.3
1.3
1.2
1.0
1.1
1.8
1.2
1.2
1.8
1.1
1.3
1.6
2.3
1.3
1.5
2.0
1.7
1.4
2.1
X


1.73
1.08
.61
.42
.38
.42
.40
.42
.48
.50
.58
.70
.94
.52
.52
.48
.50
.56
.48
.50
SD

- ppm —
.86
.53
.41
.31
.24
.35
.29
.38
.45
.42
.42
.95
.99
.36
.34
.36
.35
.62
.37
.38
X


.39
.33
.28
.27
.26
.25
.28
.35
.40
.49
.42
.31
.32
.32
.36
.31
.32
.31
.33
.37
SD


.22
.21
.22
.21
.25
.18
.21
.26
.30
.40
.36
.27
.28
.23
.25
.21
.26
.21
.27
.26
X


.42
.24
.07
.09
.08
.09
.07
.08
.07
.07
.08
.11
.08
.09
.09
.07
.08
.07
.06
,06
SD


.67
.47
.12
.13
.12
.15
.10
.12
.12
.12
.12
.23
.12
.15
.18
.11
.15
.09
.10
.09
X


.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
SD


.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
     *  Mean of 9 sites  (see Table 2) and 3 sampling dates  (7/72,  6/73  and  9/73).

    **  Standard deviation.

-------
          Table 29.   MEAN AND STANDARD  DEVIATION OF  EXTRACTABLE HEAVY METALS OF SOILS FROM
                          MUSKEGON SPRAY  AREA-BASELINE DATA AUGRES  SAND.

Depth

cm
0-15
15-30
30-46
46-61
61-76
76-91
91-107
107-122
122-137
137-152
152-168
168-183
183-198
198-213
213-229
229-244
244-259
259-274
274-290
290-305
Fe
X


77
47
27
27
25
28
23
28
29
26
22
18
22
23
23
22
21
21
22
23

SD


43
31
19
29
25
18
15
37
40
24
23
18
18
19
18
16
15
13
15
18
Mn
X


2.9
2.2
1.5
.9
.9
.9
.9
.9
.8
.9
.9
.9
.8
.9
.9
.9
.9
.9
.9
.9

SD


2.1
4.4
2.8
1.4
1.4
1.5
1.4
1.4
1.4
1.4
1.4
1.4
1.5
1.4
1.5
1.4
1.4
1.5
1.5
1.4
Zn
X


2.06
1.27
.64
.43
.64
.52
.53
.44
.48
.54
.46
.41
.49
.48
.63
1.40
.50
.61
.62
.64

SD

ppm
1.30
1.76
.47
.25
.72
.31
.54
.38
.29
.31
.25
.30
.31
.35
.40
2.35
.25
.35
.35
.46
Cu
X


.42
.23
.19
.16
.15
.15
.14
.25
.21
.22
.20
.22
.20
.23
.22
.24
.24
.16
.16
.19

SD


.56
.22
.21
.17
.17
.21
.14
.25
.21
.18
.18
.21
.17
.21
.20
.22
.21
.15
.13
.16
PI
X


.94
.19
.15
.10
.11
.11
.10
.10
.18
.13
.13
.11
.10
.13
.13
.15
.16
.13
.11
.14
5
SD


1.42
.26
.21
.12
.13
.13
.12
.13
.32
.18
.18
.15
.15
.19
.16
.18
.19
.22
.13
.22
HR
X


.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00

SD


.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
 *  Mean of 7 sites (see Table 2)  and  3  sampling  dates  (7/72,  6/73 and 9/73).

**Standard deviation.

-------
          Table 30.  MEAN AND STANDARD DEVIATION OF EXTRACTABLE HEAVY METALS  OF  SOILS  FROM
                          MUSKEGON SPRAY AREA-BASELINE DATA GRANBY SAND.

Depth
r*Tn
t-lll
0-15
15-30
30-46
46-61
61-76
76-91
91-107
107-122
122-137
137-152
152-168
168-183
183-198
198-213
213-229
229-244
244-259
269-274
274-290
290-305
Fe
X


163
123
8?
76
74
72
87
106
85
85
93
95
85
81
71
69
64
55
61
54
i
SD


158
78
64
98
98
58
60
85
62
58
80
73
67
69
59
51
50
51
45
43
M
X


2.8
1.6
1.2
1.2
1.1
1.1
.9
.9
.9
.9
1.0
.9
.9
1.1
.8
.9
.9
.8
1.0
.8
n
SD


3.3
1.7
1.4
1.9
1.7
1.7
1.1
1.1
1.1
1.1
1.0
1.1
1.2
1.1
1.0
1.0
1.1
1.0
1.1
1.1
Zr
X


3.08
2.43
.81
.80
.69
.59
.64
.65
.97
.76
.84
1.16
1.12
1.07
.99
.94
.91
.92
1.00
1.13
i
SD


1.74
3.53
.56
1.01
.70
.35
.39
.41
.84
.35
.50
.83
.71
.62
.52
.44
.58
.58
.60
.83
Cu
X


.47
.43
.36
.40
.45
.46
.40
.48
.38
.41
.46
.44
.40
.32
.40
.41
.35
.39
.42
.46

SD


.66
.35
.25
.31
.36
.39
.39
.36
.34
.42
.41
.35
.30
.28
.34
.40
.34
.36
.36
.40
Ft
X


.62
.61
.33
.38
.36
.24
.23
.24
.22
.21
.25
.23
.23
.20
.21
.21
.32
.20
.26
.21
»
SD


.87
1.00
.45
.87
.73
.40
.41
.41
.41
.41
.43
.40
.43
.40
.41
.40
.64
.40
.51
.41
Hg
X


.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00

SD


.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
.00
 *  Mean of 8 sites (see Table 2)  and 3 sampling dates (7/72,  6/73 and 9/73).

**  Standard deviation.

-------
          Table 31.   MEAN AND STANDARD DEVIATION OF TOTAL HEAVY METALS  OF SOILS FROM MUSKEGON
                              SPRAY  AREA-BASELINE DATA RUBICON SAND.

Depth
SSfY)
cm
0-15
15-30
30-46
46-61
61-76
76-91
91-107
107-122
122-137
137-152
152-168
168-383
183-198
198-213
213-229
229-244
224-259
259-274
274-290
290-305
Fe
X


4200
4100
4300
4200
3600
3300
3500
3300
2800
2900
3100
3200
3000
3100
2600
3100
3000
3200
3400
3400

SD


1300
1300
1300
1300
1100
1200
1500
1300
900
900
1100
1300
1200
1100
1300
1600
1200
1600
1600
1500
Mn
X


170
110
82
75
60
60
69
60
59
51
59
60
66
60
68
65
66
65
62
63

SD


90
56
25
24
24
25
32
26
29
16
21
25
39
23
35
36
36
26
26
30
Zn
X


35
33
27
24
22
18
18
18
15
15
17
18
32
19
20
23
26
26
22
46

SD

ppm
17
19
10
9
11
10
10
9
10
11
10
11
69
23
21
23
32
48
23
35
Ci
X


25
22
22
22
20
18
20
20
20
24
24
23
21
20
19
20
21
24
20
20
i
SD


40
34
39
42
38
37
40
38
44
53
59
45
45
44
35
39
43
55
46
41
Pb
X


.7
.7
.7
.7
.7
.7
.7
.7
.7
.7
.7
.7
.7
.7
.7
.7
.7
.7
.7
.7

SD


.9
.9
.9
.9
.9
.9
.9
.9
.9
.9
.9
.9
.9
.9
.9
.9
.9
.9
.9
.9
Hf
X


.3
.4
.3
.4
.3
.4
.5
.2
.2
.2
.3
.3
.2
.2
.2
.2
.2
.3
.2
.2
t
SD


.4
.5
.3
.4
.3
.4
.5
.0
.0
.0
.3
.3
.0
.0
.0
.0
•0 .
.3
.0
.0
 *  Mean of 8 sites (see Table 2)  and  3  sampling dates (7/72,  6/73 and 9/73).

**  Standard deviation.

-------
                   Table 32.   MEAN AND  STANDARD DEVIATION OF TOTAL HEAVY METALS OF SOILS FROM
                                MUSKEGON SPRAY AREA-BASELINE DATA ROSCOMMON SAND.
CO

Depth
PTTI
L.U1
0-15
15-30
30- /,6
46-61
61-76
76-91
91-107
107-122
122-137
137-152
152-168
168-183
183-198
198-213
213-229
229-244
244-259
259-274
274-290
290-305
F
X*


4200
4200
3700
3300
2600
2600
2500
2600
2600
2700
2800
2500
2300
2300
2500
2500
2800
2700
2400
2400
e
SD**


2400
2700
2000
1600
950
1200
1100
1100
1300
1400
1300
1100
990
990
940
980
1300
1300
990
990
Mr
X


71
59
51
55
54
56
54
59
58
61
56
55
49
48
41
50
53
66
52
53
i
SD


73
39
31
26
24
20
27
31
25
30
26
28
20
24
30
36
38
44
30
24

X


22
17
15
14
16
15
20
17
15
17
19
18
16
15
15
19
16
34
14
13
Zn
SD

	 ppra -
9.4
10
9.1
7.2
9.6
9.0
16
10
8.5
8.6
12.4
13
12
6.3
6.1
14
8.0
100
7.9
6.5
Cu
X


14
13
13
11
11
8.4
9.0
9.7
8.2
9.5
9.3
7.7
8.5
8.2
10.2
8.5
8.2
8.0
7.7
8.4

SD


13
12
15
18
18
10
10
10
9.9
12.9
11
10
10
11
12
10
9.1
10
10
11
PI
X


.7
.7
.7
.7
.7
.7
.7
.7
.7
.7
.7
.7
.7
.7
.7
.7
.7
.7
.7
.7
b
SD


.9
.9
.9
.9 .
.9
.9
.9
.9
.9
.9
1.0
.9
.9
.9
.9
.9
.9
.9
.9
1.0
HF
X


.4
.2
.2
.2
.2
.2
.2
.3
.2
.3
.3
.2
.2
.2
.3
.3
.2
.2
.2
.2
r
SD


.5
.0
.0
.0
.0
.0
.0
.2
.0
.2
.3
.0
.0
.0
.3
.3
.0
.0
.0
.0
       *  Mean of 9 sites (see Table 2) and 3 sampling dates (7/72, 6/73 and 9/73).

      **  Standard deviation.

-------
             Table 33.   MEAN AND STANDARD DEVIATION OF TOTAL HEAVY METALS OF SOILS FROM
                           MUSKEGON SPRAY AREA-BASELINE DATA AUGRES SAND.
              Fe
Mn
Zn
Cu
Pb
Hg


cm
0-15
15-30
30-46
46-61
61-76
76-91
91-107
107-122
122-137
137-152
152-168
168-183
183-198
198-213
213-229
229-244
244-259
259-274
274-290
290-305
X*


3000
2800
2600
2900
2400
2400
2400
2500
2400
2400
2400
2400
2400
2100
2100
2000
2600
2300
2300
2600
SD**


2800
2400
1900
1500
970
830
820
880
910
1100
990
1700
1100
690
980
910
1700
900
660
1200
X


60
53
4§
68
47
54
50
51
50
50
46
39
50
42
43
42
39
37
43
42
SD


34
25
26
33
26
24
22
17
19
15
27
24
29
25
24
22
18
16
25
15
X


25
28
19
18
20
19
23
22
18
19
21
19
17
26
17
17
19
20
19
18
SD

	 ppm
17
29
13
15
13
16
24
22
16
15
22
11
13
22
14
14
15
14
14
13
X


15
16
13
13
16
12
16
16
13
8.2
11
9.1
12
9.6
10
9.5
10
7.8
9.3
8.5
SD


24
' 23
25
25
25
26
27
29
20
9.1
12
12
18
13
11
13
14
10
12
11.9
X


.9
.9
.9
.9
.9
.9
.9
.9
.9
.9
.9
.9
.9
.9
.9
.9
.9
.9
.9
.9
SD


1.0
1.0
1.0
1.0
1.0
1.0
1.0
1.0
11.0
1.0
1.0
1.0
1.0
1.0
1.0
1.0
1.0
1.0
1.0
1.0
X


.4
.2
.3
.4
.2
.2
.4
.4
.3
.2
.4
.3
.2
.4
.3
.2
.4
.4
.2
.3
SD


.5
.2
.2
.6
.2
.2
.3
.4
.2
.2
.4
.3
.2
.3
.2
.2
.7
.3
.2
.3
 *  Mean of 7 sites (see Table 2)  and 3 sampling dates (7/72, 6/73 and 9/73).

**  Standard deviation.

-------
                  Table 34.   MEAN AND STANDARD DEVIATION OF TOTAL HEAVY METALS OF SOIL FROM
                                MUSKEGON SPRAY AREA-BASELINE DATA GRANBY SAND.
Ui

Depth

cm
0-15
15-30
30-46
46-61
61-76
76-91
91-107
107-122
122-137
137-152
152-168
168-183
183-198
198-213
213-229
229-244
224-259
259-274
274-290
290-305
F
X*


4800
4600
3500
3000
3000
2600
3100
2900
3200
2900
2700
2700
3000
3300
2900
2900
2800
2700
2700
2900
e
SD**


2100
2300
2200
1300
1200
660
1100
910
1400
1200
650
960
1200
1800
1000
1400
850
840
850
1200
b
X


95
91
86
76
59
52
60
63
75
66
55
52
58
58
52
52
52
50
47
54
In
SD


46
58
73
75
56
23
34
31
43
38
27
33
26
32
27
30
26
25
23
31
Z
X


40
37
32
25
29
21
22
23
25
22
23
24
23
24
27
27
23
27
25
22
n
SD

	 ppm -
29
31
26
22
31
19
19
19
26
22
21
21
22
23
25
25
20
28
25
19
Cu
X


12
15
11
8.0
8.5
5.6
5.2
6.1
5.3
6.4
7.1
8.6
6.0
8.2
7.1
9.5
8.4
9.0
6.1
6.6

SD


12
16
13
9.3
12
7.2
9.6
10.9
8.3
9.3
14
16
8.6
14
14
18
13
15
9.3
8.9
Pb
X


1.2
1.2
1.2
1.2
1.2
1.2
1.2
1.2
1.2
1.2
1.2
1.2
1.2
1.2
1.2
1.2
1.2
1.2
1.2
1.2

SD


1.0
1.0
1.0
1.0
1.0
1.0
1.0
1.0
1.0
1.0
1.0
1.0
1.0
1.0
1.0
1.0
1.0
1.0
1.0
1.0
HF
X


.2
.2
.2
.2
.2
.3
.3
.4
.3
.3
.2
.3
.3
.4
.4
.2
.3
.3
.3
.4
r
SD


.2
.2
.2
.2
.2
.4
.2
.5
.5
.4
.2
.5
.4
.6
.5
.2
.2
.2
.2
.5
      *  Mean of 8 sites (see Table 2) and 3 sampling dates  (7/72, 6/73 and 9/73).

     **  Standard deviation.

-------
                          Table  35.  CHANGES  IN CHELATE  EXTRACTABLE Fe,  Mn,  Zn and Cu
                                        AFTER APPLICATION  OF  WASTEWATER.
cr>
Chelate
Sampling*
Extractable Period
Metal
Fe

Mn

Zn

Cu

Soil Type and Depth
Rubicon
0-15cm
Bkg
Sept. 1975
Bkg
Sept. 1975
Bkg
Sept. 1975
Bkg
Sept. 1975

72
17
10
1.5
1.7
1.2
0.3
ND
135-150cm

7
4
1.6
0.4
0.3
0.1
0.2
ND
Ros common
0-15cm

107
22
2.9
2.1
1.7
1.4
0.4
ND
135-150cm

AuGres
0- 5cm

18 77
14
1.1
0.4
0.5
0.3
0.5
ND
26
3.0
0.7
2.1
0.8
0.4
ND
135-150cm

26
11
0.9
ND
0.5
0.3
0.2
ND
Granby
0-15cm

160
20
2.8
1.5
3.1
1.8
0.5
ND
135-150cm

85
16
0.9
0.2
0.8 .
0.1
0.4
ND
    * Bkg is an average of  the three sampling periods prior  to  application of wastewater,

   ND is less than  .2 ppm for Mn and Cu.

-------
CHELATE EXTRACTABLE HEAVY METALS

Chelate extractable Zn, Cu and Mn have been measured in soils to es-
timate that fraction of these heavy metals that are available for plant
uptake.  Thus, this measure has been used here to estimate the fraction
of heavy metals which may be susceptible to incorporation into our
food chain.  It is also probable that this fraction would be more sus-
ceptible to movement in soils than would precipitated forms of the
heavy metals.

Levels of chelate extractable heavy metals were much higher in the
surface horizons than in the subsurface layers.  This strong associa-
tion with soil horizons that were high in organic matter is to be ex-
pected.

The most noticeable effect of operation of the system was the reduction
in chelate extractable heavy metals, particularly Fe and Mn, by the
time of the seventh sampling in September 1975.  For example, extrac-
table Fe decreased from 72 to 17 ppm for the Rubicon sand, and the
other soils were comparable.  A large part of the extractable Fe was
probably associated with organic matter.  When the land was drained,
placed under cultivation, and irrigated, the organic matter was mixed
by implements and generally handled in a manner which resulted in its
decomposition.  This reduced the soil's ability to maintain the Fe
in a soluble or extractable form.  The pH of the applied wastewater
was about 7.2 which resulted in increases in the soil pH (see Section
IV).  This is expected to result in precipitation of the heavy metals,
particularly Fe and Mn, in the pH range of the soils at the Muskegon site.

There was no evidence of accumulation or movement of heavy metals
in the soils even after application of 380 cm (150 inches) of wastewater.
This would indicate that the site should operate effectively in heavy
metal removal for more than 50 years at the present rate of input.
                                67

-------
                            SECTION VI

                     SOIL PHYSICAL PROPERTIES

                           STUDY SITES

This section gives data and interpretation of physical properties of
the soils at the Muskegon land treatment site which may be important
to application of wastewater.  A discussion of the changes in physical
properties of the soils after application of wastewater is included.
The discussions are arranged in the following order:  study sites;
methods of study; resu?.ts and discussion; and addendum.

Originally nine study locations were selected.  These included sites
which were thought to be characteristic of each of the four main soil
series on the project.  These included AuGres, Granby, Roscommon,
and Rubicon soil series.  Two sites were selected for each series.
They were selected so that they would occur in different irrigation
circles and in large areas of occurrence of the soil series.  The sites
also had to be accessible for the infiltration equipment.  AuGres sites
were selected on circles 23 and 40, Granby sites on circles 46 and
47, Roscommon sites were on circles 42 and 48, and Rubicon sites were
on circles 3 and 5.  Initially there was a finer-textured Granby on
circle 42 which was thought to be interesting to study; however, after
the first year it was evident that this site was covered with a silt
fill, was actually not a natural soil, nor was it a major component
of the project.  Therefore, the Granby with silt fill, which was studied
the first year on circle 42, was abandoned the following year.  After
the first year and the initiation of the water spreading, the Roscommon
site on circle 48 was no longer accessible; therefore, a new site was
selected on circle 50.

METHODS OF STUDY

Infiltration

Infiltration measurements were made in the field, using concentric
ring infiltrometers with rings of 12.5 and 22.5 cm  (5 and 9 inch)
diameter.  The measurements were replicated ten times on the surface
soil and five times on the subsoil.  The rings were driven  2.5 to 5
cm  (1 to 2 inches) into the surface of the top soil or subsoil after
excavation for the measurement.  Using large automatic burets set at
2.5 cm  (1 inch) above the surface of the soil, water was measured as
it  infiltrated the center 12.5 cm  (5 inch) ring.  The outside ring
was maintained at the same water level with a constant water level
device.  Infiltration measurements were made at 5-minute intervals
for the first half hour, ten-minute intervals for the second half hour,
and at 15-minute intervals for the next four hours, for a total  in-
filtration time of 5 hours.  The average of the first hour  is considered
the initis.1 dry infiltration rate.  The average infiltration rate for
the last hour is considered the minimum dry infiltration rate.   Soil

                                68

-------
was allowed to drain naturally from 12 to 18 hours, and then the wet
infiltration run was performed in the same manner for an additional
five hours.  The initial wet is the first hour's infiltration, the
minimum wet is the fifth hour infiltration.  Before the initial dry
infiltration, moisture samples were taken and are recorded with the
infiltration analyses.

Mechanical Composition

Mechanical composition was determined by the Bouyoucos Hydrometer
Method.  Fifty grams of soil was dispersed by adding 100 ml of a 5%
hexametaphosphate solution and water and then stirring on a mixer dis-
persing unit for 5 minutes.  The two-hour hydrometer reading was used
as the measure of clay.  The dispersed sample was then washed through
a 325-mesh sieve.  The total sands were dried and weighed.  The dry
sands were split to one-quarter with a sample splitter and dry sieved
with standard sieves on a sieve shaker for 15 minutes.

Hydraulic Conductivity and Soil Water _Ch_ar_act_eris_t_ic_

Soil cores were collected at the site of the infiltration determina-
tion, using 7.5 cm (3 inch) diameter, 7.5 cm (3 inch) long cylinder,
and a standard hand driven core sampling apparatus.  These samples
were taken of the surface 3 inches, which was entitled A , of the B
horizon, and of the underlying material which was designated as C.
These samples were taken with ten replications packed in individual
cartons and transported to the laboratory.  In the laboratory, samples
were covered on the bottom with a sheet of filter paper which was held
in place by cheesecloth and a rubber band.  The samples were saturated
with water for a period of several days, and then the other analyses
were performed.

Cylinders (2.5 cm (one inch) deep) were attached to the core samples,
and the saturated core sample was placed on a Buckner funnel with 1.25
cm (1/2 inch) of water applied at a constant head using a Mariott bottle
to maintain the water lavel.  The amount of water which drained from
the sample for one-half hour was measured and the hydraulic conductivity
calculated.

The saturated samples were then weighed and placed on a series of blot-
ting paper tension tables adjusted to 0.01 atmosphere, 0.02, 0.03,
0.04 atmospheres of tension.  Samples were allowed to equilibrate
for two days, weighed, and moved to the next tension.  From there,
the samples were placed in a pressure plate apparatus and weighed after
a 2-day equilibrium at 0.1, 0.33, and 1.0 atmospheres pressure.  After
this, the samples were oven dried and reweighed.  From this data, the
soil water characteristics from saturation to one atmosphere were cal-
culated on a percent water-by-volume basis.  Bulk density was calculated
from the oven dry weight and volume of core.  Pore space was calculated
using the saturated water loss.

                                69

-------
Aeration and Redox

Aeration measurements were made using the platinum microelectrode
method of Lemon and Erickson, and Redox measurements were made with
the same electrode using a portable potentiometer.

                      RESULTS AND DISCUSSION

Mechanical Composition

The mechanical analysis of these soils indicates they are all sands.
There is some variation in the amount and distribution of the sands
between the various soil series, but there is also considerable vari-
ation between different samples taken from the same sampling area.
Only the Granby soil on circle 47 had detectable amounts of clay, and
then only 1% was present.  The bulk of the sands were in the medium
and fine sand range or from 100 to 500 microns diameter.

These soils have single grain structure except for the occasional
Fe cemented ortstein horizons.  With this exception, they should be
durable to tillage and other manipulations.  The only physical problem
is of water retention or drouthiness.

Soil Water Characteristics, Bulk Density and Hydraulic Conductivity

These determinations were all made on the same core samples.  Because
there did not appear to be any trends in these values from successive
samplings, all of the values were averaged and presented in table 36.
When the eighty values  (two sites sampled four times with ten samples
per sampling) for each soil series are compared, they are remarkably
similar.

All the A  horizons hold more water and have a lower bulk density
than the B or C horizons.  The deeper horizons decrease in water re-
tention with depth.  There is some additional water held by the  im-
perfectly drained AuGres and Roscommon that had more organic matter.

The 0.1 atmosphere moisture percentage might be considered the field
capacity  (water present in soil after free drainage) of these soils.
Considering this value, the A^ of the Roscommon averaged 30% as  com-
pared to 19% for the Rubicon.  The deeper horizons were quite variable
from sample to sample, but the averages were quite similar, ranging
from 10 to 16%, except  for Rubicon C which was lower.   If either of
the Granby soil sites had had a mucky surface, as some  01 the Granby
on the project does, the moisture characteristic would  have been higher
and the bulk density less.

The bulk densities of these  sands were similar, although these values
for the A  were altered early in the season by tillage.

All of the average hydraulic conductivities were  quite  similar except
                                 70

-------
Table 36.   SUMMARY OF AVERAGES OF SOIL PHYSICAL PROPERTIES BY
                   SOIL SERIES AND HORIZONS
Soil Type

Rubicon Sand


Granby



Ros common



AuGres



Horizon
Soil Water Characteristics
	 Tension - atm. 	
0.01 0.1 0.33 1.0

Ap
B
C
A
P
B
C
A
P
B
C
A
P
B
C
-Percent
43
38
38
42

38
35
44

35
33
44

40
34
water
19
10
8
25

16
10
30

16
10
25

15
11
by
18
9
8
18

10
6
23

10
6
20

12
7
volume-
14
8
7
15

8
5
22

8
5
18

10
6
Bulk
Density
g/cc
1.4
1.6
1.6
1.4

1.6
1.6
1.2

1.6
1.7
1.2

1.5
1.6
Hydraulic
Conduc-
tivity
cm/hr
32
54
84
16

33
40
34

28
42
38

33
38

-------
for the Granby A  which was about one-half the average and the  Rubicon
C which was twice the other values.   All these values are  high  and
confirm that these are very permeable soils.

Infiltration

The infiltration determinations are  summarized in table 37 giving
the values at each of the four samplings.  The data is extremely vari-
able, and no obvious trends are evident.  Soil variability seems to
be amplified by the infiltration measurement  even though each value
is an average of ten measurements for the surface and five for  the
subsurface.  Much of the surface had just been cleared, and the sampling
occurred as it was being brought under cultivation and irrigation.
The subsoils in these sands are also very variable.  Nevertheless,
all of the values are extremely high; the lowest reading was about
10 cm per hour. There should be no problem with water application with
infiltration rates of these soils as long as  there is adequate  under-
drainage.

Oxygen Diffusion Rates and Redox Potential

Oxygen diffusion rates were determined after  the heavy application
of wastewater that occurs at the far end of a large irrigation rig.
Even though the water suood on the surface in the lower places  for
fifteen to thirty minutes, the duration of oxygen deficient conditions,
which occurred after visible infiltration from the surface ceased,
persisted for less than thirty minutes.  Under these rapidly changing
conditions, plants would not be harmed by this stress.  The redox po-
tentials in the soil would not be reduced either.

Under several of the circles, where the drainage system has failed,
flooding of the soil has developed.   We were not aware of this as our
field crew had completed their measurements before this developed.
Under these conditions of drainage failure, oxygen deficiencies and
redox change are to be expected and plant growth may be adversely af-
fected.  The solution of this problem is to bring the drainage system
up to the original specifications.

ADDENDUM

Since this study was completed, small areas of Saugatuck and areas of
slowly permeable AuGres soils have been observed in  circle  26.  These
soils have not been studied.  They are  difficult to  locate  until after
a period of irrigation reveals their location.  Once  these  areas have
been found, they should be mapped and studied to determine what sort
of modification is necessary to overcome the  flooding  that  is  occurring
on these soils.
                                72

-------
                 Table 37.   SUMMARY  OF  INFILTRATION RATES  DETERMINED DURING 1973-1975.
Infiltration Rates
Condition
Time *
Soil Type

Rubicon
Surface

Granby
Surface

Subsurface

Roscommon
Surface

Subsurface

AuGres
Surface

Subsurface

Initial Dry

Circle
Number

3
5

46
47
46
47

42
48
42
48

23
40
23
40
1st




82
63

26
13
76
73

26
58
51
40

74
23
39
43
2nd




79
50

44
31
125
14

29
49
60
32

50
29
31
39
3rd




47
59

49
43
86
45

39
48
51
19

51
40
65
22
4th




90
80

48
39
64
93

29
23
26
35

46
67
53
51
1st




51
48

12
7
51
34

17
38
40
33

45
15
49
18
Initial Wet
2nd
__ /u —



68
46

30
17
60
6

27
31
50
21

53
15
39
26
3rd




36
28

23
20
35
19

15
27
28
11

25
16
44
13
4th




42
90

22
18
30
50

16
11
13
27

22
36
26
37
1st




51
48

9
2
36
29

12
25
44
26

37
18
34
21
Minimun Wet
2nd




64
42

39
15
61
4

23
29
57
17

38
15
37
31
3rd




48
53

14
15
36
57

12
8**
13
22**

18
38
30
37
4th




35
26

19
17
41
19

12
19
35
10

21
17
44
11
    Time of sampling was 1st in Spring 1973,  2nd in August 1973 before the application of wastewater, 3rd
    in summer 1974 after limited wastewater application and 4th in Summer 1975 after all the circles had
    a full year of application.
**  Circle 48 was not accessible for the 3rd and 4th sampling so Circle 50 was substituted.

-------
                           SECTION VII

                        MICROBIAL STUDIES

The principal objective of the work discussed in this section was
to determine the type and quantity of microorganisms present on the
Muskegon land treatment site, with particular reference to those in-
volved in nitrogen transformations.

Microbial populations were determined on three soils representative
of the soil diversity present at the Muskegon site.   The populations
were analyzed by the following methods:  nitriflers, MPN (most probable
number), using an ammonium carbonate medium and testing for the ap-
pearance of N03; denitrifiers, MPN in N03 broth incubated anaerobically
and tested for disappearance of both NO^ and NC^; aerobes, plate count
on soil extract agar; anaerobes, MPN in NOo broth and observing tur-
bidity.

The most striking result is the low numbers of nitrifiers on the Rubi-
con and AuGres soils r.t the start of irrigation  (table 38).  This
is likely due to the low pH, 4.6 and 6.0, respectively, since acidic
conditions are known to be unfavorable to chemolithotropic nitrifiers.
The high NH^  in the soil at the Rubicon site is also explained by
this nitrification limitation.  However, as wastewater was added, the
pH increased, allowing proliferation of nitrifiers at the expense of
NH^ , their energy source.  The initial low pH of the Rubicon site
was due to the forest cover.  By comparison, the farmed Granby soil
had a neutral pH, high nitrifier population, and low NH^  at the onset
of irrigation.  It maintained this quasi-steady-state condition through
the second year.

The denitrifier population increased slightly with irrigation, parti-
cularly in the Rubicon soil.  The denitrifier population relative to
total aerobes and anaerobes was quite low in all of these soils com-
pared to most other agricultural soils.  A possible explanation is
the low organic matter and aerobic conditions of these very sandy soils.

The aerobic population was fairly stable through the irrigation.
It was significantly higher  in  the Granby soil as expected because
of its higher organic matter content.

The anaerobic populations showed a c'ecrease with wastewater irrigation.
A possible explanation is that  sporeforming anaerobes, i.e., clostri-
dia, may have been stimulated to germinate but did not survive under
the aerobic conditions present.

In summary, it  is clear that the irrigation had  no detrimental effect
on the soil microbial community, and,  in the  case of the nitrifiers,
it stimulated their development, thus  assuring the conversion of
to NO^ in the soil.

                                74

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Table 38.  CHANGE IN MICROBIAL POPULATIONS AND SELECTED CHEMICAL
     PARAMETERS IN RESPONSE TO INITIAL WASTEWATER IRRIGATION
                      ON THREE SOIL TYPES.
Site

5
(Rubicon)


24
(AuGres)


46
(Granby)


Date

6-11-74
8-05-74
6-23-75
9-10-75
6-11-74
8-05-74
6-23-75
9-10-75
6-11-74
8-05-75
6-23-75
9-10-85
Microbial
Nitrifiers
(xlO1)
2.3
470
1600
4200
13
160
2800
1700
1900
420
1400
7000
populations
Denitrifiers
(xlO3)
8.4
48
46
170
22
49
42
88
46
36
320
110
(nos'g dry
Aerobes
(xlO")
3.6
4.4
1.2
15
120
4.0
5.4
8.3
18
10
9.4
12
wt"1)*
Anaerobes
(xlO5)
75
22
2.6
13
98
10
3.8
17
55
23
22
11
 Samples were taken from the same site.   Four replicate soil samples,
 each comprised of four subsamples,  were taken from the same site.
                         75

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     Table 38.  CHANGE IN MICROBIAL POPULATIONS AND SELECTED CHEMICAL
          PARAMETERS IN RESPONSE TO INITIAL WASTEWATER IRRIGATION
                     ON THREE SOIL TYPES.  (CONTINUED)
Water added
   27.8
   33.0
   41.2
pH
7.3

5.7
7.0
NH^-N
N03-N    Total C
 0.6

 2.2
 0.7
 7.0

58.2
10.6
2.2

4.4
2.1
            Site Listing
(cumula-
tive

85.
107.
148.

71.
80.
113.
in.)

1
7
7

2
7
6
(ppm)
4.
6.
6.
6.
6.
7.
6.
6.
6
8
0
6
0
0
5
2
40.
20.
3.
0.
1.
7.
2.
0.
8
0
4
2
1
8
5
2
(ppm) (%)
2.
5.
9.
8.
6.
1.
6.
9.
3
2
6
1
7
1
7
5
2.
0.
1.
1.
1.
1.
1.
2.
0
7
0
1
9
5
7
8
Forest cleared
in 1973


Abandoned
land





farm



                                                          Actively farmed
                               76

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                                SECTION VIII

                  PESTICIDES AND INDUSTRIAL TRACE ORGANICS

INTRODUCTION

It is to be expected that wastewaters from a large municipality will contain
a wide spectrum of potentially toxic trace organics originating in industry,
warehouse facilities, or distribution and trade channels.  Also, in a newly
established system, there is the probability that not all sources of storm
flow have been identified and isolated from the wastewater collection network.

In the Muskegon and Whitehall systems, such storm flows can originate in
areas of intensive vegetable production as well as in urban landscapes.
Until non-point sources are identified and isolated or otherwise regulated,
the sewage collection system can serve to channel pesticides in runoff and
sediments from scattered areas of use to a common point—the wastewater treat-
ment facility.

Data reported in this section represent a surveillance level monitoring of
soils and waters associated with the two Muskegon County wastewater manage-
ment systems.  Four objectives were in view:

     a) To obtain an inventory of readily detectable and potentially
        toxic pesticides and other trace organics in incoming raw sewage.

     b) To derive preliminary information regarding the fate of trace
        organics at various stages of treatment.

     c) To obtain a baseline inventory of trace organics in representative
        soils prior to irrigation with wastewater.

     d) To observe changes in level and profile distribution that might
        provide an early indication of the extent to which recalcitrant
        compounds in wastewater may accumulate in soils and pose a long
        term residual threat to crop production and terrestrial wildlife
        or to contiguous aquatic environments and groundwater supplies.

Attention was focused on organic species which can be detected at very low
concentrations by gas-liquid chromatography (GLC), using an electron capture
detector (ECD).  These include many of the persistent halogenated compounds
of environmental concern.

Sampling of wastewaters was initiated with the first flow of raw sewage to
the Muskegon Wastewater Management System in June 1973.  Monthly composites


                                      77

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of raw sewage from June through November 1973 were used to inventory chro-
matographic peaks, make tentative peak assignments and modify procedures for
routine analysis.  The first useful analyses of raw sewage were obtained in
December 1973, at which time routine monthly analysis was initiated (monthly
composites of twice-daily grab samples).  Beginning in April 1974,  daily grab
samples were composited for monthly analysis of discharges (after aeration
and settling) into the storage lagoons.  At this time also, monthly composit-
ing (daily grab samples) was begun at Mosquito Creek and Black Creek outfalls
(SW-05 and SW-34, Fig. 1).  After field irrigation began in May 1974, flows
out of storage (before and after chlorination) were composited periodically.
At Whitehall, routine monthly analysis of raw sewage and of treated dis-
charges into storage was begun in April 1975 (monthly composites of weekly
grab samples).

Eight special study sites, representing four soil types, were sampled twice
before wastewater was applied and twice yearly since full scale irrigation
was initiated in 1974.  Additional analyses for background were performed
on soils from 25 sites sampled in 1972 or 1973.

The special study sites at Muskegon (Fig. 1) were on AuGres sand (sites 03
and 04, circles 21 and 24), Granby sand (sites 08 and 26, circles 47 and 44),
and Roscommon sand (sites 16 and 17, circles 41 and 42).  Two sites at
Whitehall  (not shown in Fig. 1) were on Rubicon sand (sites 30 and 31,
circles W-3 and W-l).

GLC peaks which correspond to those for 29 known reference chemicals have
been encountered in soils or waters.  The corresponding peak positions  in
output from two different GLC columns were monitored routinely for all  ex-
tracts of  soils and waters.  Thin layer chromatography and, for certain
chemicals, a third or fourth GLC column were also used for confirmation.

Three additional peaks were monitored routinely, beginning August 1975, but
have not been identified with known compounds.  These were frequently prom-
inent in raw influent and in discharges to storage.  They appeared at greatly
attenuated levels in soils and in outfall waters.

PROCEDURES

Sampling methods and analytical procedures are described  in detail in
Appendix II.  They are described briefly below.

Sampling and Extraction of Soils

Four cores were  composited from depths  of 0  -  15, 46 - 61, and 91 -  107 cm
 (0 - 6", 18 - 24", and 36 - 42")—the  third  depth was not  sampled prior to
1975.  Aliquots  (100 g field moist soil) were  deactivated with water and  ex-
tracted with  two  successive 100 ml aliquots  and a third  50 ml aliquot of  2:1
benzene-isopropanol. The  isopropanol was removed with water.  The benzene
extract was dried by passing  through anhydrous sodium  sulfate and concen-
trated twice  to  a final volume of 10 ml.
                                     78

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Sampling and Extraction of Waters

Water samples were taken daily (or as noted in tables) and accumulated at
4° C over periods of 2 to 5 weeks.  Raw influent and discharges into storage
through 1975 were separated by centrifugation and filtering into aqueous and
particulate phases.  Particulate phases were extracted with 2:1 benzene-
isopropanol as for soils.  Water samples (1.5 liters) were extracted with
4 successive 50-ml aliquots of methylene chloride.  The extract was concen-
trated to 5 ml and transferred into benzene (with successive concentration
steps to remove methylene chloride).  The final volume in benzene was 10 ml.

Cleanup of Extracts

Prior to analysis, benzene extracts were cleaned up and separated into
groups of chemicals by fractional elution off from Florisil.

Detection and Quantitation of Organics

Detection and quantitation were by gas-liquid chromacography (GLC), using
1.5% OV-17/1.95% QF-1 on Gas Chrom Q in glass columns (3 mm I.D. x 1.83 m).
Identification was by retention time confirmed on one or more additional
columns and by thin layer craromatography (silica gel).  A Beckman GC-5 was
used, with a non-radioactive electron capture detector (helium arc discharge).
Instrument parameters were optimized daily for maximum sensitivity.  Integra-
tor  (Autolab System I) parameters were set to reject peaks with heights less
than 3 times baseline noise.

An injection volume of 4 yl was used for samples.  Reference standards were
injected after every third sample, at volumes ranging from 1 to 6 pi to
provide a standard curve.  Standard concentrations of 1/10 X, 1 X, or 10 X
were used to provide ranges of linear response appropriate for sample con-
centrations encountered.

Confirmation of Peak Identities

Chemicals as reported have been confirmed routinely on two columns
(1.5" OV-17/1.95% QF-1 and 6% QF-1), and by thin layer chromatography
(silica gel).  For certain chemicals and extracts, 2% SE-30 or 3% DECS
columns have also been used for confirmation.  (Table II-2, Appendix II).

TRACE ORGANICS IN WATERS

With the exception of diethylhexylphthalate (DEHP), chemicals reported for
incoming wastewaters in this study are pesticides or isomers or metabolites
of pesticides.  Identification of sources was beyond the scope of the in-
vestigation.  However, some consideration of probable sources and modes of
entry for trace organics into wastewater flows at Muskegon and Whitehall
will be helpful in evaluating the data.
                                    79

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Probable Sources and Modes of Entry

Sewage treated at Muskegon and Whitehall comes  from 14 municipalities, with
approximately 140,000 residents and 200 industries.  Most  of  it  (27 MGD  in
1975) goes into the Muskegon system.   Flows at  Whitehall are  about 1 MGD
(Muskegon County Dept. of Public Works, 1975; USEPA, Region V, 1976).

Sixty percent of the flows at Muskegon come from industry, with  the major
contributor a paper manufacturer.  A major contributor at  Whitehall is a
tannery.  Manufacturers of chemicals include several companies that produce
primary chemicals and intermediates, pesticides, plastics, resins, elasto-
mers.  Other industries that undoubtedly use organic chemicals of environ-
mental concern are manufacturers of foundry products, heavy machinery,
automotive engines, parts and accessories (Directory of Michigan Manufac-
turers, 1976).

Supporting these basic industries are warehousers and distributors serving
local, state, national and international trade  channels by rail  and truck,
as well as through the Port of Muskegon and the St. Lawrence  Seaway.   There
are also numerous operators involved in various aspects of industrial  waste
disposal:  waste haulers, waste takers and processors, barrel Tenderers, etc.

This complex of activities affords numerous opportunities  for point  source
contamination due to accidents, inappropriate handling or  storage, or  in-
adequately controlled disposal or discharge.

"Truth in pollution" legislation (Act 200, Mich. P.A.  1970, and  later  amend-
ments to Act 245, P.A. 1929) requires that industrial  and  commercial  pro-
ducers of wastewaters (other than sanitary sewage) file  annual reports with
the Michigan Water Resources Commission, listing critical  materials  and waste-
water outfalls.  A fee is assessed to cover costs of surveillance  by  the
Commission.

Types of outfall registered by industries in the Muskegon  and Whitehall areas
include discharges into surface waters  (directly or through storm sewers)  and
a variety of discharge methods that may lead ultimately  to groundwater  (la-
goons or seepage ponds with no outlet, septic tanks and  tile fields,  overland
flow).  Large quantities of noxious liquid wastes and recoverable by-products
are  transported by licensed waste haulers to independent  industrial  waste
processors operating locally, elsewhere in Michigan, or  out of state.    Sludges
that accumulate in lagoons and seepage ponds have in the past leen inciner-
ated y buried in landfills, or abandoned in favor of new discharge sites.

Since the two county treatment systems became operational, state and local
authorities have encouraged the diversion of compatible wastewaters  from
industry into sanitary sewers connected to the  county systems.  The major
contributor to flows at the Muskegon site  (the  paper mill) initiated diver-
sion in June 1973.  The tannery at Whitehall connected up  in late 1974.
The  number of connected discharges has  increased over the  period of this
study.  Diversions of 50  to 80% or more were registered by a number of
companies in 1975.  However, numerous  industries and a number of smaller
municipalities were either not connected or had diverted  less than 50%  of

                                     80

-------
their wastewater into either system through 1975 (Michigan Water Resources
Commission, Surveillance Fee Listings,  1973, 1974,  1975).

Increasing numbers and diversity of source discharges may have contributed
to changes in spectrum of trace organics encountered in this study.   It is
likely that wastewaters will become increasingly complex and variable in
composition as more of the existing discharges from industry and from sub-
urban residential and commercial areas are connected to the system and as
new industries, attracted by the county's wastewater treatment capabilities,
move into the area.

A wide range of chemicals is used or produced in large volume.  The bulk of
these are identified in critical materials registrations only by broad cate-
gories (chlorinated benzenes, nitrobenzenes, aromatic amines, etc.).  The
probable range of organic species which may appear in wastewaters is aug-
mented by unknown or unlisted by-products of manufacturing or of pretreat-
ment before discharge.  Discharges can vary widely from time to time with
production schedules chat may involve a succession of weekly campaigns for
production of two or more intermediates leading to a major product.   Waste-
waters from paper manufacturing are extremely complex and vary with pulping
method, pulp species, and with treatment given to palping effluents before
discharge (Hrutfiord et al., 1975).

Numerous instances of contamination of surface and groundwaters associated
with chemical industries in the Muskegon and Whitehall areas have occurred
(Muskegon Chronicle, December 12, 1975; Detroit Free Press, December 29, 1976
and April 12, 1977).  The Michigan Water Resources Commission has determined
that contaminated groundwaters shall be purged by pumping into the county
wastewater treatment systems.  It is unlikely that much of this was done
during the period of this study, however.

At the present state of the art, both dischargers and control agencies are
handicapped by uncertainties regarding parameters which should be monitored
and by analytical difficulties in resolving complex mixtures and positively
identifying individual organic species.

The lack of positive identification by other than chromatographic parameters
seriously limits the credibility of chemical assignments given in this report.
Phthalates are listed as critical materials by a number of companies, sup-
porting the identification here of DEHP.  Of the pesticides, only phorate
(ThimetR) is known to have been produced in the Muskegon area where it was
identified frequently in wastewaters in 1975.  However, it appears that major
production may not have been undertaken until early 1976.

Circumstantial support for several pesticides is to be found in known pat-
terns of use and in known sales for "restricted use" pesticides which must
be reported by licensed dealars (Michigan Department of Agriculture, Regula-
tion No. 633, 1972).  There is good reeson to expect that pesticides in
current use or persistent residues frot. past use will enter wastewater flows,
directly or indirectly, from hydrologic systems that converge in the
Muskegon and Whitehall areas.
                                    81

-------
Major industrial dischargers in the Muskegon area take their feedwaters from
Muskegon Lake, Mona Lake or streams that flow into them,  or from contiguous
groundwaters.  Sixty percent of the annual wastewater flow at the Muskegon
treatment site comes from the paper mill, which takes essentially all of its
processing water from Muskegon Lake.  Contaminants in Muskegon Lake may well
appear at the treatment site at levels reduced by less than fifty percent.
Much greater dilution would be expected for contaminants from Mona Lake or
other lesser sources of feedwater.

Pesticides and other pollutants in these lakes can originate locally in
storm flows from residential, commercial and industrial areas.  Chronic con-
tamination of surface and groundwaters by discharges from chemical industries
has occurred along streams entering both lakes.  Both receive drainage from
watersheds extending northeasterly, hence normally downwind.  Thus, airborne
pollutants generated locally can be intercepted and returned.  Vegetables,
mainly celery, are grown in drained lowlands just east of both lakes.  Flood-
waters of the Muskegon River occasionally wash across the diked fields near
its mouth.

Water and sediments entering Muskegon and Mona Lakes can also carry contam-
inants from point and non-point sources scattered widely over extensive river
basin areas.  The Muskegon River basin is one of the largest in Michigan
(2660 nn/, or 6890 knr).  Fifty percent of the area is forested and includes
a large proportion in recreational areas and concentrated resort development;
25% is in agriculture, including important areas of cash crop and intensive
vegetable production.  Over 20 industries and 9 municipalities use the sur-
face waters of the river for wastewater assimilation  (Great Lakes Basin Com-
mission, 1976; Wright, 1974; see also National Cooperative Soil Surveys for
Counties of Muskegon, Newaygo, Mecosta and Osceola).

The Black Creek watershed lies almost entirely in lluskegon County.  There
are areas of agricultural production in the eastern half of the basin  in-
cluding vegetables and cash crops on organic soils just east of the waste-
water irrigation site.  A large chemical plant is located in a thinly  popu-
lated marginal area along the middle reaches of the stream.  The lower half
of the basin becomes increasingly urbanized on approach to Mona Lake,  but
there are scattered farms, including areas near the lake, that are managed
intensively  for celery and other vegetables.

A number of  pesticides implicated in this study were  currently and widely
used for insect control in agriculture and forestry and for landscaping and
other uses in urban, suburban, resort and recreational areas.  These,  and
persistent chemicals like DDT and endrin that were  used extensively prior
to the 1970's, can appear in substantial concentrations in  streams during
periods of heightened or turbulent  flow resulting from runoff and  erosion
 (Miles, 1976; Snow, 1977; Truhlar and Reed, 1976).

Soluble materials and pesticide-enriched fine  sediments carried by streams
can be widely dispersed in receiving lakes.  Heavier  bottom wash sediments
are also enriched with pesticide residues.  Deposition of sediments  in flood-
ing lowlands a^d in quiescent waters near the mouths  of streams  is a concen-
trating mechanism.  The presence of such deposits increases  the probability

                                    82

-------
that persistent chemicals will be found in associated surface waters
(Glooschenko, 1976).   Flooding lowlands are often important groundwater
recharge areas.  Deposition of enriched sediments in these areas also in-
creases the potential for contamination of groundwaters (Garrett et al.,
1976).

Thus, there is good reason to expect that pesticides and other contaminants
from basin-wide sources will appear in feedwaters used by industry.  At times
the concentrations may be substantial, and little change will occur between
points of intake and discharge where water is used for cooling or for large
volume processes compatible with low-grade water.  This would be the primary
mode of entry into flows received at the treatment site.  System failures
can occur, as when a malfunctioning sluice gate allowed high waters in
Muskegon Lake to flow directly into municipal sewerage for periods during
this study.  Flows measured in the system indicate that infiltration of sew-
ers occurs also in low-lying areas during periods when the watertable is high
and that there are places in the system where storm sewers and sanitary sew-
ers are still interconnected.  Unusual flows associated with storm events
or high water are, however, small when compared to base flow or to industrial
flows that are known to originate in feedwaters taken from lakes or streams.

Some of the circumstances described above for the Muskegon system undoubtedly
exist also at Whitehall.  Celery is grown in lowlands near the mouth of White
River and along its lower tributaries in Muskegon County.  The basin includes
important areas of vegetable production and general farming in Oceana and
Newaygo Counties (Wright, 1974; also see National Cooperative Soil Surveys
for these counties).   Some of the fruit areas in Oceana County drain to White
River.  There are scattered resort developments and recreational areas in
the basin and several small communities along the river.

The White River discharges into White Lake which opens on Lake Michigan.
White Lake also receives discharges and storm flows from a concentration of
industry around the lake as well as runoff from residential, commercial and
resort areas.  Well over 90% of the wastewater volume registered in 1975 for
industrial outfalls in the Whitehall-Montague area was surface discharged
and came mainly from a basic producer of chlorinated hydrocarbons.  The plant
is not connected to the Whitehall wastewater system; however, chemicals dis-
charged to the lake or airborne and intercepted on downwind landscapes might
well appear in feedwaters of other industries which do discharge into the
Whitehall system.

To monitor the full range of chemicals known or suspected of being input at
either the Muskegon or Whitehall treatment sites is beyond available funding
and probably beyond presently available methodology.  Analytical difficulties
are complicated further by the likelihood that individual source chemicals
are variously altered in diverse environments along pathways of local and
regional circulation before coming together at the treatment sites.  Fluc-
tuations in volume and composition of flows from individual point or non-
point sources make sampling to estimate loadings at a confluence point dif-
ficult if not impossible (Lake Michigan Interstate Pesticides Committee,
1972).
                                    83

-------
Only electron capturing species were monitored in this study.   Electron cap-
ture was used for detection and quantitation because of its sensitivity for
a number of chlorinated hydrocarbons that are known to be widely distributed
and most likely encountered.  DDT, dieldrin and PCB's are of particular con-
cern in the Great Lakes Basin because of their known impact on fish and
waterfowl and their persistence in soils and sediments (International Joint
Commission, 1976; Schacht, 1972).  These and other refractory organics can
be useful for tracing pathways of circulation through the environment (Arthur
et al., 1977; Miles, 1976; Roan, 1975; Snow, 1977).  Abroad spectrum of
organics which might be expected from industry would not have been detected
(Garrett et al., 1976).

Chemicals reported here were identified by chromatographic methods and con-
firmed on three or more media.  Nevertheless, identities are presumptive
rather than specific.  The chromatographic parameters  (Appendix II) are re-
producible.  The methods used and the data themselves are compatible with
a large volume of data accessible in STOR.ET  (Merkle and Bovey, 1974) and with
historical documentation categorized by geographical location, water types,
sources, etc. in such compilations of available data as DAM (Hall et al.,
1976) and Water DROP (Shackleford and Keith, 1976).

Raw Influent and Discharges in^o Storage

Because of the large number of probable sources and fluctuating flows from
each, the composition of incoming wastewater can vary  greatly over short
periods of time.  Chemicals entering sporadically may not be detected in
grab samples taken at a given station.  Some GLC peaks which were not found
in raw influent did appear during the same compositing period in discharges
into storage lagoons.  Peaks for most chemicals did not decline in frequency
or indicated range of concentration during aeration and settling.  For these
reasons, data for raw influent and for discharges into storage are best con-
sidered together for purposes of characterizing incoming wastewaters.  Data
for monthly composites are given in Tables 39 to 43.   Frequencies and
ranges of occurrence are summarized for 1974 and 1975  in Tables 47 and 48.

Industrial organics —

Diethylhexylphthalate  (DEHP) was the only industrial  organic  identified in
this study.  Phthalates, as a class, have appeared on  lists of critical
materials from local industries.  DEHP was found frequently at Muskegon at
concentrations of 10^ to 10^ ng/1 (Tables 39 to 42).   An important source
would have been from manufacture of paper products.   It appeared at Whitehall
in late 1974 at about the  time  the  leather company reported its hook-up to
the system  (Table 43).

Numerous unknown peaks were not monitored.   Beginning in August 1975,  three
unknown peaks that were frequently  observed  and often prominent were  inte-
grated, and their percentage contribution to total integrated peak area was
recorded.  These were at 115-118 sec, 164-168 sec  and  247  to  253 sec  on
1.5% OV-17/1.95% QF-1  (Rt  ratios  relative to aldrin  = 0.9,  1.27 and 1.92).
The first two peaks were not close  co any major peak for any  of the common
Arochlors examined  (1242,  1248,  1254, 1260).  The  third  corresponded  closely

                                     84

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                                                  Table 39.  TRACE ORGANICS IN RAW INFLUENT, MUSKEGON, DECEMBER 1973 TO DECEMBER 1974.$
00
Ol

Month


Dec
Dec- Jan
Feb
Mar
Mar
Apr
May
May
Jun- Jul
Jul
Aug
Sep
Oct
Nov
Dec- Jan
Detected
Compositing Period

(twice daily
grab samples)
12-1-73 to 12-21-73
l?-22-73 to 1-21-74
2-1 to 2-27-74
2-28 to 3-19-74
3-20 to 4-4-74
4-8 to 4-30-74
5-1 to 5-14-74
5-15 to 5-31-74
6-1 to 7-11-74
7-12 to 7-31-74
7-31 to 8-29-74
8-30 to 9-30-74
10-1 to 10-29-74
10-30 to 12-1-74
12-2-74 to 1-10-74
means (ng/l)

'"r
i

nd*
nd
nd
nd
nd
324
35
nd
nd
nd
nd
nd
nd
nd
nd
180

I
1
fi-

nd
nd
nd
nd
nd
nd
lot
nd
nd
nd
nd
nd
nd
nd
nd
10
a:
CD
*o
rt
1
O

nd
nd
nd
nd
nd
123
363
464
nd
22
nd
nd
nd
nd
nd
243
1
n it
•o fa
o n
X cr
E o*
it 1

nd
nd
nd
nd
nd
106
2 t
nd
nd
7
nd
nd
nd
3t
nd
30
M
o"cL
an
0
!H

nd
nd
nd
nd
nd
225
nd
270
nd
lot
nd
nd
nd
nd
nd
168

p
i
W
o

nd
nd
nd
nd
nd
nd
193
nd
nd
340
nd
nd
nd
nd
nd
266

H*
g.
i

- ng/l -
89
140
nd
nd
nd
nd
323
57
79
97
268
100
6
nd
5t
116

N
§

nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
404
nd
nd
404

n
»
rt
III

nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
6.3xl03
6.3xl03
Is)
f
O
§

nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
l.JxlO3
nd
nd
nd
nd
1.2xl03

•<
O OQ
n n

nd
nd
nd
nd
nd
323
nd
nd
nd
nd
nd
nd
nd
nd
nd
323

Q


75xl03
109x10 ~
63x10
20xl03
91xl03
358x10 3
650xl03
172xl03
21xl03
36xl03
nd
nd
199xl03
175xl03
nd
164x10 3
              *nd  - not detected
              tBelow usual range  of  confident quantitation (Appendix II, Table 2).


             *GLC  peaks for all  chemicals listed in Table 2, Appendix II, were monitored.   Only chemicals detected and confirmed
              on  two or more GC 
-------
                                                          Table 40.   TRACE ORGANICS IN RAW INFLUENT, MUSKEGON,  JAN TO DEC 1975.1
oo


Monti


Jan
Feb
Mar
Apr
May
Jun
Jul
Aug
Sep
Oct
Nov
Dec
Detected

Compositing
period
(twice daily
grab samples)
1-6 to 1-31-75
2-4 to 2-28-75
3-4 to 3-31-75
4-1 to 4-30-75
5-2 to 6-2-75
6-2 to 7-2-75
7-2 to 7-30-75
8-2 to 9-2-75
9-2 to 10-2-75
10-2 to 11-4-75
11-4 to 11-28-75
12-2-75 to 1-2-76
means (ng/1)

It
$


nd*
4t
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
4
a
H1
(X
H-
a


nd
nd
nd
nd
nd
nd
nd
tr**t
nd
nd
nd
nd
tr
fo
fa
I
s


28
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
28
ff
•0
rt
cr
o
hi


nd
nd
nd
nd
nd
nd
8
nd
nd
nd
90
nd
49
8?
•a
•a ID
86-
O. 0
rt n


nd
194
nd
nd
nd
nd
nd
nd
nd
nd
21
nd
108

f
OS
o


nd
nd
nd
nd
nd
34
nd
nd
nd
517
96
nd
216
P
8.
g


31
374
nd
nd
102
20
30
611
20
815
575
83
266
a
N
g-
g


nd
nd
nd
nd
nd
nd
nd
3.5xl03
nd
nd
nd
nd 3.
l.SxlO3 1
o
r
rt
cr
o
i?


347
nd
nd
nd
nd
nd
nd
nd
nd
nd
833
2x103

fT
O
rt
ft
IB


- - ng/1
rid
3.5xl03
nd
nd
2.X103
32.xlOJ
nd
9,xlQ3
6.6x103 9
7. 5x10 3
88.X103
nd
' 21.X1Q3

r
CD
O


nd
nd
nd
nd
nd
nd
nd 4
200 1
. 3x10 3
nd
nd
200 5.
3. 2x10 3
NJ
V
O
5


nd
nd
nd
nd
nd
nd
.xlO3
nd
nd
nd
SxlO3
3.5x10
V
a
W
M
M

nd
nd
nd
630
nd
nd
nd
nd
nd
nd
nd
nd
3 630
V
o
DJ
s
H

nd
nd
nd
nd
nd
nd
nd
nd
200
nd
nd
nd
200
**
a
M
•U
RJ
*^>

nd
nd
l.lxlO3
nd
nd
nd
nd
nd
nd
nd
nd
500
800


D
t§

2,6Mxl03
nd
nd
nd
677xl03
5 3x10 J
60x10 3
55xl03
nd
1,067x103
SOxlO3
193xl03
597x103
              *nd - not detected
              **tr = Trace
              tflelow usual range of continent quantitation (Appendix II,  Table 2).
               +GLC peaks for all chemicals listed in Table 2,  Appendix II,  were monitored.   Only chemicals  detected and confirmed on two or more
                GC columns are reported.   Confirmation by thin  layer was  required,  also,  except  at concentrations too low for spots to be
                visualized.

-------
                                                Table 41.  TRACE ORGANICS IN DISCHARGES INTO STORAGE LAGOONS, MUSKEGON, APRIL TO DEC. 1974.-)
co
Month



April
May
May
Jun-Jul
Jul
Aug
Sep
Oct
Nov.
Dec-Jan
Detected i
Compositing
period
(dally grab
samples)


4-8 to 4-30-74
5-1 to 5-14-74
5-15 to 5-31-74
6-1 to 7-11-74
7-12 to 7-31-74
7-31 to 8-29-74
8- 30 to 9-30-74
No sample
No sample
12-2-74 to 1-10-75
Deans (ng/1)
Dieldrin



nd*
nd
nd
nd
nd
16
nd
__
—
nd
16
	 F° 	
I
O
s



244
345
nd
nd
nd
nd
nd
	
	
nd
294
leptachlor



nd
199
nd
nd
37
nd
nd
	
	
nd
118
Heptahior
epoxlde



nd
nd
nd
nd
80
nd
nd
	
—
nd
80
L-hydroxy-
chlordene



341
nd
144
187
512
nd
25
— .—
	
255
244
p
k
n



nd
nd
18
51
40
nd
nd
	
—
nd
36
Llndane


- ng/1 - -
224
155
92
73
151
nd
nd
	 	
	
151
141
I



nd
nd
nd
nd
nd
nd
127
	 	
	
nd
127
parathion



nd
nd
nd
nd
nd
nd
38t
__
—
nd
38
Lasso
J.4-h..1



nd
nd
nd
nd
nd
nd
12.8x103
	
	
nd
12.8xl03
Vegadex



nd
nd
nd
nd
10
nd
nd
	
—
nd
10
o



419xl03
348x10^
269x10^
67xl03
60xl03
nd
1,233x103
	 . 	
— 	 	
nd
216xl03
                *nd  •  not  detected
                tBelow usual  range of confident qualification  (Appendix II, Table  2).
               +GLC peaks for all chemicals listed in Table 2, Appendix II, were monitored.  Only  chemicals detected  and  confirmed  on  two
                or more GC columns aire reported.   Confirmation by thin layer was required, also, except at concentrations too low for spots
                to be visualized.

-------
                                                 Table 42.  TRACE ORGANICS IN DISCHARGES  INTO STORAGE  LAGOONS,  MUSKEGON,  JAN.  TO DEC.  1975.
00
00
MoTif-h


Jan
Feb
Mar
Apr
May
Jun
Jul
Aug
Sep
Oct
Nov
Dec
Detected
Compositing
period
(daily grab
sauries)
1-6 to 1-31-75
2-4 to 2-28-75
3-4 to 3-31-75
4-1 to 4-30-75
5-2 to 6-2-75
6-2 to 7-2-75
7-2 to 7-30-75
8-2 to 9-2-75
9-2 to 10-2-75
10-2 to 11-4-75
11-4 to 11-28-75
12-2-75 to 1-2-76
means (ng/1)
Aldrln


nd
nd
26
nd
nd
nd
ml
nd
nd
nd
hd
nd
26
Endrin


35
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
35
lo
I
o


nd
nd
nd
nd
nd
nd
ud
tr**t
nd
nd
nd
nd
tr
1°
S
w


nd
nd
3t
11
nd
nd
nd
nd
nd
nd
nd
nd
7
i


nd
nd
nd
nd
nd
nd
nd
nd
18
nd
nd
nd
18
Heptachlor


nd
nd
nd
nd
nd
nd
nd
nd
nd
955
nd
7
481
Heptachler
epoxide


nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
18
18
l-tiydroxy-
chlordene


nd
nd
nd
nd
nd
nd
nd
nd
7t
nd
2t
2t
4
B
1


nd
nd
nd
nd
nd
nd
nd
nd
nd
nd

nd
98
p.


56
111
9
nd
tr
3t
nd
84
58
729
463
168
168
Diazinon


- ng/i - - -
3. 8x10 3
nd
nd
910
nd
nd
561
nd
nd
nd
nd
nd 1.
1.6xl03
Dlmethoate


290
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
,7xl03
995
Fhorate


nd
nd
nd
nd
nd
nd
nd
3. 3x10 3
nd
nd
31.X103
2.4xl03
12.xlO<
t*
0


nd
nd
nd
nd
260
nd
2.xl03
1.4xl03
lot
nd
1.3xl03
nd
994
2,4-D(IPE)


nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
1.6xl03
nd
1.6xl03
0


332. 103
289xlOJ
nd
106xl03
nd
nd
nd
183xl03
167xl03
350xl03
2,017xHT
142xl03
448. xlO3
               *nd ™ not detected
               i*tr _ Trace
               '''Below usual range of confident quantitation (Appendix II,  Table 2).
               tGLC peaks for  all chemicals listed in Table 2,  Appendix II,  «ere monitored.  Only chemicals detected ar.d confirmed on two or
               more  GC  columns  are  reported.   Confirmation by  thin layer was  required,  also,  except  at concentrations too low for spots to
               be visualized.

-------
                                        Table 43.  TRACE ORGANICS IN RAW INFLUENT AND IN DISCHARGE INTO STORAGE, WHITEHALL, APR. TO DEC. 1975. j
00

Month




Compositing
Period
(Random grab
samples)

>
3.
0



1-
1
§
o


ff
S*
ai
a. M
It 0
*


V
&«
82
s-s
§ '


R
1
3
o



C
P
8-
g



RAW INFLUENT
Apr
May
Jun
Jul
Aug
Sep
Oct
Nov
Dec
DISCHARGE
Apr
May
Jun
Jul
Aug
Sep
Oct
Nov
Dec
4-1 to 4-30-75
5-2 to 6-2-75
6-2 to 7-2-75
7-2 to 7-30-75
No sample
9-2 to 10-2-75
No sample
11-4 to 11-28-75
No sample
INTO STORAGE
4-1 to 4-30-75
5-2 to 6-2-75
6-2 to 7-2-75
7-2 to 7-30-75
No sample
9-2 to 10-2-75
No sample
11-4 to 11-28-75
No sample
nd*
nd
nd
nd
	
8
	
nd
—

nd
nd
10
nd
	
nd
	
nd

nd
nd
nd
nd
	
nd
	
nd
	

404
nd
nd
nd
	
nd
. 	
nd

9
nd
nd
nd
	
nd
	
nd
	

26
nd
nd
nd
	
nd
	
nd

nd
nd
nd
nd
	
nd
	
nd
	

nd
3t
nd
nd
	
nd
„. 	
nd

nd
nd
nd
nd
	
nd
	
nd
	

404
nd
nd
nd
	
nd
	
nd

nd
22
51
14
	
97
	
113
	

nd
3t
47
25
	
137
	
nd

0
3-
Q
ft
n



770
nd
nd
nd
	
nd
	
nd
	

2.5xl03
nd
nd
nd
	
nd
	
nd

F
M
o




nd
nd
nd
nd
	
nd
	
nd
	

nd
312
nd
nd
	
nd
	
nd

Kl
V
O
§




nd
lid
nd
nd
	
nd
	
300
	

nd
nd
nd
nd
	
nd
	 .
4.2xl03

M
V
a
w
w
M
M


nd
nd
9t
nd
	
nd
	
nd
—

nd
nd
nd
ltd
	
nd
	
nd

M
V
a
/-*
M
•a
•2



S.xlO3
nd
nd
962
	
nd
	
500
	

1.4xl03
nd
nd
nd
	
210
	
6.X103

a
n




nd
nd
nd
nd
	
nd
	
nd
	

nd
nd
nd
nd
	
2.xlo3t
	
5.xl03t

B ns
n «
ptachlo
tabollt
2"



9
nd
nd
nd
	
nd
	
nd
	

26
3t
nd
nd
	
nd
	
nd

M. P
a> -a ft
1*1




nd
22
51
14
	
97
	
113
—

404
It
nd
25
	
137
	
nd

              *nd - not detected
              tflelow usual range  of confident  quantitation  (Appendix  II, Table  2).

             *GLC  peaks for all chemicals listed in Table 2, Appendix II,  were monitored.  Only chemicals detected and confirmed on two or more
              GC columns are reported.   Confirmation by thin layer was required,  also,  except at concentrations too low for spots
              to be visualized.

-------
                                      Table 44.  TRACE ORGANICS IN PRE-CHLORINATION FLOWS AND IRRIGATION WATER, MUSKEGON, JUNE 1974 TO DEC. 1974.
VO
O
Month

Compositing
period
(Random
grab samples)

Frechlorination flows (out of storage
Jun-Jul
Jul
Aug
Oct
Nov
Dec
Irrigation
Jul #1
#2
Aug #1
#2
Sep #1
Oct
Nov #1
n
Dec
6-1 to 7-11-74
7-12 to 7-31-74
7-31 to 8-29-74
10-1 to 10-29-74
10-30 to 12-1-74
No sample
waters (pumps fl and #2)
7-12 to 7-31-74
7-12 to 7-31-74
8-12 to 8-31-74
8-12 to 8-31-74
9-12 to 9-31-74
No sample


No sample
Detected means (ng/1)
Dleldrin


lagoons)
nd*
nd
nd
nd
nd
	

nd
nd
nd
nd
146
— —
nd
nd

146
ha.
i
g
in



3t
3t
nd
nd
nd
	

nd
nd
nd
nd
nd
- ...
nd
nd

3
1-hydroxy-
chlordene



57
nd
nd
62
nd
	

nd
nd
nd
nd
nd
__
nd
nd

60
P
8



nd
nd
nd
nd
nd
	 	

nd
nd
nd
nd
nd
	 	
43
143

69
P



nd
nd
nd
nd
133
- —

nd
nd
nd
nd
nd
-_.
nd
nd

133
Lindane
.


36
nd
95
32
nd
— —

371
nd
nd
nd
nd
—
41
42

93
o



315
nd
nd
nd
nd
	

nd
nd
nd
nd
nd
—
nd
rd

315
1



19xl03
nd
nd
nd
nd
	

112xl03
5 3x10 3
nd
nd
32xl03
	
nd
nd
_
54xl03
S
ui rt
•g&
Ho
a a
in H



3
3
nd
nd
nd
	

nd
nd
nd
nd
nd
—
nd
nd

3
                *nd ~ not detected
                t Below usual range of confident  quarvtitation  (Appendix  II,  Table  2).

                tGLC ; eaks for  all chemicals listed in Table  2,  Appendix II, were monitored.  Only chemicals detected and  confirmed
                 on two or more GC columns are reported.  Confirmation by thin layer was required, also, except at concentrations too low
                 for spots to be visualized.

-------
                                         Table  45.   TRACE  ORGANICS IN  NORTH OUTFALL WATERS (SW-05,  MOSQUITO CREEK),  MUSKEGON; APR 74 TO DEC 75.
VO
Month


Apr
May
May
Jun-Jul
Jul
Aug
Sep
Oct
Nov.
Dec-Jan
Jen
Feb
Mar
Apr
May
Jun
Jul
Aug
Sep
Oct
Nov
Dec
Detected
Compositing
period
(daily grab
samples)


4-8 to 4-30-74
5-1 to 5-14-74
5-15 to 5-31-74
6-1 to 7-11-74
7-12 to 7-31-74
7-31 to 8-29-74
8-30 to 9-30-74
10-1 to 10-29-74
10-30 to 12-1-74
12-2-74 to 1-6-75
1-6 to 1-31-75
2-4 to 2-28-75
3-4 to 3-31-75
4-1 to 4-30-75
5-2 to 6-2-75
6-2 to 7-2-75
7-2 to 7-30-75
8-2 to 9-3-75
9-2 to 10-2-75
10-2 to 11-4-75
11-4 to 11-28-75
12-2-75 to 1-2-76
means (ng/1)
Aldrin


nd*
nd
nd
14
nd
nd
nd
. nd
nd
nd
nd
ud
nd
nd
4t
nd
nd
nd
nd
nd
nd
nd
9
a
H.
H*
o


nd
nd
nd
nd
31
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
31
h>
i
o
s


7t
8t
8t
6t
6t
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
7
Heptachlor


nd
nd
nd
5t
47
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
5t
nd
nd
19
Heptachlor
epoxide


nd
nd
nd
ncl
25
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
It
nd
13
1-hydroxy
chlordene


nd
nd
nd
nd
145
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
145
e
S
O


nd
nd
25
nd
53
nd
nd
nd
112
lit
nd
4t
19
nd
nd
nd
nd
lh
nd
nd
nd
nd
37
T
£
o


nd
nd
nd
nd
nd
nd
nd
46
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
46
(0


nd
nd
nd
11
37
nd
nd
84
375
nd
5t
2t
178
150
nd
nd
nd
It
nd
2t
nd
nd
84
Diazlnon


nd
nd
nd
nd
nd
nd
48t
521
483
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
334
Atrazine


nd
nd
nd
nd
nd
nd -
292xlOJ
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
292xl03
1
o


298
119t
183
415
625
nd
nd
loot
nd
350
nd
nd
nd
nd
359
33t
Ifft
nd
nd
nd
nd
25t
226
2,4-D(BE)Il


nd
nd
nd
nd
203
nd
nd
nd
nd
nd
nd
nd
nd
650
195
nd
nd
nd
nd
nd
nd
nd
349
Vegadex


nd
nd
nd
32
136
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
84
I


nd
r.d
15x10
lOxlO3
3xl03t
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
115xl03
nd
nd
10xlOJ
31.xl03
              *nd - not detected
              tBelow usual range of confident  quantitation  (Appendix  II, Table 2).
             +GLC  peaks  for all chemicals listed in Table 2, Appendix II, were monitored.  Only chemicals detected and  confirmed on  two
               or :uore GC columns  are  reported,  Confirmation by  thin layer was  requirfd,  also,  except at concentrations too low for spots to
               be visualized.

-------
                            Table 46.   TRACE  ORGANECS  IN  SOUTH  OUTFALL WATERS  (SW-34,  BLACK CREEK),  MUSKEGON, APR 74 TO DEC 75. t


Month



Apr
May
May
Jun-Jul
Jul
Aug
Sap
Oct
Nov
Dec- Jan
Jan
Feb
Mar
Apr
May
Jun
Jul
Aug
Sep
Oct
Nov
Dec
Detected


Compositing
period
(dally grab
samples)

4-8 to 4-30-74
5-1 to 5-14-74
5-15 to 5-31-74
6-1 to 7-11-74
7-12 to 7-31-74
'/• il to 8-29-74
8-30 to 9-30-74
10-1 to 10-29-74
10-30 to 12-1-74
12-2-74 to 1-6-75
1-6 to 1-31-75
2-4 to 2-28-75
3-4 to 3-31-75
4-1 to 4-30-75
5-2 to 6-2-75
6-2 to 7-2-75
7-2 to 7-30-75
8-2 to 9-2-75
9-2 to 10-2-75
10-2 to 11-4-75
11-4 to 11-28-75
17-2-75 to 1-2-76
means (ng/1)
>
M
a.
*i
H>
a



nd*
nd
nd
22
39
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
30
h»

h>_
i
o
O
to


nd
nd
5t
2t
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
4
X
(0
•0
rt
I
M
o
n

nd
nd
It
9
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
5
«
IB
It V
•O rt
O f»
M n
H- =r
a. M
n o
H

nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
6
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
6
0
i
1



nd
nd
nd
nd
nd
nd
16
nd
nd
13
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
14
f
H.
8.
i



nd
nd
39
10
3t
42
12
8
2t
15
11
137
2t
nd
nd
nd
nd
It
nd
It
nd
nd
22
o»
i
8


- ng/l
nd
nd
nd
nd
nd
nd
7
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
7
a
H*
tu
N
|
8


nd
nd
nd
207 t
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
207
V
3-
o
2
rt
n



nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
63t
nd
nd
nd
nd
nd
nd
nd
nd
nd
63
f
o»
(n
CD
O



141
nd
nd
nd
nd
200
nd
100 1
nd
nd
nd
nd
nd
nd
7.xlO
nd
nd
nd
32t
nd
nd
nd
1.5x103
W

**
1
a
to
M
M

nd
nd
nd
69
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
69
ro

*>
1
o
^
H<
Ht

nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
217
217


ro
V
Q

T»
PI

nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
,,d
40 1
nd
nd
nd
nd
40


f
00
8.
5


nd
nd
nd
S
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
8


o



nd
nd
nd
2.8x10 t
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
40.X10
nd
21.X103
*nd » not detected
tbelow usual  range of confident quantitatiou (Appendix II, Table 2).
*GLC peaks for all chemicals listed in Table  2,  Appendix  II,  were monitored.   Only chemicals detected and confirmed on two
 or more GC columns are reported.   Confirmation  by  thin layer was required,  also,  except at concentrations too low for spots to
 be visualized.

-------
                           Table 45.
                                      TRACE ORGANICS IN NORTH OUTFALL WATERS  (SW-05, MOSQUITO CREEK), MUSKEGONj  APR 74  TO DEC 75.  J
Month


Apr
May
May
Jun-Jul
Jul
Aug
Sep
Oct
Nov.
Dec- Jan
Jsn
Feb
Mar
Apr
May
Jun
Jul
Aug
Sep
Oct
Nov
Dec
Detected
Compositing
period
(daily grab
samples)


4-8 to 4-30-74
5-1 to 5-14-74
5-15 to 5-31-74
6-1 to 7-11-74
7-12 to 7-31-74
7-31 to 8-29-74
8-30 to 9-30-74
10-1 to 10-29-74
10-30 to 12-1-74
12-2-74 to 1-6-75
1-6 to 1-31-75
2-4 to 2-28-75
3-4 to 3-31-75
4-1 to 4-30-75
5-2 to 6-2-75
6-2 to 7-2-75
7-2 to 7-30-75
8-2 to 9-3-75
9-2 to 10-2-75
10-2 to 11-4-75
11-4 to 11-28-75
12-2-75 to 1-2-76
means (ng/1)
Aldrin


nd*
nd
nd
14
nd
nd
nd
. nd
nd
nd
nd
ud
nd
nd
4t
nd
nd
nd
nd
nd
nd
nd
9
Dieldrin


nd
nd
nd
nd
31
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
31
i
g
W


7t
8t
8t
6t
6t
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
7
Heptachlor


nd
nd
nd
5t
47
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
5t
nd
nd
19
Heptachlor
epoxide


nd
nd
nd
nd
25
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
It
nd
13
an
p


nd
nd
nd
nd
145
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
145
S
0


nd
nd
25
nd
53
nd
nd
nd
112
lit
nd
4t
19
nd
nd
nd
nd
If
nd
nd
nd
nd
37
T
1


nd
nd
nd
nd
nd
nd
nd
46
nd
nd
nd '
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
46
Llndane


nd
nd
nd
11
37
nd
nd
84
375
nd
5t
2h
178
150
nd
nd
nd
It
nd
2t
nd
nd
84
Dlazlnon


nd
nd
nd
nd
nd
nd
48t
521
483
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
334
Atrazine


nd
nd
nd
nd
nd
nd
292xlOJ
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
292xl03
o


298
119t
183
415
625
nd
nd
lOOt
nd
350
nd
nd
nd
nd
359
33t
18t
nd
nd
nd
nd
25t
226
2,4-D(BE)d


nd
nd
nd
nd
203
nd
nd
nd
nd
nd
nd
nd
nd
650
195
nd
nd
nd
nd
nd
nd
nd
349
1
s-
K


nd
nd
nd
32
136
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
84
1


nd
r.d
15x10
lOxlO3
3x10 3t
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
115xl03
nd
nd
10x10
31.X103
 *nd  - not  detected
 tBelow  usual  range of confident quantttatlon (Appendix II, Table 2).
*GLC peaks for all chemicals listed  in Table  2, Appendix  II,  were monitored.   Only chemicals detected and confirmed on two
 or  .uore GC columns are reported,   Confirmation by thin layer was required, also, except at concentrations  too low for  spots to
 be visualized.

-------
                                         Table 46.  TRACE ORGANECS IN SOUTH OUTFALL WATERS  (SW-34, BLACK CREEK), MUSKEGON,  APR 74  TO DEC  75. t
VO
N3

Month

Apr
May
May
Jun-Jul
Jul
Aug
Sep
Oct
Nov
Dec- Jan
Jan
Feb
Mar
Apr
May
Jun
Jul
Aug
Sep
Oct
Nov
Dec
Detected

Compositing
period
(dally grab
samples)
4-8 to 4-30-74
5-1 to 5-14-74
5-15 to 5-31-74
6-1 to 7-11-74
7-12 to 7-31-74
?• ji to 8-29-74
8-30 to 9-30-74
10-1 to 10-29-74
10-30 to 12-1-74
12-2-74 to 1-6-75
1-6 to 1-31-75
2-4 to 2-28-75
3-4 to 3-31-75
4-1 to 4-30-75
5-2 to 6-2-75
6-2 to 7-2-75
7-2 to 7-30-75
8-2 to 9-2-75
9-2 to 10-2-75
10-2 to 11-4-75
11-4 to 11-28-75
17-2-75 to 1-2-76
means (ng/1)
>
M
a.
1
0

nd*
nd
nd
22
39
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
30
fo
fr.
1

nd
nd
5t
2t
nd
nd
nd
nd
ud
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
4
s
n
n
O
n
o
rt
nd
nd
It
9
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
5
ts
a> TJ
o v
as-
O. M
n o
n
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
6
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
6
0
i
8
o

nd
nd
nd
nd
nd
nd
16
nd
nd
13
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
14
f
H*
s.
1

nd
nd
39
10
3t
42
12
8
2t
15
11
137
2t
nd
nd
nd
nd
It
nd
It
nd
nd
22
o.
t
Qd
8

- ng/1
nd
nd
nd
nd
nd
nd
7
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
7
0
iazlnoo

nd
nd
nd
207 t
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
207
•0
horate

nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
63t
nd
nd
nd
nd
nd
nd
nd
nd
nd
63
r1
CO
CO
0

141
nd
nd
nd
nd
200
nd
100 1
nd
nd
nd
nd
nd
nd
7.xlO
nd
nd
nd
32t
nd
nd
nd
1.5xlfl3
NJ
,4-D(BE)
M
nd
nA
nd
69
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
69
to
O
I
K-5
H
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
217
217

V
o
3
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
ud
40 1
nd
nd
nd
nd
40

00

nd
nd
nd
8
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
8

I

nd
nd
nd
2.8xl
-------
                                             Table 47.  FREQUENCIES OF OCCURRENCE, TRACE ORCAN1CS IN WATERS, MUSKEGON, DEC 73 TO DEC 75.
VO
Chemical




Total samples
Aldrin
Dieldrln
Endrin
DDT species
Hepcachlor and/or metabolites
Lindane and/or isooers
Dlazinon
Dlmethoate
Parathion (methyl)
Phorate
Atrazine
2,4-D species
Lasso
Vegadex
DEHP
After aeration
Raw :
Dec 73
to
Dec 74
15
nd*
nd
1
2
5
10
1
nd
nd
1
nd
1
nd
1
12
sewage
Jan 75
to
Dec 75
12
1
1
nd
1
3
10
1
3
nd
7
nd
6
3
nd
8
and
Apr
to
Dec
8
nd
1
nd
2
7
7
nd
nd
1
nd
nd
nd
1
1
6
settling^
74 Jan 75
to
74 Dec 75
12
1
nd
1
4
4
10
3
2
nd
3
nd
1
5
nd
8
After
storage*
Jun 74
to
Dec 74
13
nd
1
nd
2
2
7
nd
nd
nd
nd
nd
nd
1
nd
4

Mosquito
Apr 74
to
Dec 74
10
1
1
nd
5
2
6
3
nd
nd
nd
1
1
7
2
3

Creek
Jan 25
to
Dec 75
12
1
nd
nd
nd
2
6
nd
nd
nd
nd
nd
2
4
nd
2

Black
Apr 74
to
Dec 74
10
2
nd
nd
2
2
8
1
nd
nd
nd
nd
i
3
nd
1

Creek
Jan 75
to
Dec 75
12
nd
nd
nd
nd
1
5
nd
nd
nd
1
nd
2
2
1
1
                                  ' Prechlorlnatlon flows  (  6  samples)  and Irrigation pump feed waters (7 samples).

                                  *nd - not detected.

                                  t Number of samples In which chemical was detected.
                                 tGLC peaks  for all  chemicals listed in Table  2,  Appendix II,  were monitored.   Only  chemicals detected and confirmed
                                  on  two or  more GC  columns are reported.  Confirmation by thin layer was  required,  also,  except  at  concentrations too low
                                  for spots  to be  visualized.

-------
                                        Table  48.   DETECTED RANGES OF CONCENTRATION, TRACE  ORGANTCS  IN  WATER.  MUSKEGON.  DEC 73 TO DEC 75. i
vO
Chemical
Aldrln
Dleld^ln
Endrln
DDT
Ueptachor &
metabolites
Lindane + isomers
Dlazinon
Dimethoate

min
max
mln
max
min
max
min
max
min
max
min
max
min
max
mln
max
Raw
Dec 73
to
Dec 74

nd*
nd
lot
35
324
3f
734
5t
516
404
nd
sewage
Jan 75
to
Dec 75

4t
trt
nd
28
8
194
20
1.3x10
l.SxlO3
347 ,
3. 2x10 J
After aerating
and settling
Apr 74
to
Dec 74

nd
16
nd
244
345
25
629
110
224
nd
nd
Jan 75
to
Dec 75

26
nd
35
tr
18
2t
955
tr
729
56^
2.8x10
290
1.7xlOJ
After
Storage"
Jun 74
to
Dec 74

nd
146
nd
3t
3t
57
62
32
371
nd
nd
Mosquito
Apr 74
to
Dec 74

14
31
nd
6t
Si
5t
217
11
487
48t
521
nd
Creek
Jan 75
to
Dec 75

4+
nd
nd
nd
It
5*
11
197
nd
nd
Black
Apr 74
to
Dec 74

22
39
nd
nd
2t
5*
it
9
2t
42
207f
nd
Creek
Jan 75
to
Dec 75

nd
nd
nd
nd
6
it
137
nd
nd
(continued)

-------
                                                             Table 48.   (continued)
Chemical
Parathion (methyl) min

Phorate mln
max
Atrazine min
max
2,4-D species mln
max
Lasso min
max
VO
*"" Vegadex min
max
DEHP min
max
Raw
Dec 73
Co
Dec 74
nd

6.3x103
nd
1.2xl03
nd

323
20.xl03
650.XNT
Sewage
Jan 75
to
Dec 75
nd

2.xl03
88.X103
nd
200
6.xl03
200
9,3xl03

nd
50. xlO3
2.6xlOb
After aerating
and settling

Apr 74 Jan 75
to to
Uec 74 Dec 75
38t

nd
nd
nd
12. 8x1 O3

10
68.X103
1.2xl06
nd

2.4xl03
31.xlOJ
nd
1.6xl03
lot
2.xlOJ

nd
106. XlO3
2.X106
After
Storage*
Jun 74
to
Dec 74
nd

nd
nd
nd
315

nd
19-xlO3
112xl03
Mosquito
Apr 74
to
Dec 74
nd

nd
292xl03
203
loot
625

32
136
3.xl03t
15.xlOJ
Creek
Jan 75
to
Dec 75
nd

nd
nd
195
650
18 1
359

nd
10. xlO3
115. xlO
Black Creek
Apr 74 Jan
to to
Dec 74 Dec
nd

nd
nd
69
loot
200 7.

8t
2.8xl03f 40.
75
75
nd

63t
nd
40*
217
32!
xlOJ

nd
xlO3
ffPrechlorination flows (6 samples)  and Irrigation pump feed waters (7 samples).

*nd "not detected.

tGLC peaks for all chemicals listed in Table 2,  Appendix II,  vere monitored.   Only chemicals detected and confirmed on two
 or more CC  columns are  reported.   Confirmation  by  thin  layer was required, also,  except  at  concentrations too low for spots to
 be visualized.

tBelow usual range of confident quantitation (Appendix II,  Table 2).

-------
to a major peak in Arochlors 1254 and 1260.

The third peak (247-253 sec) appeared in the first (petroleum ether)  eluant
from Florisil, as did the reference Alachlors.   In 10 of 19 chromatograms
for the first Florisil eluant for aqueous and particulate phases of influent
and discharges to storage at Muskegon, it represented 20% or more of  the in-
tegrated peak area.  In 3 of 8 chromatograms for incoming wastewater  at
Whitehall, the area for this peak represented 50 to 90% of the total  for all
monitored peaks.

The other two peaks, when encountered, appeared in varying proportion in all
three Florisil eluants.  The peak at 115-118 sec appeared more frequently
at Muskegon than at Whitehall (peak area percentages greater than 20% in 8
of 57 chromatograms vs none greater than 20%, of 24 at Whitehall).  The peak
at 164-168 sec appeared mainly in the aqueous phase at Whitehall where it
was the principal peak in the second Florisil eluant (28 to 95% of total
area).  When encountered at Muskegon, it was a minor peak (less than 10% of
peak area in most cases) and was variously distributed between aqueous and
particulate phases and among the three Florisil eluants.

The unknown peaks varied independently of each other and independently of
peaks which might be assigned to major diagnostic PCB components of the
common Arochlors.  GC-MS scans of the first Florisil eluant for raw influent
samples taken in 1976 have shown no evidence for the degree of chlorination
required of PCB species in regions of prep chromatograms where they might
be expected.  Positive identification has been hampered by inadequate sample
size and the number of parent species encountered  (Pesticide Research Center,
Michigan State University).

Thus, it appears that PCB's were not present in the substantial concentra-
tions that might be inferred from these unknown peaks.  Nevertheless, low
concentrations may well have been present.  Individual PCB species would
have appeared at peak positions monitored for several pesticides which also
appear in the first Florisil eluant  (Table II-3, Appendix II). The probabil-
ity for confounding is augmented further by the array of other organics which
might have been expected from industry.

Persistent organochlorine insecticides —

Among the pesticides in Tables 39 to 43 are several organochlorine insecti-
cides that were widely used prior to the mid-sixties.  Persistent  residues
of aldrin, dieldrin, endrin, DDT, heptachlor and lindane were widely  distri-
buted in soils, waters and  sediments  (Edwards, 1973; Carey et al., 1976;
Crockett et al., 1974; Glooschenko et al., 1976; Lake Michigan  Interstate
Pesticides Commission, 1972; Schacht, 1974).  Manufacture and use  of  these
chemicals in  the U.S. and Canada have declined as  more degradable  insecticides
became available.  This has been reflected in declining  frequency  of  en-
counter with  these chemicals in  surface waters since 1966  (Lichtenberg  et
al., 1970).   Nevertheless,  dieldrin  and DDT, along with  PCB's,  are still con-
sidered to be the most widely distributed environmental  pollutants in the
Great Lakes Basin  (Joint International Commission, 1976).


                                     96

-------
During the present decade, persistent organochlorine residues retained in
soils and sediments continue to appear in streams during periods of
heightened or turbulent flow associated with runoff or erosion from agri-
cultural, residential or recreational areas (Miles, 1976; Miles and Harris,
1973; Snow, 1977; Truhlar and Reed, 1976).  Frequencies and ranges of con-
centration reported in these studies were similar to those reported here
for aldrin, dieldrin and endrin (Tables 47 and 48).  DDT species were en-
countered more frequently in the cited studies than here, and maximum con-
centrations in two of the studies were 50 to 100-fold greater (Snow, 1977;
Truhlar and Reed, 1976).  Heptachlor and lindane or related species were
encountered more frequently here than in the cited studies and at generally
higher concentrations.

There is no evidence that any of these insecticides were produced locally
during or immediately preceding the study period.  If the GLC peak identi-
fications given here are valid, the implicated compounds must have origi-
nated in areas of residual accumulation or current use.  Concentrations in
contributing runoff or stream flows would have had to be substantially
greater than these encountered at treatment sites.  Since more than 50% of
the flows at the Muskegon site come from the paper mill, periodic concentra-
tions in Muskegon Lake, double those in Tables 39 to 42, would suffice to
explain the data.  The cited stream load studies indicate that such concen-
trations are not unreasonable.

The only independent analyses found for direct comparison were for one samp-
ling station near the outlet channel from Muskegon Lake to Lake Michigan
(Station 610030, Comprehensive Studies Section, Environmental Services Divi-
sion, Michigan Department of Natural Resources).  These analyses are for
seven samplings  (36-hr collections) made at irregular intervals over the
period from March 1971 through July 1976.  All of the chlorinated hydrocarbon
pesticides of concern here were searched for, but none were detected except
for DDT species  (12 ng/1) in the March 1971 sampling.  Arochlors 1242, 1254
and 1260 were searched for, and 1254 was reported once at 37 ng/1  (1971).
Phthalates were searched for in 1974 and 1976, and DEHP was found at 2,000
to 3,000 ng/1 in the one sample taken in 1974 and in one of two taken in 1976.

These data are non-supportive but do not preclude the probability that sub-
stantial concentrations of pesticides from non-point sources will be found
from time to time in areas of the lake that receive direct discharges from
streams and metropolitan storm flows.  Concentrations associated with heavy
runoff, turbulent flow in streams, or turbulence in areas of sedimentation
within the lake itself, will be attenuated quickly by sedimentation (Edwards,
1973; Merkle and Bovey, 1974).  Further attenuation will occur by numerous
continuing processes:  volatilization, concentration in aquatic biota and
bottom sediments, biological and catalytic degradation, photochemical altera-
tion, and dilution by more normal stream flows of low concentration (Kaufman,
1974; Matsumura, 1973; Sanborn, 1974).

       Heptachlor, lindane and related species — When encountered here,
values for heptachlor and its metabolites (Heptachlor epoxide and 1-hydroxy-
chlordene) and for lindane and other BHC isomers were often higher than
reported over the period 1965 to 1969 in streams and surface waters of the

                                     97

-------
U.S. (Edwards, 1973) and much higher than most values reported over the
period 1969 to 1972 in streams entering Lake Michigan (Lake Michigan Inter-
state Pesticides Committee, 1972; Schacht, 1974).   Confounding with PCB's
or other industrial organics may well have occurred.   However, peaks for
lindane were well separated from significant peaks in chromatograms run con-
currently for Arochlors which might reasonably have been expected (1242,
1248, 1256, 1260).

Chronic inputs of heptachlor and lindane or technical BHC at point or non-
point sources would be required to sustain levels  indicated here.  Heptachlor
is converted rather quickly in soils to the epoxide or to 1-hydroxychlordene,
both of which are subject to further alteration and degradation.  Lindane
and other BHC isomers are degraded rapidly under anaerobic conditions.
Isomerization (conversion of one isomer to another) may also occur.  There
is evidence that B-BHC may accumulate as the most  persistent isomer in areas
where BHC has been used extensively (Kaufman, 1974; Matsumura, 1973).

Both heptachlor and BHC isomers are relatively volatile, and lindane is the
most soluble of the persistent organochlorine insecticides  (Biggar and Riggs,
1974; Edwards, 1973).  It would be expected that local concentrations asso-
ciated with current use would be diluted rather quickly by dispersion into
the general environment.  Nevertheless, insecticidal activity associated with
these compounds persists iu soils for periods of 2 to 3 years.  The compounds
themselves can be retained in soils and sediments for much longer periods
of time and can be found in streams receiving runoff from areas treated
several years earlier  (Hiltbold, 1974; Merkle and Bovey, 1974).

Concentrations of BHC  isomers 10-fold greater than reported here have been
observed in streams receiving heavy runoff from forest areas sprayed one and
two years earlier with BHC  (Jackson et al., 1974).  A concentration of  170
ng/1 had been found four years after an earlier spray treatment.

Both lindane and technical BHC are used for insect control  in Christmas  tree
plantations which occupy significant acreages in Muskegon County, in the
immediately adjacent counties in the Muskegon River basin  (Newaygo) and  the
White River basin  (Oceana), and  in Missaukee and Wexford Counties in the
uppe.: basin of the Muskegon River  (Manthy et al., 1973; Wallner, 1975).
Lindane and heptachlor are active  ingredients in proprietary products  that
are widely distributed for use by homeowners and landscape  services on  trees
and other ornamentals.  Important uses call for spray applications  in  spring
or  early summer or  in  the  fall,  although  applications may be made at any
time during the growing season.

In  1974, twice-normal  rainfall was reported each month  from April through
August at one or more  stations in  the immediate tri-county  area  (stations  at
Hart, Hesperia, Muskegon and Newaygo).  Rains through the balance of 1974
were less  than normal  at most stations  (NOAA, 1974).

The  coincidence of  high rainfall with the spring and  summer season  of  spray
application would  explain  the frequency and  level  of  encounters  with hepta-
chlor and metabolites  and  with lindane and  other BHC  isomers  at  Muskegon
during this period  (Tables 39 and  41).  Entry into wastewater  flows  could

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have occurred by runoff from areas of current use or residual accumulation
or directly through drift, accidents or inappropriate disposal.

Wintertime encounters in 1974 (Tables 39 and 41)  or in 1975 (Tables 40 and
42) could be expected from runoff due to a combination of snowmelt plus
rain which often occurs in this part of Michigan.

Spring rainfall in 1975 was less than normal until May when higher than nor-
mal precipitation was reported for stations in the upper basin of the
Muskegon River.  Rains were more general in June, with near twice-normal
totals in the immediate tri-county area.  Heavy rains over the entire region
in August resulted in totals 2- to 4-fold greater than normal at all stations
in the Muskegon River and White River basins (Cadillac, Lake City, Higgins
Lake, Houghton Lake, Big Rapids, Evart, Hesperia, Muskegon).  September and
October were dry, but rainfall 50 to 100% greater than normal was again re-
ported in November at most of these stations.

Encounters with lindane from May to September 1975 (Tables 40 and 42) could
have originated in areas of residual accumulation or current season's use.
Sharply increased concentrations in October and the appearance of a-BHC and
heptachlor suggest origin in drift, runoff or other direct inputs associated
with current fall spraying operations.  These unusually high concentrations
in October would have been associated also with reduced volume of stream flow
after several weeks of dry weather with consequent lesser dilution.  The
later appearance of heptachlor epoxide in November (Table 40) and December
(Table 42) suggests a period of exposure to soils and points to origin in
runoff from areas of earlier application.

The above relationships to probable uses and climatic conditions in river
basin areas support the identifications given here.  Quantities distributed
through wholesale or retail channels are not known since sales; of lindane,
BHC or of the proprietary products containing heptachlor are not reported.
Heptachlor is a restricted use pesticide.  As such, sales for agricultural
uses have been reported since 1972 by dealers licensed under Regulation 633
of the Michigan Department of Agriculture.  The reported sales have been
mainly for use on grains and forages and have not exceeded I metric ton
annually statewide.  Negligible quantities have been reported for counties
in the White River or Muskegon River basins  (annual summaries of restricted
use pesticide sales, 1972-1976, Plant Industry Division, Michigan Department
of Agriculture).

       Aldrin and dieldrin — Usage of aldrin and dieldrin declined during
the late sixties in Michigan, as elsewhere in the U.S.  However, sales in-
creased again when uses of DDT were banned in the state in 1969 and nation-
wide in 1972.  The following sales have been reported by licensed restricted
use pesticide dealers in Michigan:
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                                      Licensed  sales  (metric  tons)

                                      Aldrln           Dieldrin

            1972                       13.2                 5.3
            1973                       22.5                13.8
            1974                       24.9                11.0
            1975                        3.3                 2.0
            1976                         .07                .4

In 1974, 18 metric tons of aldrin (70% of the state total)  was  sold  in one
county in the upper Muskegon River basin. Of the dieldrin in 1974,  37% was
sold in 9 councies which lie wholly or in part  in the basins  of the  Muskegon
and White Rivers.  Rapidly diminishing quantities have moved  from stocks on
hand since U.S. registrations for both chemicals were cancelled in 1975.
Intended uses reported by dealers were for aldrin mainly  on grains and for-
ages and for dieldrin mainly on fruits and vegetables. Lesser uses  for both
compounds were for ornamentals, forest and Christmas trees, and "other uses."

These figures give only an approximate indication of actual use since these
river basins do not define a merchandising area.  Also it is  likely that
stockpiling occurred after the first rebuttable notice of cancellation was
announced in 1971.  Nevertheless, the reported sales indicate that signifi-
cant quantities were used in 1973 and 1974 and probably also  in 1975.

Aldrin was encountered in wastewaters only three times.  A questionable
detection at Muskegon in February 1975 (Table 40) is supported by its detec-
tion a month later in discharges to storage  (Table 42).  It was detected
only once at Whitehall, in September 1975 (Table 43).

Dieldrin was not encountered at Whitehall.  It was observed entering storage
lagoons at Muskegon in August 1974 (Table 41) and in irrigation water coming
out of storage a month later (Table 44).

The most probable sources for aldrin would have been in areas of current or
recent application since aldrin is converted quickly in soils to dieldrin.
Current or recent applications would likely  have been required, also, for
dieldrin to appear.  The probability that dieldrin could have originated in
persistent older residues is remote since it is usually found in soils  and
sediments at much lower concentrations than DDT  (Edwards, 1973; Carey et al.,
1976; Crockett et al., 1974; Roan, 1975).  Neither aldrin nor dieldrin was
found in the same monchly composites with DDT species or endrin.  The latter
compounds would have originated, almost necessarily, from applications  made
prior to 1972 and probably earlier.

The encounters with dieldrin in wastewaters came after unusually heavy
rainfall in the Muskegon River basin from April  through August 1974.  The
encounters with aldrin in 1975 were associated with unusual sales in  the
region  in 1974 and occurred during the late winter to early spring  runoff
period  in 1975 or after 2- to 4-fold greater than normal rainfall in August.

It is significant that the indicated levels of use did not result in  chronic
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appearance or high concentrations of aldrin or dieldrin in wastewaters.
The relation to sales reported in contributing river basin areas gives a
rough indication of the extent to which pesticides of low solubility and de-
signed primarily for soil application may appear at these treatment sites.
Reported sales in Michigan of aldrin and dieldrin during these last few years
before cancellation can provide a useful reference for evaluating the resid-
ual environmental impact of dieldrin in the Great Lakes Basin.

     DDT species and endrin — Negligible quantities of DDT or endrin were
sold in Michigan from 1972 to 1976 and none in the nine watershed counties
of the White River and Muskegon River basins where significant non-point
sources might exist (Clare, Mecosta, Missaukee, Muskegon, Newaygo, Oceana,
Osceola, Roscommon, Wexford).  Permissible uses remain for DDD (TDE) on
fruits and vegetables, but sales statewide were less than 2 metric tons in
1972 and 1973 and declined sharply to less than 200 kg in 1975 and 1976.
No sales of DDD were reported in the above listed counties.

It is unlikely that insecticides containing endrin or DDT species (other
than DDD) have been used in significant quantities during the present decade
in Michigan.  Prior to the mid-1960's, DDT was for two decades the most
widely used insecticide in agriculture and forestry as well as in urban and
recreational areas.  Combined sales of aldrin plus dieldrin had overtaken
sales of DDT in the U.S. by 1965 (Edwards, 1973).

The relative cumulative impact of usage prior to 1970 is reflected in soil
residues reported in synoptic surveys made in 1970 (Carey et al., 1976;
Crockett et al., 1973).  At 54 cropland sites in Michigan, DDT species and
dieldrin were encountered with equal frequency (7 of 54 sites), but the mean
concentration for total DDT species was 50-fold greater than for dieldrin
(530 vs_ 1C ng/g), and the maximum concentration was 100-fold greater  (25,590
vs 220 ng/g).  At 23 urban sites in Muskegon's metropolitan neighbor, Grand
Rapids, dieldrin was not detected in 1970, but DDT species were found at 19
sites in concentrations up to 6,660 ng/g, with a mean of 660 ng/g.

Most frequently encountered in 1970, and at highest concentrations, were
_p_,jDf-DDT and £,£T-DDE, but _p_,£T-DDD was also found as well as all c^,j3 iso-
mers.  Neither aldrin nor endrin was encountered in Michigan, but both were
found occasionally at agricultural sites elsewhere in the country.

DDT species continue to be the most frequently encountered chlorinated hydro-
carbons in soils.  Concentrations up to 20,000 ng/g have been reported in
national surveys as recently as 1974 (Roan, 1975).  Such high values are
unusual, but their continuing appearance in surveys is evidence that local-
ized high residue concentrations persist in areas of discontinued use.

All of the persistent chlorinated hydrocarbons have been reported in runoff,
sediments or stream flows associated with agricultural, urban and recreation-
al areas.  DDT species continue to be found with greatest frequency and at
much the highest concentration as recently as 1974 (Roan, 1975) and 1976
(Snow, 1977).  Concentrations reported for DDT species in streams during base
flow or normal runoff events are lower than reported here for wastewaters
(Miles, 1976; Miles and Harris, 1973; Minnesota Pollution Control Agency,

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1971).  Occasional concentrations 10- to 100-fold greater than reported here
have been reported for storm events when suspended sediments were high due
to erosion or turbulent stream flow (Snow, 1977;  Truhlar and Reed, 1976).

The parent DDT species tend to be protected against alteration in soils and
may be the dominant species in runoff from land surfaces.  Runoff and erosion
expose soil residues to a wide range of aerobic to anaerobic environments
in streams.  Both DDE (aerobic metabolite) and ODD (anaerobic metabolite)
tend to increase relative to DDT in bottom wash sediments over time and with
distance downstream from the source (Miles, 1976; Miles and Harris, 1973).
The ratios DDE:DDT:DDD will reflect the quality of water in a given stream
as well as stream geometry conducive to greater or lesser aeration or dis-
turbance of bottom sediments (Snow, 1977).

In the present study, _p_,£*-DDE was encountered at concentrations up to
345 ng/1 at Muskegon during April and May of 1974 (Tables 39 and 41).  Ear-
lier snow accumulations were greater than normal, and twice-normal precipi-
tation was reported for March, April and May at individual stations in the
immediate tri-county area.  The presence of DDE isomers was indicated twice
in 1975, once in association with spring runoff in April and again in Septem-
ber after 2- to 4-fold greater than normal rainfall in August (Table 42).

ODD was encountered only once—at Whitehall in April 1975 at 400 ng/1  (Table
43).  Again, the absence of peaks for other DDT species suggests origin in
suspended bottom sediments.  Since DDD is formed during anaerobic metabolism,
this would imply that bottom environments in the White River or its tribu-
taries are less well aerated than in the Muskegon River or in areas of sedi-
mentation in Muskegon Lake where disturbance can occur by wave action or by
heavy stream discharge.  It is possible also that DDD  (TDE) may have been
used recently on fruits or vegetables in the White River basin, although no
sales have been reported in the area since 1972.

Unaltered DDT was encountered only once—in January 1975 at Muskegon  (Table
40).  It may have been accompanied at this time by endrin which was indicated
in discharges to storage  (Table 42).  Both could have  originated  in runoff
due to snowmelt plus rain, perhaps from areas where unusual residue accumula-
tions had been exposed to erosion by a change in management as, for example,
new construction or subdivision development.

The identification here of peaks for endrin and DDT species in wastewaters
is  supported by their association with weather conditions conducive  to heavy
runoff, erosion and turbulent straam flow  in contributing watersheds.  The
most  probable mode of entry would be through wastewater  discharges from in-
dustries that take feedwaters from lakes or streams.   This would  imply that
concentrations in surface waters near points of  intake for  the paper  mill
at Muskegon may, at these  times, have been double  those  observed  at  the treat-
ment  site.  The cited literature indicates that  this is  not an unreasonable
expectation.  The proportional  contribution from the tannery  at Whitehall
is not known, but it is considered a major contributor since  it  connected
to  che system in late 1974.   In both systems, direct inputs from intercon-
nected storm flows or through sewerage  failures  in areas of flooding  may
have  occurred also.

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Less persistent pesticides —

A number of less persistent pesticides in current use were encountered in
incoming wastewaters at concentrations of 10^ to 10^ ng/1.  These included
2,4-D esters, phorate (ThimetR),  diazinon, dimethoate, LassoR and Vegadex8-
(CDEC).

     2,4-D esters — Ester formulations of 2,4-D are used for control of
broadleaved weeds in small grains, forage legumes, pastures, along fence-
rows, ditchbanks, highway rights-of-way, and appear in proprietary products
for use on turf.  Applications are normally made in spring or fall.  The
chemicals are degraded rather rapidly (1 to 5 weeks).  Encounters were con-
sistent with applications in spring or fall and with carryover from late
spring or early summer applications to periods of heavy runoff in August or
from late fall applications to periods of winter snowmelt or early spring
runoff (Tables 39 to 43).  Appearances in July, August, or September could
have come from summer applications for control of woody brush species along
ditchbanks, in which case the 2,4-D esters would likely have been accompanied
by 2,4,5-T.  Peaks for 2,4,5-T were not monitored.

The methyl ester was encountered most frequently at Muskegon (Tables 39 to
42).  The isopropyl ester was indicated most frequently at Whitehall (Table
43) but appeared at Muskegon only in 1975 (Tables 40 and 42).  Patterns of
merchandising and use might account for such variations in frequency for the
different esters, but actual sales or usage are not known.

     Phorate (Thimet ) — Peaks for phorate were first encountered at Muskegon
in December 1974, but were found in 7 of 12 influent composites in 1975
(Tables 39 and 40) and in three samples of discharge into storage  (Table 42).
Phorate was not encountered at Whitehall.

As a systemic insecticide, phorate has limited used on vegetable crops.  It
is used for control of corn rootworm, and there may have been a substantial
increase in 1975 due partly to cancellation of aldrin and partly to entry
into the area of the western corn rootworm with developed resistance to the
chlorinated hydrocarbons (Ruppel, 1975).

However, the uses of phorate involve placement in soil before or at planting
time or at the time of first cultivation.  Also, phorate is quickly degraded
in soil (persistence, about 2 weeks).  Parathion, which is only slightly less
persistent than phorate, was never detected in wastewaters, although it is
much more widely used for both soil and foliar applications (sales of para-
thion reported by restricted use pesticide dealers in 1974 and 1975 were
about 50 metric tons statewide).   Thus, the chronic appearance of phorate
through 1975 cannot be explained by usage.

Major production of phorate by a chemical company on Black Creek appears not
to have been undertaken until early 1976.  Whether pilot production may have
been undertaken earlier is not known.  Processing discharges from this plant
were not diverted to the county sewage collection system until May 1976.
The company did report two episodes of holding lagoon failure in April and
in August 1975 (Muskegon Chronicle, December 21, 1975).  These were


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associated with fish kills in Black Creek and Mona Lake.   Phorate was not
analyzed for in samples of discharges,  lagoon seepage or  fish taken during
this period by state water quality control personnel.

The knoxm circumstances are inconclusive.  If phorate had in fact been
present in these accidental discharges,  it could have entered wastewater
flows through industries that take their feedwaters from Black Creek or Mona
Lake.  The proportion of total flow originating in these  industries is not
known.  If it were as much as 1%, a 100-fold dilution might have been ex-
pected at the treatment site.  This would imply that chronic concentrations
of the order of 10^ to 10^ ng/1 were maintained in Black Creek and Mona Lake
for periods of months after each discharge.  Whether this is a reasonable
expectation is uncertain since the persistence of phorate in sediments or
subsurface seepage is not known.  Phorate itself is soluble to the extent
of 5 x 107 ng/1 (50 ppm).

Confounding of phorate and a-BHC may have occurred in quantitation on the
OV-17/QF-1 column.  However, these two  species are differentiated by RF
values and by color on thin layer chromatograms which were used for con-
firmation with all extracts (Appendix II).  Peaks for these compounds are
clearly separated on a DECS column which was used, in addition to routine
confirmation on QF-1, with several extracts where both phorate and a-BHC
were indicated.  The possibility remains that unknown industrial organics
may have interfered with these determinations.  These uncertainties empha-
size the need for back-up analytical capability for positive confirmation
of presumptive identifications based on chromatographic parameters.

     Diazinon — Diazinon has extensive uses involving soil and foliar ap-
plications on field crops and horticultural crops.  As in the case of
phorate, soil applications for control of corn rootworm increased sharply
about 1975.  Spray applications for control of the six-spotted leafhopper
(vector for aster yellows) for several vegetable crops must extend over
field margins and ditchbanks for effective control.  In muck soil areas
these applications are frequently made from the air, increasing the likeli-
hood for direct entry into surface waters.  Applications must be repeated
every 3 to 6 days.

In spite of extensive usage and the vulnerability of surface waters to  con-
tamination, diazinon was encountered infrequently in wastewaters at Muskegon
(Table 47) and was not detected at Whitehall  (Table  43).  Concentrations  in
the ppb range  (10-^ ng/1) were indicated  for raw influent in association with
unusually heavy rainfall in August 1975  (Table 40) and in discharges  into
storage in January 1975  (Table 42).  The wintertime  encounter is not  incon-
sistent with the accepted persistence for  this compound  (3 months  in  soil
under growing  season conditions).

     Dimethoate — Identification of peaks for dimethoate at Muskegon  (Tables
40 and 42) and at Whitehall  (Table 43) is  to be questioned,  since  the
reference chemicc.1 was not recovered from  Florisil  (Appendix II, Table II-3) .
There are reasons to expect  that it might  appear.  In addition  to  uses  in
production of  crops and ornamentals, dimethoate is used as a residual  insect-
icide around farm buildings, homes and commercial establishments.   It  is  the

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material most commonly used in the custom pest control industry for fly
control.  It is among the most soluble pesticides (2 to 3% in water).
Residues picked up in cleaning water would likely be dumped directly into
sanitary drains and might well appear in wastewaters associated with seasonal
cleaning or renovating in homes, stores, warehouses, etc.

Encounters with peaks assigned to dimethoate in fall, winter and spring would
be consistent with this expectation.  However circumstantial inference must
be discounted, since analytical protocol was inappropriate for this chemical.

     Lasso  (alachlor) — This herbicide is used as a preemergence surface
spray for control of emerging broadleaved weeds and annual grasses.
Probably the only crops in contributing watershed counties on which it may
have been used would have been field corn, sweet corn and potatoes.

Lasso is readily degraded in moist soil but may persist for considerable
periods in dry soil.  Following a drier than normal early season in 1975,
the presence of Lasso at concentrations in the ppb range was indicated in
discharges to storage in July after heavy rains in June in areas near
Muskegon (Table 42).  After basin-wide heavy rains in August (2 to 4 times
normal), similar concentrations were indicated for both influent and dis-
charges to storage (Tables 40 and 42).  Encounters in November and December
were again associated with widespread heavy rains in November.

The previous season (1974) was wetter than normal through August.  This would
have promoted more rapid dissipation of Lasso.  However, weather records re-
flect a scattered distribution until August when heavy rains were general in
the immediate tri-county area.  Peaks for Lasso were not found for influent,
but 12  ppb was indicated in September discharges to storage (Table 41).

Circumstances of weather in relation to use practices support the indenti-
fication given here.

     Parathion (ethyl and methyl) — Ethyl parathion was not encountered at
any time.  Methyl parathion was indicated at levels below reliable quanti-
tation on one occasion at Muskegon (Table 41).

Failure to detect parathion is significant since ethyl parathion is the most
widely used of the restricted use pesticides.  Fifty metric tons were sold
in 1974 and 1975, mainly for use on fruits and vegetables but with signifi-
cant usage on grains, forages and ornamentals.  Less than 2 metric tons of
methyl parathion were sold, mainly for use on vegetables.

Parathion is used in many of the same areas and frequently in the same tank
mix with diazinon.  Direct entry into surface waters can occur from spraying
of field margins and ditch banks or from aerial sprays in muck soil areas.
Diazinon, with a persistence in soil of 3 months, was detected infrequently.
Failure to detect parathion reflects its susceptibility to rapid degradation
(persistence in soil, about 1 week).

     VegadexR (CDEC) — This is not a widely used herbicide but is used in
preemergence sprays for control of emerging annual weeds in certain vege-


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table crops and ornamentals.   It is more persistent than parathion (about
6 weeks in soil).   The appearance of peaks for Vegadex in influent at
Muskegon in April 1974 coincides with the season of most probable use (Table
39) and with unusually heavy rainfall in the immediate tri-county area.

Pre-chlorination Flows and Irrigation Water (1974)

Samples of water after the storage phase of treatment were obtained only
during the summer and fall of 1974 (Table 44).  Six samples of pre-chlorina-
tion flows were taken and 7 at irrigation pumps—not enough to draw any in-
ferences regarding effects of chlorination.  The 13 observations, as a group,
can be compared with data for incoming wastewaters in 1974 (Tables 39 and
41) to draw some tentative inferences regarding effects of storage.

Heptachlor (and/or its metabolites) and £,jp'-DDE were observed entering
storage at concentrations of the order of 10^ ng/1.  Only p,p'-DDE and
1-hydroxychlordene were detected in waters out of storage, both at greatly
reduced concentrations.  Lindane and/or isomers were found with similar high
frequency before and after storage (Table 47).  In 17 samples of incoming
wastewater where BHC isomers were detected in 1974 (Tables 39 and 41), their
mean sum was 163 ng/1.  The mean sum for 7 of 13 samples coming out of stor-
age (Table 44) was similar (134 ng/1).  DEHP was detected less frequently
after storage  (Table 47), and concentrations were substantially lower than
maximum concentrations before storage (Table 48).

These comparisons indicate that significant quantities of £,_p_'-DDE, hepta-
chlor and metabolites, and DEHP were removed from wastewater flows during
storage.  Such losses could have occurred by degradation, volatilization or
retention in sediments.  The benzene hexachlorides, as a group, were not at-
tenuated, although some isomerization may have occurred.  For example, $-BHC
was not found  in incoming wastewater but was indicated in water coming out
of storage lagoons in November  (Table 44).  This would be consistent with
reports that g-BHC may accumulate differentially as the most persistent
isomer (Kaufman, 1974; Matsumura, 1973).

Single observations for dieldrin, Lasso and Vegadex do not allow for infer-
ences drawn from the data.  Dieldrin would be expected to persist, whereas
the acetanilide and the carbamate might well be degraded extensively or
removed into sediments during storage.

Outfall Waters
General hydrologic considerations —

The area occupied by the Muskegon wastewater management system included what
was formerly the upper reach of Black Creek.  In preparing the site, drainage
patterns were altered so that some areas which formerly drained to Black
Creek and  then to Mona Lake now drain to the north outfall on Mosquito Creek,
which is a tributary of the Muskegon River.

The system also intercepts Cranberry Creek and two large county drains (Hall
Drain and  Big Drain).  The intercepted drainage originates in agricultural
areas east of the site, including a substantial area of drained organic soils
in Moorland Township.  The organic soils and associated artificially drained

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mineral soils are used for production of vegetables and cash crops (National
Cooperative Soil Survey, Muskegon County, 1968).   This off-site drainage has
been diverted to pass through the site via an open ditch which discharges
into Black Creek at a point west of the site.

The extent to which off-site drainage was, in fact, isolated from on-site
drainage collected to either of the outfalls during the period of this study
is not known.  Routine monitoring by management system personnel indicates
that input chloride is diluted in the system, but this has been attributed
to precipitation and groundwater intrusion.

Underdrainage from about two-thirds of the irrigated circles is now
directed to Mosquito Creek (the north outfall).  Drainage from the southern
third of the site is directed to the Black Creek outfall.  The soils in this
southern third are somewhat less permeable than those to the north and are
inadequately drained by tile at 500 ft spacing (150 m).  As a result, they
have accepted less water.  During the period of this study, the south-drain-
ing circles received wastewater at the rate of 0 to 130 cm over a 25 to 30-
week season each year, as compared with 130 to 190 cm on most circles to the
north.  Some of the north-draining circles received 250 cm or more (USEPA,
Region V, 1976).

These differences in drainage area and wastewater loadings are reflected in
summertime flows at the two outfalls:  33 to 35 MGD at the north outfall,
5 to 8 MGD at the south (Municipal Wastewater Surveys for August 26-27, 1975,
and July 6-7, 1976, Muskegon Wastewater Management System No. 1, Michigan
Water Resources Commission).

Total flow for the two outfalls was about 40 MGD, which compares with 28 MGD
of wastewater being received at the time of the two surveys.  This difference
between inflow and outflow is reasonable since approximately 50 MGD must be
applied over a 7-month irrigation season to dispose of 12 months' influent.
Drainage during the summer will normally be less than input due to evapo-
transpiration and consumptive use by the crop.

Chemicals encountered —

Monthly composites of drainage at the two outfalls at the Muskegon site were
monitored, beginning April 1974 (Tables 45 and 46).  The outfall on Silver
Creek at Whitehall was not monitored.

Two composites were taken before the first application of wastewater was
made in the latter half of May 1974.  The only chemical encountered in
quantifiable concentrations was LassoR.  Encounters at both outfalls could
have originated in soil residues from earlier use by private operators on
the site, although Lasso had not been detected in background soil samples.
It is possible, at this early stage of design implementation, that agricul-
tural chemicals could have entered the system in off-site drainage from the
east.

Lasso and atrazine were used each year for weed control on essentially all
of the irrigated acreage on the site.  The principal encounters with Lasso

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in drainage were associated with planting (May)  and the  early growing  season
(Tables 45, 46).  Lasso encountered at other times could reasonably have  en-
tered in wastewater (cf. Tables 40 to 42).

Peaks for atrazine were not observed in incoming wastewater.   One encounter
in drainage at the north outfall in September 1974 (Table 45) can be ascribed
to leaching of applied atrazine under conditions of heavy hydraulic loading
on north-draining circles.  A number of these were irrigated  at rates  greatly
in excess of design because less than 30 of the 52 circles were operational
by the beginning of the 1974 season, and storage lagoons were dangerously
full.

Diazinon was used on site in 1974 as insurance against corn rootworm.   Its
appearance in quantifiable concentrations at the north outfall in October
and November 1974 (Table 45) can be ascribed to this application.  Diazinon
was not used on site in 1975, but peaks for it were observed  in incoming
wastewater (Tables 40, 42).  It was not detected at outfalls  in 1975.

SutanR (butylate) was used on some circles in 1975 for control of nutsedge.
It could not be confirmed satisfactorily in sample extracts because of inter-
ference from contaminants with similarly short retention times (Rt relative
to aldrin = 0.23 on OV-17/QF-1).

Peaks for aldrin and dieldrin were observed in drainage during the early
growing season of 1974  (Tables 45, 46).  Because of the large regional sales
reported in 1973 and 1974, these restricted use pesticides may well have  been
present in wastewater which had been accumulating in storage  lagoons since
June 1973.  Dieldrin, but not aldrin, had been indicated also in background
samples of surface and subsoils (Tables 50, 51, 52).  The very low levels
of residual dieldrin in soils would not account for finding 31 ng/1 at the
north outfall in July 1974, however  (Table 45).  Localized areas of higher
soil residues may well have existed  in association with former residences
or earlier farming operations.  However, input wastewater would have been
the more likely source for this level of breakthrough into drainage.  Heavy
irrigation during the early weeks of operation in 1974 would have favored
rapid downward displacement of chemicals from both wastewater and soil
sources.

Quantifiable concentrations of £,p/-DDE were indicated  in 35 of  49 back-
ground samples of soil  (Tables 50, 51, 52) and in incoming wastewater in
April and May of 1974  (Tables 39, 41).  Levels approaching the quantifiable
limit were detected at the north outfall from April through July 1974 (Table
45) and at the  south outfall just after irrigation was  initiated in May 1974
(Table 46).  Disturbance  of soils during site preparation may well have ex-
posed sites of  residual accumulation to leaching under  conditions of heavy
local rainfall  in March,  April and May, followed by the period of unusually
heavy irrigation on the limited number of circles that were operational at
the beginning of the 1974 season.  The indicated presence of ]3,p^-DDE in  the
applied wastewater would  have contributed, also, to breakthrough at outfalls.

Heptachlor and/or its metabolites  (heptachlor epoxide,  1-hydroxy-chlordene)
were indicated  in quantifiable concentrations at outfalls only in July 1974

                                    108

-------
(Tables 45, 46).  Peaks for one or more of these species had been present
in 9 of 10 samples of incoming wastewater composited from April through July
(Tables 39, 41).  Frequencies of encounter at the two outfalls are consistent
with earlier and heavier irrigation on north-draining circles than on circles
draining to Black Creek.

Heptachlor and its metabolites have not appeared in credible concentrations
at outfalls since July 1974, even though concentrations of the order of 10
to 10^ ng/1 have been indicated for incoming wastewater through 1975 (Tables
40, 42).  There is evidence in background soil analyses that heptachlor may
have been used on site in the past (Tables 50, 51, 52).  Thus, microbial pop-
ulations adapted to metabolizing heptachlor and derivative intermediates may
have been present before wastewater was applied.  These species are also ad-
sorbed strongly by soil organic colloids.  Thus, interception by adsorptive
and degradative processes would account for their virtual absence in drainage
except when they were ostensibly present in wastewater applied at excessive
rates.

Lindane and/or other BHC isomers were encountered frequently at outfalls from
the time irrigation was initiated in 1974 through early spring of 1975 (Ta-
bles 45, 46).  Scattered occurrences since then have been at or below limits
of quantitation.  However, indicated inputs in wastewater did not decrease
in frequency or concentration from 1974 through 1975 (Tables 39 to 42).

Lindane or its isomers were not detected in background samples of soils.
Enzymatic competence to degrade BHC species would not have developed in their
absence.  The data suggest that adaptive populations may have developed in
soils after BHC species were first introduced with wastewater in 1974.

A further consideration is the larger annual production and return of plant
residues from irrigated corn, as compared with that from native cover,
stressed for water and nutrients, that existed on substantial portions of
the site before present management was imposed.  Thus, an increased rate of
turnover of organic matter can be expected to lead to an increasing organic
content in soils that were initially low in organic content.  With irrigation,
it can be expected that stabilized humic materials will be distributed to
greater depth in the profile also.

It is early to assess these expected changes with confidence because of the
very great variability introduced by land clearing and leveling operations.
Organic carbon has increased in surface soils and subsoils in a number of
north-draining circles.    As has been noted, irrigation commenced earlier
in north-draining areas of the site, and loadings have been consistently
heavier than in areas which drain to Black Creek.  Increased organic content
in the soil mantle will increase interception of both organic and mineral
species by adsorption and complexation.

Other pesticides which have been indicated occasionally at outfalls (Tables
45, 46) have also been encountered in incoming wastewater (Tables 39 to 42).
These include VegadexR (CDEC) and three 2,4-D esters (butyl, isobutyl, iso-
propyl).  The methyl ester of 2,4-D was not detected at outfalls, although
peaks for it were found in raw influent on several occasions in 1974 and 1975

                                     109

-------
(Tables 39, 40).  It was not detected in discharges to storage  after pre-
treatment (Tables 41, 42) but was indicated in soils in 1975  (Tables 54  and
55).  None of these herbicides has been used on site since the  land came
under county control.

The industrial chemical, DEEP appeared at outfalls in detectable  concentra-
tions (10-* to 10^ ng/1) at times when a substantial proportion  of the irri-
gated acreage was being subjected to exceptionally heavy hydraulic loading.
Thus, it appeared in late May, June and July of 1974 when water had to be
dumped on 20 or 30 operational circles to lower dangerously high  water in
storage lagoons.  It appeared again at the north outfall in September 1975
after 21 cm (8.3 inches) of rain in August, combined with normal  irrigation,
resulted in total water inputs of 40 to 50 cm (averaging 10 to  13 cm per
week) on most of the circles draining to the north (operational data, Muskegon
County Wastewater Management System).

In 1975, irrigation was discontinued (for periods of 3 to 6 weeks on indivi-
dual circles) to accommodate grain harvest in September and October.  After
this interruption, heavy irrigations were employed (10 to 15  cm/week on many
circles) to empty lagoons for winter storage.  These season-end applications
were accompanied by the appearance of DEHP at both outfalls in  November or
December.

Except during these periods of excessive hydraulic loading, DEHP  has been
reduced by passage through the system, from incoming concentrations of 10
to 10^ ng/1 to less than 10^ ng/1 (the limit of quantitation) at  outfalls.
Changes in frequency of detection and in ranges of concentration  at sampled
flow points (next section) indicate that removals of DEHP occurred both in
storage and during passage through soil systems.

Frequencies of Occurrence and Ranges of Concentration in Waters

Frequencies and ranges of concentration for trace organics detected by GLC/
ECD in waters associated with the Muskegon system are summarized in Tables
47 and 48.

Chemicals encountered most frequently in incoming wastewater were lindane
(or isomers), heptachlor (or metabolites), and the industrial chemical,  di-
ethylhexylphthalate  (DEHP).  Frequencies of encounter and maximum concentra-
tions give no evidence of change from 1974 to 1975 in the chronic nature of
input for these compounds.  There is no evidence that influent  levels were
reduced by aeration and settling.  In fact, there is a suggestion that extrac-
tability may have been increased by physical or metabolic comminution of oc-
cluding structures  (tissue fragments, fibers, floe, etc.).

Data for flows after storage  (obtained only in 1974) indicate that heptachlor
and heptachlor epoxide were removed during lagoon storage and that the flux
of 1-hydroxychlordene and DEHP out of storage was reduced substantially from
input  (cf. Tables 39, 40, 44).  By contrast, the frequency of BHC isomers,
as a group, and their summed  concentration did not change materially  (the
mean sum for BHC species in 17 samples before storage was 163 ng/1 vs 134 ng/1
for 13 samples after storage).  The spectrum of isomers was  different after
storage.
                                     110

-------
Levels detected at outfalls will reflect dilution by precipitation and by
waters entering from underlying aquifers or from intercepted off-site drain-
age.  However, the virtual disappearance of heptachlor and its metabolites
from drainage after July 1974 indicates that these compounds are being re-
moved effectively in the system, whether in lagoons or in soils or both.
The virtual disappearance of BHC isomers at outfalls since early spring of
1975 indicates a marked increase in interception over the first year of op-
eration (Tables 45, 46).

As noted in the previous section, DEHP appeared at outfalls during periods
of heavy hydraulic loading.  Analytical sensitivity for this chemical was
two or three orders of magnitude less than for chlorinated species.  Concen-
trations less than 10 ppb would not have been detected.  Nevertheless, changes
in frequency and concentration in 1974 (Tables 47, 48) indicate that removals
of DEHP occurred both in lagoons and in soils.  Interception in sediments
and soils would be expected, since phthalates are not exotic to natural sys-
tems.  They are found among biosynthetic products of plants and microorganisms
and in stable complexes with humic acids (Ogner and Schnitzer, 1970).  Enzy-
matic competence to degrade simple aromatics is widely distributed (Alexander,
1977).

Thus, it is to be expected that DEHP will be removed efficiently from waste-
waters if given sufficient residence time in lagoons or in soils.  Chronic
inputs should result in enrichment of sediments and soils with competent or-
ganisms and, consequently, in more rapid degradation.  As management operations
are routinized to avoid periodic excesses in wastewater application, episodes
of breakthrough at outfalls should decline.  Increased production and return
of crop residues should contribute to increased interception by products of
humification and to increased size and diversity of competent populations.
Increased vigor of the vegetative cover will serve, also, to reduce net per-
colation and increase retention times during seasons of active growth.

Three pesticides used in connection with farming operations on the Muskegon
site were encountered at outfalls.  These were diazinon, atrazine and Lasso^.
A fourth (Sutan^), used only in 1975, may have been present on occasions,
but the corresponding peak could not be resolved credibly by the methods em-
ployed.  Diazinon and Lasso were input, also, with wastewater.

Principal encounters with Lasso at outfalls were associated with planting
and the early growing season, whereas credible peaks for diazinon and atrazine
occurred later in the season and only in 1974 (Table 45).  Atrazine would
not have been detected at concentrations less than 1 ppb (Appendix II, Table
2).  Nevertheless, the data suggest that Lasso was intercepted less effective-
ly by soil materials than the other two pesticides under conditions of heavy
hydraulic loading.

On the other hand, peaks for Lasso were encountered less frequently at out-
falls in 1975 than in 1974 in spite of an indicated greater frequency in in-
coming wastewater (Tables 47, 48).  This result would be consistent with
developmental changes leading to more effective interception in soils.  A
more rational irrigation regime in 1975 and more vigorous growth of corn would
have been contributing factors.

                                    Ill

-------
Other pesticides encountered at outfalls would appear to have originated
primarily in wastewaters (aldrin, dieldrin,  DDT species, phorate,  2,4-D
esters, Vegadex^-) .   Others indicated in wastewater but not detected at out-
falls were endrin,  dimethoate, 2,4-D(ME) and 2,4-D(BE)I.

The various esters  of 2,4-D are rapidly hydrolyzed in soils and sediments
(Loos, 1975).  For  the esters to appear at outfalls, it would be necessary
for them to pass through the system quickly.

The secondary butyl ester, 2,4-D(BE)II, was encountered most frequently at
outfalls and at highest concentration.   Encounters at the north outfall (Table
45) were during periods of heavy hydraulic loading, at which times 2,4-D(BE)II
was associated with other trace organics, notably Lasso.  A single appearance
at the south outfall in December 1975 (Table 46) was associated with heavy
rains and breakthrough of DEHP in November.

There is experimental evidence that different ester derivatives of 2,4-D vary
in their susceptibility to hydrolysis (Aly and Faust, 1964).  Failure to de-
tect 2,4-D(ME) at outfalls, in spite of relatively frequent encounters in
incoming wastewater, suggests that the methyl ester may have been hydrolyzed
more rapidly in the system than the others.

Unfortunately, the peak for the free 2,4-D acid was not monitored.  It is
known that adaptive populations develop in soils and sediments amended re-
peatedly with 2,4-D (Aly and Faust, 1964; Loos, 1975).  Degradation by
adapted populations is rapid, and the adapted populations can persist for
periods of months or longer in the absence of 2,4-D in the substrate.  Adap-
tation to 2,4-D frequently confers competence to degrade related aromatics
such as 2,4,5-T.  Thus, the indicated periodic inputs of 2,4-D may, in fact,
be beneficial for inducing and maintaining a broader range of enzymatic com-
petence in soils.

Data for "unknown" peaks have not been  tabulated.  The compounds responsible
for unreferenced peaks monitored in 1975 may be sufficiently exotic that
degradative capability will, at best, be slow to develop.  Two or more of the
three peaks appeared in nearly all outfall samples.  The indicated concentra-
tions were reduced substantially from input, but peak areas as percent of
the total for all monitored peaks tended to increase.  Thus, the unknown chem-
icals may be more persistent or more mobile than many of the chemicals respon-
sible for referenced peaks.

The data summarized in Tables 47 and 48  indicate that the Muskegon system
has operated most effectively to intercept organics  that are strongly ad-
sorbed by soils or sediments  (endrin, heptachlor, DDT,  dieldrin, and related
species) and chemicals that are readily metabolized  (dimethoate, phorate).
There is evidence of improved performance in the second year of operation
over the first in removal of several relatively recalcitrant compounds  input
during farming operations on site or, at ppb to ppm  levels,  in wastewater
(BHG isomers, diazinon, atrazine, Lasso).

The effectiveness of wastewater renovation with regard  to trace organics can
be expected  to improve as irrigation regimes are rationalized and as agro-
nomic limitations are identified and corrected.  A  questionable operational
practice is  that of discharging wastewater  through disconnected sprinkler

                                      112

-------
headers in spring and fall.  Channeling of percolate through a severely re-
stricted soil volume may have contributed to breakthrough of a number of chem-
icals into drainage at these times.

It is probable that industrial wastes include potentially hazardous organics
that are more recalcitrant or more mobile in soils than DEHP or the pesticide
species monitored here.  For this reason, it appears important to utilize
the total soil area accessible to the sprinkler system at all times.

Particulate-Phase/Aqueous-Phase Distributions

The fate of trace organics adsorbed on particulate matter will be closely
linked with the fate of solids in the waste.  Removal of adsorbed chemicals
by sedimentation in settling basins and lagoons and by filtration in soils
are important mechanisms for reducing concentrations in wastewater flows.
On the other hand, these deposits represent reservoirs for maintaining con-
centrations in the transport stream by partitioning or by resuspension of
colloidal fractions. Also, their possible impact on desirable biotic communi-
ties in lagoons and soils must be considered, as well as their effect on ter-
restrial systems when sludges are removed for land application.

Distribution coefficients  (Kd) have been shown to be related to the degree of
inactivation of bioactive compounds in the presence of adsorbing surfaces,
as well as to their persistence in soils and sediments.  Also, Kd values pro-
vide an indication of the extent to which partitioning may serve to maintain
the concentration of persistent chemicals residually in waters passing through
the system.

Distribution coefficients for raw sewage and treated discharges into storage
have been calculated in Table 49 for those chemicals which were present in
sufficient concentration to be detected in both solid and liquid phases.  The
Kd values obtained are in the range of 1(P to 10^.  These are greater by 2 or
more orders of magnitude than have been reported for numerous chemicals in
laboratory equilibrations with soils (Hamaker and Thompson, 1972).  Values
as great as 10^ have been reported for j3,p>'-DDT, however, in slurry equilibra-
tions with plant tissues, fungal mycelium and muck soils (Shin et al., 1970).

Thus, the distribution coefficients in Table 49 appear valid in the qualita-
tive sense that they illustrate the great capacity of waste solids for con-
centrating trace organics.  They do not provide strong support for more re-
fined interpretation because of the limited number of observations.  Certain
trends are evident which will warrant detailed investigation in the future.

It is to be expected that different chemicals will be adsorbed to different
degrees by any given solid waste component and that adsorption patterns will
change as BOD substrates are dissipated.  Solids loadings were reduced 50
percent by aeration and settling (from a mean of 253 mg/1 to 120 mg/1).  The
concentration of chemicals associated with residual solids increased (Table
49).

The indicated increase in adsorptive capacity is not unexpected.  Adsorptive
surface would increase as tissue fragments and aggregated solids are commi-

                                     113

-------
Table 49.   DISTRIBUTION OF TRACE ORGANICS BETWEEN PARTICIPATE AND AQUEOUS PHASES, MUSKEGON WASTE WATER, DEC 73 TO DEC 75.




Source

RAW INFLUENT
(27 samples total)
Particulate phas :
(125 to 576 mg/1)
(mean 253 mg/1)
Aqueous phase

Distribution coefficient*
DISCHARGE INTO STORAGE
(20 samples total)
Particulate phase
(49 to 245 mg/1)
(mean 120 mg/1)
Aqueous phase


Distribution coefficient






No. of samples*

Range: Min
(ng/g) Max
Mean (ng/g)
Range: Min
(ng/1) Max
Mean (ng/1)

No. of samples
Range: Min
(ng/g) Max
Mean (ng/g)
Range : Min
(ng/1) Max
Mean (ng/1)

*No. of samples in which chemicals were detected

Particulate phase
«  M
o
1

43


6

7. 2x10 3
1
50


6


8.3xl03
0 V ?
a- s- M
t-"< S
oo. n
n »
&. o
IP j
1 1

29 113


219 305

.IxlO3 .4xl03
4 0
39
1.2x103
535
5
137
96
5.6xl03
ft "0
H. jj*



P rt

11 3

25 4.xl03
2.8x10 23.xlO
494 15.9xl03
H 4.8xl03
233 87-x10^
iiS 33.3xl03
2. IxlO3 .5xl03
9 0
250
•i
1.4x10
561
3 	
717
158
3.6xl03
f
CO
CD
O


2

145
983
564
20
9.3x10,
4.7x10
.IxlO3
1
25-xlO3


17


1.5x10°
o





9

30.xl03
3.3x10°
767jd03
ll.xlO3
930. xlO3
152. xlO
5.0xl03
8
1.3xl03
2.5x10°
1.03xl06

l.OxlO3
2.0x10°
318. xlO3
3.2xl03
and aqueous phases.





                                                       = Kd

-------
nuted by metabolic degradation and physical detrition in aeration lagoons.
Also respiratory processes will alter the nature of exposed surfaces, and
probable changes would increase specific adsorption of many organic species.

An increase in adsorptive capacity of residual solids would lead to increased
distribution coefficients, as evidenced for most chemicals in Table 49.  On
the other hand, degradation of occluding structures might expose more of a
complexed chemical for partitioning and result in a relatively greater in-
crease in concentration in the aqueous phase than in the solid phase, and
a decrease in distribution coefficient, as indicated for DEHP.

The distributions in Table 49 are consistent with the evidence in Tables 47
and 48 that incidence and total recoveries of frequently encountered chemi-
cals were not affected (or may have been increased in some cases) by detrital
changes during treatment before storage.

Data for 1974 (Tables 47 and 48) suggest that reductions in incidence and
concentration of several chemicals may have occurred in consequence of
storage.  Sedimentation in lagoons would have been a contributing factor.
On the other hand, no attenuation during storage was indicated for lindane-
related species.  This reflects both the recalcitrance of the chlorinated
cyclohexanes and their relatively much greater solubility relative to other
chlorinated hydrocarbons  (Biggar and Riggs, 1974; Gunther et al., 1968).

TRACE ORGANICS IN SOILS

Background Samples

Background data are given in Table 50 for surface soils (0-15 cm) from 25
circles and for subsoils  (46-61 cm) from 17 circles sampled at various times
in 1972 or 1973.  Eight circles were selected to represent four major soil
types for routine twice-a-year sampling.  These special study stations were
sampled for background in spring 1973 and again in spring 1974 just before
irrigation with wastewater was initiated.  Background data for the six special
study sites at Iluskegon are given in Tables 51 and 52 and, for the two sites
at Whitehall, in Table 56.

Both £,£T-DDT and _p_,_p_'-DDE were encountered in nearly all surface samples,
less frequently and at lower concentrations In subsoils.  The corresponding
c^,_p_ isomers were encountered less frequently, but at similar concentrations.
The anaerobic metabolite, £,£*-DDD, was indicated in a few samples, but peaks
for £,£-DDD were not detected.

Peaks for dieldrin were encountered in about half of the surface soils, less
frequently and at lower concentrations in subsoils.  Heptachlor was indicated
at only one station.  This was in circle 44 (MSU site No. 26) in 1973, at
which time it was accompanied by the highest value for dieldrin encountered
at any time during this study (Table 51).

In later samplings, values for both dieldrin and DDT species have varied
widely in circle 44 as compared with other stations (cf. Tables 51 to 55 and
next section).  The highest values for DDT species in this study were obtained

                                     115

-------
Table 50.  TRACE ORGANICS IN SOILS, MUSKECON AND WHITEHALL SYSTEMS,  BACKGROUND SAMPLES TAKEN SUMMER 72 OR JUNE 73 (25 SURFACE SAMPLES, 17 SUBSOIL SAMPLES).!
HSU
Site
No.

03

04

05

06

08

11

14

16

17

Circle
No.

21*

24*

23#

23*

47§

It

11 »

41§

42§

a
H-
ro
CL
£
Sample depth
cm

0-15
46-61
0-15
46-61
0-15
46-61
0-15
46-61
0-15
46-61
0-15
46-61
0-15
46-61
0-15
46-61
0-15
46-61

tr**t
nd
nd*
nd
nd
	
.3
	
nd
nd
nd
	
nd
	
nd
nd
nd
nd
Ip
P
i
§
H

nd
nd
nd
nd
nd
	
nd
	
nd
nd
nd
	
nd
	
nd
nd
nd
nd
lo
to
i
a
a

nd
nd
1.4
nd
nd
	
nd
	
nd
nd
nd
	
nd
	
nd
nd
nd
nd
(a hi
fa b_
i i
§ §
H 0

- ~ ng/g
5.0
nd
1.2
nd
nd
No
nd
No
5.0
nd
nd
No
.2t
No
1.3
nd
1.1
nd

nd
nd
nd
nd
nd
Analysis
nd
Analysis
nd
nd
nd
Analysis
nd
Analysis
nd
nd
nd
nd
to
K
i
§
ca

1.4
nd
.6
.It
.7
	
.4
	
1.2
nd
.8
	
.5
	
.8
nd
.5
.it
Heptachlor

nd
nd
nd
nd
nd
	
nd
	
nd
nd
nd
	
nd
	
nd
nd
nd
nd
Heptachlor
epoxlde

nd
nd
nd
nd
nd
	
nd
	
nd
nd
nd
	
nd
	
nd
nd
nd
nd
Total DDT
species

6.4
nd
3.2
.It
.7
	
.4
	
6.2
nd
.8
	
.7
	
2.1
nd
1.6
.It
n n
p TJ rr
O* H* B>
O C O
M » y
H- 1-
rt o
ID n
O)

nd
nd
nd
nd
nd
	
nd
	
nd
nd
nd
	
nd
	
nd
nd
nd
nd
     #Sltes  draining to north outfall  at Muskegon
     SSites  draining to south outfall
     tBelow  usual range of confident quantitation  (Aypendix II., Table  2).
                                                                                                                                (continued)

-------
                                                                Table 50. (continued)

MSU Circle
Site No.
No.


18 3#

19 7#

21 19 f

23 27#

25 401

26 445

27 40 i

29 W-2

30 W-3


Sample
depth
cm


0-15
46-61
0-15
46-61
0-15
46-61
0-15
46-61
0-15
46-61
0-15
46-61
0-15
46-61
0-15
46-61
0-15
46-61
a
H.
n>
3


tr** t
	
.7
nd
nd
	
nd
nd
nd
nd
48.0
.2
.It
.4
.It
	
nd
nd
\o
l
1


1.9
	
nd
nd
nd
	
nd
nd
3.1
nd
2.0
nd
2.5
nd
2.0
	
3.4
nd
L0
l-a
l
o
8


nd
	
nd
nd
nd
	
nd
nd
nd
nd
nd
nd
nd
nd
nd
	
nd
nd
I?
l-o
o
s

- - ng/g
1.9
No
1.2
nd
5.8
No
nd
nd
2.7
nd
5.0
nd
.4
.8
2.7
No
1.6
nd
Ijo
l-o
i
§
e>


nd
Analysis
nd
nd
nd
Analysis
nd
nd
.3
nd
nd
nd
nd
.8
.6
Analysis
1.1
nd
1?
l-o
i
1


1.3
	
5.6
.2
3.5
	
2.0
.It
2.1
.8
1.4
.2
1.6
1.0
2.2
	
4.1
.2
i?
•o
rr
|


nd
—
nd
nd
nd
—
nd
nd
nd
nd
1.5
nd
nd
nd
nd
	
nd
nd
»!
O ft*
P. s-
O. V-*
ID o


nd
—
nd
nd
nd
—
nd
nd
nd
nd
tr
nd
nd
nd
nd
	
nd
nd
o
a ft
•o (a
o
sr§
• H


4.1
	
6.8
.2
9.4
	
2.0
.1
8.2
.8
8.4
.2
4.5
2.6
7.5
	
10.2
.2
§ if
rr "O
P> •O rt
g-ss-
H- M
S S

-------
                                                                                 Table 50.   (continued)
00




MSU Sample
Site Circle depth
a
H*
a.
ft
a
lo
fa
|
§
lo
fa
|
1
to
~
1
O
q
No. No. cm "*
31 W-l

32 W-2

33 33»

34 30*

35 435

36 465

37 42§

0-15
46-61
0-15
46-61
0-15
46-61
0-15
46-61
0-15
46-61
0-15
46-61
0-15
46-61
Frequency of detection (no
25 samples
17 samples
Range when



analyzed: 0-15
analyzed :46-61
detected (ng/g)
0-15
46-61

Mean for samples in which


0-15

.It
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
—
. of samples)
8
2

Min tr I
Max 48.0 3
Min .4
.4
detected (ng/g)
6.2 2
.3
nd*
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
—

6
0

.9
.1



.5
—
nd
nd

nd

nd

nd

nd

nd

	

1
0

1.4



1.4
— — ~
2.2
.5
1.8
nd
2.3
.2t
4.3
.2t
2.5
nd
1.4
.2t
.2t
No

21
5

.2t
5.8
.2t
.8

2.4
.4
fa
™
i
a
o
o
1.0
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
Analysis

4
1

.3
1.1

* 8

.8
.8
V
*°L

i
§
w
1.8
.5
1.1
.It
1.2
.It
1.3
.2
.8
.It
.8
.It
nd
—

24
14

.4
5.6
.It
1.0

1.6
.3
1
s
o
ET
M
O
n
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
—

1
0

1.5



1.5
	
» i?
•a -o
8 U
g.0

nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
—

1
0

tr



tr
	
*s
*S w
H> O
(D O
a H

5.0
1.0
2.9
.It
3.5
.3t
5.6
.4
3.3
.It
2.2
.3t
>2t
	

25
14

.2t
10.2
.It
2.6

4.2
.4
g ff
ft "O
O* M B»
o c ^
H* 5 3*
It 0
It M
[a
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
—

1
0

1.5
	


1.5
	
                     GLC peaks for all chemicals listed in Table 2, Appendix II, were monitored.   Only chemicals detected and confirmed on two or more GC
                     Columns are reported.  Confirmation by thin layer was required, also, except at concentrations too low for spots to be visualized.

-------
                  Table 51.  TRACE ORGANICS  IN SOILS,  SPECIAL  STUDY  SITES, MUSKEGON,  BACKGROUND SAMPLES  TAKEN JUNE 73  AND APRIL  74  (SURFACE  SOILS,  0-15  cm).  T
VO
MSU
Site Circle
No. No.

034»

04*

085

26 §

16 §

17§


21

24

47

44

41

42

Frequency of detection
(12 samples
Detected range
(ng/g)
Detected mean
analyzed)
Min.
Max.
(ng/g)
Year

73
74
73
74
73
74
73
74
73
74
73
74
(no. of




o
H.
1
M.
a


tr**t
.It
nd*
.It
nd
.4
48.0
3.1
nd
.8
nd
.4
samples)
8
tr
48.
6.6
|o
I*
§


nd
.2
nd
.2
nd
.6
2.0
.5
nd
.4
nd
.6

7
.2
2.0
.6
I?
to
B


nd
nd
1.4
nd
nd
nd
nd
nd
nd
nd
nd
nd

1
1.4

1.4
t?
*.
1
1
/

5.0
1.1
1.2
1.2
5.0
.9
5.0
2.0
1.3
.9
1.1
1.4

12
.9
5.0
2.2
h)
hJ_
g
o


nd
.4
nd
nd
nd
nd
nd
.8
nd
.6
nd
.4

4
.4
.8
.6
b>
k
1


1.4
.4
.6
.4
1.2
.4
1.4
1.0
.8
.5
.5
.3

12
.3
1.4
.7
Heptachlor


nd
nd
nd
nd
nd
nd
1.5
nd
nd
nd
nd
nd

1
1.5

1.5
a, S
US
O H
ffo
.0


6.4
2.1
3.2
1.8
6.2
1.8
8.4
4.4
2.1
2.4
1.6
2.8

12
1.6
8.4
3.6
                 *nd - not detected
                 **tr • trace
                 #Sites 03 and 04 drain  to north outfall  (Mosquito Creek).
                 SSites 08,  26,  16 an
-------
Table 52.  TRACE ORGANICS IN SOILS, SPECIAL STUDY SITES,  MUSKEGON, BACKGROUND SAMPLES TAKEN JUNE 73 AND APRIL 74 (SUBSOILS, 46-61 cm). I


MSU
stte
No.

03#

04*

08 §

26§

16 S

175

Frequency






c
•H
•a
Circle "3
No.

21

24

47

44

41

42

Year

73
74
73
74
73
74
73
74
73
74
73
74
of detection (no.
(12 samples analyzed)
Detected
(ng/g)
range

Detected mean
Min
Max
(ng/g)
-H
Q

nd*
nd
nd
.It
nd
.3
.2
.5
nd
.It
nd
.It
of samples)
6
.1
.5
.2
H
a
a
i
°-l
o"l

nd
nd
nd
.2
nd
nd
nd
nd
nd
nd
nd
nd

1
2

.2
g
a
i

-------
                  Table 53.  TRACE ORGANICS IN SOILS, SPECIAL STUDY SITES, MUSKEGON (NOVEMBER 1974 SAMPLING).
HSU

site
no.

n-i A
U Jtf
04 #

085

265

165

175



Circle
no.



24

47

44

41

42

Detected means




Depth


0-1 S
j. j
46-61
0-15
46-61
0-15
46-61
0-15
46-61
0-15
46-61
0-15
46-61
0-15
46-61
g
|
cJ
ol

•) o
£ * y
.it
nd*
nd
nd
.5
nd
nd
nd
nd
nd
nd
2.9
.3
§

P.J
oTs

2Q
• 7
nd
nd
nd
nd
1.7
nd
nd
nd
.It
nd
nd
2.9
.9
1

aj
oJ


nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
1.4
	
1

O.J
fxl


2.3
nd
nd
nd
1.0
nd
nd
.9
nd
nd
nd
3.2
1.6
droxy-
chlordene
^
.c
i
.-t


nd
.It
nd
nd
nd
nd
nd
nd
nd
nd
nd
.1
— —
u

i
a


1.0
1.9
.It
1.2
nd
3.0
nd
.It
nd
.It
nd
1.3
.6


.5
hJ
i
- ng/g-
nd
nd
nd
nd
.4
nd
nd
1.0
.1
.5
.1
.8
.2
c
0
c
•H
N
01
•H
Q


nd
nd
4.0t
nd
12.0
nd
nd
nd
nd
nd
9.0

8.4
u
e
N

U
*J


A i n
*t J.U.
nd
230.
nd
490.
nd
nd
nd
nd
nd
nd
nd
377.
	
o
GO
0)
0)


6.0
4.0
4.0
nd
11.0
3.0
nd
nd
nd
nd
nd
nd
7.1
3.3

PL,
U
P

27Av1fi3
> /'fXAU-'
2.61x103
2.84x103
nd
nd
nd
. 33xl03
nd
nd
nd
nd
nd
1.97x103
2.61x103
(0
10
•H
U
01
a
01
H
§
T-t
(0
o
H

12 7
2.4
nd
nd
nd
3.1
nd
nd
.9
.It
nd
nd
6.8
1.9
ane plus
isomers

•H
t-1

1C
. J
1.0
1.9
.It
1.2
.4
3.0
nd
1.2
.1
.6
.1
1.6
.3
 *nd * not detected
 # sites 03 and 04 drain to north outfall (Mosquito Creek).
 i sites 08, 26, 16, and 17 drain to south outfall (Black Creek).
 t Below usual range of confident quantisation (Appendix II, Table 2).
tGLC peaks for all chemicals  listed  in Table 2,  Appendix II,  were monitored.   Only chemicals detected and confirmed
  on two or more GC columns are reported.  Confirmation  by  thin  layer was  required, also, except  at  concentrations  too
 low for spots to  be  visualized.

-------
                                                Table 54.  TRACE ORGANICS IN SOILS, SPECIAL STUDY SITES, MUSKEGON (APRIL 1975 SAMPLING).
N5
K3
>
£
HSU H.
site Circle Depth °
No. No. cm
Dieldrin
1°
'?
1°
(•d
I
r?
f0.
O
O
H
p
f0.
1
'?
f°.
1
Q
1
r*
H-
g.
Methoxy-
chlor
Atrazine
1
o
ro
*•
o
§
2,4-D(lPE)
CO
•o
a n
w o
P« h*
CD
H H- f
0 CO V H-
n O M P
» g C £.
• M K to ft
n p


030 21


04# 24


08§ 47


26 § 44


16 § 41


17 § 42


0-15 nd*
46-61 nd
91-107 nd
0-15 nd
46-61 nd
91-107 nd
0-15 nd
46-61 nd
91-107 nd
0-15 2.0
46-61 nd
91-107 nd
0-15 nd
46-61 tr**t
91-107 nd
0-15 nd
46-61 nd
91-107 nd
Detected means 0-15 2.0
(ng/g)
lb-61 tr
nd
nd
nd
nd
nd
nd
nd
nd
nd
29.0
nd
nd
nd
nd
nd
nd
nd
nd
29.0

28.0
nd
nd
nd
nd
nd
1.0
nd
nd
15.0
.It
nd
nd
nd
nd
nd
nd
nd
14.7
.1
nd
nd
nd
nd
nd
nd
nd
1.0
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
—
1.0
3.0
nd
nd
4.0
nd
nd
4.0
nd
nd
58.0
nd
nd
1.0
nd
nd
3.0
nd
nd
12.2

nd
nd
nd
nd
nd
nd
.6
nd
nd
14.0
nd
nd
nd
nd
nd
nd
nd
nd
7.3

.2
nd
nd
1.0
nd
nd
1.0
nd
nd
10.0
nd
nd
.4
nd
nd
.9
nd
.It
2.2

.It
nd
nd
nd
nd
nd
nd
nd
nd
1.0
nd
nd
.It
nd
nd
1.0
nd
nd
.6

nd
nd
nd
.1
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
6.0
.2
.1
3.1
.1
nd
nd
.4t
nd
nd
nd
nd 1.4xl03
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
—

nd
nd
12. Of
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
7. 0x10 3

17
3
3
39
nd
nd
2t
nd
nd
nd
nd
nd
tr
nd
nd
2t
2 +
nd
12.1
2.5
nd
nd
nd
23.0
3.0
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
23.0
3.0
nd
nd
nd
tr
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
.3

nd
nd
nd
6.5xl03
nd
nd
nd
nd
nd
31.2
nd
nd
5.0
nd
nd
6.6
1.0
nd
nd 97.0
16. 0x10 J
nd
4.0xl03
nd
nd
nd
nd
nd
5.2xl03
• 16.0x103
.It
nd
1.4
nd
nd
3.9
nd
nd
24.2
.6
.It
nd
nd
.1
nd
nd
nd
nd
nd
1.0
nd
nd
.It
tr
nd
7.0
.2
.1
1.7
.1
                              *nd • not detected
                              **tr - trace
                              #sites 03 and 04 drain to north outfall (Mosquito creek).  § Sites 08, 26, 16 and 17 drain to south outfall (Black creek).

                              tBelow usual range of confident quantitation  (Appendix II, Table 2).
                              +GLC peaks for all chemicals listed in Table 2,  Appendix II,  were monitored.   Only chemicals detected and confirmed on two
                                or more GC columns are reported.  Confirmation by thin  layer was required, also, except at concentrations too  low for spots  to
                               be visualized.

-------
                                           Table  55.  TRACE ORGANICS IN SOILS.  SPECIAL  STUDY  SITES, MUSKEGON  (OCT.  1975  SAMPLING).!
N5
U)
HSU
site Circle
No. No.


031 21


04* 24


089 47


265 44


165 41


17$ 42


Detected means
(ng/g)
Depth
en


0-15
46-61
91-107
0-15
46-61
91-107
0-15
46-61
91-107
0-15
46-61
91-107
0-15
46-61
91-107
0-15
46-61
91-107
0-15
46-61
o
1


.4
nd*
nd
tr**t
nd
nd
nd
nd
nd
17.0
.2
nd
nd
nd
nd
nd
nd
nd
5.8
.2
Ip


nd
nd
nd
• It
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
.1
—
(?


1.4
nd
nd
.8
nd
nd
1.9
nd
.It
1.3
nd
.It
2.5
tr
nd
.7
nd
nd
1.4
tr
l-o
l-o,
i
g
n


nd
nd
nd
.2
nd
nd
.8
.2
nd
nd
nd
nd
.4
nd
nd
.1
nd
nd
.4
.2
Haptachlor
•pozldc


nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
.1
nd
nd
nd
nd
nd
.1
— —
a


nd
nd
nd
.4
nd
nd
.6
nd
nd
2.0
nd
nd
2.5
nd
nd
nd
nd
nd
1.4
~— —
1


4.4
.3
nd
nd
nd
nd
3.9
nd
nd
5.8
nd
nd
4.0
nd
nd
.7
nd
nd
4.0
.3
Diazlnon


4.6
nd
nd
10.0
nd
nd
3.7t
nd
nd
nd
nd
nd
6.0
nd
nd
.8t
nd
nd
5.0
—
Phoratt


nd
nd
nd
nd
nd
nd
9.0
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
9.0
___
Atrazln*


nd
nd
nd
108.
nd
nd
31.
nd
nd
36.
nd
nd
nd
nd
nd
nd
nd
nd
58.
—
1*
o


8
nd
nd
4
ad
tr
It
nd
nd
58.
tr
nd
11.
nd
nd
5.
nd
nd
16.5
.1
ro
I


nd
nd
nd
5.0
nd
nd
nd
nd
nd
1.0
nd
nd
nd
nd
nd
nd
nd
nd
3.0
—
.? !
IE !
t* i
• o


1.4
nd
nd
1.1
nd
nd
2.7
.2
.It
1.3
nd
.It
2.9
tr
nd
.8
nd
nd
4.7
.1
iif


4.4
.3
nd
.4
nd
nd
4.5
nd
nd
7.8
nd
nd
6.5
nd
nd
.7
nd
nd
4.1
.3
               *nd - not detected
               **tr - trace
                fsites 03  and 04  drain to north outfall  (Mosquito Creek).  Ssites 08, 26,  16 and  17 drain  to south outfall  (Black Creek).
               t Below usual range of confident  quantltatlon (Appendix II,  Table 2).
               tGI.C peaks for all chemicals listed in Table 2, Appendix II, were monitored.  Only chemicals detected and confirmed on two
                or more CC columns are reported.   Confirmation by thin layer was required, also,  except at concentrations too low for spots to
                be visualized.

-------
                             Table  56.  TRACE ORGANICS IN SOILS, SPECIAL STUDY SITES, WHITEHALL, BACKGROUND  SAMPLES TAKEN JUNE  1973 AND APRIL  1974.:f
S3
-C-
MSU
site Circle
no. no.

30 W-3



31 W-l



Frequency of detection
(of 4 samples
analyzed)
Detected range



Detected means
(ng/g)
Depth
cm

0-15

46-61

0-15

46-61

(no. of
0-15
46-61
0-15

46-61

0-15
46-61
Year

73
74
73
74
73
74
73
74
samples)


Min
Max
Min
Max


Dieldrin

nd*
nd
nd
nd
.It
.It
nd
nd

2
0
.1
.1
	
	
.1
	
8

3.4
.2
nd
nd
nd
nd
nd
nd

2
0
.2
3.4
	
	
1.8
	
§

nd
nd
nd
nd
nd
nd
nd
nd

0
0

	
	
	
—
	
Q
"p.
a.
	 ng,
1.6
.9
nd
nd
2.2
1.3
.5
nd

4
1
.9
2.2

.5
1.4
.5
1
1
P.
'g 	 •
1.1
.It
nd
nd
1.0
.4
nd
nd

4
0
.it
1.1
	
	
.6
	
w
o
1
0.
o."

4.1
.11
.2
nd
1.8
1.2
.5
nd

4
2
.It
4.1
.2
.5
1.8
.4
Hept achlor

nd
nd
nd
nd
nd
nd
nd
nd

0
0
_..
	
	
	
._.
	

-------
                            Table 57.   TRACE ORCANICS  IN  SOILS,  SPECIAL STUDY SITES,  WHITEHALL (SAMPLINGS OF NOV. 1974, APR. 1975 AND OCT. 1975). I
NJ
Ul
MSU
site Circle Sampling
no. no. date


30 W-3 Nov 74

Apr 75


Oct 75


31 W-l Nov 74

Apr 75


Oct 75


Detected uieans
(ng/g)
Depth
cm


0-15
46-61
0-15
46-61
91-107
0-15
46-61
51-107
0-15
46-61
0-15
46-61
91-107
0-15
46-61
91-107
0-15
46-61
W
g
1
0*1


nd*
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
.2
nd
nd
.2
—
|
al


1.5
nd
tr**t
nd
nd
2.8
nd
nd
nd
nd
.2t
nd
nd
1.5
tr
nd
1.2
tr
w
Q
e>
pJ


.8
nd
nd
nd
nd
.9
nd
nil
nd
nd
tr
nd
nd
.It
nd
nd
.4
___
u
g
0


.6
.3
nd
nd
nd
nd
nd
nd
.3
nd
nd
nd
nd
nd
nd
nd
.4
.3
Lindane


.2
.2
nd
nd
nd
nd
nd
nd
.1
.1
tr
tr
nd
tr
nd
nd
.1
.1
Phorate
i

nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
64.
nd
nd
64.
	
O
i


nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
nd
tr
nd
nd
nd
nd

.6
I
Q
1
CS


nd
nd
nd
nd
nd
3.6
nd
nd
nd
nd
nd
nd
nd
13.9
nd
nd
8.8
— —
U)


nd
nd
nd
nd
nd
nd
700.
700.
nd
nd
nd
nd
nd
1850.
nd
nd
1850
700
(0

-------
for samples taken at this station in April 1975 (Table 54).

The general area of this sampling station was examined just  before corn was
planted in May 1976.  Fragments of boards and timbers were found at one point,
together with a number of woven nylon bags of a type used at one time by the
basic producer of heptachlor for protective packaging.  A service shed was
apparently located here and used in connection with farming  operations on
surrounding areas of predominantly Granby soils.  Immediately east of the
building site, however, was a sizeable area of shallow muck  (5 to 10 ha).
Aerial photos taken about 10 years earlier show a north-south field boundary
at about the location of the sampling station (near the center of the NW
quarter of Sec. 29, R.14W, T.10N; Sheet No. 67, National Cooperative Soil
Survey, Muskegon County, 1968).

Thus, the sampling-to-sampling variability in analyses for dieldrin and DDT
species in circle 44 can be ascribed to a complex of soils and previous
management bordering within the area designated for sampling.  The unusual
(for this study) values for dieldrin and DDT species can be ascribed to
localized concentration of soil residues associated with storage and handling
of these chemicals at a field service facility over periods of time in the
past.

Maximum values for dieldrin (48 ng/g) and DDT species (97 ng/g) at this sta-
tion are, in fact, low relative to ranges of concentration reported in
national surveys made as recently as 1974  (Roan, 1975).  Values reported here
for other sampling stations are no more than might be expected in soils after
equilibration with global circulation through the atmosphere  (Edwards, 1973;
Woodwell et al., 1971).

The relative frequencies and concentrations of DDT, dieldrin and heptachlor
at this station over the period of this study are consistent with their
relative persistence in soils:  DDT > dieldrin > heptachlor  (Hiltbold, 1974).
Other limited local areas of unusual residual concentrations of these per-
sistent insecticides, perhaps others also, undoubtedly exist elsewhere in
the Muskegon system at sites associated with earlier  farming operations or
residences.

Numerous small unreferenced peaks were present  in extracts of background soil
samples.  However, peaks for dieldrin and DDT species were, normally, the
dominant peaks differentiated from background.

Post-Irrigation _S_amples_

Referenced Compounds —

Data for three samplings of soils made since wastewater  irrigation was initi-
ated at Muskegon  (May 1974) are given in Tables 53, 54,  55.  At Whitehall,
no wastewater was applied until late in the season, shortly before the first
post-irrigation samples were taken in Nov. 1974  (Table 57).

With the exception  of DDT species, dieldrin and heptachlor or  its metabolites,


                                    126

-------
none of the chemicals in Tables 53, 54, 55, and 57 had been detected in
background samples taken before the start of irrigation and farming opera-
tions in 1974 (cf. Tables 50, 51, 52, and 56.

Frequencies of Occurrence and Ranges of Detected Concentration

The frequency with which trace organics were encountered pre- and post-
irrigation in soils at special study sites is summarized in Table 58
(Muskegon) and Table 59 (Whitehall).  The ranges of concentration when
detected are given in Tables 60 and 61.

With few exceptions, individual chemicals were encountered more frequently
in surface soils  (0-15 cm) than in subsoils  (46-61 cm) and usually at higher
concentrations.  Samples were taken also at 91-107 cm in spring and fall of
1975, but only p,p'-DDT, lindane, lasso and methoxychlor were encountered,
at near limits of quantitation and only once for each chemical (Tables 53,
54, and 55).

Of the chemicals which have been detected in soils only after irrigations
began in 1974, all have been detected at some time in incoming wastewater—
except methoxychlor and atrazine.  Methoxychlor was detected in soil only
once and in trace quantities, so its identification is questionable.  The
presence of atrazine in soils is explained by its use on-site for weed
control, both in 1974 and 1975.  Lasso was used as an herbicide both years,
but also appeared frequently in incoming wastewaters, at concentrations
ranging up to 10^ ng/1 (Tables 47 and 48).

Diazinon was used for control of corn rootworm at Muskegon only in 1974.
This would have been the likely source for encounters with this chemical at
outfalls and in subsoils in the fall of 1974.  However, its frequent occur-
rence in surface soils in the fall of 1975 (Tables 58 and 60) must be
ascribed to wastewater inputs in 1975 ranging up to 10^ ng/1 (cf. Tables 47
and 48).

On-site applications of pesticides have not been made at Whitehall.  Traces
of Lasso detected in subsoils in April 1975  (Tables 59 and 61) may well have
entered in wastewater.  Wastewater samples for organic analysis were first
taken at Whitehall in April 1975, and Lasso was detected in samples taken in
May (Table 43).

Lindane and/or its isomers and DEHP have been the most frequently encountered
chemicals in incoming wastewaters at Muskegon (Table 47). They were first de-
tected in soils after irrigations began (Table 58).  Incoming concentrations
of lindane plus isomers have been less at Whitehall (Table 43) than at Muske-
gon (Table 48), and concentrations in soils have been less (Table 61 vs_ Table
60).  At Whitehall, DEHP was not detected in incoming wastewater until Sep.
1975 (Table 43), and it was first detected in soil in Oct. 1975 (Table 59).

Significant quantities of lindane and a-BHC appear to have been intercepted
in surface soils (Tables 53, 54, 55).  The indicated concentrations of
lindane in surface soils increased from 1974 to 1975. Immobilization in
surface layers undoubtedly contributed to the much lower concentrations in

                                     127

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                                          Table 58.  FREQUENCIES OF OCCURRENCE, TRACE ORGANICS IN SOILS, MUSKEGON, JUNE 73 TO OCTOBER 754
OO
Chemicals
Jun
Total samples
Aldrln
Dieldrtn
DDT species
Lindane & isomers
Heptachlor & metabolites
Methoxychlor
Dlazinon
Phorate
Atrazlne
Lasso
2,4-D species
DEHP

73
6
nd*
2
6
nd
1
nd
nd
nd
nd
nd
nd
nd
Surface
Apr 74*
6
nd
6
6
nd
nd
nd
nd
nd
nd
nd
nd
nd
soils (0-15 cm)
Nov 74
6
nd
nd
2
6
1
nd
nd
nd
3
3
nd
3
Apr 75
6
1
1
6
5
nd
nd
nd
nd
2
5
1
2
Oct 75
6
nd
3
6
6
1
nd
5
1
3
6
2
nd
Jun 73
6
nd
1
3
nd
nd
nd
nd
nd
nd
nd
nd
nd
Subsoils ( 46-61 cm)
Apr 74*
6
nd
5
5
nd
nd
nd
nd
nd
nd
nd
nd
nd
Nov 74
6
nd
nd
3
5
nd
nd
3
nd
nd
2
nd
1
Apr 75
6
1
nd
2
2
nd
nd
nd
nd
nd
2
1
1
Oct 75
6
nd
1
2
1
nd
nd
nd
nd
nd
1
nd
nd
                            f Numbers of  samples in which detected.
                            * nd * none detected.
                            # First wastewater applications were made in late May 1974, after the Apr. 1974 sampling.
                             iGLC peaks for all chemicals listed  in Table  2,  Appendix II,  were monitored.   Only chemicals detected and confirmed
                              on cwo  or more  GC columns are reported.  Confirmation by  thin  layer was  required,  also,  except  at  concentrations  too  low for
                              spots to be visualized.

-------
             Table 59.   FREQUENCIES OF OCCURRENCE, TRACE ORGANICS IN SOILS, WHITEHALL, JUNE 73 TO OCTOBER 75.t


Total samples
Dieldrin
DDT species
Lindane £, isomers
Phorate
Lasso
2,4-D species
DEHP

Jun 73
2
1
2
nd*
nd
nd
nd
nd
Surface i
Apr 74
2
1
2
nd
nd
nd
nd
nd
soils ( 0-15 cm)
Nov 74#
2
nd
]
2
nd
nd
nd
nd
Apr 75
2
nd
2
1
nd
nd
nd
nd
Oct 75 Jun 73
2
nd
2
1
1
nd
2
I
2
nd
2
nd
nd
nd
nd
nd
Subsoils (46-61 ciu)
Apr 74
2
nd
nd
nd
nd
nd
nd
nd
Nov 74#
2
nd
nd
2
nd
nd
nd
nd
Apr 75
2
nd
nd
1
nd
1
nd
nd
Oct 75
2
nd
1
nd
nd
nd
nd
1
tNumber of  samples in which detected.
tfFirst wastewater applications were made in the fall of 1974, before the Nov.  74 sampling.
*nd=none detected
+GLC peaks for all chemicals  listed in Table  2,  Appendix II,  were monitored.   Only  chemicals detected and
confirmed on  two  or more GC columns are reported.  Confirmation  by  thin layer  was  required,  also,  except at
 concentrations too low for spots  to be visualized.

-------
                                       Table  60.  DETECTED RANGES OF CONCENTRATION.  TRACE ORGANICS IN SOILS, MUSKEGON, JUNE  73  TO  OCT  75.-
I-1
U>
O
Chemicals
Aldrin

Dteldrln

DDT species

Lindane plus
Isomers
Heptachlor plus
metabolites
Dlazlnon
Phorate
Atrazine
Lasso

2,4-D Species

DEHP
Surface soils (0-15 cm)

min
max
min
max
min
max
min
max
min
max
min
max
min
max
min
max
min
max
min
max
min
max
June 73
nd*

tr**
48.0
1.6
8.4
nd

1.5

nd
nd
nd
_ J
uQ
nd

nd
Apr 74#
nd

.1
3.1
1.8
4.4
nd

nd

nd
nd
nd
_ J
uQ
nd

nd
Nov 74
nd

nd

.9
12.7
.6
3.0
.1

nd
nd
230.0
490.0
4.4
11.4
nd

. 33x10:?
2. 84x10 J
Anr 75
Oct 75
- 2>0- ng/g -d

29.0

1.4
97.0
.1
7.0
nd

nd
nd
12.0
1.4x10
tr
39.0
23.3

4.0x10?
6.5x10

tr
17.0
.8
2.9
.4
7.8
.1

.8
10.0
9.0
31.0
108.0
1.0
58.0
1.0
5.0
nd
June 73
nd

.2

.1
.2
nd

nd

nd
nd
nd
nd

nd

nd
Subsoils (46-61cm)
Aor 74#
nd

.1
.5
.5
1.1
nd

nd

nd
nd
nd
nd

nd

nd
Nov 74
nd

nd

.1
3.1
.1
1.0
nd

4.2
12.0
nd
nd
2.7
3.9
nd

2.6xl03
Apr 75
tr

nd

.1
1.0
tr
.2
nd

nd
nd
nd
2.0
3.0
3.0

16.0xl03
Oct 75
nd

.2

tr
.2
.3

nd

nd
nd
nd

tr
nd

nd
                 *nd - not detected
                 **tr ** trace
                 t First wastewater applications were made In late May 1974, after the Apr 74 sampling.
                 i CLC peaks for all chemicals listed In Table 2, Appendix II, were monitored.  Only chemicals detected and
                   confirmed on two or more GC columns are reported.  Confirmation by thin layer was required, also, except at
                   concentrations too low for spots to be visualized.

-------
       Table 61.   DETECTED RANGES OF CONCENTRATION, TRACE ORGANICS IN SOILS. WHITEHALL, JUNE 73 TO OCTOBER 75.
Chemicals

Dieldrln

DDT species

Lindane plus
isomers
Phorate

Lasso

2,4-D species
DEHP



min
max
min
max
min
max
min
max
min
max
min
max
min
max
Surface soils (0-15 cm)
Jun 73 Apr 74 Nov 74J t
.1 .1 nd

4.8 1.3 2.3
10.2 2.8
nd* nd .4
.8
nd nd nd

nd nd nd

nd nd nd
nd nd nd


ipr 75 Oct 75
	 ng/g
nd nd

tr 1.8
.2 3.7
tr** tr

nd 64.0

nd nd

nd 3.6
13.9
nd 1.8x103

Subsoil!
Jun 73 Apr 74 1
nd nd

.2 nd
1.1
nd nd

nd nd

nd nd

nd nd
nd nd

J (46-61 cm)
tov 74* Apr 75 Nov 75
nd nd nd

nd nd tr

.1 tr nd
.5
nd nd nd

nd tr nd

nd nd nd
nd nd 700.

 * nd = not detected

** tr - trace


 #First wastewater  applications were made in Fall 1974,  before the Nov. 74 sampling.
*GLC peaks for all chemicals listed in Table 2, Appendix II, were monitored.  Only chemicals detected and
 confirmed on two or more GC columns are reported.  Confirmation by thin layer was required, also, except at concen-
 trations  too low for spots to be visualized.

-------
subsoils.  However, microbial populations with competence to degrade chlor-
inated cyclohexanes are favored by anaerobic conditions (Kaufman,  1974;
Matsumura, 1973).  With frequent irrigation, even on these well-drained soils,
appropriately oxygen-deficient conditions would likely attain for  significant
periods at some point in the profile.

Thus, enrichment of subsoils with adaptive microbial populations could have
contributed to low recoveries of lindane or other isomers in subsoils and
would account for the virtual disappearance of BHC species from drainage at
outfalls since early spring of 1975 (Tables 45, 46).

In the case of DEHP, substantial concentrations have continued to appear at
outfalls through 1975 (Tables 45 and 46).  However, these occurrences have
been associated with high hydraulic loadings.  The incidence of DEHP in waters
passing through the system has declined from sampling point to sampling point
(Table 47), and there has been a strong tendency for maximum concentrations
to decline also (Table 48).  This suggests that populations adapted to de-
grading DEHP are developing in lagoons and in soils.

Thus, it may be significant that DEHP was not found at any of the 6 special
study sites at Muskegon in Oct. 1975 (Table 58).  These samples were taken
at harvest time and no wastewater had been applied for periods of two weeks
or longer on any of the sampled circles.  There was very little rain during
this period either.  The increased retention time afforded by interrupted
 water applications may have permitted degradation of the latest inputs of
DEHP to non-detectable levels.

Lasso has been found in most surface soil samples taken since waste irriga-
tion and agronomic applications were initiated in 1974 (Table 58).  Concen-
trations encountered have increased in surface soils but not in subsoils
(Table 60).  It appears that this chemical is being intercepted to a large
extent in surface soil, but the combined inputs from wastewater and agronomic
applications have exceeded the capacity of microbial populations in the sur-
face soil to degrade it.

On the other hand, the incidence of Lasso at outfalls has declined  (Tables
45, 46, and 47).  Major appearances are associated with planting operations
and periods of heavy hydraulic loading.  Thus, it may be that mechanisms  for
removal of Lasso are developing in the soil profile.

Phorate was input frequently with wastewater and in substantial concentra-
tions in 1975 at Muskegon, and 2,4-D species at both Whitehall and Muskegon
(Tables  43, 47, and 48).  They were encountered in  soils for the first  time
in 1975  (Tables 58 and 59).  All except the methyl  ester of 2,4-D have
appeared at outfalls (Tables 45 and 46).

Phorate  is oxidized quickly in soils  (Getzin and Shanks, 1970; Hiltbold,  1974;
Kaufman, 1974), and 2,4-D esters are quickly hydrolyzed  (Loos,  1975).   It is
to be expected that they might be detected  transiently in soils, but  for
only short periods after input.

Phorate was encountered in soil once in 1975,  at Muskegon  (Table 55).

                                     132

-------
The methyl ester of 2,4-D was encountered on three occasions at Muskegon
(Tables 54, 55) and twice at Whitehall (Table 57).  The other 2,4-D esters
were not encountered at credible concentrations in soil, although their
presence was indicated in incoming waste water (Tables 39 to 43) and, at
Muskegon, in drainage at outfalls (Tables 45, 46).

Soil samples were taken before planting in the spring and during or immedi-
ately after corn harvest in the fall.  At these times, it was observed that
wastewater was being discharged on a number of circles through disconnected
sprinkler headers.  Areas affected by this off-season dumping of wastewater
were avoided in sampling.

The indicated appearance of readily altered compounds, such as phorate and
ester derivatives of 2,4-D, in drainage is evidence of excessively rapid
transit through the soil.  Since soil areas affected by dumping in spring and
fall were not sampled, chemicals input at these times would not have been
detected in soils even though they did appear in drainage.

"Unknown" Peaks —

Of the three "unknown" peaks monitored in 1975, only one appeared in extracts
of soils sampled in October.  This peak (Rt = 247-253 sec) was encountered
at all three depths in all circles sampled.  Peak areas were much less in
subsoils than in surface soil.  Nevertheless, this was the principal peak in
subsoils at Muskegon, accounting for 70 to 99% of total integrated peak area.
Proportionate areas for surface soils ranged from 20 to 40% and, for subsoils
at Whitehall, from 25 to 55%.

A qualitative assessment, based on these observations, suggests that the
chromatographic entity at Rt = 247-253 sec may be a fairly recalcitrant com-
pound.  It appears to react rather strongly with surface soil materials but
can be displaced downward under conditions of heavy hydraulic loading.  It
appeared as a prominent peak in 3 of 10 outfall samples taken from August
through December 1975 (28 to 37% of total integrated area in the first Flori-
sil eluant).  Retention time and behavior on Florisil corresponded to a
prominent peak in reference standards for Arochlors 1254 and 1260, but other
peaks characteristic for these formulations were not present.

The entity at Rt = 115-118 sec may not interact so strongly with soil
materials since the peak did not appear in soil extracts but was prominent
in 7 of 10 outfall samples (20 to 40% of total integrated area).  It is pos-
sible that this is not a single compound, since the peak appeared variably
in one or another of the three Florisil fractions.

The third "unknown" (Rt = 164-168 sec) did not show in chromatograms for soil,
and the peak encountered in occasional outfall samples was small.  The indi-
cated level of input at Muskegon was low.  Also more than one species was
probably involved, since the distribution among Florisil eluants varied.
                                     133

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EVALUATION OF METHODS

The identification of trace organics in this study was  presumptive,  based
on chromatographic parameters only.   Nevertheless, identities  were corro-
borated on three or more media.   Circumstantial support for  most pesticide
species was found in known sales or  known patterns of use in river basin
areas which drain to Muskegon Lake,  Mona Lake or White Lake.  Encounters with
specific pesticides were associated  with weather conditions  conducive to
runoff and heightened stream flow in these drainage basins.

The observed patterns of encounter with pesticides in wastewaters are
significant mainly as evidence that  chemicals from non-point sources in ex-
tensive regional watersheds can enter these sewage collection  systems through
connected discharges from industries that draw feedwaters from these lakes or
tributary streams.  In addition to pesticides and other non-point-source
chemicals, the potential exists for  entry of chemicals that  originate in in-
dustrial and municipal discharges at remote outfalls along the tributary
streams.  For example, twenty industries and nine municipalities use the
Muskegon River for wastewater assimilation.

The very much greater and immediate  hazard from chemicals input within areas
served by the two sewage collection  systems was addressed only superficially
by methods employed here.  In the broad, diverse category of industrial
organics, credible data were obtained only for DEHP.  At least three other
electron-capturing species were present chronically and at indicated concen-
trations that were frequently greater than for referenced compounds.
Numerous small peaks and occasional prominent peaks at retention times not
programmed for routine integration were ignored.

The monitored peaks probably account for much of the total mass of electron-
capturing species in the GLC column effluent from sample injections.  Many
chemicals volatile enough to move with the carrier gas stream would not have
been detected by electron capture.  Derivitization was not employed to permit
detection of non-volatiles.  Not all polar compounds would have partitioned
into the initial methylene chloride extracts, and others would have been
eliminated during cleanup and final transfer into hexane.

It has been estimated that no more than 10 or 20 percent of the organics
in wastewaters are accounted for by established methods for sampling, ex-
traction, concentration, separation and detection  (Donaldson, 1977).  The
percentage accounted for in the present study was undoubtedly even  less.

With regard to sampling, the use of grab samples here was particularly  in-
appropriate for incoming wastewaters because of the episodic nature of  inputs,
from both industrial and non-point sources.  With normal operation, less
short-term variation would be expected in  irrigation water  or drainage  because
of the  large mixing volumes and relatively long retention times in  lagoons
and soils  (Robert S. Kerr Environmental Research  Laboratory, 1977).  Never-
theless, observed breakthroughs of labile  compounds like phorate and 2,4-D
esters  are evidence that significant short-term discharges  to surface streams
can occur when unusual operating procedures are employed, as when storage
lagoons are by-passed or when wastewater is applied through disconnected


                                    134

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sprinkler headers.

Continuous sampling devices would appear essential for incoming waste-waters
and at least desirable for other flow points.   Analyses should be scheduled
more frequently than once a month to increase the likelihood for detection
of chemicals input sporadically and to reduce the opportunity for loss or
chemical alteration during cumulative storage.  To assess performance, for
purposes of surveillance and as a guide for on-site management, the frequency
of analysis at different flow points should be related to retention times in
various components of the system, with due regard for seasonal and ad hoc
changes in modes of operation.

Methods used in this study for extraction, concentration, separation and
detection were limited in the number of organics which could be detected as
well as in the discreteness of separation of such important classes of com-
pounds as chlorinated hydrocarbon pesticides and polychlorinated biphenyls.
The range of detectable chemicals can be extended and separations greatly im-
proved by moderately greater detail in preparatory protocol.  Substantially
greater detail can be achieved, together with increased efficiency, by such
measures as the use of selective accumulators in continuous sampling devices
to effect preliminary fractionation and concentration, thereby eliminating
some of the time consuming steps in the laboratory (Donaldson, 1977).

Electron capture is appropriate for detection of many of the compounds of
known concern in industrial discharges into the Muskegon and Whitehall
systems.  Numerous detection methods are available, covering a wide range of
sensitivity and specificity for different types of compounds.

Protocols are being developed for comprehensive analysis of organics in
wastewaters, using advanced instrumentation and computer methodologies (Robert
S. Kerr Environmental Research Laboratories, 1977).  The cost, if large num-
bers of compounds are to be monitored, will be high.  In particular, costs
and time constraints will preclude indiscriminate monitoring for the hundreds
of compounds of known or suspected hazard.

A feasible protocol for monitoring the Muskegon County systems, or any other,
must evolve around a rational ordering of compounds to be monitored.  Priori-
ties should be based primarily on known or reasonably suspected consequences
of environmental release.  National guidelines for establishing priority
among potential toxicants are being developed (TSCA Interagency Testing
Committee, 1977).  However, the determination for a given system should be
guided also by the best available information regarding chemicals which are
known or reasonably expected to enter the system.

In the case of the Muskegon County systems, several compounds and categories
of compounds of recognized hazard have been identified in recent surveys and
special studies conducted by state water quality control personnel.  These
compounds should be given immediate attention in terms of defining input and
fate in the treatment systems.  Priorities and analytical protocols can be
expanded as additional critical compounds are identified in source discharges
or as chronic or unusual chromatographic entities at treatment sites.  Of
crucial importance to this end will be the responsible disclosure of critical


                                    135

-------
materials and campaign schedules by industries within the service areas and
in tributary river basins.

Back-up analytical capability for positive identification should be provided,
initially at least, by federal or state agencies.  Once a chemical has been
identified as a chronic input or an expected occasional input from a given
source or scheduled process, retention times on appropriate chromatographic
media can be used for monitoring.  It is possible that recognition by industry
of its stake in the integrity of these systems might lead to local funding
to support the sophisticated back-up facilities necessary for positive veri-
fication or ab jjjlijtio. identification of chromatographic entities encountered
in source discharges or in combined flows entering the treatment systems.

It is apparent that each compound may interact uniquely with different com-
ponents of the treatment system.  The fate of each should be followed—as a
guide both for on-site management and for regulation by public agencies.
Data for the referenced chemicals in this study illustrate the influence of
operational procedures on renovative effectiveness at the Muskegon site.
Observed developmental trends for chronically input species  (lindane, hepta-
chlor, related species, DEHP) are encouraging.  They suggest that, with ap-
propriate management, land application in combination with economical pre-
treatment and a period of detention in storage lagoons can very greatly
reduce, if not eliminate, the hazards associated with exotic organic
toxicants in industrial and municipal wastes.
                                     136

-------
SUMMARY — TRACE ORGANICS

1.  Local and regional hydrologic systems were described  in  some  detail with
a view to identifying probable sources and modes  of  entry for  trace  organics
into wastewater collection systems at Muskegon and Whitehall.

2.  Patterns of encounter with 26 pesticide parameters provide evidence that
chemicals from non-point sources can enter these  systems  through  connected
discharges from industries that take their feedwaters from Muskegon  Lake,
Mona Lake, White Lake or tributary streams.  By inference, chemicals origin-
ating at extramural point-sources can be expected also.

3.  A wide range of industrial chemicals which have  become the focus of con-
cern in these systems was not addressed by analytical methods  used in this
study.  Credible evidence for chronic entry of DEHP  was obtained.  Peaks  for
several unreferenced electron capturing species were present frequently in
incoming wastewater but were not identified.

4.  In background soil samples, dieldrin and DDT species  were  indicated at
the very low concentrations that might be expected from global circulation,
with evidence at one sampling station for locally higher  residues from
earlier use.

5.  Chromatographic peaks observed in incoming wastewaters and peaks for  pes-
ticides used on site were found in extracts of soils after the systems were
placed in operation in 1974.  Both referenced and unreferenced species were
found mainly in surface (0-15 cm) and shallow subsurface  layers (46-61 cm).
Encounters at 91-107 cm were infrequent or at levels approaching  the limit
for quantitation.

6.  Outfalls were monitored only at the Muskegon site. Significant break-
throughs, observed for a number of chemicals, were associated  with heavy
rains or with seasonally expedient modes of operation that resulted in un-
usually heavy applications of wastewater on limited  soil  areas.

7.  Data for successive flow points at Muskegon indicate  that  removals of
trace organics occurred both in storage lagoons and  during passage through
the soil mantle.  Chemicals intercepted most effectively  were  those that  are
Strongly adsorbed by soils or sediments and those that are readily metabo-
lized.  Chemicals responsible for unreferenced GLC/ECD peaks appeared to  be
more recalcitrant or more mobile in soils than the referenced  species.

8.  Chemicals observed frequently in incoming wastewater  (lindane, heptachlor,
related species, DEHP) declined in frequency and concentration at outfalls
from 1974 to 1975.  This is hopeful evidence that the efficiency  of the system
in removing exotic chemicals may improve over time.   Beneficial developmental
changes may include the induction of adaptive enzymes in  lagoons  and soils,
increasing volume and adsorptive surface of sediments in  lagoons, and in-
creased annual return of crop residues and exudates  to support co-metabolism
of recalcitrant compounds in soils and residual increases in adsorptive soil
organic matter.
                                    137

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RECOMMENDATIONS

Monitoring Priorities

In recent surveys and special studies by control agency  personnel,  several
compounds and categories of recognized hazard have been  identified  in  surface
and groundwaters in the Muskegon area.  These chemicals  should be given  im-
mediate but orderly attention in terms of defining input and fate in these
treatment systems.  An ordering of priorities among candidate compounds  is
essential for selecting analytical methods that are specific for the com-
pounds sought and realistic in relation to available facilities, personnel
and funds.

Relations with Industry

Responsible reporting of critical materials is essential for developing  moni-
toring priorities.  In addition to raw materials and major products, listings
should include by-products, known or likely, and best determined by the  manu-
facturer.  Appropriate confidentiality should be accorded proprietary  pro-
cesses.  However, production schedules should be reported in sufficient
detail to serve as a guide for monitoring.  In particular, monitoring  per-
sonnel at the treatment sites should be alerted to anticipated  critical
discharges.

Regulatory pressures and essential adversary positions should be tempered by
recognition of the mutual concerns of industry and the general  public  in main-
taining beneficial production consistent with beneficent control of products
and by-products.  Recent events make  it clear that industry's good faith in
these matters is  essential.  In turn, industry should be brought into delib-
erations leading  to choice of regulatory priorities, since cost-benefit dis-
tributions are a  necessary consideration.

Also, specialized expertise  in  industry can contribute  to development of con-
trol technologies.  Integration of public and private resources and analyti-
cal capabilities  can contribute to the effectiveness of monitoring for pur-
poses of surveillance  as well as  for  control of processes both in production
and in waste  treatment.

On-Site Monitoring

Routine monitoring  of  waters at key  flow  points  is essential for rational
management of the wastewater treatment  systems.   This can best be  done by
personnel  and analytical facilities  at  the Muskegon site.

Points  to  be  monitored should  permit assessment of changes  that occur during
 important  phases of treatment:  pretreatment,  storage,  chlorination,  passage
 through  the soil mantle.   Continuous sampling at all points is desirable but
would  appear  essential for incoming  wastewater and at outfalls.  Continuous
 sampling of incoming wastewater may  be  more feasible at point of discharge
 into  storage  than for raw  influent.

 Chemicals  to  be followed within the  system should be selected from those for


                                     138

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which compliance monitoring is required at outfalls.   Internal priorities,
must, however, allow for following individual chemicals over  sufficient
periods of time for their behavior to be reasonably understood and for
developmental trends to be expressed.  Useful operational data can be ob-
tained most readily for compounds that are input chronically.   Flexibility
should be developed, also, for following critical chemicals that  enter only
occasionally.

Frequency of analysis (and frequency of sampling if grab samples  are used)
should be related to periodicity of inputs and to retention times in dif-
ferent components of the system.  It is in this connection that it is impor-
tant for industries to give accurate and timely notice of production schedules
that involve critical discharges into the system.

Requirements for obtaining sound operational data within the treatment systems
should be recognized by control agencies in establishing priorities for  moni-
toring in compliance with external regulations.  Priorities should be revised
as new criteria appear for assessing hazard, or as appropriate analytical
capabilities are realized.

RESEARCH NEEDS

Analytical Methods

The development of analytical procedures must proceed hand in hand with the
development of monitoring priorities.  Both must recognize limitations of
available instrumentation, personnel and funds.  Methods for a given chemical
or group of chemicals should be evaluated and quality control parameters es-
tablished before routine monitoring is undertaken.

Backup capabilities for positive identification are costly and will need to
be supplied, initially at least, by federal or state agencies or through con-
tract with public or private research organizations.  Once identities have
been established by definitive methods, chromatographic parameters can be
used for monitoring and for confirmation with reasonable assurance.

To expedite processing, sampling devices equipped to effect initial fraction-
ation and concentration should be investigated.

Fate of Trace Organics

Useful operational data can be obtained by routine monitoring of waters at
key flow points in the system.  However, evaluation of management alternatives
for prediction purposes over the long term must be based on a fundamental
understanding of the extent to which individual chemicals are detained,  par-
titioned, altered or metabolized in different components of the system.

On the basis of data reported here, immediately useful studies might be  under-
taken with lindane, heptachlor, related species, and DEHP since they appear
to be input chronically and because a great deal is known about their inter-
actions (or those of closely related compounds) in natural systems.  Of
specific concern would be the extent to which induced enzymes, cometabolism


                                     139

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or adsorption in soils  or  sediments may have contributed to increasing effec-
tiveness in removal,  as evidenced by  decreasing  frequencies and concentrations
at outfalls.

Chemicals received from industry undoubtedly include numerous photosensitive
and photo-sensitizing species.   Because of  the large area for exposure in
storage lagoons, significant photochemical  alterations  can be expected and
should be investigated.  Changes due  to chlorination after storage  should be
examined also.

In anticipation of the time when sludges  may need  to be removed from pretreat-
ment basins or storage lagoons,  an  inventory should be  made of potential toxi-
cants that may have accumulated. Patterns  of release during decomposition  of
sludges in soil should be examined.   A continuing  concern will be  the possi-
bility that specific toxicants may  be transferred  from  sludges or  from waste-
water into animal feeds and human food channels.

Modeling

Many kinds of information from many sources bear on the successful management
and responsible regulation of these systems.  To facilitate accumulation, re-
trieval and manipulation of relevant  information,  continuing attention should
be given to developing comprehensive  conceptual  models  that will  include
wastewater collection and wastewater  treatment in  their relation  to hydrolo-
gic and other systems that can influence  or be influenced by them.

Provision should be made to accommodate surveillance  fee  listings,  opera-
tional schedules and monitoring  data  for  directly  connected point  sources as
well as for point sources in contributing watersheds.   Feedwater  sources and
volumes for connected industries should be  known.   Other  useful  information
would include land use parameters,  weather  data, stream flow data,  and sales
or management practices that reflect  use  of critical  materials  in contribu-
ting watersheds.
                                     140

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                                 REFERENCES

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     New York.  (2nd edition).

Aly, 0. M. and S.  D. Faust.  1964.  Studies on the fate of 2,4-D and ester
     derivatives in natural surface waters.  J.  Agr. Food Chem. 12:541-546.

Arthur, R. D., J.  D. Cain and B. F. Barrentine.   1977.   DDT residues in air
     in the Mississippi Delta,  1975.  Pestic. Monit. J. 10(4):168.

Biggar, J. W. and R. L. Riggs.   1974.  Apparent solubility of  organochlorine
     insecticides in water at various temperatures.  Hilgardia 42(10):383-391.

Carey, Anne E., G. B. Wiersma and H. Tai.  1976.  Pesticide Residues in urban
     soils from 14 United States cities, 1970.  Pestic. Monit. J. 10(2):
     54-60.

Crockett, A. B., G. B. Wiersma, H. Tai, W. G. Mitchell, P. F.  Sand and
     Anne E. Carey.  1974.  Pesticide residue levels in soils  and crops,
     FY-70—National Soils Monitoring Program (II).  Pestic. Monit. J.
     8(2):69-97.

Directory of Michigan Manufacturers.  1976.  Published by Michigan Manufac-
     turer and Financial Record, Detroit.

Edwards, C. A.  1973.  Pesticide residues in soil and water.  Pp. 409-458.
     In C. A. Edwards (ed.) Environmental pollution by pesticides.   Plenum
     Press, New York.

Filonow, A. B., Y.-O. Shin and A. R. Wolcott.  1977.  Sequential extractions:
     An approach to characterizing pesticide-organic matter interactions.
     ^n_A. Banin (ed.) Agrochemicals in Soils.  Proceedings, International
     Congress of Commissions II, IV and V, International Society of Soil
     Science, Israel, 1976.  (In Press).

Garrett, D., F. P. Maxey and H. Katz.  1976.  The impact of intensive appli-
     cation of pesticides and fertilizers on underground water recharge areas
     which may contribute to drinking water supplies.  EPA 560/3-75/006.

Getzin, L. W. and G. H. Shanks, Jr.  1970.  Persistence,  degradation, and
     bioactivity of phorate and its oxidative analogues in soils.  J. Econ.
     Entom. 63:52-58.
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Glooschenko, W.  A.,  W.  M.  J.  Strachan and R.  C.  J.  Sampson.   1976.   Distri-
     bution of pesticides  and polychlorinated biphenyls  in water,  sediments
     and seston of the  upper  Great Lakes—1974.   Pestic. Monit.  J.  10(2):
     61-67.

Gunther, F. A.,  W. E. Westlake,  and P. S. Jaglan.   1968.  Reported solubili-
     ties of 738 pesticide chemicals in water.  Res.  Rev. 20:1-148.

Hall, J. R., E.  A. Jarecki, T. J.  Monteith,  W. E.  Skimin and W.  C.  Sonzogni.
     1976.  Existing river mouth loading data in the  U.  S. Great Lakes Basin.
     International Joint Commission on the Great Lakes.  Great Lakes Basin
     Commission, Ann Arbor.

Hamaker, J. W.  1972.   Diffusion and volatilization,  Pp. 341-397.  T-n
     C. A. I. Goring and J. W. Hamaker (eds.) Organic chemicals in the soil
     environment.  Marcel Dekker,  New York.

Hamaker, J. W. and J.  M. Thompson.  1972.  Adsorption.  Pp.  49-143.  In
     C. A. I. Goring and J. W. Hamaker (eds.) Organic chemicals in the soil
     environment.  Marcel Dekker,  New York.

Hiltbold, A. E.   1974.   Persistence of pesticides in soil.   Pp. 203-222.
     _In_ W. D. Guenzi (ed.) Pesticides in soil and water.  Soil Sci. Soc.
     Amer., Madison, WI.

Hrutfiord, B. F., T. S. Friberg, D. F. Wilson and J.  R.  Wilson.  1975.
     Organic compounds in pulp mill lagoon discharges.  EPA-660/2-75-028.

International Joint Commission, Great Lakes Water Quality Board.  1976.
     Great Lakes Water Quality, 1975.  Annual report, June 1976.

Jackman, J. A., A. W.  Bloomer and D. L. Haynes.  1976.  Pesticide use and
     residues in a Michigan community.  Res. Rpt. 303, Mich. Agr. Exp. Sta.

Jackson, M. D., T. J.  Sheets and C. L. Moffett.  1974.  Persistence and
     movement of BHC in a watershed, Mount Mitchell State Park, North
     Carolina—1967-72.  Pest. Monit. J. 8(3):202-208.

Kaufman, D. D.  1974.   Degradation of pesticides by soil microorganisms.
     Pp. 133-202.  In_ W. D. Guenzie  (ed.) Pesticides in soil and water.
     Soil  Science Society of America, Inc., Madison, WI.

Lake Michigan Interstate Pesticides Committee.  1972.  An evaluation  of DDT
     and dieldrin in Lake Michigan.  EPA-R3-72-003.

Lichtenberg, J. J., J. W. Eichelberger,  R. C. Dressman and J. E. Longbottom.
     1970.  Pesticides in surface waters in  the United States—a 5-year
     summary, 1964-1968.  Pestic. Monit. J.  4:71-86.

Loos, M. A.  1975.  Phenoxyalkanoic acids.   Pp. 1-128.  In P. C. Kearney  and
     D. D. Kaufman  (eds.) Herbicides:  Chemistry, degradation, and mode of
     action.  (Vol. 1).  Marcel Dekker,  New  York.

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Manthy, R. S., L. M. James and H.  H.  Huber.  1973.   Michigan timber produc-
     tion—now and in 1985.  Research Rpt. 192.  Michigan Agricultural
     Experiment Station and Cooperative Extension Service.

Matsumura, F.  1973.  Degradation of pesticide residues in the environment.
     Pp. 494-513.  T-n_ C. A. Edwards (ed.) Environmental pollution by pesti-
     cides.  Plenum Press, New York.

Merkle, M. G. and R. W. Bovey.  1974.  Movement of pesticides in surface
     water.  Pp. 99-106.  In W. D. Guenzi (ed.) Pesticides in Soil and
     Water.  Soil Sci. Soc. Amer., Madison WI.

Metcalf, R. L.  1973.  A century of DDT.  J. Agr. Food Chem. 21:511-519.

Michigan Water Resources Commission.   1973,74,75.  Surveillance Fee Listings
     and Industrial Wastewater Surveys.  Water Quality Control Div.,
     Mich. Dept. of Natural Resources.

Miles, J. R. W.  1976.  Insecticide residues on stream sediments in Ontario,
     Canada.  Pestic. Monit. J. 10(3):87-91.

Miles, J. R. W. and C. R. Harris.  1973.  Organochlorine insecticide
     residues in streams draining agricultural, urban-agricultural, and
     resort areas of Ontario, Canada—1971.  Pestic. Monit. J. 6(4):363-368.

Minnesota Pollution Control Agency.  1971.  Pesticide inputs and levels.
     Minnesota waters—Lake Superior Basin.  USEPA 16050 EYT 06/71 (108pp.)

Muskegon County Department of Public Works.  1975.  Muskegon County, Where
     Wastes are Resources.  Public Information Leaflet.

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     1968; Newaygo County, 1973; Oceana County, 1972; Osceola County, 1969.
     Michigan Agricultural Experiment Station.

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     Jan. to Dec. 1974.  Entomological Special Study No. 44-011-75/76.
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     EPA Report 660/3-74-002.

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                                 APPENDIX 1

                     METHODS OF ANALYSIS FOR NUTRIENTS

PROCEDURES

Total Carbon

Reagents —

1.  Tin Metal Accelerator, Leco Co.
2.  Iron Chip Accelerator, Leco Co.
3.  Carbon Steel Standards, Leco Co.  (0.074 to 0.862% C).

Procedure —

Grind soil samples in a SPEX Industries ball grinder to reduce the particle
size.  Weigh 50 to 100 rag of soil sample (depending on the carbon content)
into ceramic cups.

Add 0.8 g of each accelerator and mix.   The sample is placed in the furnace
and ignited and total carbon read from the instrument.

Total Nitrogen

Reference —

Bremner, J. M.  1965.  Total Nitrogen.   Chapter 83 in Methods of Analysis.
Agronomy No. 9, part 2.  Chemical and Microbiological Properties.

Reagents —

1.  Sulfuric acid(H2SO^), concentrated.

2.  Sodium Hydroxide (NaOH), approximately 10 N:  Place 4.2 kg of NaOH in a
heavy-walled 10-liter Pyrex flask, add 4 liters of water,  and swirl the flask
until the alkali is dissolved.  Cool  and allow to stand for several days to
settle out N32C03, and siphon the clear supernatant liquid into a large Pyrex
bottle which contains about 1.5 liters of C02~free water and is marked to in-
dicate a volume of 10 liters, and make the solution to 10 liters by addition
of C02~free water.  Mix well and protect from entry of atmospheric C02.

3.  Boric acid-indicator solution:  Place 80 g. of pure boric acid (HoBOo)
in a 5-liter flask marked to indicate a volume of 4 liters, add about 3,800
ml of water, and heat and swirl the flask until the ^BO-^ is dissolved.  Cool
the solution and 100 mis of methyl purple indicator (Fisher's) or add 2 drops
of indicator just prior to titration.
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4.  Potassium sulfate-catalyst  mixture:   Prepare an  intimate mixture of 100
g of K2S04,  10 g of copper sulfate  (CuS04'5H20) , and 1 g of Se.  Powder the
reagents separately before mixing,  and  grind  the mixture in a mortar to pow-
der the cake which forms during mixing.

5.  Sulfuric (or hydrochloric acid) (I^SO^ or  HC1) , 0.01 N  standard.

Procedure —

Place a sample containing about 1 mg of N in  a dry micro-Kjeldahl  flask,  add
2 ml of water, and after swirling the flask for a few minutes,  allow it to
stand for a further 30 minutes.  Then add 1.1 g of K^SO^-catalyst  mixture and
3 ml of concentrated I^SO^, and heat the flask cautiously  on  the digestion
stand.  When the water has been removed and frothing has ceased, increase the
heat until the digest clears, and thereafter  boil the mixture gently for  3
hours.  Regulate the heating during this boiling  so  that the  t^SO^ condenses
about one-third of the way up the neck  of the digestion flask.

After completion of digestion,  allow the flask to cool, and add about  20  ml
of water (slowly, and with shaking). Then swirl  the flask to bring any in-
soluble material into suspension.  Place 5 mis of boric acid  indicator in a
50 ml Erlenmeyer flask and place the flask under  the condenser. Connect  the
micro-Kjeldahl flask to the distillation unit, add  15 mis  of  NaOH  solution
(reagent 2) and steam distill until 35  mis of volume is collected. Remove
the 50 ml flask, disconnect the steam,  and rinse  the tip of the condenser in-
to the flask and titrate the ammonium present with  0.01 N  acid  from a  10  ml
graduated burette  (graduated in 0.01 ml intervals).

Extractable Ammonium

Reagents —

1.  2N KC1.  Weigh 149.2 g KC1  into a one liter volumetric flask.   Add dis-
tilled water to give one liter.

2.  0.1N NaOH.  Weigh 4 g of NaOH pellets into a  one-liter volumetric  flask.
Add distilled water to give one liter.

3.  Sulfuric  (or hydrochloric acid)  (^SO  or HC1) ,  0.01 N standard.
4.  Boric acid-indicator solution:  Place 80 g of pure boric acid (H^BOg) in
a 5-liter flask marked to indicate a volume of 4 liters, add about 3,800 ml
of water, and heat and swirl the flask until the ^603 is dissolved.  Cool
the solution and add 100 mis of methyl purple indicator (Fisher's) or add 2
drops of indicator just prior to titration.

Procedure —

Weigh 10 gms of moist soil into a 125 ml Erlenmeyer flask, add 50 ml of
2N KC1.  Shake for 2 hours on a rotary shaker at 200 rpm.  Filter through
Whatman //42 filter paper.  Pipette 10 mis of filtrate into Kjeldahl flask,
attach to steam distillation apparatus, add 10 mis of 0.1N NaOH and steam

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distil the NHg into 5 ml of boric acid-indicator solution.   Titrate  to  end-
point with standard sulfuric acid.

Ammonium Acetate Extractable Cations

Reagents —

1.  Ammonium acetate extracting solution:   Dilute 114 ml of glacial  acetic
acid (99.5%) with water to a volume of approximately 1 liter.   Then  add 138
ml of concentrated ammonium hydroxide (NH^OH),  and add water to obtain  a
volume of about 1,980 ml.  Check the pH of the  resulting solution, add  more
NH^OH as needed to obtain a reaction of pH 7, and dilute the solution to a
volume of 2 liters with water.

2.  Standard solutions:

     Calcium:  Dry CaC03 at 105° c.  Then weigh 2.497 g into a 1 liter  volu-
     metric flask, add 200 mis distilled water  and 75 mis of 2 N HC1.  Agi-
     tate until dissolved, then dilute to volume with distilled water.   Final
     solution = 1000 ppm Ca.

     Magnesium;  Clean magnesium ribbon with 0.1 N HC1 and wash with distilled
     water.  Dry at 105° c.  Weigh 1.0000 g into a 1 liter volumetric flask,
     add 90 mis 2N HC1 and agitate until dissolved.  Dilute to volume with
     distilled water.  Final solution = 1000 ppm Mg.

     Potassium;  Dry KC1 at 105° c.  Then weigh 1.9066 g into a 1 liter vol-
     umetric flask.  Add 50 mis 2N HC1 and dilute to volume with distilled
     water.  Final solution = 1000 ppm K.

     Sodium:  Dry NaCl at 105° c.  Then weigh 2.542 g into a 1 liter volumet-
     ric flask.  Add 50 mis of 2 N HC1 and dilute to volume with distilled
     water.  Final solution = 1000 ppm Na.

Procedure —

Weigh 5 g of soil into a 125 ml Erlenmeyer flask and add 50 ml of ammonium
acetate extracting solution.  Shake for one hour on a rotary shaker  at  200
rpm, filter through Whatman No. 2 or equivalent paper, and determine Ca and
Mg by comparison with standards on an Atomic Adsorption spectrophotometer and
Na and K by comparison with standards on a flamephotometer.

Chelate Extractable Heavy Metals

Reference —

Lindsay, W. L. and W. A. Norvell.  1969.  Development of a DTPA Micronutrient
Soil Test.  Agronomy Abstracts, p. 84.

Reagents — 1.  Extracting solution (0.005 M DTPA, 0.01 N CaCl2 and  0.1 M
Triethanolamine):   Weigh 3.96 g DTPA 2.22  g CaCl2 and 29.84 g Triethanolamine
into a two liter volumetric flask and bring to  volume with re-distilled water.

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Procedure —

Weigh 10 g soil into 250 ml polypropylene  bottles, add 20 ml of extracting
solution.  Shake on a reciprocal shaker  for  2 hours, filter through Whatman
number 2 filter paper and analyze the  filtrate  for Cu, Fe, Mn, Zn, and Pb by
comparison with standards on an atomic absorption spectrophotometer .

Digestion with Hydrofluoric and Perchloric Acids for Total Analysis

Reference —

Pratt, P. F.  1965.  Chapter 60.  In Methods of Soil Analysis Chemical and
Microbiological Properties.  Agronomy  No.  9, Part 2.

Reagents —

1.  Hydrofluoric acid (HF) , 48%
2.  Perchloric acid (HC104), 70-72%
3.  Hydrochloric acid (HC1) , 6 N
4.  Nitric acid (HN03) ,  70%.

Procedure —

Weigh a 0.5 g sample of  finely ground  soil in  a 30 ml  platinum crucible.  Wet
the soil with a few drops of water, and  add  5  ml of HF and 0.5 ml  of  HC104.
(With surface soils, add 3 ml of HNOo, heat  at 200 C until dry,  cool  and  add
3 ml of HN03 and 1 ml HCIO^ and heat on  a  hot  plate until the white fumes
of HC104 appear.  Cool and add 5 ml HF.)  Place the crucible  in  a  sand bath
and cover with about nine-tenths of the  crucible top with a platinum  lid.
Heat the crucible to 200 to 225 C and  evaporate the contents  to  dryness.
Cool the crucible, and add 2 ml of water and a few drops of HC104. Replace
the crucible in the sand bath, and evaporate the contents to  dryness. If or-
ganic matter stains are still present  on the sides or  lid of  the crucible,
direct the flame of a Meker burner onto  the  sides and  lid until  the organic
matter is oxidized.  Remove the crucible,  cool, add 5  ml of 6N HC1 and about
5 ml of water.  Heat until the solution boils  gently.   If the sample  does not
dissolve completely, evaporate the solution to dryness and repeat  the proce-
dure, starting with 5 ml of HF and 0.5 ml of HCIO^.  When the residue com-
pletely dissolves in HC1, transfer the sample  to a  50-ml volumetric flask,
and dilute the content to volume.

Extractable P

Reagents —

1.  Extracting solution.  Add 15 ml of 1.0 N NH4F  and  25 ml  of 0.5 N  HC1  and
460 ml of distilled water to prepare each 500  mis  of  extracting  solution.
 2.  Ammonium molybdate-HCl-H3B03 solution.  Dissolve 100 g (NE^ ^NoO 2^ '4^0
 in 850 mis distilled water, filter and cool.  Add 1700 mis concentrated HC1
 to 160 mis water, cool.  Mix the two solutions slowly and add 100 g of boric
 acid.

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3.  Reducing agent mixture.   Mix 10  g  l-amino-2-naphthol-4-sulfonic acid with
20 g sodium sulfite and 584  g sodium bisulfite, meta.  Grind mixture to a
fine powder with morter and  pestle.

4.  Reducing solution.   Dissolve 15.4  g  of  reagent no. 3  in 100 mis warm dis-
tilled water.  Cool and filter.

5.  Standard phosphate  solution:   Dilute 0.4393 g of oven-dry KI^PO^ to 1
liter in a volumetric flask  with distilled  water.  Working standards are
prepared by dilution of this 100 ppm P stock solution.

Procedure —

Weigh 5 g of soil into  a 125 ml Erlenmeyer  and add 20 mis of extracting solu-
tion (reagent no. 1).  Shake on a rotary shaker at 200 ppm for one minute,
and filter the contents through Whatman  No. 2 or 42 filter paper.   (1  g of
acid washed activated charcoal is added  if  the filtrates  are not clear).

Pipette a 5 ml aliquot  of the filtrate into a 50 ml flask.  Adjust pH  to 3.0
using 2,4 dinitrophenol as an indicator. Add 2 mis of ammonium molybdate
solution and about 40 mis distilled  water.    Shake and add 2 mis of reducing
solution, and make to volume with distilled water.  Mix and after 10 minutes,
but before 15 minutes,  measure the color photometrically  using 660 mu  incident
light.

Water Soluble Nitrate

Reagents —

1.  Saturated calcium sulfate (CaSO^).  Add slightly more than two grams
CaSO^ per liter, shake  thoroughly and  allow to equilibrate overnight before
using.

2.  Standard nitrate.  Weigh 7.216 g of  KNO^ (previously  dried for 24  hours
at 105 C) into a one liter volumetric  flask and add distilled water to give
one liter.  Working standards of 1 to  50 ppm N are prepared by appropriate
dilution of this standard with the calcium  sulfate solution.

Procedure —

Weigh 20 grams of freshly sampled soil into a 125 ml Erlenmeyer flask, add
50 mis of saturated calcium  sulfate  solution. Shake for  1/2 hour on a rotary
shaker at 200 rpm.  Decant liquid into a 50 ml beaker and measure nitrate
content with a specific ion  electrode.  (Orion electrod for nitrate in con-
junction with an Orion  801 meter is  presently used in this laboratory.)
Standardize the electrode and meter  each time with known  standards covering
the range of nitrate that is in the  samples being measured.  Also recheck
standards after each few analyses.
(Note:  For low nitrate contents, the  method of Lowe and  Hamilton is recom-
        mended.)
(Note:  Moisture determinatiors are  carried out simultaneously on the  soils
        and the nitrate nitrogen values  are reported on a dry wt. basis.)

                                    149

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                                APPENDIX II.

                    ANALYTICAL PROCEDURES FOR TRACE  ORGANICS

                            IN SOILS  AND WATERS

                A.  B.  Filonow, R.  Cabrera and A.  R.  Wolcott

                     Department of Crop and Soil  Sciences

                         Michigan  State University

                               February 1976

Methods used in these studies have been drawn from numerous  sources.   The
following (see list of references) have been consulted for guidance  in
adapting procedures for routine analysis:  Pionke and Chesters,  1968;
Thompson, 1972; Federal Working Group on Pest Management, 1974,  1975.

The several phases of the operation are considered separately:   sampling of
soils; sampling of waters; soil extraction; water extraction;  separation and
clean-up; gas-liquid chromatography;  thin layer  chromatography;  analytical
quality control.

SAMPLING OF SOILS

Separate samples are taken at arbitrary increments of depth,  depending on
the monitoring or other objective.  Surface samples  through  the  plow layer
may be taken with a core sampler designed to minimize contamination  of in-
cluded increments.  Ten cores per  sample are composited.

Where subsoils are sampled, a standard 3-inch bucket auger  is used.   An
uncontaminated sample for each desired depth is  retained  from the central
and lower sections of the bucket.   A minimum of  four auger  cores is  com-
posited per depth sample.

Composite samples are combined and mixed in the  field.  The  composites are
first passed through a stainless steel sieve (5  mm openings)  and mixed
thoroughly in a 3-gal stainless steel pot.  A representative subsample is
passed through an 8-mesh stainless steel sieve (about 2mm openings)  and
again thoroughly mixed before a representative aliquot is taken  for  the
final sample.

Samples are placed in 8 oz brown glass jars with foil—lined  screw caps and
are stored at 4° C for no longer than one week before extraction.

                                     150

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SAMPLING OF WATERS

For the Muskegon Project,  analyses are performed monthly on variously  com-
posited water samples.   Twice daily grab  samples of  raw influent  and daily
grab samples of discharge  into storage lagoons and outfalls at Mosquito and
Black Creeks have been  composited by Muskegon Waste  Management System  em-
ployees and accumulated under refrigeration (4° C) to  provide 2 to  3 liters
of sample monthly.  Collections of pre-chlorination  flow and irrigation pump
feed water or pan samples  from irrigation booms have varied with  changes in
management routines and availability of personnel.

Water samples are accumulated and stored  in brown glass reagent bottles  (1
gal cap'y.) with Teflon-lined screw caps.

SOIL EXTRACTION

As soil samples are removed from refrigerated storage, they are stirred and
a 10 g sample taken for moisture determination (24 hr  at 105° C).  Prior to
extraction, water is added to a field-moist aliquot  (100 g) to adjust  to
25% moisture.  One hour is allowed for equilibration.

The equilibrated soil sample is extracted with 100 ml  of benzene-isopropanol
(2:1) in a stainless steel mixing cup.  The extraction slurry is  mixed for
5 min with a high-speed blender, then allowed to stand overnight.  The
solvent is carefully decanted into a 500  ml separatory funnel. An additional
100 ml of solvent is added to the mixing  cup and the contents blended  again
for 2 minutes.  After standing for 2 hrs, the solvent  is transferred to the
separatory funnel.  A final 50 ml extraction is made by swirling  occasionally.
This final extract plus benzene-isopropanol rinsings of the cup are added to
the separatory funnel.

Five successive 30 ml water washings are  used to remove isopropanol.   The
benzene layer plus benzene washings of the separatory  funnel are  passed
through freshly activated anhydrous sodium sulfate held in a glass  funnel
into a 100 ml round bottom flask.  The benzene is concentrated at 40 - 50° C
to less than 10 ml in a rotary evaporator.  Then an  equal amount  of benzene
is added, swirled thoroughly, then concentrated almost to dryness.  With
repeated rinsings of the round bottom flask, the benzene extract  is adjusted
to 10 ml in a 10 ml vol. flask.  The extract is transferred into  a  glass vial
with a Teflon-lined screw cap and is stored at 4° C  until cleanup.

WATER EXTRACTION

Water samples may be extracted as received or, if the  distribution  of
chemicals between particulate and aqueous phases is  of concern,  they may be
centrifuged before extraction.  Samples of raw sewage  and of discharge into
storage lagoons at Muskegon were centrifuged routinely through 1975.

Water Extraction for Whole Samples (as received).

The water sample is vigorously shaken by  hand and 1.5  liters is immediately
extracted in a two liter separatory funnel with 50 ml  of methylene  chloride.

                                     151

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The solvent layer is then transferred  into  a  500 ml  Erlenmeyer flask.  Water
is extracted three more times with  50  ml methylene chloride each time.  The
extract plus rinsings of the funnel are combined in  the  500 ml flask.  The
combined extract is dried by passing through  anhydrous sodium sulfate and
concentrated by rotary evaporation  to  5.0 ml.   An equal  amount of benzene is
added, then concentrated almost to  dryness.  The residue is quantitatively
transferred to a 10 ml volumetric flask, brought up  to volume in benzene,
and transferred into a glass vial (Teflon-lined cap)  for storage at  4° C un-
til separation and cleanup.

Water Extraction for Separating Particulate and Aqueous  Phases

A water sample of known volume (1.5 1  or more)  is distributed in stainless
steel bottles and centrifuged in a  Sorvall  RCB-2 refrigerated centrifuge,
equipped with a GSA rotor.  Centrifugation  at 13,000 rpm (27,300 g)  for 20
to 30 min removes most particulate  matter from the aqueous  phase.   Complete
separation of particulates can be achieved  with excess CaCl2 as flocculating
agent.

The supernatant is decanted through a pre-weighed glass  fiber filter.  A  1.5
1 aliquot of the filtered supernatant is  extracted immediately  in  the manner
described above for whole samples.

The sedimented solids are transferred quantitatively from the centrifuge
bottles to the same glass fiber disc as used  to filter the  supernatant.   The
disc is then placed in a solvent-washed  glass storage dish  and  stored at  4°C
until it can be prepared for extraction.

When removed from storage, the glass fiber  discs  and retained solids are
dried in a vacuum oven at 50° C (4  hours) and re-weighed.  Ten  to  20 ml of
water is added to the sample in the dish  and  the  cover  is taped securely.
After 8 hours of standing, 50 ml of benzene-isopropanol  (2:1)  is  added,  the
cover is securely taped and the contents  rotary shaken  (100 rpm)  for 2 hours.
The solvent is decanted into a 250  ml separatory  funnel.  Two  successive
50 ml extractions with 2 hours shaking are  then made. After each  extraction,
the solvent is carefully transferred into the separatory funnel.   Three
rinsings are made of the filter disc and  storage  dish.

The benzene-isopropanol extract is  washed four times with water to remove
the alcohol.  The benzene extract is dried  by passing through anhydrous
sodium sulfate.  Dried extract is then concentrated  by rotary evaporation
and volume adjusted to 10 ml before storing at 4° C  until separation and
cleanup.

SEPARATION AND CLEANUP

Preparation of Micro Column

Place a small loose plug of Pyrex glass wool in the tip of a 11.2 cm x 1  cm
glass column.  Pack the column with 2.0 grams of 60/100 mesh Florisil pre-
activated at 130° C.  The column packing is added in increments,  each
followed by gentle  tapping with a vibrator.  Place a small loose plug of

                                    152

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glass wool again above the surface of the packed absorbent.   Store  columns
in a 130° C oven for at least 48 hours before use.

Florisil Fractionation

(1) Remove Florisil column from the oven and cool to room temperature  in a
dessicator (1 hr).

(2) Deactivate column with 10 ml of 1% methyl alcohol in benzene mixture.

(3) Elute the column with 10 ml petroleum ether.  Discard the eluate.   How-
ever, take precaution to not allow the column to "run dry" at any time.

(4) Introduce the 10.0 ml of sample extract in benzene slowly into  the
column, taking care not to disturb the surface of the column absorbent.
Begin collection of eluate immediately in a 100 ml round bottom flask.
Follow introduction of sample with the first eluant, 50 ml petroleum ether.
The fraction eluted by this addition of petroleum ether contains most
organochlorine insecticides like lindane, aldrin, heptachlor, o_,j>_-DDE  and
other compounds like polychlorinated biphenyls.

(5) Elute column with the second eluant:  50 ml of 10% methylene chloride
in benzene.  Collect eluate in another 100 ml round bottom flask.

(6) Finally collect a third fraction by eluting the column with 50  ml  of a
mixture of 50 ml benzene, 49 ml methylene chloride and 1 ml acetonitrile.
This fraction usually contains most herbicides and phthalates (DEHP).   The
column can be allowed to drain dry into this final eluant fraction.

Each of the three fractions is concentrated to about 20 ml by rotary evapo-
ration.  An equal amount of benzene is added and concentrated to near  dryness,
The residue is taken up quantitatively in benzene and adjusted to 10 ml.
Each fraction is analyzed separately by gas-liquid chromatography and  thin-
layer.  When a chemical is confirmed in more than one eluant fraction, the
sum for those fractions is reported.

The use of Florisil as adsorbent and the fractional elution procedure  have
been adapted from procedures described by Mills (3) and Thompson (5).
Various modifications of these procedures, whereby Florisil is partially
deactivated with water or other polar solvents  (1), have improved the
recovery of certain pesticides.  The use of a micro—column was proposed by
Law and Goerlitz (2).  With the micro-column, pesticides are efficiently
separated from many interfering coextractives, and the miniaturization con-
tributes to both speed and economy of analysis.

GAS-LIQUID CHROMATOGRAPHY

Identification, confirmation and quantitation of pesticide fractions is per-
formed on a Beckman GC-5 gas chromatograph equipped with a non-radioactive
(helium arc discharge) electron capture detector, a 10-in (1 mV) Beckman
recorder and an Autolab System I electronic integrator.
                                     153

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Glass columns (3 mm l.D.  x 1.83  m)  are  used, with  Gas  Chrom Q as  solid
support.  The stationary phase for  quantitation  is 1.5%  OV-17/1.95%
QF-1.  A second column (6% QF-1)  is used  routinely for confirmation.  Two
other columns (2% SE-30 and 3% DECS)  are  used  occasionally for  confirmation
of certain chemicals (Table II-2).

Ultrapure helium (Matheson) is used for detector discharge and  as carrier
gas.  The detector is operated at 250°  C  with  a  discharge helium  flow of
80 ml/min.  Column flow rates and temperatures vary with the column
(Table II-2).

Instrument parameters are set daily for maximum  sensitivity.  Normally,
amplifier output is attenuated to 2 x 10~~" amps  =  full scale on the  recorder.
At this output, maximum C02 response at a polarizing voltage of .57  x 150  V
is 70 to 80% of full scale.  Background current  is set with C02 slightly  in
excess of this peak response. Optimum peaks are obtained with  a  bias voltage
of 0.2 to 0.4 x 150 V.

Integrator parameters are set to reject peaks  with heights  less than 3  times
baseline noise; initial peak width is set at 3 to  5 sec, depending on column,
and is updated at pre-selected  intervals  during  a  run.

Four yl of sample is injected.   A multiple standard (in  benzene)  is  injected
before each group of three Florisil eluant injections  for  a given sample.
Reference chemicals are selected for each combined standard to  assure that
the peaks in standard chromatograms are discretely resolved (Table II-2).
A separate standard is used for  DEHP.

Identification is based on retention time.  Quantitation is based on peak
area (mV-sec), integrated electronically.  During  the course of a day's run,
the volume of each appropriate standard (Table II-2) is  varied  from 1 yl to
6 yl (in increments of 2 or 3 yl) to provide coordinates for a  standard
curve.  Response over this range is linear (log-log plot)  to about 75%  of
background current  (50 to 60% full scale  at attenuated amplifier  output =
2 x 10~9 amps).  If injected sample quantities do  not fall in this range,  a
new set of standards covering a  1/10 X or 10 X range of  concentrations  is
injected to provide an appropriate standard curve.  If extremely high con-
centrations are encountered, the sample is diluted.

THIN LAYER CHROMATOGRAPHY

Thin layer chromatography is used to substantiate the identity of pesticides
detected with two or more GLC columns.  The procedure is as follows:

Sample Preparation

Evaporate sample left from G.C.  analysis to near  dryness (in the vial used
for storage) with a flow of high grade nitrogen gas.  Add ethyl acetate,
shake vigorously and blow down again almost to dryness with N£.  Finally
adjust  to 0.2 ml with ethyl acetate.
                                     154

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Application of Sample

F-254 silica gel G 250 u plates (Brinkman 66 14180-2)  are prescored and acti-
vated at 135° C.  The pesticide solutions are spotted  with disposable
capillary tubes at 1 cm intervals along an origin 2 cm from one edge of the
plate.  Parallel to the origin and 15 cm distant, a second scored line sets
the limit for advance of the solvent front.  Standard  solutions of pesticides
to be confirmed are spotted on the same plate as the sample in question.

Development

The developing solvent is a mixture containing 4 ml glacial acetic acid plus
196 ml of a 10% solution of methylene chloride in benzene.

Each plate is developed by ascending chromatography under conditions of
equilibrium with free solvent, until the solvent front reaches the second
line. Development generally takes 45 min and should be completed within 2
hours of spotting.  The plate is then removed from the tank and dried at
60-80° C for 10 minutes.

Detection

The plate is cooled to room temperature, then exposed to short-wave ultra
violet light until the spot for the standard of lowest concentration appears,
or approximately 10 minutes.

A system similar to one described by Wood (6) is used to make the spots
visible for examining later.  After developing fluorescence, spray the plate
immediately with AgN03 - bromophenol blue chromogenic  reagent.  Dry the
plate and neutralize excess chromogenic reagent by spraying with iodine
solution (Ig 12 + 2 g KI in 300 ml t^O, diluted 1:1 with acetone just before
using).

QUALITY CONTROL

Reagents

Solvents (methylene chloride, benzene, petroleum ether, acetonitrile,
methanol) are distilled-in-glass, chromatographic grade (Burdick & Jackson,
Muskegon, Mich.).  For each new lot a 500 ml aliquot is concentrated to 10
ml and a chromatograph prepared to check for electron-capturing contaminants.

Water for deactivation of soil samples and for use in analytical procedures
is double-distilled in glass and adjusted to pH 4.0 before storage in an 18
1 Pyrex carboy with a spigot at the bottom equipped with a Teflon stopcock.
Each new batch is analyzed as for a water sample to assure absence of
electron-capturing species.

Florisil — 60/100 PR grade (Floridin Co., 3 Penn Center, Pittsburgh, Pa.
15235) — is transferred immediately upon receipt to glass containers with
ground glass stoppers or foil-lined closures and stored in the dark.  Each
new lot is sampled for extraction with methylene chloride to check for

                                    155

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contaminants.  Two or three days before  use,  quantities needed are activated
at 130° C for at least 48 hrs,  cooled and  stored  in  a  desiccator  (over P20s)•
The micro-columns for cleanup are loaded 2 or 3 days before use,  stored in
an oven at 130° C, then cooled in a desiccator (^2^5^  Just before use.
Glass wool plugs are Soxhlet-extracted with methylene  chloride for 16 to  20
hrs.  Residual methylene chloride is evaporated under  an  infrared lamp.
The plugs are then wrapped in foil and heated at  130°  C for 24 hours before
they are used in loading the micro-columns.

Glass fiber filter discs (A. H.  Thomas 4750 D55)  are Soxhlet-extracted with
methylene chloride for 24 hours, dried at  130° C,  cooled  in a desiccator
(1*205) and weighed.  The weights are scribed  on pieces of foil used to
separate the discs in a glass storage dish which  is  kept  in the  desiccator.

Anhydrous sodium sulfate is Soxhlet-extracted with methylene chloride
(50 g/500 ml) for at least 36 hours and  dried at  130°  C for 48 hours just
before use.  It should be cooled in a desiccator  for an hour before use.   For
each new lot received from a supplier, the first  methylene chloride wash
solution is concentrated and taken up in benzene  for injection to provide
a chromatographic record of possible interfering  impurities.

Glassware

Utmost care is taken to avoid contamination of samples or reagents  through
contact with materials other than glass, stainless steel  or aluminum  foil.
All glass connections (or Teflon-to-glass) are used  in tubing  for transfer
of liquids.  Teflon or foil liners are used in all closures.

Rigorous washing procedures are necessary to avoid contamination from
glassware:

1.  Tap water rinse immediately after use.
2.  Hot soak with detergent  (Liquinox) and vigorous  brushing
    to remove visible surface deposits.
3.  Copious hot water rinse.
4.  12-hour dichromate soak.
5.  Copious hot water rinse.
6.  Three small rinsings with acetone followed by hexane.
7.  Cap with foil until use.
8.  Just before use, flush with the solvent to be used at the time.

Reference Standards

Purified reference chemicals are used.  Sources are identified in Table 1.

Identification and Confirmation of GLC Peaks

Peaks  corresponding to the  reference  chemicals in Table  2 have been monitored
routinely in soils and water from Muskegon and Whitehall.  Peaks encountered
have been confirmed on two  or more GLC columns and by TLC.  Three peaks which
occur  frequently have not been  identified  (R  on 1.5% OV-17/1.95% QF-1 =
115-118 sec, 164-168 sec, 247-253 sec; Rt  relative  to aldrin = 0.9, 1.27,

                                      156

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1.92).

Peaks for most reference chemicals are resolved satisfactorily  on  the
OV-17/QF-1 column used for quantitation and on the 6% QF-1  column  used most
frequently for confirmation (Table II-2).   For identification of sample  peaks,
a variation of ± 2 sec is allowed in the retention time for peaks  with R^  <
300 sec, increasing to ± 10 for peaks with Rt > 900 sec.

Phorate and a-BHC are separated satisfactorily only on DECS.  On TLC plates,
these two chemicals are separated spatially (phorate, Rf  =  0.63; a-BHC,  Rf
= 0.73), and the spot for phorate is purple, whereas the  spot for  a-BHC  is
yellow.

In the case of the sediment phase in untreated sewage influent  and of surface
soil  (0-6 in), there is some ambiguity in resolving peaks for chemicals  with
retention times on the OV-17/QF-1 column less than 100 seconds  (Table II-2).
The ambiguities relate primarily to identifying an appropriate  baseline  on
the trailing edge of a broad fused peak for coextracted contaminants.  The
problem is encountered mainly in the first eluant fraction  from Florisil
cleanup (Table II-3).

Arochlors that have been examined are eluted almost quantitatively in the
first eluant.  If present, peaks for PCB components would confound the deter-
mination for a number of chemicals in this fraction.  Families  of  peaks
typical for commercial Arochlors have not been observed.   In particular,
frequently prominent unknown peaks at retention times on OV-17/QF-1 of 115 -
118, 164 -168, and 247 - 253 sec were not accompanied by other  prominent
peaks that would be expected in common Arochlors.  Nevertheless, the "windows"
specified for selecting referenced peaks for integration would  not have  ex-
cluded a number of PCB species.  The possibility that PCB's may have been
present at low concentrations cannot be ruled out.

PCB's can be separated from a number of chemicals referenced in this study by
available methods (Thompson, 1972).  Because of time constraints,  these  have
not been used.

Problems of separation increase with the number of chemicals to be considered
in a given survey.  Fractional recoveries in Table II-3 provide less than
satisfactory separation for the range of chemicals considered in this study.
Separations for selected groups of chemicals can be improved by manipulating
elutant composition or eluant volumes.  Other procedures  for fractional
separation and concentration are available or are being developed.

The variability in fractional and total recoveries in Table II-3 derives,  in
part, from the fact that determinations were made by different  analysts  at
widely spaced time intervals during the course of the investigation.  Florisil
recoveries ware not used to adjust values reported in Section VIII of this
report.

Extraction Efficiencies

Recoveries of reference chemicals from spiked water samples have ranged  from

                                     157

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80 to 110 percent.   No  attempt  has been made  to assess efficiency of extrac-
tion from spiked soil samples.

Sensitivities and Limits of Quantitation

Instrument parameters are optimized  daily for maximum sensitivity.  Integrator
parameters are set to reject peaks with heights less than  3  times baseline
noise.  Typically,  peak heights representing  50 percent  reduction in back-
ground current are achieved with injections of 1.3  ng £,£'-DDT  or 0.1 ng
lindane.

Peak areas for 1 pi standard injections on the quantitating  column  are  given
in Table II-2.  Quantitation limits  in the last column allow for inter-
ferences from early-eluting contaminants  in sample  injections and for decreas-
ing resolution capabilities as  peaks widen with increasing elution  time.
Instrument capabilities vary from time to time.   Under optimum  operating
conditions, smaller peaks can be resolved satisfactorily.

OVERALL ASSESSMENT

Experience in this study serves to  emphasize  the  need  to develop and validate
analytical protocols for specific chemicals of concern prior to initiation
of routine monitoring for those chemicals. Provision must be made  for
routine assessment of recoveries and possible artifacts  at each step.   Iden-
tification and confirmation by  chromatographic procedures  should be substan-
tiated by definitive methods as characteristic or unusual  wastewater  compon-
ents are encountered.  Effective quality  control  will  represent a  substantial
portion of the total cost for trace organic analysis.
                                     158

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TABLE II-l.  REFERENCE CHEMICALS (PURIFIED GRADE) AND SOURCES
  Chemical
            Chemical name
    Source
Aldrin
Dieldrin
Heptachlor
Heptachlor
  Epoxide
1-Hydroxy-
chlordene
Lindane
cx-BHC

B-BHC

6-BHC

£,£'-DDT


£,£f-DDD


£,£f-DDE


£,£T-DDT


£,£'-DDD


£,£f-DDE


Methoxychlor
l,2,3,4,10,10-hexachloro-l,4,4a,5,8,8a-
hexahydro-1,4-endo,exo-5,8-
dimethanonaphthalene

1,2,3,4,10,lQ-hexachloro-exo-6,7-
epoxy-1,4,4a,5,6,7,8,8a-octahydro-
1,4-endo,exo-5,8-dimethanonaphthalene

1,4,5,6,7,8,8-heptachloro-3a,4,
7,7a-tetrahydro-4,7-methanoindene

1,4,5,6,7,8,8-heptachloro-2,3-epoxy-
3a,4,7,7a-tetrahydro-4,7-
methanoindene

1,7,8,9,10,10-hexachloro-2,3-6,5
endo-tricyclo [5.2.1.0] deca-
4,-8-diene-exo-3-ol
Perrine Repository
Triangle Park
Research Center

Perrine Repository
Perrine Repository
Perrine Repository
Perrine Repository
gamma isomer of hexachlorocyclohexane    Perrine Repository
alpha isomer of hexachlorocyclohexane

beta isomer of hexachlorocyclohexane

delta isomer of hexachlorocyclohexane

1,1,1-trichloro-2-(o-chlorophenyl)-
2- (£-chlorophenyl)ethane

2-(o-chlorophenyl)-2-(£-chlorophenyl
-1,1-dichloroethane

2- (p_-chlorophenyl) -2— Cp-chlorophenyl) -
1,1-dichloroethylene

2 ,2-bis Cp_-chlorophenyl) -1,1,1-
trichloroethane

2, 2-bis (£-chlorophenyl) -.1,1-
dichloroethane

2,2-bis(£-chlorophenyl)-1,1-
dichloroethylene

2,2-bis(£-methoxyphenyl)-
1,1,1-trichloroethane	
Perrine Repository

Perrine Repository

Perrine Repository

Perrine Repository


Perrine Repository


Perrine Repository
City Chem. Corp.
New York, N. Y.

Perrine Repository
Perrine Repository
Perrine Repository
                                    159
                                                           (continued)

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                         Table II-l. (continued)
     P
Lasso


M. Parathion


E. Parathion


Atrazine


Diazinon



Endrin



Phorate


Dimethoate


DEHP


2,4-D(ME)


2,4-D(BE)I


2,4-D(BE)II


2,4-D(IPE)


Vegadex^
2-chloro-2',6'-diethyl-N-
(methoxymethyl)-acetanilide

(},0-dimethyl-0-(p-nitrophenyl)
phosphorothioate

£,0-diethyl-0-Cp_-nitrophenyl)
phosphorothioate

2-chloro-4-ethylamino-6-
isopropylamino-a-triazine

£,0-diethyl-0- (2-isopropyl-
4-methyl-6-pyrimidinyl)
phosphorothioate

1,2,3,4,10,10-hexachloro-6,7-
epoxy-1,4,4a,5,6,7,8,8a-oc tahydro-
1,4-endo,endo-5,8-dimethanonaphthalene

£,0-diethyl-S_-(ethyl thiomethyl)
phosphorodithioate
Weed Science Soc.
(City Chem. Corp.)

Perrine Repository
Perrine Repository
CIBA-Geigy Chem.
Corp.

Perrine Repository
Applied Sci. Labs
(ANSPEC, Ann Arbor,
 MI)

Perrine Repository
0^0-dimethyl-^-(N-methylcarbamoylmethyl) Perrine Repository
phosphorodithioate
diethylhexylphthalate
methyl ester of 2,4-dichloro-
phenoxyacetic acid

n-butyl ester of 2,4-dichloro-
phenoxyacetic acid

isobutyl ester of 2,4-dichloro-
phenoxyacetic acid

isopropyl  ester of  2,4-dichloro-
phenoxyacetic acid
Analabs,  Inc.
New Haven,  CT

Perrine Repository
Perrine Repository
 Perrine  Repository
 Perrine  Repository
 2-chloroallyl-N^-diethyldithiocarbamate  Weed Science Soc.
                                    160

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Table II-2.   STANDARD  SOLUTIONS IN  (BENZENE):  RETENTION TIMES (Rt) ON FOUR GLC COLUMNS
             AND  TYPICAL SENSITIVITIES AND DETECTION LIMITS FOR THE QUANTITATING COLUMN.


Chemicals


STANDARD A

a-BHC

Lindane

6-BHC

1-OH-chlordene

Dieldrin

pp'-DDD

pp'-DDT

Methoxychlor

STANDARD B

Phorate

Aldrin

Heptachlor
Heptachlor
Epoxide
pp'-DDE
STANDARD C

2,4-D (ME)

2,4-D (IPE)

2,4-D (BE) I

2,4-D (BE)II

Lasso

Retention times (Rt) sec

22 SE-30 6% QF-1 3% DECS |oV-17/Qf-l
Column Temperatures ( C)
200 185 185 200
Column flow rates (ml/min)
50
60
25 J 60


49

59

60

108

198

246

324

498

101

131

168

217

462

558

608

936

102

145

103

370

273

683

683

	

70

90

141

167

314

454

545

1055



94

108

90
132
198
101

160

137
298
320
63

83

90
132
198
67

130

108
204
292


80

100

147

169

180

108

132

191

212

295

98

85

109

128

146

62

73

105

122

145

Quantitating column
Icw I-.TT IT/I Q^y OF—I
. Jfu UV-"X/ / JL • 7 Jh Vf J.
Sensitivities)? Quantitation
1 ul Peak
Injection area
ng*

mv-sec



.010

.005

.008

.016

.008

.016

.020

.104

200

200

500

800

500

700

400

2,200



.120

.005

.005
.004
.012
100

300

400
200
500


.030

.040

.040

.030

.142

200

200

200

200

600

limits?
Water: ng/1
Soil: ng/g



HO:
Soil:
HO:
Soil:
HO
Soil:
H20:
Soil:
H,0:
Soil:
H,0:
Soil:
HoO:
Soil:
H20:
Soil:
15.
.3
8.
.1
8.
.1
20.
.3
10.
.2
20.
.3
20.
.3
80.
1.


H2°
Soil:
HO:
Soil:
HO:
Soil:
HO:
Soil:
HO:
Soil:
300.
5.
8.
.1
8.
.1
6.
.1
15.
.3
1

H20:
Soil:
H,0:
Soil:
H20:
Soil
HjO:
Soil
H,0:
S&il
50.
.8
100.
2.
100.
2.
60.
1.
150.
3.
                                                                         (continued)
                                           161

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                                Table II-2.   (continued)


Chemicals



STANDARD D

Diazinon

Dimethoate

op-DDD

op-DDT

Ethyl parathion

STANDARD E

Atrazine

6-BHC

op-DDE

Methyl parathion

Endrin

Vegadex

DEHP

Retention times (Rt) sec
	 column 	 ; 	
2% SE-30| 6% QF-1
3%DEGS 1 OV-17/QF-1
Column Temperatures (°C)
200
185 185 200
- - - - Column flow rates (ml/im
50 60
25
Ln"*
n; - - - - -
60


66

64

198

258

125



_

180

162

80

222

.__

702

115

300

382

407

583



135

151

295

442

547

_._

1,133

62

442

396

385

-



193

398

185

346

317

___

426

84

132

343

410

240



84

105

237

188

385

73

980

Quantitating column
1.5% OV-17/1.95% QF-1
Sensitivities)1/
1 ul Peak
injection area
ng*

rav-sec



.220

.098

.010

.020





.990

.020

.010

0.063

.010

.010

L0.5

400

200

400

300





200

400

400

300

500

200

1,100

Quantitation
limits?
Water: ng/1
Soil: ng/g



H20: 350.
Soil: 6.
H20: 150.
Soil: 3.
H20: 10.
Soil: .2'
H20: 20.
Soil: .3
H20: 100. i
Soil: 2.

;
H20: 1,500.
Soil: 25.
H20: 30. i
Soil: .5,
H20: 10.
Soil: .2
H20: 100. ;
Soil: 2.
H20: 15.
Soil: .3
H20: 15.
Soil: .3
H20:10,000.
Soil: 170.
    ng/ul » ppm.   Primary  standards  are made  up  in  benzene  to  contain 10  x this  concentration.
    They are stored at  4°C in Teflon-capped vials.   Injection  standards  are prepared at time
    of use by diluting  the primary standard 10~3, 10"'*  or 10~5.   Electron capture detector
    response is linear  on  log—log paper for injections  of 1 to 6  ul  at a given dilution of
    standard.  Sample peaks are quantified by reference to  the appropriate linear response
    curve.  Unusually high sample concentrations are diluted.
#   Sensitivities at amplifier output attenuated  to 2
    recorder.
10~9 amps « full scale on the
    Quantitation limits were estimated from standard curves (6 to 18 runs per chemical),
    with allowances for baseline noise (3x),  for interference from contaminants in sample
    chromatograms,  and for decreasing resolution as peaks widen with increasing retention
    time.  Recoveries from spiked water samples  ranged from 80 to 110%.   Recovery from
    spiked soil samples was not determined.
                                                162

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   Table II-3.
FLORISIL ELUANTS:  FRACTIONAL DISTRIBUTIONS AND
TOTAL RECOVERIES FOR REFERENCE CHEMICALS.*
Distribution Total
% of recovered recovery
w c
Chemical
Aldrin
Dieldrin
Endrin
Heptachlor
Heptachlor epoxide
1-OH-Chlordene
Methoxychlor
o , p-DDT
o",p~-DDD
cT,"p-DDE
p.p'-DDT
p,p'-DDD
p,p'-DDE
=-BHC
S-BHC
Y-BHC (lindane)
S-BHC
2,4-D (ME)
2,4-D (BE) I
2,4-D (BE) II
2,4-D (IPE)
Diazinon
Dimethoate
Parathion (ethyl)
Parathion (methyl)
Phorate
Atrazine
Lasso
DEHP
PCB's:
Arochlor 1016
1221
1242
1248
1254
1260
5432
Eluant #1
100
50 - 90
60 - 90
100
100
30 - 40
90 - 95
100
90 - 100
100
100
100
100
90 - 100
100
100
90 - 100
tr - 10
5-20
5-20
10 - 15
	
	
60 - 80
45 - 60
100
	
tr - 5
	

100
100
95
100
100
100
100
Eluant #2 Eluant #3 column
loading
85 - 105
10 - 50 	 70 - 110
10 - 40 	 105 - 145
85 - 95
90 - 110
60 - 70 	 90 - 100
5-10 	 80
95 _ us
tr - 10 	 70 - 100
80 - 115
100 - 120
80 - 100
115
tr - 10 	 80 - 100
80 - 100
70 - 105
tr - 10 	 75 - 110
0-10 90 50 - 110
15 - 25 65 - 70 60 - 150
10 - 20 70 - 75 60 - 90
10 75 - 80 60 - 65
tr - 5 95 - 100 70 - 80
100 tr
20 - 40 	 90 - 100
40 - 55 	 80 - 100
80 - 100
tr - 20 80 - 100 70
95 - 100 50 - 130
10 - 25 75 - 90 95 - 100

tr 	 80
tr tr 115
tr 5 100
tr tr 90 - 100
tr tr 100 - 105
tr tr 90 - 120
120
*  Two determinations for each chemical,  using OV-17/QF-1  or  SE-30
   columns.
                                  163

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                           APPENDIX III.

The following table has been developed to estimate the nutrients removed
by harvested corn grain.  They are average values obtained from Ellis
et al. 1973.1

        Table III-l.  ESTIMATED NUTRIENT CONTENT OF CORN GRAIN
                      (15.5% MOISTURE).
Nutrient

N
P
K
Ca
Mg
S
Fe
Mn
Cu
An
Na
Cl
Content

1.46%
0.26%
0.33%
0.03%
0.12%
0.12%
50 ppm
10 ppm
5 ppm
15 ppm
0.03%
0.03%
Quantity Removed
by 100 bu/A Corn
kg /ha
93
16.5
21.0
2.2
7.5
7.5
0.3
0.06
0.03
0.10
2.2
2.2
 Ellis, B. G., A. E. Erickson, B. D. Knezek, R. J. Kunze, I. F.
 Schneider, E. P. Whiteside, A. R. Wolcott and R. L. Cook.  1973.
 Land Treatment of Wastewater in Southeastern Michigan.  Detroit Dist,
 U.S. Army Corps of Engineers,  pp 65 and 68.
                                 164

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                              APPENDIX IV
              AVAILABILITY OF DATA FROM U.S. EPA STORAGE




                AND RETRIEVAL COMPUTER SYSTEM "STORET"









     Much of the data collected has been entered into the U.S.  Environ-




mental Protection Agency's storage and retrieval computer system called




"STORET".  Access to STORET and use of this data may be obtained directly




by authorized users or indirectly through any of the ten different EPA




Regional Offices or STORET User Assistance, U.S. EPA, 401 M Street, S.W.,




Washington, D. C. 20460, phone (202) 426-7792.  The applicable codes




for gaining access to this data are:  Agency Code No. 21 MI MUSK;




State Code No. 26; County Code No. 121.
                                  165

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                                  TECHNICAL REPORT DATA
                           (Please read Instructions on the reverse before completing)
1  REPORT NO
EPA-905/9-79-006-B
                                                           3. RECIPIENT'S ACCESSION NO.
4. TITLE AND SUBTITLE
Applicability of Land Treatment of Wastewater  in  The
Great  Lakes  Area Basin
Effectiveness of Sandy Soil at Muskegon County, MI  for
             5. REPORT DATE
               May 1979
             6. PERFORMING ORGANIZATION CODE
            Wastewater
B.G.  Ellis,  A.E.  Erickson, A.R. Wolcott, B.  D.Knezek
I.M.  Tiedje,  and  S.  Butcher
                                                           8. PERFORMING ORGANIZATION REPORT NO.
9. PERFORMING ORGANIZATION NAME AND ADDRESS
Crop  and  Soil Sciences, Entomology
Michigan  State University
East  Lansing, Michigan 48824
             10. PROGRAM ELEMENT NO.
               2BA645
             11. CONTRACT/GRANT NO.
                                                           EPA Grant No. G005104
12. SPONSORING AGENCY NAME AND ADDRESS
U.S.  Environmental Protection Agency
Great Lakes  National Program Office
536  South Clark Street, Room 932
Chicago,  Illinois  60605
             13. TYPE OF REPORT AND PERIOD COVERED
             Final-April 1972-June 1976	
             14. SPONSORING AGENCY CODE
15. SUPPLEMENTARY NOTES
 The  Muskegon County, Michigan Wastewater  Management System
16. ABSTRACT
 The Muskegon County Wastewater Management System is a lagoon impoundment,  spray irriga-
 tion facility which treats about  102,000 cubic meters of wastewater per  day and irri-
 gates 2,160 hectares of corn land.   About 60% of the flow is industrial.   Data was
 collected over a three year period  to  determine the changes from background condi-
 tions of the native infertile sandy soil as wastewater was irrigated  and crops
 grown.   Data analyzed include major crop nutrient elements and heavy  metals, the
 soil physical properties and electron  capturing organic chemical species.

 The knowledge gained was used to  estimate the useful life of the system  for removing
 critical contaminants such as phosphorus and metals relative to the amounts of
 contaminants and wastewater applied.   With proper management phosphorus  can be removed
 by soils and crops for at least fifty  years.   It is not expected that soil physical
 properties will offer any major problem hydraulicly for the rate and  type  of waste-
 water being applied.  Removals of trace organics from the wastewater  occurred in
 storage lagoons and as the water  passed through the soil mantle, however,  with
 partial pass through of certain organics occurring when the wastewater application
 rate was excessive.  This system  apparently became more effective with time in
 removing many of these trace organic chemicals.
17
a.
                                KEY WORDS AND DOCUMENT ANALYSIS
                  DESCRIPTORS
 Land Treatment of Wastewaters
 Removal of Nutrients by Soils
 Phosphorus
 Heavy Metals
 Electron Capturing organic Chemical  Species
 Muskegan
                                              b.IDENTIFIERS/OPEN ENDEDTERMS
                           c. COSATI Field/Group
18 DISTRIBUTION STATEMENT
 Available to Public from sponsoring agency
 and NTIS, Springfield, Virginal  22151
19. SECURITY CLASS {This Report)
Unclassified
21. NO. OF PAGES
    166
2O. SECURITY CLASS (This page)
Unclassified
                           22. PRICE
EPA Form 2220-1 (Rev. 4-77)
                      PREVIOUS EDITION IS OBSOLETE

                                           166
              US GOVERNMENT PRINTING OFFICE 1979—652-041

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