United States
                Environmental Protection
                Agency
                Industrial Environmental Research  EPA-600 2 80-1 39
                Laboratory            June 1980
                Cincinnati OH 45268
                Research and Development
v>EPA
Sulfide
Precipitation of
Heavy Metals

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                RESEARCH REPORTING SERIES

Research reports of the Office of Research and Development, U.S. Environmental
Protection Agency, have been grouped into nine series. These nine broad cate-
gories were established to facilitate further development and application of en-
vironmental technology. Elimination of traditional grouping was  consciously
planned to foster technology transfer and a maximum interface in related fields.
The nine series are:

      1.  Environmental Health  Effects Research
      2.  Environmental Protection Technology
      3.  Ecological Research
      4.  Environmental Monitoring
      5.  Socioeconomic Environmental Studies
      6.  Scientific and Technical Assessment Reports (STAR)
      7.  Interagency Energy-Environment Research and Development
      8.  "Special" Reports
      9.  Miscellaneous Reports

This report has been assigned  to the  ENVIRONMENTAL PROTECTION TECH-
NOLOGY series. This series describes research  performed to develop and dem-
onstrate instrumentation, equipment, and methodology to repair or prevent en-
vironmental degradation from point and non-point sources of pollution. This work
provides the new or improved technology required for the control and treatment
of pollution-sources to meet environmental quality standards.
This document is available to the public through the National Technical Informa-
tion Service, Springfield, Virginia  22161.

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                                               EPA-600/2-80-139
                                               June 1980
      SULFIDE PRECIPITATION OF HEAVY METALS
                         by

           Alan K. Robinson and 3oyce C. Sum
         Manufacturing Research and Development
          Boeing Commercial Airplane Company
               Seattle, Washington  98124
                    Grant: S805413
                    Project Officer

                   Hugh B. Durham
           Industrial Pollution Control Division
       Industrial Environmental Research Laboratory
                Cincinnati, Ohio 45268
INDUSTRIAL ENVIRONMENTAL RESEARCH LABORATORY
      OFFICE OF RESEARCH AND DEVELOPMENT
     U.S. ENVIRONMENTAL PROTECTION AGENCY
               CINCINNATI, OHIO  45268

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                                  DISCLAIMER

    This  report  has  been  reviewed  by  the  Industrial  Environmental  Research
Laboratory—Cincinnati, U.S.  Environmental  Protection  Agency,  and  approved for
publication.  Approval  does not signify that  the contents necessarily reflect the views
and policies of the U.S.  Environmental Protection Agency, nor does mention of trade
names or commercial products constitute endorsement or recommendation for use.
                                       11

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                                   FOREWORD

    When energy and material resources are extracted, processed, converted, and used,
the related pollutional impacts on our environment and even on our health often require
that new and increasingly  more  efficient  pollution control  methods  be used.   The
Industrial  Environmental   Research   Laboratory—Cincinnati  (lERL-Ci)   assists   in
developing and demonstrating new and improved  methodologies that will meet  these
needs both efficiently and economically.

    This report describes work undertaken to assess the merits of a method for removing
heavy metals from wastewater by precipitation of  the metals  as sulfides instead of the
usual  hydroxide method.  The results of the work can  be used as a source of technical and
cost data to compare the  relative merits of  the  sulfide and hydroxide  processes for
removing heavy metals from industrial wastewaters.
                                                     David G. Stephan
                                                         Director
                                        Industrial Environmental Research Laboratory
                                                        Cincinnati

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                                     ABSTRACT

    This research program was initiated with the objective of evaluating a new process,
the suifide precipitation of heavy metals from  industrial wastewaters.  The process was
expected  to  effect a more complete removal  of heavy metals than conventional  lime
processing because of the much lower solubilities of metal sulf ides than hydroxides.

    Five processes were compared in bench-scale, continuous-flow equipment:  conven-
tional  lime  processing,  conventional  lime processing  plus filtration, lime  with a  suifide
polishing and filtration,  lime with suifide, and lime with suifide plus filtration.

    Samples of actual  wastewaters from 14 metal  working industries (including Boeing)
were processed through  the bench-scale equipment using all five processes.  Reductions in
the concentrations of cadmium, chromium,  copper, nickel, and zinc,  plus selected other
metals, were measured by atomic absorption  chemical analysis.

    Capital  and operating costs for  the five  processes were compared for three plant
sizes:  37.85 m3/day  (10,000 gal/day),  757  m3/day  (200,000 gal/day), and 1,893  m3 /day
(500,000 gal/day).

    The report recommends that,  to reduce the levels of cadmium, copper, nickel, or zinc
from a wastewater treatment plant using conventional lime processing, the addition of a
final filtration should be considered first. > If filtration does not achieve the desired low
levels, then  a suifide polishing process with added filtration is recommended.  If reduction
of the levels of chromium, lead, silver, or tin is required, the conventional lime process
plus filtration is recommended. The suifide process did not significantly reduce the levels
of these metals.

    Details are included on the use of a specific ion  electrode for the control of suifide
additions.   The report  does not include comparison  testing of the  commercial Sulfex
process.

    This  report  was submitted in fulfillment  of Grant S805413  by Boeing under  the
sponsorship  of  the U.S. Environmental  Protection Agency.  This  report  covers  a period
from October 1977 to July  1979; work was completed as of July 1979.
                                         IV

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                                    CONTENTS

Foreword	'.,....'	       iii
Abstract	       iv
Figures	       vii
Tables	        x
Abbreviations and Conversions	       xi
Acknowledgment	       xii

   1.   Introduction	        1
   2.   Conclusions	        2
            Overview	.*	        2
            Effectiveness of processes for removing heavy metals	        2
            Operating and capital equipment costs	        2
            Sludge disposal costs .  .'	        3
            Effectiveness of specific processes for removing
              heavy metals	        3
            Control of sulfide  concentration by specific ion electrode	        5
   3.   Recommendations	        6
   i*.   Description of the Lime Processes (LO-CL and LO-CLF)	        7
            General.	'	        7
            Outline of lime process	        7
   5.   Description of the Lime-With-Sulfide Processes (LWS-CL and
         LWS-CLF)	        9
            General	        9
            Outline of lime-with-sulfide process	        9
            Control of sulfide  additions	       10
   6.   Description of the Lime, Sulfide Polished and Filtered
         Processes (LSPF)	       11
            General	       11
            Outline of lime, sulfide polished and filtered process	       11
   7.   Reason for Omission of Tests on the Sulfex Process	       13
   8.   Removal of Cyanides and Hexavalent Chromium From Wastewaters ...       14
            General	       14
            Removal of cyanides	       14
            Removal of hexavalent chromium	       14
   9.   Bench-Scale Equipment Used in the Tests	       15
            General	       15
            Equipment details	       15
 10.   Description of the Fourteen Wastewaters Treated  .  .	       20
 11.   Presentation of the Analytical Results	       21
 12.   Capital Costs of Full-Scale Plants	       24
 13.   Operating Costs of  Full-Scale Plants	       28
            General	       28
            Assumptions used in the calculations	       28
 14.   Electron Photomicrographs of Sludges	       33

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 15.  Slide and Cassette Tape Presentation  ................       35
 16.  Confidence Levels of the Chemical Analyses  .............       3°
            General ...........................       36
            Analysis of EPA standards ...................       36
            Statistical repeatability tests  .................       36
 17.  Consultant's Report ........................       38
References
Appendices
  A.   Case history data of 16 test runs  ..................       ^2
  B.   Analytical methods ........................       59
  C.   Comparison plots of five metal concentrations for all samples ......       60
  D.   Sign test statistical analysis  ....................       71
  E.   Wilcoxon matched-pair, signed-rank statistical analysis  ........       76
  F.   Capital cost of full-scale plants ...................       78
  G.   Graphic presentation of results ...................       98
  H.   Criteria for selecting pH value for precipitation ...........  •
                                          VI

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                                    FIGURES

Number                                                                     Page

1     Lime-only process flow diagram	       8

2     Lime-with-sulfide process flow diagram	       10

3     Lime, sulfide polished and filtered process flow diagram	       11

4     Bench-scale unit for processing industrial wastewater by'the
       LO-CL, LO-CLF, LSPF, LWS-CL, and LWS-CLF processes	       16

5 .    Flow diagram of multipurpose bench-scale equipment	       17

6     Bench-scale unit showing instrumentation and air vent hood	       18

7     Wastewater being charged into sample reservoir of
       bench-scale unit from sample drum	       19

8     Electron photomicrograph of lime-with-sulfide
       sludge (magnified at 46,500x)	       34

C-l   Comparison of LO-CL process and LSPF process using
       Cd, Cu, Cr, Ni, and Zn effluent metal concentrations
       for all wastewater samples	       61

C-2   Comparison of LO-CLF process and LO-CL process using
       Cd, Cu, Cr, Ni, and Zn effluent metal concentrations
       for all wastewater samples	       62

C-3   Comparison of LSPF process and LWS-CL process using
       Cd, Cu, Cr, Ni, and Zn effluent metal concentrations
       for all wastewater samples	       63

C-4   Comparison of LWS-CL process and LO-CLF process using
       Cd, Cu, Cr, Ni, and Zn effluent metal concentrations
       for all wastewater samples	       64

C-5   Comparison of LO-CLF process and LWS-CL process using
       Cd, Cu, Cr, Ni, and Zn effluent metal concentrations
       for all wastewater samples	       65

C-6   Comparison of LO-CL process and LWS-CLF process using
       Cd, Cu, Cr, Ni, and Zn effluent metal concentrations
       for all wastewater samples	       66

C-7   Comparison of LSPF process and LO-CLF process using
       Cd, Cu, Cr, Ni, and Zn effluent metal concentrations
       for all wastewater samples	       67
                                       VI1

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Number                                                                     Page

C-8   Comparison of LWS-CLF process and LSPF process using
       Cd, Cu, Cr, Ni, and Zn effluent metal concentrations
       for all wastewater samples ....................       68
C-9   Comparison of LWS-CLF process and LWS-CL process using
       Cd, Cu, Cr, Ni, and Zn effluent metal concentrations
       for all wastewater samples ....................       69
C-10  Comparison of LWS-CL process and LO-CL process using
        Cd, Cu, Cr, Ni, and Zn effluent metal concentrations
        for all wastewater samples  ....................       70

D-l   Hierarchy of wastewater treatment processes
        established from sign test statistical analysis  ............       71

D-2   Agreement between LO-CLF and LO-CL not significant
        at 75-percent confidence level ...................       72

D-3   Agreement between LSPF and LO-CL not significant
        at 75-percent confidence level   ..................       72

D-4   Agreement between LWS-CL and LWS-CLF not significant
        at 75 -percent confidence level   ..................       72

D-5   Agreement between LO-CLF and LWS-CL significant
        at 75-percent confidence level ...................       73

D-6   Agreement between LSPF and LWS-CL not significant
        at 75-percent confidence level ...................       73

D-7   Agreement between LO-CL and LWS-CL not significant
        at 75-percent confidence level ...................       73

D-8   Agreement between LWS-CLF and LO-CL not significant
        at 75-percent confidence level ...................       74
D-9   Agreement between LO-CLF and LSPF not significant
        at 75-percent confidence level
D-10  Agreement between LO-CLF and LWS-CLF not significant
        at 75-percent confidence level .....  .N  .............       74
D-ll  Agreement between LSPF and LWS-CLF significant
        at 75-percent confidence level ...................       75

E-l   Hierarchy of wastewater treatment processes established from
        Wilcoxon matched-pair, signed-rank statistical analysis ........       77
F-l   Small LO-CL and LO-CLF plant schematic ..............       82

F-2   Small LSPF, LWS-CL, and LWS-CLF plant schematic  .........       83
F-3   Medium-sized LO-CL and LO-CLF plant schematic ..........       84
F-4   Medium-sized LSPF plant schematic .................       85
F-5   Medium-sized LWS-CL and LWS-CLF plant schematic .........       86

F-6   Large LO-CL and LO-CLF plant schematic ..............       87
                                       via

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Number                                                                    Page
F-7   Large LSPF plant schematic	      88
F-8   Large LWS-CL and LWS-CLF plant schematic	      89
F-9   Small plant layout—all processes (LO-CL,
       LO-CLF, LSPF, LWS-CL, and LWS-CLF)	      90
F-10  Medium-sized LO-CL and LO-CLF plant layout	      91
F-ll  Medium-sized LSPF plant layout	      92
F-12  Medium-sized LWS-CL and LWS-CLF plant layout	      93
F-13  Large LO-CL and LO-CLF plant layout	      94
F-14  Large LSPF plant layout  .	      95
F-15  Large LWS-CL and LWS-CLF plant layout	      96
F-16  Cross section of medium-sized arid large plants—all
       processes (LO-CL, LO-CLF, LSPF, LWS-CL, and LWS-CLF)	      97
G-l   Relationship of LO-CL process effluent concentration to raw
       feed concentration for Cd, Cu, Cr, Ni, and Zn	      99
G-2   Relationship of LO-CLF  process effluent concentration to raw
       feed concentration for Cd, Cu, Cr, Ni, and Zn	     100
G-3   Relationship of LSPF  process effluent concentration to raw
       feed concentration for Cd, Cu, Cr, Ni, and Zn	     101
G-4   Relationship of LWS-CL process effluent concentration to raw
       feed concentration for Cd, Cu, Cr, Ni, and Zn	     102
G-5   Relationship of LWS-CLF process  effluent concentration to raw
       feed concentration for Cd, Cu, Cr, Ni, and Zn	     103
H-l   Effect of pH on effluent  concentration of heavy metals	
                                       IX

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                                     TABLES
Number                                                                      Page
1   Comparison of Operating Costs
2   Comparison of Capital Costs
3   Arithmetic Mean Influent and Effluent Concentrations for
       the Five Processes
4   Logarithmic Mean Influent and Effluent Concentrations for
       the Five Processes
5   Arithmetic Mean Influent and Effluent Concentrations for
       the Five Processes  ........................      21
6   Logarithmic Mean Influent and Effluent Concentrations for
       the Five Processes  ........................      22
7   Summary of Plant Capital Installation Costs ..............      24
8   Small Plant Construction Costs ....................      25
9   Medium -Sized Plant Construction Costs ................      26
10  Large Plant Construction Costs ....................      27
1 1  Summary of Operating Costs .....................      28
12  Operating Costs for Small Plant ....................      30
13  Operating Costs for Medium -Sized Plant ................      31
14  Operating Costs for Large Plant  ............  .  ......      32
15  Analysis of EPA Standards ......................      37
16  Effluent From LO-CL Process  ....................      37
17  Effluent From LO-CLF Process ....................      37
18  Confidence Levels of the Analyses  ..................      37
19  Zinc Removal From Waste No. 12 ...................      39
20  Metal Removal From Waste No. 9 ...................      39
Data Sheets for Test Runs 1 through 16  ..................   43-58
E-l  T- Values of Wilcoxon Matched-Pair, Signed-Rank Statistical
        Analysis  ................  ............      77
H-l  Proposed EPA Guideline Levels  ...................      105
H-2  Effluent Concentration Related to EPA Proposed Limitations  ......      105

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                      ABBREVIATIONS AND CONVERSIONS
ABBREVIATIONS

LO-CL      —lime only, clarified
LO-CLF     —lime only, clarified and filtered
LSPF       —lime, sulfide polished and filtered
LWS-CL     —lime with sulfide, clarified
LWS-CLF    —lime with sulfide, clarified and filtered
Be          — Baume degrees
v/v         —volume per volume ratio
jumho/cm    — micromho per centimeter (same as /iS/cm)
L           -liter

METRIC CONVERSIONS

To Convert                    To                              Multiply by
gal	L	3.785 412 E+00
gal/min	L/min	3.785 412 E+00
gal/hr	L/h	3.785 412 E+00
gal/day	L/day	3.785 412 E+00
gal/mo	L/mo	3.785 412 E+00
inches	cm	2.540 000 E+00
Ib/hr	 kg/h	4.535 924 E-01
Ib/day	kg/day	4.535 924 E-01
ppb	Mg/L  .	1.000 000 E+00
ppm	mg/L	1.000 000 E+00
                                      XI

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                              ACKNOWLEDGMENT

    We would like to acknowledge the assistance of the following.

For assistance in locating metal finishing companies willing to supply wastewaters: Mr.
E. P.  Durkin, president of Metal Finishers Foundation.

For their cooperation in supplying wastewaters:

        The Advance Plating Company, Cleveland, Ohio
        Dixie Industrial Finishing Company, Atlanta, Georgia
        Automation Plating Corporation, Glendale, California
        Chrome-Rite Company, Chicago, Illinois
        ADI Industries, Inc., Chicago, Illinois
        Franke Plating Works, Inc., Fort Wayne, Indiana
        Alco Cad-Nickel Plating Corporation, Los Angeles, California
        Lincoln Plating Company, Lincoln, Nebraska
        Superior Plating, Inc., Minneapolis, Minnesota
        Heath Techna Corporation, Kent, Washington
        Holley Carburetor Division of Colt Industries, Warren, Michigan
        Federated Metals Corporation,  New York, New York

For information on the Sulfex process: Mr.  R. Schiauch, Mr. M. Scott, Mr. W. Schwoyer,
and Mrs. C. Glover of the Permutit Company, New 3ersey.

Of  the many Boeing  colleagues  who  have contributed to  this  program, particular
acknowledgment goes to Mr. W. Larsen and Mr. I. Woods for chemical analysis.

For consultation services:   Dr.  D.  Bhattacharyya of  the  Department of  Chemical
Engineering, University of Kentucky, Lexington, Kentucky.

To Dr. H.  B. Durham and Mr. D. Wilson  of the Environmental Protection Agency Labor-
atories, Cincinnati, Ohio, who have been EPA project officers on the program.
                                        Xll

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                                    SECTION 1

                                 INTRODUCTION

    The  purification  of industrial process wastewaters that contain  heavy metals, such
as cadmium, copper,  chromium, nickel,  and  zinc, is commonly  accomplished by pre-
cipitating these metals as hydroxides.  The process is relatively inexpensive and is well
established. However, removal of metals by the hydroxide process is incomplete, either
because of slight solubility of the metal hydroxides or because of incomplete settling out
of small particles of the hydroxides.

    A much more complete  removal of metals from wastewaters could be expected for
processes using sulfides  instead of  hydroxides for  precipitation.   In general,  metal
sulfides have  solubilities several  orders  of magnitude smaller than  the  corresponding
hydroxides.

    The  work  described  in  this report is  a  side-by-side  comparison of three sulfide
methods and two hydroxide methods of wastewater treatment. The tests were conducted
on actual wastewaters from  the nonferrous metal producing and metal finishing industry
in the United States.

    The  wastewater  treatments  were conducted  on  a continuous-flow, bench-scale
model treatment plant.  The plant was of a size suitable for  providing test runs lasting
several hours from each 190L (50-gal) sample of wastewater.

    The Permutit Company's Sulfex process (1, 2, 3), which uses an insoluble iron sulfide,
originally was  to be  included in  this  study;  however, legal difficulties  prevented  its
inclusion.

    This report  is concerned  only  with soluble forms of  sulfide precipitant, such as
Na2S, NaHS, and H2S.

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                                    SECTION 2

                                 CONCLUSIONS
OVERVIEW

     Three suifide precipitation processes that use soluble sulfides have  been demon-
strated (in a  continuously operated bench-scale plant) as practical  waste treatment
processes for removing heavy metals  from wastewater.   the levels to  which  heavy
metals  can  be reduced, and the  costs  of  treatment  compared  to  conventional lime
treatment, are developed in this report.

     The lime, suifide  polished and  filtered (LSPF)  process  is  the optimum  suifide
process. For many wastewaters, treatment by the lime process followed by filtration is
almost as effective as the LSPF process and costs far less.

EFFECTIVENESS OF PROCESSES FOR REMOVING HEAVY METALS

     Based only  on  the reduction in  concentration of five heavy  metals (cadmium,
chromium, copper, nickel, and  zinc) in  the  effluents analyzed  and without considering
cost:
     •    The lime only,  clarified (LO-CL) process is the least effective.
     •    Processes lime only,  clarified  and  filtered (LO-CLF) and lime  with suifide,
         clarified (LWS-CL) are equally effective and better than the LO-CL process.
     •    Processes LSPF  and lime with suifide, clarified and filtered (LWS-CLF) are
         equally effective and better than any of the other three.

OPERATING AND CAPITAL EQUIPMENT COSTS

     Each of  the improvements to the  basic  LO-CL   process  carries a cost penalty.
Tables 1 and 2 show that:
     •    The  addition of a filtration operation  (conversion to the LO-CLF  process) adds
         from 0.4 to 0.7 percent to the operating costs and from  0.8  to 1.7 percent to
         the capital costs.
     •    The  addition of a suifide  polishing operation,  which includes filtration (conver-
         sion to the LSPF process), adds from 4.8 to 8.6 percent to the operating costs
         and from 8.6 to 11.6 percent to the capital  costs.
    •    Conversion  to  a  lime-with-sulfide process increases the  capital cost by  6.2 to
         11.6 percent; for a small  plant, the process increases the operating cost  by 7.1
        to 7.8 percent, and for  a  medium or large  plant, the  process increases the
        operating cost by 26.4  to 39.5 percent.

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                   TABLE 1.  COMPARISON OF OPERATING COSTS
\
N. Operating
>v cost of :
N^
Plant ^v
capacity ^v

Conventional lime
plant with no
filtration


LO-CL
37.85 m3/day $5.96/m3
(10,000 gal/day) ($22.6/1 ,000 gal)
757 m3/day $0.90/m3
(200,000 gal/day) ($3.39/1 ,000 gal)
1 ,893 m3/day $0.55/m3
(500,000 gal/day) ($2.08/1 ,000 gal)

Lime plant
with
filtration
added (%)


LO-CLF
+0.7

+0.4

+0.5

TABLE 2. COMPARISON OF
Nv
N. Capital
N. cost of:

N.
>.
Plant ^v
capacity N^

Conventional lime
plant with no
filtration


LO-CL
37.85 m3/day $233,000

Lime plant
with
filtration
added (%)


LO-CLF
+1.7
Lime plant
with sulfide
"polish"
operation,
including
filtration (%)

LSPF
+4.8

+8.0

+8.6


Lime-with-
sulfide plant
with no
filtration (%)


LWS-CL
+7.1

+26.4

+39.0


Lime-with-
sulfide plant
with filtration
added (%)


LWS-CLF
+7.8

+26.8

+39.5

CAPITAL COSTS
Lime plant
with sulfide
"polish"
operation.
including
filtration (%)

LSPF
+11.6

Lime-with-
sulfide plant
with no
filtration (%)


LWS-CL
+9.4

Lime-with-
sulfide plant
with filtration
added (%)


LWS-CLF
+11.6
  (10,000 gal/day)

  757 m3/day
  (200,000 gal/day)
  1,893 m3/day
  (500,000 gal/day)
 $799,000

$1,296,000
+0.8

+1.1
+11.6


 +8.6
+9.1

+6.2
+10.0

 +7.2
SLUDGE DISPOSAL COSTS

    The costs developed here include estimates for sludge disposal, which are based on
the assumption that a sulfide sludge will not carry any significant cost penalty.  At this
stage,  we do  not  know  the  additional surcharge, if any, that might be added to the
disposal charges for a sulfide sludge.

EFFECTIVENESS OF SPECIFIC PROCESSES FOR REMOVING HEAVY METALS

    The same order of preference as that given on page  2,  with more details about
individual metals, can be seen in Tables 3 and 4, which show the mean levels of the five
metals before and after treatment.

    The tables show that cadmium, copper, and zinc follow the same hierarchy as we
established on page 2; that is, LO-CL is least effective, LO-CLF and LWS-CL are more

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effective, and LSPF and LWS-CLF are most effective. The logarithmic mean removal of
these three metals is 96.3 percent or greater for the two most effective processes, with
a logarithmic mean effluent concentration of less than 50
    Nickel removal  does  not  follow the  established  hierarchy  completely;  when  the
logarithmic means are considered, the five processes are roughly equivalent.  When the
arithmetic means  are considered,  the  hierarchy  is the same as that  established  for
cadmium, copper,  and zinc.  The logarithmic mean nickel removal is 88.4 percent or
               TABLES.  ARITHMETIC MEAN INFLUENT AND EFFLUENT
                         CONCENTRATIONS FOR THE FIVE PROCESSES
  Concentrations in M9/L (values in parentheses are percentage reductions from raw feed)
Heavy metal
Cadmium
Copper
Chromium
Nickel
Zinc

Concentrations
Heavy metal
Cadmium
Copper
Chromium
Nickel
Zinc
* 1 /^rt awora/io .nf
Raw feed
4,805
4,136
26,006
18,617
259,865
TABLE 4.
in jug/L (values
Raw feed
135
673
1,039
976
23,904
v thr^iinH v
LO-CL
144
(97.00)
963
(76.72)
603
(97.68)
2,021
(89.14)
8,385
(96.77)
LO-CLF
103
(97.86)
673
(83.73)
58
(99.78)
1,561
(91.62)
6,629
(97.45)
LWS-CL
25
(99.48)
521
(87.40)
370
(98.58)
1,506
(91.91)
491
(99.81)
LSPF
13
(99.37)
96
(97.68)
58
(99.78)
652
(96.50)
517
(99.80)
LWS-CLF
8
(99.83)
70
(98.31)
86
(99.67)
751
(95.97)
422
(99.84)
LOGARITHMIC MEAN* INFLUENT AND EFFLUENT
CONCENT RA TIONS FOR THE FIVE PROCESSES
in parentheses are
LO-CL
31
(77.04)
109
(83.80)
136
(86.91)
156
(84.02)
820
(96.57)
TT7 l™~1 1 '
percentage
LO-CLF
18
(86.67)
63
(90.64)
24
(97.69)
118
(87.91)
210
(99.12)
'9* \
reductions from raw
LWS-CL
8
(94.07)
49
(92.72)
108
(89.61)
155
(84.12)
195
(99.18)

feed)
LSPF
5
(96.30)
21
(96.88)
24
(97.69)
93
(90.47)
46
(99.81)


LWS-CLF
4
(97.04)
16
(97.62)
32
(96.92)
113
(88.42)
31
(99.87)


-------
greater for the two most effective processes, and the logarithmic mean nickel level in
the effluents is 113  jug/L or less.

    Chromium removal is not significantly improved  by the presence of sulfides.  That
is, the  unfiltered  effluents (LO-CL and LWS-CL processes) showed logarithmic  mean
concentrations that were about equal at 136 and 108 jug/L, and the logarithmic means for
the filtered effluents (LO-CLF, LSPF, and LWS-CLF) were also about equal at 24,  24,
and 32 /xg/L, respectively. This grouping clearly indicates that filtration after clarifica-
tion had exerted a marked effect.  Logarithmic mean chromium removal rates are 86.9
percent  or  greater for  the unfiltered  effluents and  96.9 percent  or  greater for  the
filtered.  Logarithmic mean chromium levels of  32 jug/L  or  less were  obtained in  the
effluents from the filtered processes and 136 /ug/L or less in the unfiltered.

    These findings agree with  the observation that chromium,  unlike the other metals
considered, precipitates a hydroxide, not a sulfide, in the presence of sulfide ions.  Thus,
no difference would be anticipated between the removal rates of  hydroxides precipitated
by lime and hydroxides precipitated by sulfides.  The solubility constant of the hydroxide
would govern in both cases.

    Lead was removed effectively in some tests, such as Runs 5, 8, 14,  and  15. In each
of  these, the  removal efficiency is  96.6 percent or  greater  for  all  five processes.
However, in  many other  runs,  the efficiency of removal  is poor,  ranging from 0  to 77
percent.  In two cases, Runs 1 and 4, a striking improvement  was noted  in the effluents
from filtered processes compared with the effluents from unfiltered processes. In Run 1,
the removal efficiency of the filtered process is 91.1 percent or  greater, but  virtually no
removal took place in the unfiltered process. In Run 4, the filtered-process removal
efficiency is 82 percent  or greater, but the  efficiency is only 30 to  64  percent for the
unfiltered process.  Further work is needed to determine the underlying causes of  these
variations in  the  effectiveness  of the  processes.  Based on the present tests,  for lead
removal, the sulfide processes apparently have no advantage over the lime process.

    When  the sulfide processes are  used, silver  removal is  not significantly different
from conventional lime processing.

    Tin is removed efficiently  by all  processes in Runs 3, 7, and 12, with greater than
95-percent removal efficiency.  Runs 4 and  5 are less efficient, with removal ranging
from 19 to 86 percent. The sulfide processes are no more efficient than the conventional
lime processes.

CONTROL OF SULFIDE  CONCENTRATION BY SPECIFIC ION ELECTRODE

    The dependability of the sulfide specific ion electrodes  that  were  used to control
sulfide  levels was  excellent during the 6-month period while the bench-scale  plant was in
operation. Ruggedness,  freedom  from drift, and ease of  electrode maintenance  were
roughly intermediate when compared to those of a typical combination pH electrode and
to those of an oxidation-reduction-potential (ORP) probe.

-------
                                    SECTION 3

                               RECOMMENDATIONS

    To use conventional  lime processing for reducing the levels of cadmium, copper,
nickel, or zinc in the effluent from a wastewater treatment plant, we recommend that:
    a.   The addition of a filtration operation should be considered;
    b.   If reduction of these heavy metals to the desired levels cannot be achieved by
         filtration alone,  the use of the LSPF process described in this report should be
         considered.
Details about costs and about the anticipated levels that would be achieved by courses a
and b are given in this report.

    The LWS processes are recommended only for small plants (37.85 m3/day or 10,000
gal/day),  because  of the  high  consumption of soluble  sulfide.  The high consumption
results in prohibitive chemical costs in larger  plants (757 m3/day or 200,000 gal/day and
larger).

    If reduction of  the levels of chromium, lead, silver, or tin in the  effluent from  a
waste treatment plant that uses conventional lime processing is required, we recommend
filtration.  The sulfide processes tested in this study  did  not significantly reduce the
levels of these metals and are not recommended.

    Finally,  we recommend  that research be initiated to determine information  about
the leaching  and about other characteristics of  the sulfide  sludges generated by the
processes described in this report and to determine the availability of disposal sites for
such sludges.

-------
                                   SECTION 4

                     DESCRIPTION OF THE LIME PROCESSES
                              (LO-CL AND LO-CLF)
GENERAL
    The lime process for removing heavy metals from wastewater consists essentially of
raising the pH of the normally acid or neutral wastewater to a predetermined value that
is within the range 8.0 to 11.0 pH. A lime slurry is added, and the resultant precipitate,
containing the bulk of the heavy metals, is separated.

    The lime process will not remove chromium  in the form of chromates or dichro-
mates (for example, hexavalent chromium Cr6+ ),  and it will not remove  heavy metals
complexed with cyanide.   Therefore,  when these  ions  are present in the wastewater,
pretreatment is necessary to remove  them.  In this program, the methods used to remove
hexavalent chromium and cyanides are  described in Section 8.

OUTLINE OF LIME PROCESS

    The sequence of unit operations for  the lime  process used in this work is shown in
Figure 1.    Notes  on  each operation are  provided  in the  following  paragraphs;  a
description of the actual test hardware is  given in Section 9.

Input Filter

    A filter (0.1  p.m  nominal) at the input made-sure that a uniform  sample, free from
variable amounts of  suspended matter, would be processed.   The filter was for sample
uniformity only and is not recommended for a full-sized industrial plant.

Lime Slurry

    This was composed of a suspension of 50 g/L CaO, continuously stirred.

Flash Mix Tank

    In  this continuously stirred tank, the  pH of  the raw feed  water was  raised  to a
preselected value.  (Criteria for selecting the pH are given in Appendix H.) The value
was maintained at ±0.1  pH  unit by rnetered additions of  lime slurry that were controlled
by a pH probe.  Polyelectrolyte additions were made to the pH-adjusted stream at the
exit of the flash mix tank.

-------
                           LIME
                           SLURRY
 FEED
          INPUT
          FILTER
                pH
              CONTROLLER
                             \ '
                              • *
                             L \
                I
               .J
FLASH
MIX
SETTLING
COLUMN
CLARIFIER
                          POLYELEC-
                          TROLYTE
FINAL
FILTER
                                                                            EFFLUENT
                         SAMPLE POINT
                         FOR LO-CL
                              SAMPLE POINT
                              FOR LO-CLF
                        Figure 1. Lime only process flow diagram.
Polyelectrolyte

     This  substance  was  a freshly prepared  concentrate  of  a  proprietary, anionic
polyelectrolyte that improves the flocculation of precipitated metals in wastewaters.

Settling Column Clarif ier

     The pH-adjusted wastewater from the flash mix tank was continuously fed upward
through a settling  column, and the precipitated sludge  was allowed to collect at the
bottom of the column.  Clarified effluent was  passed continuously from the top of the
column.   Liquid rise  rate  in  the column  was  10.3 mm/min,  and the  sludge settling
velocity was generally 40 mm/min or greater; thus good separation was readily obtained.
In all tests, except Runs  1, 2, and 9, sampling of  the process effluents was delayed until a
sludge bed at least 50 mm thick had formed; more complete clarification is expected
when the effluent passes through  such  a bed.   For Runs 1, 2, and  9, insufficient
precipitate was  generated, and it was impossible to build up a thick sludge bed with the
limited 190L samples  that were available.

Final Filter

     A final  filter (0.1 jum nominal) removed traces of precipitate that were carried over
from the clarifier.  Samples drawn from points  before and after the filter  were used to
determine the amount of carryover; the  LO-CL samples were taken before  the filter,
and the LO-CLF samples were  taken after it.

-------
                                    SECTION 5

             DESCRIPTION OF THE LIME- WITH -SULFIDE PROCESSES
                             (LWS-CL AND LWS-CLF)
GENERAL
    The lime-with-sulfide process for  removing heavy  metals from  wastewater is a
modification of the lime process described in Section k.  In the modified process, suifide
is  added to the  flash mix tank simultaneously with  the lime slurry.  Coprecipitation of
heavy metal sulfides and hydroxides occurs in the tank.

    For each wastewater in this study, the same pH value was used for the lime process
and the lime-with-sulfide process.

    Suifide additions were made continuously to the flash mix tank to maintain a small
(about 0.5 mg/L) excess of S=.

OUTLINE OF LIME-WITH-SULFIDE PROCESS

    The sequence of unit operations of the lime-with-sulfide process, shown in Figure 2,
involves suifide additions controlled by a specific ion electrode.  Soluble suifide is added
to the flash  mix tank simultaneously with the lime slurry. The input filter, lime slurry,
polyelectrolyte,  clarifier, and final filter  were operated in the same manner  as in the
lime process (see  Section 4).  A description of the  additional test hardware is given in
Section 9.  Notes on the additional operation and the flash mix tank are provided in the
following paragraphs.

Soluble Suifide

    This was composed of a freshly prepared solution of 10 g/L Na2S'9H2O.

Flash Mix Tank

    Metered additions  of lime slurry and suifide solution were made to the  raw feed
water in this continuously stirred  tank.  The pH of  the raw feed water was raised to a
preselected value.  (Criteria for selecting the pH are given in Appendix H.)  The value
was maintained at ±0.1  pH unit by metered additions of the lime slurry, as controlled by
the pH probe.   Simultaneously, metered additions  of the suifide  solution, which  were
controlled by a reference electrode pair to detect the suifide specific ion, maintained a
preselected potential  of -550 mV ±10 mV  with respect to the  reference  electrode.
Polyelectrolyte additions were made to the pH- and suifide-adjusted stream at the exit
of  the flash mix tank.

-------
FEED
SULFIDE
CONTROLLER
Ii
l—
1 	
INPUT
FILTER


	
	 >
SOLUBLE
SULFIDE
\
/
1
I
7
i


r
i
1 	 ' 	 r
* FLASH *
MIX
t
i
POLYELEC-
TROLYTE

^^^H •••••

LIME
SLURRY
4

pH
CONTROLLER
1 1
J 1

A "
	 J
SETTLING
COLUMN
CLARIFIER


1
SAMPL
FOR LV
k-
r
E P(
VS-<
FINAL
FILTER
EFFLUENT

DINT SAMPLE POINT
2L FOR LWS-CLF
                     Figure 2. Lime-with-sulfide process flow diagram.
CONTROL OF SULFIDE ADDITIONS

    The preselected value of -550 mV corresponds to about 0.5 mg/L of free sulfide and
was selected for two reasons:
    •    The curve of electrical potential versus sulfide concentration  has its  maximum
         gradient in this region, thus giving a large response to a small change in free-
         sulfide concentration.
    •    The concentration of 0.5 mg/L  was the minimum excess sulfide that gave  no
         detectable odor from solutions at pH 8 to 9.

    The electrode was nearly troublefree and  had negligible  drift.   Fouling  of the
electrode surface by precipitated materials usually was countered by wiping with a paper
tissue.   At about 2-month intervals, the response of the electrode became noticeably
sluggish  when tested  in a reference solution.   Light  abrasion  with  600-mesh  silicon
carbide corrected this condition and restored the response rate.  The  electrode  usually
was used for 6 hours per day and stored overnight  in clean water.
                                         10

-------
                                   SECTION 6

                 DESCRIPTION OF THE LIME, SULFIDE POLISHED
                         AND FILTERED PROCESS (LSPF)
GENERAL
    The  lime,  sulfide polished and filtered process  for  removing heavy metals from
wastewater is a modification of the lime process described in Section 4.  In the modified
process, sulfide is added to  the wastewater after the  bulk of  the heavy metals has been
removed by a lime process.  The precipitation and removal of the small amount of heavy
metals that remain after lime processing is the polishing operation.

OUTLINE OF LIME, SULFIDE POLISHED AND FILTERED PROCESS

    The  sequence of unit operations of the lime, sulfide polished and filtered process,
shown in Figure 3, involves  sulfide additions, controlled by a specific ion electrode, to
the sulfide polishing tank, which contains  lime-processed and  clarified wastewater.  The
input filter, lime slurry, polyelectrolyte, clarifier, and final filter  were  operated in the
same manner  as  they were in the lime process (see Section 4).  A description of  the
additional test  hardware used in this process is given in Section 9.  Notes on the sulfide
polishing operation are provided in the following paragraphs.

Soluble Sulfide

    This was composed of a freshly prepared solution of 10 g/L Na2S'9H2O.
SOLUBLE
SULFIDE
\
i
r
i
SULFIDE
POLISHING


r
1
I




SULFIDE
CONTROLLER
j '
1
	 1
FINAL
FILTER

EFFLUENT

                                                                      SAMPLE POINT
                                                                      FOR LSPF
              Figure 3.  Lime, sulfide polished and filtered process flow diagram.
                                         11

-------
Suifide Polishing

    Metered additions of the soluble sulfide solution were made to the pH-adjusted and
clarified wastewater in  this continuously stirred tank.  The metered additions, which
were  controlled  by  a reference  electrode  pair  to  detect the sulfide specific ion,
maintained a preselected potential  of  -550 mV  ±10 mV  with respect to the reference
electrode.   The behavior of the  electrodes was similar  to  their behavior  in the  LWS
process.  The notes  in Section  5 under  "Control  of Sulfide Additions" apply also to the
LSPF process.
                                         12

-------
                                    SECTION 7

                        REASON FOR OMISSION OF TESTS
                            ON THE SULFEX PROCESS

    The Sulfex  process for removing heavy metals from processed waste streams  by
sulfide precipitation is a proprietary system developed by The Permutit Company (2). It
differs from others described in Sections 5 and 6 of this report in that it uses relatively
insoluble iron sulfide, instead of highly  soluble  sodium  sulfite or  hydrosulfide,  as  its
source of sulfide ions for precipitation. Descriptions of  the Sulfex process are  given in
References 1, 2, and 3.

    Although we originally intended to include the Sulfex process in this study, to enable
its merits to  be  objectively determined in direct comparison with conventional lime and
soluble  sulfide methods, problems with commercial secrecy prevented its inclusion in the
program.

    The Sulfex process relies  partly on an existing patent (4) and partly on  commercially
secret knowledge, some of which is included in a new patent application.   The Permutit
Company understandably declined to reveal details of their process until an acceptable
secrecy agreement had been signed  between Permutit and Boeing.   Protracted negotia-
tions  failed to reach this agreement, and  the  comparative tests on this  process  were
deleted from the program.
                                         13

-------
                                  SECTION 8

                  REMOVAL OF CYANIDES AND HEXAVALENT
                       CHROMIUM FROM WASTEWATERS
GENERAL

    Heavy  metals complexed with cyanides are not removed by the lime process, and
neither  is chromium in the form of chromates  and dichromates, that is,  hexavalent
chromium (5).  Consequently, the removal of cyanides and hexavalent chromium from a
wastewater before subsequent lime processing is a common practice.

REMOVAL OF CYANIDES

    The alkaline chlorination process (5, 6) was used to remove cyanides when they were
present  in the  raw wastewater, that is, in Runs 5 and 9.  The process, which was carried
out in 100L batches, is as follows:
    a.  Raise pH to  10.0 or higher (not necessary with the samples for Runs 5 and 9
        because they  were already in this condition).
    b.  Add  5-percent  sodium  hypochlorite  solution  until oxidizing  conditions are
        present,  as indicated by an oxidation-reduction potential (ORP) (7)  of 400 mV
        minimum to convert the cyanide to cyanate.
    c.  Reduce pH to 2.5 by the addition of sulfuric acid.  After  about  5  min, the
        cyanates in the wastewater are converted to carbon  dioxide and nitrogen.

REMOVAL OF HEXAVALENT CHROMIUM

    Reduction of the  hexavalent chromium found in all raw feed wastewaters (except
Runs 5,  8, 12, and 13) was accomplished by adding sulfuric acid  wherever necessary to
lower the pH to 2.5.  This was followed by the addition of  sodium sulfite until a 10- to
15-mg/L excess of SO3 was indicated by iodometric titration (8). The wastewater was
allowed  to stand for a minimum of 1 hour after  reduction before treatment in the bench-
scale plant.

-------
                                   SECTION 9

                 BENCH-SCALE EQUIPMENT USED IN THE TESTS
GENERAL
    Wastewaters were processed through a single bench-scale unit (Figure 4) that was
capable of operation in  each  of  the five  process  modes:  LO-CL,  LO-CLF, LSPF,
LWS-CL,  and LWS-CLF.  Changeover from one mode to another  was accomplished  by
opening the appropriate valves and actuating the necessary feed  pumps.  Wastewater
flow rate through the equipment was 130 mL per minute.

    Process details are given in Sections 4 (lime process), 5 (lime-with-sulfide process),
and 6 (lime,  sulfide  polished and filtered process).  Figure  5 is a  flow diagram for the
multipurpose bench-scale unit.  Figures 4, 6, and 7 show the actual equipment.

EQUIPMENT DETAILS

    Individual items  of equipment are detailed  in  the  following  list (located by key
number in the flow diagram, Figure 5).

     1.  Sample  drum: ACT  1 poly-drum  (black,  polyethylene,  55-gal shipping and
        storage  drum);  ACT  Poly-drum Division,  1100 South Azusa Ave., City  of
        Industry, California 91748
    2.  Tank: 350L stainless steel
    3.  Stirrer:  J£ hp, 1,725 rpm, 32-in stainless steel shaft, with propeller
    4.  Tank: Polyethylene, 150L, with lid
    5.  Pump:  Peristaltic type, 130 mL per minute
    6.  Filter:  Disposable, wound polypropylene  fiber type, nominal removal rating 0.1
        jum;  Motor  Guard  Corporation  Model D-15, P. O.  Box  1834, San  Leandro,
        California 94577
    7.  Pump:  Peristaltic  type, variable  speed  6 to 120 mL per minute, Masterflex
        7545 drive and 7014 pump head;  Cole-Parmer Industrial Co., 7425 N. Oak Park
        Ave., Chicago, Illinois  60648
    8.  Tank: Polyethylene, 7.5L capacity
    9.  pH controller: Chemtrix type 45 with 500W output and high and low  adjustable
        setpoints; Chemtrix Inc., 163  S.W. Freeman Ave., Hillsboro, Oregon 97123
    10. Sulfide  controller:  Chemtrix type 45 with 400W output and high and low
        adjustable setpoints; Chemtrix Inc., 163 S.W. Freeman Ave.,  Hillsboro, Oregon
        97123
    11. Tank: Polyethylene, 3L capacity
    12. Clarifier: Plexiglas column,   127-mm (5-in) diameter, 610-mm (24-in) water
        height
                                       15

-------
•-
                       POLYELECTRO-
                       LYTE FEED PUMP ,
                           VARIABLE-
                           SPEED
                           PUMP FOR
                           LIME
                           SLURRY
                           FEED .
                                               pH ELEC
                                               TRODE
            SULFIDE
            ELECTRODES
                                                                                         SAMPLE
                                                                                         TANKS
                                                 FLASH
                                                 MIX
                                                 TANK
LIME
SLURRY
TANK
SULFIDE
POLISH
TANK
                   CONTROLLER
               "I   FOR VARIABLE
                   SPEED PUMP
                            Figure 4. Bench-scale unit for processing industrial wastewater by the LO-CL,
                                    LO-CLF, LSPF, LWS-CL, and LWS-CLFprocesses.

-------
                                     SULFIDE
                                     CONTROLLER

LER
(io)



SULFIDE
TANK
©
1
^

                                                                             STIRRER
Note.. See text for identity of key-numbered equipment.

               Figure 5.  Flow diagram of multipurpose bench-scale equipment.
    13.  Stirrer: Variable-speed laboratory stirrer, 1/75 hp, with 50-mm-diameter stain-
        less  steel  propeller,  T-Line No.   101,  Tallboys  Engineering  Corporation,
        Emerson, New 3ersey 07630
    14.  Pump:  Peristaltic type, 2.8 mL per  minute; Cole-Farmer Industrial Co., 7425
        N. Oak Park Ave., Chicago, Illinois 60648
    15.  Valve:  Pinch-type tubing  control valve, Dura-Clamp®, United States  Plastic
        Corporation, Lima, Ohio 45801       ':
    16.  pH electrode: Chemtrix, No.  H005; Chemtrix Inc.,  163  S.W.  Freeman Ave.,
        Hillsboro, Oregon 97123
    17.  Sulfide  specific ion electrode: Orion  94-16A  used  with reference electrode
        Orion 90-02, Orion Research Inc., 380 Putnam Ave., Cambridge, Massachusetts
        02139;  or, Sensorex S1015M used with reference electrode, Sensorex RD1015F,
        Sensorex, 502 Armstrong Ave., Irvine, California  92705
                                        17

-------
SAMPLE
POINT
FILTER
pH CON-
TROLLER
STIRRER
 LIME
 SLURRY
 TANK
SAMPLE
RESER-
VOIR
                                                                        VENT HOOD
                                                                        FOR AIR
                                                                        EXTRACTION
                                                                           SOLUBLE
                                                                           SULFIDE
                                                                           SUPPLY
                                                                           TANK
                                                                        SULFIDE
                                                                        CONTROLLER
                                                                        SULFIDE
                                                                        ELECTRODES
                                                                            pH ELEC-
                                                                            TRODE
               FLASH
               MIX
               TANK
       CONTROLLER
       FOR VARIABLE
       SPEED PUMP
VARIABLE-SPEED
PUMP FOR LIME
SLURRY FEED
             Figure 6. Bench-scale unit showing instrumentation and air vent hood.


-------
                                    VENT HOOD FOR
                                    AIR EXTRACTION
Figure 7.  Wastewater being charged into sample reservior of bench-scale unit from sample drum.


                                         19

-------
                                  SECTION 10

           DESCRIPTION OF THE FOURTEEN WASTEWATERS TREATED

    The wastewaters collected for treatment in the bench scale plant were representa-
tive of wastewaters generated by  the nonferrous metal producing and metal finishing
industries  in the  United States.   Because  the  chelating  agents  usually  present  in
electroplating wastewater are known to inhibit precipitation (9,  10), emphasis was placed
on obtaining  wastewater samples from as wide a  variety of electroplating sources  as
possible.   Twelve samples of electroplating, anodizing, and other metal finishing rinse
waters plus one  nonferrous metal smelter's wastewater (Run 8) and one copper printed
circuit etching wastewater  were collected.   All the samples  were collected in new
polyethylene 190L (50-gal) drums.

    The samples were  supplied from companies spread over 10 states to minimize the
effects  of local geographical conditions.  About  half  of  the samples were average
samples collected over a few days; the remainder were "grab" samples.

    Brief  individual descriptions of each  sample are  given in Appendix A (case history
data); the identity of the wastewater supplier companies is kept confidential at their
request.
                                       20

-------
                                  SECTION 11

                 PRESENTATION OF THE ANALYTICAL RESULTS

    To  simplify the  data  on the efficiency  of  removing heavy  metals  by the five
processes, the detailed results of Appendix A are condensed into two tables and a number
of graphic presentations.         v

    Tables 5 and 6 show the mean concentrations of cadmium, copper, chromium, nickel,
and zinc in the raw feed and in the effluents from each of the processes.  Conventional
mean determinations may be  misleading when applied  to sets having an extremely wide
range (such as the nickel effluent concentrations, which range from <4 to 11,000 Mg/L f°r
one process).  Thus, both the conventional mean and the logarithmic  mean are used.
Table 5 shows the conventional mean,  and Table 6, the mean based on a logarithmic
scale. That is, for n observations (x.	x ):
                                    vn
                                    ' I
    Conventional (arithmetic) mean = 	
                                      -      log x
    Logarithmic mean              = log


    Tables 5 and 6 also show the percentage reduction of the heavy metal concentra-
tions for each process.
              TABLE 5.  ARITHMETIC MEAN INFLUENT AND EFFLUENT
                        CONCENTRA TIONS FOR THE FIVE PROCESSES
  Concentrations in M9/L (values in parentheses are percentage reductions from raw feed)
Heavy metal
Cadmium
Copper
Chromium
Nickel
Zinc
Raw feed
4,805
4,136
26,006
18,617
259,865
LO-CL
144
(97.00)
963
(76.72)
603
(97.68)
2,021
(89.14)
8,385
(96.77)
LO-CL F
103
(97.86)
673
(83.73)
58
(99.78)
1,561
(91.62)
6,629
(97.45)
LWS-CL
25
(99.48)
521
(87.40)
370
(98.58)
1,506
(91.91)
491
(99.81)
LSPF
13
(99.37)
96
(97.68)
58
(99.78)
652
(96.50)
517
(99.80)
LWS-CLF
8
(99.83)
70
(98.31)
86
(99.67)
751
(95.97)
422
(99.84)
                                       21

-------
              TABLE 6.  LOGARITHMIC MEAN* INFLUENT AND EFFLUENT
                        CONCENTRA TIONS FOR THE FIVE PROCESSES
  Concentrations in jug/L (values in parentheses are percentage reductions from raw feed)
Heavy metal
Cadmium
Copper
Chromium
Nickel

Zinc


* Log average of >
Raw feed
135
673
1,039
976

23,904


<1 through xn
LO-CL
31
(77.04)
109
(83.80)
136
(86.91)
156
(84.02)
820
(96.57)
/]C, '°9:
1 u-M 1
log I n
LO-CLF
18
(86.67)
63
(90.64)
24
(97.69)
118
(87.91)
210
(99.12)
A
I

LWS-CL
8
(94.07)
49
(92.72)
108
(89.61)
155
(84.12)
195
(99.18)


LSPF
5
(96.30)
21
(96.88)
24
(97.69)
93
(90.47)
46
(99.81)


LWS-CLF
4
(97.04)
16
(97.62)
32
(96.92)
113
(88.42)
31
(99.87)


    Two main types of graphic plots are given in the Appendices.  Appendix C plots
compare the effluent concentrations  of pairs of processes.  Each point plotted has two
coordinates:   the concentration of  a metal  in process  A effluent (x-axis), and  the
concentration of the same metal in process B effluent (y-axis).  A point below the H5-deg
line results when there  is a higher concentration of  the metal in process A effluent; if all
the points are below the line, then process A is clearly less effective in removing  that
metal than process B.  For example,  in the following diagram the LO-CL process is less
effective than the LSPF process in removing copper.
                      cr
                      LU
                      u-3- iee
                      O v)

                      2o
                      h-O
                      
-------
C-2 diagrams compare the LO-CLF and LO-CL processes
C-3 diagrams compare the LSPF and LWS-CL processes
C-4 diagrams compare the LWS-CL and LO-CLF processes
C-5 diagrams compare the LO-CLF and LWS-CLF processes
C-6 diagrams compare the LO-CL and LWS-CLF processes
C-7 diagrams compare the LSPF and LO-CLF processes
C-8 diagrams compare the LWS-CLF and LSPF processes
C-9 diagrams compare the LWS-CLF and LWS-CL processes
C-10 diagrams compare the LWS-CL and LO-CL processes
  £
  , Appendix G  bar charts show the  relationship between the raw feed concentrations
and effluent concentrations for each heavy metal.  For example, the following bar chart
shows raw feed and effluent concentrations for copper in the LWS-CLF process.
             teeeee
           O
           u
           u_
           O
           z
           O
           CE
           8-1
              leeee
1990
               199
                  COPPER
                                            Raw feed


                                            LWS-CLF process
                  1 2 3 4 5  6  7 8 9 10 11 1213
                          TEST RUN NUMBER
                                              16
     The bar charts of Appendix G are as follows:

G-l  diagrams display raw feed and effluent concentrations of cadmium, copper,
     chromium, nickel, and zinc for the LO-CL process
G-2  diagrams display raw feed and effluent concentrations for the LO-CLF process
G-3  diagrams display raw feed and effluent concentrations for the LSPF process
G-4  diagrams display raw feed and effluent concentrations for the LWS-CL process
G-5  diagrams display raw feed and effluent concentrations for the LWS-CLF process

     The use of the graphic presentations  of Appendices C and G  enables rapid  visual
comparisons to be made for any desired sets of the experimental results.
                                       23

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                                    SECTION 12

                    CAPITAL COSTS OF FULL-SCALE PLANTS

    The estimated costs of  installing full-scale wastewater treatment plants are given
in this section.  Not included in  the estimates are: land acquisition costs; sewer, road,
and other  utility connection costs; preparation costs for environmental impact state-
ment; or site survey and test boring costs.

    Table  7 compares the estimated capital costs of small,  medium-sized, and large
plants for the five treatment processes.

    Tables 8, 9, and 10 are detailed cost estimate summaries for constructing plants for
each of the five processes.

            TABLE 7.  SUMMARY OF PLANT CAPITAL INSTALLATION COSTS
                 Process
        Plant
        capacity
          Capital costs (thousands of 1978 dollars)
LO-CL
LO-CLF
LSPF
LWS-CL
LWS-CLF
         37.85 m3/day          233        237        259        255
         (10,000 gal/day)

         757 m3/day            799        805        892        872
         (200,000 gal/day)

         1,893 m3/day         1,296       1,310       1,407       1,376
         (500,000 gal/day)
                                               259
                                               879
                                              1,389

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                  TABLES.  SMALL PLANT CONSTRUCTION



Plant capacity = 37.85 m3 (10,000 gal) per day
COSTS
Item
Capital Expense
Total
Process 1, LO-CL
Architectural
Mechanical
Electrical
Subtotal
A&Efee + CM,* 12.5%
Total
$ 42,700
139,500
19,000

$5,400
$201,200 $5,400
25,200 700
$226,400 $6,100
$ 48,100
139,500
19,000
$206,600
25,900
$232,500
Process 2, LO-CLF
Architectural
Mechanical
Electrical
Subtotal
A&Efee + CM/ 12.5%
Total
$ 43,464
141,996
19,340

$5,400
$204,800 $5,400
25,600 700
$230,400 * -$6,100
$ 48,864
141,996
19,340
$210,200
26,300
$236,500
Process 3, LSPF
Architectural
Mechanical
Electrical
Subtotal
A&E fee + CM,* 1 2.5%
Total
$ 52,100
152,300
19,000

$6,400
$223,400 $6,400
27,900 800
$251,300 $7,200
$ 58,500
152,300
19,000
$229,800
28,700
$258,500
Process 4, LWS-CL
Architectural
Mechanical
Electrical
Subtotal
A&Efee + CM,* 12.5%
Total
$ 52,100
148,800
19,000

$6,400
$219,900 $6,400
27,500 800
$247,400 $7,200
$ 58,500
148,800
19,000
$226,300
28,300
$254,600
Process 5, LWS-CLF
Architectural
Mechanical
Electrical
Subtotal
A&Efee + CM,* 12.5%
Total
$ 52,945
151,214
19,308

$6,400
$223,467 $6,400
27,933 800
$251,400 $7,200
$ 59,345
151,214
19,308
$229,867
28,733
$258,600
*A&E fee + CM = architectural and engineering fee plus central management
                                        25

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               TABLE 9. MEDIUM-SIZED PLANT CONSTRUCTION
 Plant capacity = 757 m3 (200,000 gal) per day
                                          COSTS
Item
Capital Expense
Total
Process 1, LO-CL
Architectural
Mechanical
Electrical
Subtotal
A&E fee + CM,* 1 2.5%
Total
$287,400
326,900
91,700

$3,800
$706,000 $3,800
88,300 400
$794,300 $4,200
$291,200
326,900
91,700

$709,800
88,700
$798,500
Process 2, LO-CL F
Architectural
Mechanical
Electrical
Subtotal
A&E fee + CM,* 12.5%
Total
$289,770
329,596
92,456

$3,800
$711,822 $3,800
88,978 400
$800,800 $4,200
$293,570
329,596
92,456

$715,622
89,378
$805,000
Process 3, LSPF
Architectural
Mechanical
Electrical
Subtotal
A&E fee + CM,* 12.5%
Total
$296,800
373,500
118,800

$3,800
$789,100 $3,800
98,600 400
$887,700 $4,200
$300,600
373,500
118,800

$792,900
99,000
$891 ,900
Process 4, LWS-CL
Architectural
Mechanical
Electrical
Subtotal
A&E fee + CM,* 12.5%
Total
$296,800
361,200
113,600

$3,800
$771,600 $3,800
96,600 400
$868,200 $4,200
$300,600
361,200
113,600

$775,400
97,000
$872,400
Process 5, LWS-CL F
Architectural
Mechanical
Electrical
Subtotal
A&E fee + CM,* 12.5%
Total
$299,074
363,967
114,470

$3,800
$777,511 $3,800
97,1 89 400
$874,700 $4,200
$302,874
363,967
114,470

$781 ,31 1
97,589
$878,900
Note:  Piling costs for medium-
* A&E fee + CM = architectural
sized plants represent 12% to 16% of the total cost.
and engineering fee plus central management
                                           26

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                  TABLE 10.  LARGE PLANT CONSTRUCTION COSTS
Plant capacity = 1,893 m3 (500,000 gal) per day
Item
Capital Expense
Total
Process 1, LO-CL
Architectural
Mechanical
Electrical
Subtotal
A&E fee + CM,* 12.5%
Total
$621,800
425,200
93,900

$11,300
$1,140,900
142,600
$1,283,500
$11,300
1,400
$12,700
$633,100
425,200
93,500
$1,152,200
144,000
$1 ,296,200
Process 2, LO-CL F
Architectural
Mechanical
Electrical
Subtotal
A&E fee + CM/ 12.5%
Total
$628,343
429,674
94,872

$11,300
$1,152,889
144,111
$1,297,000
$11,300
1,400
$12,700
$639,643
429,674
94,872
$1,164,189
145,511
$1,309,700
Process 3, LSPF
Architectural
Mechanical
Electrical
Subtotal
A&E fee + CM,* 12.5%
Total
$631,200
487,000
121,000

$11,300
$1,239,200
154,900
$1,394,100
$11,300
1,400
$12,700
$642,500
487,000
121,000
$1,250,500
156,300
$1,406,800
Process 4, LWS-CL
Architectural
Mechanical
Electrical
Subtotal
A&Efee + CM,* 12.5%
Total
$631,200
464,700
115,800

$11,300
$1,211,700
151,500
$1,363,200
$11,300
1,400
$12,700
$642,500
464,700
115,800
$1,223,000
1 52,900
$1,375,900
Process 5, LWS-CLF
Architectural
Mechanical
Electrical
Subtotal
A&Efee + CM,* 12.5%
Total
$637,468
469,315
116,950

$11,300
$1,223,733
152,967
$1,367,700
$11,300
1,400
$12,700
$648,768
469,315
116,950
$1,235,033
154,367
$1 ,389,400
Note:  Piling costs for large plants represent 12% to 16% of the total cost.
*A&E fee + CM = architectural and engineering fee plus central management

                                           27

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                                   SECTION 13

                  OPERATING COSTS OF FULL-SCALE PLANTS
GENERAL

    Operating costs for  three  full-scale  plants based on the principles of the bench-
scale plants is developed  in this section. A summary of the operating costs is presented
in Table 11. Details on which the costs are based are given in Tables 12, 13, and  14.

ASSUMPTIONS USED IN THE CALCULATIONS

    a.  All costs are in 1978 dollars.

    b.  Amortization of plant cost (purchase price plus installation cost)  is calculated
        at 8 percent over a 12-year life.

    c.  Operating  labor costs  are  $30/hr total, including basic wage, overtime, fringe
        benefits, and management and overhead burden.

    d.  One operator working half of an 8-hr shift will be required for the  smallest
        plant, 37.85  m3/day (10,000 gal/day).   Three part-time operators (with total
        labor of 8  man-hours per day), will be  required for each of the larger plants, at
        757 m3/day (200,000 gal/day), and 1,893  m3/day (500,000 gal/day).  A  three-
        shift operating  schedule increases  the total operating labor cost but  allows a
        reduction in capital equipment cost (the major cost item); the equipment  can be
        sized to handle one-third of the load of a single-shift operation.


                     TABLE 11. SUMMA RY OF OPERA TING COSTS
^~\^^ Process
Plant ^\^
capacity ^\^

LO-CL
37.85 m3/day 5.96
(10,000 gal/day) (22.57)
757 m3/day 0.90
(200,000 gal/day) (3.40)
1,893m3/day 0.55
(500 ,000 gal /day) (2.08)
Operating cost.
LO-CLF
6.00
(22.72)
0.90
(3.42)
0.55
(2.09)
$/m3 ($/
LSPF
6.24
(23.65)
0.97
(3.68)
0.60
(2.26)
1,000 gal)
LWS-CL
6.38
(24.17)
1.13
(4.30)
0.76
(2.89)

LWS-CLF
6.42
(24.32)
1.14
(4.32)
0.77
(2.90)
                                        28

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  e.   The  following items are not taken into  account in  this study:  startup costs,
      operating profit, site purchase cost, preparation costs for environmental impact
      statement, sewage disposal charges, tax credits, costs of cyanide destruction in
      the  case of wastewaters that  contain  cyanides, special additives (such as
      antifoaming agents), electric  power  costs, and laboratory chemical  analysis
      charges.

  f.   Costs  of process  consumables  (for example,  lime,  sulfide) are based on the
      average  value of  each' consumable required for the  14  wastewaters, at  prices
      published in Chemical  Marketing Reporter for December 4,  1978  (12).  These
      prices are:

           Sulfuric acid, 66 B£                               $ if9.4I/ton
           Sodium sulfite anhydrous, technical*               $ 13-75/100 Ib
           Lime, pebble  quicklime                            $31.88/ton
           Sodium hydrosulfide, 71 percent*                   $305.00/ton
           Polyelectrolyte, Betz Laboratories No. 1110        $  2.55/lb
For calculations in this report, sodium sulfite and sodium hydrosulfide are assumed to
be used in full-scale plants.  Cost savings might accrue through the use of equivalent
forms  of  these reactants.   For example, many treatment plants use sulfur  dioxide
acquired in cylinders instead of sodium sulfite.  Hydrogen sulfide in cylinders, though
considerably  less  costly ($0.24/kg of sulfur) than sodium  hydrosulfide  ($0.827/kg of
sulfur), would incur extensive development costs (to overcome potential mass transfer
problems) and would increase equipment costs (to  preclude release to the atmosphere).
For handling  convenience, sodium sulfite Na2SO3  and sodium sulfide Na2S-9H2O were
used in the laboratory.

                                       29

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                     TABLE 12.  OPERATING COSTS FOR SMALL PLANT
Plant capacity = 37.85 m^/day
(10,000 gal/day)
Equipment amortization*
Operating labor t
Chemicals t
Maintenance**
Sludge disposal Tt
Totals

LO-CL
88.15
120.00
4.35
12.00
1.16
225.66

LO-CLF
89.66
120.00
4.35
12.00
1.16
227 .17
Cost per day ($)
LSPF
98.00
120.00
5.29
12.00
1.16
236.45

LWS-CL
96,53
120.00
11.96
12.00
1.16
241.65

LWS-CLF
98.04
120.00
11.96
12.00
1.16
243.16
  * Equipment amortization tt
        (LO-CL)      $232,500  x
        (LO-CLF)     236,500  x
        (LSPF)        258,500  x
        (LWS-CL)     254.600  x
        (LWS-CLF)    258,600  x
0.1326957 350 days
0.1326957 350 days
0.132695 7 350 days
0.132695 7350 days
0.132695 7 350 days
$88.15 pur day
 89.66 per day
 98.00 per day
 96.53 per day
 98.04 per day
  t Operating labor:  $30/hr x 4 hr/day = $120.00 per day
   Chemicals
       Sulfuricacid:    290 mg/L x $0.0507/kg x 37.85 m3/day
       Sodium sulfite:  120 mg/L x $0.280/kg x 37.85 m3/day
       Lime (LO and LSPF): 2,090 mg/L x $0.032/kg x 37.85 m3/day =
       Lime (LWS):     1.635 mg/L x $0.032/kg x 37.85 m3/day
       IMaHS (LWS):  260 mg/L x $0.827/kg x 37.85 m3/day
       NaHS(LSPF): 30 mg/L x $0.827/kg x 37.85 m3/day
       Polyelectrolyte: 0.8 mg/L x $5.62/kg x 37.85 m3/day
            Total chemical cost per day

 "Maintenance:  10% of operating labor cost = $12.00 per day


ttSludge disposal:  1 m3/month at $35/m3 = $1.16 per day

ttCapital cost x 0.132695 = annual repayment for annuity, 8%, 12 years (11).
Cost
LO-CL,
LO-CLF
0.55
1.21
2.43
-
-
- ,
0.16
$4.35
per day
LSPF
0.55
1.21
2.43
—
—
0.94
0.16
$5.29
($)
LWS-CL.
LWS-CLF
0.55
1.21
—
1.90
8.14
—
0.16
$11.96
                                            30

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               TABLE 13.  OPERATING COSTS FOR MEDIUM-SIZED PLANT
Plant capacity = 757 m^/day
. (200.000 gal/day)
Equipment amortization*
Operating labor t
Chemicals 4
Maintenance**
Sludge disposaltt
! Totals
Cost per day ($)
LO-CL
302.73
240.00
90.96
24.00
23.20
680.89
LO-CLF
305.20
240.00
90.96
24.00
23.20
683.36
LSPF
338.14
240.00
109.74
24,00
23.20
735.08
LWS-CL
330.75
240.00
242,66
24.00
23.20
860.61
LWS-CLF
333.22
240.00
242.66
24.00
23.20
863.08
 * Equipment amortization tt
       (LO-CL)   $798,500  x
       (LO-CLF)   805.000  x
       (LSPF)      891.900  x
       (LWS-CL)   872.400  x
       (LWS-CLF)  878,900  x
0.132695/350 days
0.132695 7350 days
0.132695/350 days
0.132695/350 days
0.132695/350 days
$302.73 per day
 305.20 per day
 338.14 per day
 330.75 per day
 333.22 per day
 t Operating labor: $30/hr x 8 hr/day = $240 per day
  Chemicals
       Sulfuric acid:    290 mg/L x $0.0507/kg x 757 m3/day
       Sodium suitite:  120 mg/L x $0_280/kg x 757 m3/day
       Lime (LO and LSPF);. 2,090 mg/L x $0.032/kg x 757 m3/day =
       Lime (LWS):   1,635 mg/L x $0.032/kg x 757 m3/day
       NaHS(LWS): 260 mg/L x $0.827/kg x 757 m3/day
       NaHS (LSPF): 30 mg/L x $0.827/kg x 757 m3/day
       Polyelectrolyte: 0.8 mg/L x $5.62/kg x 757 m3/day
           Total chemical cost per day

Cost per day
LO-CL, LSPF
LO-CLF
11.17
25.54
50.83
-
-
_
3.42
$90.96
11.17
25.54
50.83
-
-
18.78
3.42
$109.74
($)
LWS-CL.
LWS-CLF
11.17
25.54
-
39.76
162.77
-
3.42
$242.66
 1 Maintenance: 10% of operating labor cost = $24.00 per day
ttSludge disposal: 20 m3/month at $35/m3 = $23.20 per day

ttCapital cost x 0.132695 = annual repayment for annuity, 8%, 12 years (11).
                                             31

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                   TABLE 14. OPERATING COSTS FOR LARGE PLANT
Plant capacity = 1,893 m3/day
( 500,000 gal/day)
Equipment amortization*
Operating labor t
Chemicals t
Maintenance**
Sludge disposal tt
Totals

LO-CL
491.43
240.00
226.19
24.00
58.00
1,039.62

LO-CLF
496.54
240.00
226.19
24.00
58.00
1,044.73
Cost per day ($)
LSPF
533.36
240.00
273.16
24.00
58.00
1,128.52

LWS-CL
521.64
240.00
605.70
24.00
58.00
1,444.69

LWS-CLF
526.76
240.00
605.70
24.00
58.00
1,450.21
 * Equipment amortization tt
       (LO-CL)     $1,296,200   x
       (LO-CLF)      1,309,700   x
       (LSPF)         1,406,800   x
       (LWS-CL)      1,375,900   x
       (LWS-CLF)     1,389,100   x
0.132695/350 days
0.1326957 350 days
0.132695/350 days
0.132695/350 days
0.132695/350 days
$491.43 per day
 496.54 per day
 533.36 per day
 521.64 per day
 526.76 per day
 t Operations labor: $30/hr x 8hr/day = $240 per day
 t Chemicals
                                                                          Cost per day ($)
       Sulfuric acid:    290 mg/L x $0.0507/kg x 1,893 m3/day
       Sodium sulfite:   120 mg/L x $0.280/kg x  1,893 m3/day
       Lime (LO and LSPF): 2,090 mg/L x $0.032/kg x 1,893 m3/day
       Lime (LWS):   1,635 mg/L x $0.032/kg x  1,893 m3/day
       NaHS (LWS): 260 mg/L x $0.827/kg x 1,893 m3/day
       NaHS (LSPF):  30 mg/L x $0.827/kg x 1,893 m3/day
       Polyelectrolyte:  0.8 mg/L x $5.62 x 1,893 m3/day
             Total chemical cost per day
LO-CL,
LO-CLF
27.79
63.50
126.40
-
-
-
8.50
LSPF
27.79
63.50
126.40
-
-
46.97
8.50
LWS-CL,
LWS-CLF
27.79
63.50
—
98.88
407.03
-
8.50
                             $226.19    $273.16    $605.70
** Maintenance: 10% of operations labor cost = $24,00 per day
tt Sludge disposal: 50 m3/month, $35/m3 =  $58.00 per day
tiCapital cost x 0.132695= annual repayment for annuity, 8%, 12 years (11),

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                                   SECTION 1*

                 ELECTRON PHOTOMICROGRAPHS OF SLUDGES

    A  few of the sludges obtained from actual  wastewaters and from laboratory-made
dilute solutions that contain copper ions were examined at magnifications up to 50,000x.
At low magnifications, the sludges invariably appeared amorphous.  Only when magnifi-
cations greater than 10,000x were employed could any structure be seen.  At this power,
the sludges  showed  a  granular appearance, with  particles about  0.1 to  0.5 /zm in
diameter. No difference could be observed between sludges generated by lime alone and
those generated by lime with sulfide.

    The  results of these exploratory photomicrographs did not suggest that further work
would be particularly fruitful.  Accordingly, research in this direction was discontinued.

    Figure  8  shows  a typical high-power  (46,500x) electron photomicrograph of  a
iime-with-sulfide sludge.
                                        33

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 ,
 •

rn
 r


 :

•


 i



;
  '\


 ,

 ,

-------
                                   SECTION 15

                   SLIDE AND CASSETTE TAPE PRESENTATION

    A  35-mm color slide presentation with accompanying synchronized cassette tape
narration is available on request.

    The 38-slide presentation lasts about 20 min.  It describes the background of sulf ide
precipitation of heavy metals and the purpose of  the program; it contains photographs of
the bench-scale equipment;  it includes a condensed table of results plus the conclusions
drawn from the program.

    The slides are standard 35-mm, 2-in by 2-in format, and the narration is on a two-
track tape cassette with sound on one channel and a 1,000-Hz slide-advance pulse on the
other.   Suitable  equipment  for  viewing includes (but  is not  restricted to) a Kodak
Ektographic projector and a Wollensak Model 2570 AV  tape player.

    Inquiries regarding the slide  presentation  should  be  addressed to Dr. H. B. Durham,
Industrial  Environmental Research Laboratory,  Office of Research and Development,
U.S. Environmental Protection Agency, Cincinnati, Ohio  45268.
                                        35

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                                  SECTION 16

              CONFIDENCE LEVELS OF THE CHEMICAL ANALYSES
GENERAL
    The  primary  objective of  this program is to document the relative abilities of the
five processes to remove heavy metals from wastewater, so the accuracy and reliability
of the chemical analyses are of fundamental importance. Accordingly, considerable time
and effort were  devoted  to  testing the reproducibility of  the  results obtained by
chemical analysis.

ANALYSIS OF EPA STANDARDS

    Two solutions of composition known only to  the EPA were  supplied to test the
accuracy of Boeing analyses.  The results for the seven principal metals of  interest to
the EPA  are detailed in Table  15.  All Boeing analyses were within the acceptance limits
designated by the EPA.
                    \
STATISTICAL REPEATABILITY TESTS

    Two  12L samples of  a treated  wastewater  (Run  5,  LO-CL  and  LO-CLF) were
analyzed three times  over (on  three separate  days) by the  two  atomic  absorption
methods, flame and flameless, to give a total of six analyses for each of the five heavy
metals tested in this study. Tables 16 and 17 show the results.

    Table 18 gives the calculated limits  within which the true  concentrations would be
expected to fall,  with a  90-percent  confidence level, for 99 percent of a series of
estimations, based on 8.97 standard deviations (13).
                                                       i
    The remaining conclusions  drawn from the repeatability tests are that:
    a.   A statistically significant reduction exists at the 0.975 confidence level in the
        filtered,  compared with the unfiltered, samples;
    b.   A significant difference  exists at the 0.95 confidence level  between the flame
        and  flameless methods  so that, in  order  to  compare  metal levels, the same
        method should be used for both metals being estimated.
                                       36

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              TABLE 15.  ANALYSIS OF EPA STANDARDS
Solution 1
Cug/L)


Metal
Cd
Cr
Cu
Hg
Ni
Pb
Zn

Boeing
analysis
12
79
55
1.5
107
79
71

EPA
actual
10
60
40
3.0
70
80
60
EPA
acceptance
limits
2.84 to 18.0
2 1.2 to 93.6
4.53 to 85.3
0 to 7. 19
21.4 to 119
30.3 to 132
23.8 to 105

Boeing
analysis
65
237
334
2.0
279
381
388,
Solution 2
fofl/U

EPA
actual
70
250
350
8.0
300
400
400
EPA
acceptance
limits
47.5 to 85.8
102 to 368
267 to 415
Oto 17.6
161 to 452
185 to 608
206 to 61 2
               TABLE 16.  EFFLUENT FROM LO-CL PROCESS
Flame method
Flameless method

-------
                                    SECTION 17

                             CONSULTANT'S REPORT

                         Consultant: Dr. D. Bhattacharyya
             Department of Chemical Engineering, University of Kentucky

     Industries  engaged  in  metal  finishing  or  metal  production  operations  use large
quantities  of contact  process  water, and the spent process wastewater  (rinse water)
streams contain  heavy metals, such as  Cu, Cd,  Pb, Zn, Ni, Cr, Sn, Ag, and cyanides.
Although hydroxide (lime) precipitation of heavy metals,  followed by settling, is the
process that is used most often to treat industrial wastewaters,  the amphoteric nature of
some precipitates  [ M (OH)2  (ppt)  + OH~ ^ M  (OH)^ ] , settling  problems,  and the
presence of complexing agents  may reduce metal removal efficiency.   With  sulfide
precipitation, the high reactivity of sulfides (S=, HS~,  H2S) with heavy metal ions and
the  very low solubility  of heavy  metal sulfides  over  a broad  pH range are attractive
features when this  process is compared to the  corresponding hydroxide  precipitation
process.  The  optimum  sulfide dosage  and  pH  adjustments  depend, of course,  on the
wastewater characteristics.

     Although heavy metals can be precipitated with soluble sulfide salts (Na2S or NaHS)
or with  sparingly soluble metal sulfides (such as FeS), the use of  FeS often requires
higher  than  stoichiometric  dosages.    The Boeing   Company  conducted  extensive
experimental investigation of the  soluble sulfide process and lime precipitation process
with various industrial metal finishing (anodizing, metal cleaning, printed circuit etching,
and several types of electroplating) wastewaters.

     A side-by-side  comparison of continuous-flow sulfide precipitation and  hydroxide
precipitation processes  has  not been reported  previously in  the  literature.   Sulfide
precipitation experiments were conducted in the  pH 8.0 to 9.0 range. Lime precipitation
with settling followed  by  sulfide precipitation  and filtration (LSPF process) and  a
combined lime-sulfide-settling-filtration (LWS-CLF) process were  consistently better
than the hydroxide processes.  In several  cases (moderate Zn and Cu concentration in the
influent), lime  precipitation-settling  followed by filtration (to remove fine precipitates)
was  also highly  effective  in removing heavy  metals from  the  wastewaters.    The
precipitation results also indicated that  with  several wastes (higher concentrations), the
lime precipitation process produced sludge volumes 1.3  to 1.9 times higher than the LWS
(sulfide) process.

     Sulfide precipitation was considerably better than  the lime precipitation process for
waste number 12, which  contained a high concentration  of Zn (440 mg/L), in the presence
of ammonium ion, and for waste number 9, which contained 24  mg/L Cu and 99 mg/L Ni
at a high pH of 11.it (high pH  may indicate  presence of complexing agents).   Table 19
shows  the  Zn  removals  (waste No.  12) obtained with various precipitation processes.
With waste number 9,  both Cu and Ni removals are considerably better with the sulfide
processes, as shown in  Table 20.


                                        38

-------
                  TABLE 19. ZINC fiEMOVAL FROM WASTE NO. 12
pH

8.5
9.0
Zinc removal (%}
LO-CL
83.0
91.5
LO-CLF
84.1
93.4
LSPF
89.9
99.5
LWS-CL
99.4
99.8
LWS-CLF
99.0

                  TABLE 20.  METAL REMOVAL FROM WASTE NO. 9
                                               Metal removal (%)
IV1GLC1I
Copper
Nickel
yn
8.8
8.8
LO-CL
58.3
83.5
LO-CLF
66.7
87.8
LSPF
" 99.7
98.8
LWS-CL
89.2
92.9
LWS-CLF
98.3
95.8
    For all  the wastewaters studied, although LSPF and LWS-CLF gave similar effluent
quality, the sulfide  polishing (LSPF)  process would  be  preferred  on  the  basis  of
considerably lower sulfide dosage (thus lower sulfide chemical cost) requirements.  With
the LSPF process, two separate reaction stages would be required.  The total operating
costs  (NaHS as sulfide) with the LSPF process would be 5 to 9 percent higher than the
conventional lime precipitation process.

    Although  the sulfide  precipitation studies conducted at Boeing were at pH 8 to  9,
the sulfide precipitation of heavy metals is highly effective even  at  lower  pH values.
Among the heavy metals,  HgS has the lowest solubility, and ZnS and NiS have the highest
solubility. The precipitates' solubility sequence is HgS  < CuS < CdS < PbS < ZnS  <
NiS.  Hg, Cu,  Cd, and Pb can be precipitated with sulfide (Na2S or NaHS) even at pH 3>
without any H2S gas formation. Effective precipitation  of Zn and Ni occurs  at pH >  6.
Sulfide  precipitation  is quite effective, even in  the acidic pH; thus, selective metal
recovery and the  obtaining of effluent water of low calcium content (for possible water
recycling because no lime may be required) are possible.

    A full-scale sulfide precipitation process (Na2S as sulfide source) with a capacity  of
1.0 x  106  gallons per day is operating at Boliden Metall Corporation of Sweden to treat
smelter (Cu, Pb, Zn smelting) wastewaters.  One copper smelter in Japan  has a sulfide
precipitation process  to recover heavy metals  as sulfides.  A New Hampshire aluminum
company operates a chrome removal treatment system with FeCl3  and Na2S to remove
both  hexavalent  and  trivalent  Cr.  The  Permutit Company  and Holley  Carburetor
Division of Colt Industries demonstrated the use of the sulfide  process (Sulfex process
uses freshly prepared FeS  by reacting NaHS  with FeSO4) at  Paris, Tennessee, and
obtained effluent waters  containing Cr  and Zn at less than a  0.05-mg/L  level.   An
extensive  bench-scale study involving lime-sulfide  precipitation of  heavy metals and
arsenic from smelter (Cu) wastewaters is also in progress at the University of Kentucky.

-------
                                 REFERENCES

 1.  Schlauch, R.M., and A. Epstein,  Treatment of Metal Finishing  Wastes by Sulfide
    Precipitation.  EPA  report  number  EPA-600/2-77-049,  Feb.   1977,  IERL,  U.S.
    Environmental Protection Agency, Cincinnati, Ohio 45268, 86 pp.

 2.  Suliex Heavy Metals Waste Treatment  Process, Technical  Bulletin, Vol. 13, No.  6,
    Code 4413.2002, Oct. 1976, The Permutit Company, E. 49 Midland Avenue, Paramus,
    N.3. 07652, 4 pp.

 3.  Scott, M.C., Sulfex—A New  Process Technology for Removal of Heavy Metals from
    Waste Streams, Paper  presented at Purdue  Industrial Waste Conference,  May  10,
    1977, The Permutit Company, Inc., Paramus,  N.3. 07652, 18 pp.

 4.  Anderson, Cranbury, and Weiss, Patent No.  3,740,331, Method for  Precipitation of
    Heavy Metal Sulfides, 3une 19, 1973

 5.  Patterson and Minear, Wastewater Treatment Technology, Illinois Institute  of Tech-
    nology report number IIEQ 71-4, Illinois Institute of Technology, Chicago, 111., Aug.
    1971

 6.  Water Pollution Control for Metal Machining,  Fabricaton, and Costing Operations,
    prepared  for  the U.S.  Environmental Protection  Agency Technology  Transfer
    Program by Centec Consultants, Inc., 11800 Sunrise Valley Drive, Reston, Va. 22091,
    May 1977, 180 pp.

 7.  Considine, et  al.,  Process Instruments  and Controls Handbook, McGraw-Hill Book
    Company, New York, N.Y., 1974, pp. 6.85-6.87

 8.  Standard Methods for  the Examination of Water and  Wastewaters, 13th Edition,
    1971, p. 337,  American Public Health Association, 1015 18th St.  N.W., Washington,
    D.C.  20036

 9.  Nilsson, R., Removal of Metals by Chemical Treatment of Municipal Waste Water,
    Water Research, Pergamon Press, Elmsford, N.Y., 1971, Vol. 5, pp. 51-60

10.  Hartinger,  L.,  Metallkomplexe in der Abwassertechnik,  Galvanotechnik D.7698,
    Eugen G. Leuze Verlog, Postfach 8,  Saulgau, Wurttemberg, Germany, 1975, No.  5,
    pp. 366-373

11.  Gushee, C.H., Financial Compound Interest  and Annuity Tables, Boston Financial
    Publishing Company, p. 884
                                                                                 <
12.  Chemical Marketing Reporter, December 4,  1978, Schnell  Publishing Company, 100
    Church St., New York, NY 10007, p. 68
                                       40

-------
13.  Rickmers, A.D.,  and H.N. Todd,  Statistics, An  Introduction,  McGraw-Hill  Book
    Company, New York, N.Y., 1967, Ch. 18, "Non-Parametric Statistics," pp. 386-407

14.  Development Document  for  Proposed Effluent  Limitation Guidelines,  Effluent
    Guidelines Division, U.S. Environmental Protection Agency, Washington, D.C. 20406,
    Aug. 1973, EPA-440/1-73-003, Fig. 6, p. 65

15.  Stumm,  Werner, "Chemical  Interaction  in Particle  Separation,"  Environmental
    Science and  Technology, Vol. 11, No. 12, Nov. 1977, pp. 1066-1070

16.  Bowker and Lieberman, Engineering Statistics, Prentice-Hall, 1960, Sec. 8.12 and
    Table 8.2

-------
                                  APPENDIX A

                     CASE HISTORY DATA OF 16 TEST RUNS

    The  test runs are arranged in this appendix in the order of  increasing electrical
conductivity of the raw feed.  Each case history includes data on the wastewater sample
raw feed analysis, processed effluent analysis, process consumables, and sludge volume.

    The  data were generated from  14 wastewater  samples that  represented nonferrous
metal smelting,  electroplating, anodizing,  cleaning, and  etching operations.   Samples
came from industrial plant sources across the United States.  Each wastewater sample
was used in a test run at a pH value selected as an optimum for precipitation of its heavy
metals.   Two samples were tested at  a second pH  value where doubt  existed as to the
true optimum pH value.

-------
                                             TEST RUN 1
                  Description of wastewater:  Rinse from copper printed circuit etching and copper
                                             deposition (electrolytic and electroless)

                  Source area: Seattle, Washington
Treatment process details*
Precipitation pH for
lime-only and lime-
with-sulfide processes

8.5


Chemical analysis
Measurement
Cd
Cr (total)
Cu
Ni
Zn
PH
Conductivity*
Color
Cr6+
Hg
Pb
Ag
Sn




Sludge volumet
LO: <2

LWS: < 2

Process consumables (mg/L)
H2S04 for Cr6+ reduction:
IMa2S03 for Cr^+ reduction:
CaO for LO process:
S for LWS process:
S for LSPF process:

120
31
86
18
3.5
(all values except conductivity and pH in jug/L)
Before-
raw feed
8
215
2.3 x 103
209
770
5.2
115
colorless
73
<1
192
<3
3.3 x 103
Value after
LO-CL LO-CLF
2 «1
203 3
1.8x103 200
217 86
430 53





185 17
1 1
308 139
treatment by process of*:
LSPF LWS-CL
«1 1
2 215
67 1.9 x103
77 209
14 424





15 192
1 1
348 432

LWS-CLF
«1
6
5
88
13





13
1
279
* Process code:  LO = lime only; LSPF = lime, sulfide polished and filtered; LWS = lime with sulfide;
                CL = clarified; CLF = clarified and filtered
t Volume per volume, percentage after 1 hr settling
t jumho/cmat 18.5°C

-------
                                             TEST RUN 2
                  Description of wastewater:  Rinse from electroplating
                  Source area:  Portland, Oregon
Treatment process details*
Precipitation pH for lime-
only and lime-with-sulfide
processes
Sludge volume
 Process consumables (mg/L)
           8.5
  LO:   <2

  LWS:   < 2
H2S04 for Cr6+ reduction:   264
Na2S03 for Cr6+ reduction:  132

CaO for LO process:         132
S for LWS process:            1
S for LSPF process:            1
Chemical analysis (all values except conductivity and pH in jug/L)
Measurement
Cd
Cr (total)
Cu
Ni
Zn
pH
Conductivity'*
Color
Cr6+
Fe
Hg
Before—
raw feed
LO-CL
268 179
949 459
87 59
19 18
112 100
8.0
217
colorless
396
408 56
<1
Value after treatment by process of*:
LO-CLF LSPF LWS-CL LWS-CLF
22 23 139 19
15 29 484 57
24 14 36 8
18 8 16 7
20 10 78 10




12 20 150 21

 *Process code:  LO = lime only; LSPF = lime, sulfide polished and filtered; LWS = lime with sulfide;
               CL = clarified; CLF = clarified and filtered
t Volume per volume, percentage after 1 hr settling
           at 17°C

-------
                                               TEST RUN 3
                    Description of wastewater:  Rinse from electroplating and metal finishing by carburetor
                                              manufacturer

                    Source area: Warren, Michigan
 Treatment process details"
 Precipitation pH for lime-
 only and lime-with-sulfide
 processes
Sludge volume t
Process consumables (mg/L)
8.75
Chemical analysis
Measurement
Cd
Cr (total)
Cu
Ni
Zn
PH
Conductivity
Color
Cr6+
Hg
Pb
Ag
Sn
H2SO4 for Cr6+ reduction:
L0: 24 Na2S03 for Cr6+ reduction:
CaO for LO process:
LWS: 19 S for LWS process:
Sfor LSPF process:
(all values except conductivity and pH in Mg/D
R , Value after treatment by process of*:
raw feed |_0-CL LO-CLF LSPF LWS-CL
4
200 x103 1,060 76 56 437
30 22 22 14 7
106 10 ~ 17 8 4
90x103 1,000 210 10 490
4.5
550
yellow
91 x 103
<1
<25
20
1.2 x103 <2 <2 <2 <2
370
610
290
43
25


LWS-CLF

58
5
4
15






<2
'Process code:  LO = jime only; LSPF = lime, sulfide polished and filtered; LWS = lime with sulfide;
               CL = clarified; CLF = clarified and filtered
t Volume per volume, percentage after 1 hr settling
tjumho/cm at  18.5°C

-------
                                               TEST RUN 4
                    Description of wastewater:  Rinse from anodizing and electroplating
                    Source area: Minneapolis, Minnesota
  Treatment process details*
Precipitation pH for lime-
only and lime-with-sulfide
processes
9.0
Chemical analysis
Measurement
Cd
Cr (total)
Cu
Ni
Zn
PH
Conductivity*
Color
Cr6+
Pb
Ag
Sn

(all values except
Rpfnrp • LJ
raw feed
400
12.6 x103
800
3.2 x103
11x103
7.05
700
pale yellow
10.4 x 103
17
29
350
Sludge volume ^
LO: <4
LWS: <4
conductivity and pH in /zg/L)
Value after
LO-CL LO-CLF
98 11
2,200 178
69 20
467 69
2,145 167



<5
12 <2
3 3
215 155
Process consumables (mg/L)
H2S04 for Cr6+ reduction:
Na2S03 for Cr6+ reduction:
CaO for LO process:
Sfor LWS process:
S for LSPF process:

treatment by process of*:
LSPF LWS-CL
16 55
237 957
18 40
102 350
331 1,200



<5 <5
<2 6
3 3
185 169

140
200
20
1
0.5


LWS-CLF
29
470
24
197
560




3
3
213
* Process code:   LO = lime only;  LSPF = lime, sulfide polished and filtered; LWS = lime with sulfide;
                 CL = clarified; CLF = clarified and filtered
t Volume per volume, percentage after 1 hr settling
* jumho/cm at 21°C

-------
                                                TEST RUN  5
                    Description of wastewater:  Rinse from anodizing and electroplating
                    Source area:  Lincoln, Nebraska
  Treatment process details*
  Precipitation pH for lime-
  only and lime-with-sulfide
  processes
Sludge volume t
Process consumables (mg/L)
10.5
Chemical analysis
Measurement
Cd
Cr (total)
Cu
Ni
Zn
pH
Conductivity*
Color
Hg
Pb
Ag
Sn
CN
LO: 6
LWS: 4
(all values except conductivity and pH
Before 	 -
raw feed LO-CL
9 3
18 18
24 12
789 125
33 6
7.1
1,320
colorless
<10
211 1
600 2
280 40
1 x 103
H2S04 for Cr6+ reduction : 0
Na2S03 for Cr6+ reduction: 0
CaO for LO process: 98
S for LWS process: 19
S for LSPF process: 14
in Mg/L)
Valu • after treatment by process of*:
LO-CLF LSPF LWS-CL
<3 <3 <3
12 14 9
864
100 100 69
335




1
232
36 131 103




LWS-CLF
<3
13
5
111
5





2
228

 *Process'code:  LO = lime only; LSPF = lime, sulfide polished and filtered; LWS = lime with sulfide;
               CL = clarified; CLF = clarified and filtered
t Volume per volume, percentage after 1 hr settling
t/imho/cm at  22°C

-------
                                               TEST RUN 6
                    Description of wastewater:  Rinse from electroplating
                    Source area:  Cleveland, Ohio
  Treatment process details51
  Precipitation pH for lime-
  only and lime-with-sulfide
  processes
Sludge volume
  Process consumables (mg/L)
          8.5
    LO:   5

    LWS.   6
H2S04 for Cr6+ reducti on:   339
Na2S03 for Cr6+reduction:   25

CaO for LO process:         145
S for LWS process:           91
S for LSPF process:           67
Chemical analysis (all values except conductivity and pH in jug/L)
Measurement
Cd
Cr (total)
Cu
Ni .
Zn
PH
Conductivity*
Color
Fe
Pb
Ag
Before-
raw feed
<40 <1
1.7x103 109
21 x 103 1,300
119x103 12x103
13x103 625
7.1
1,500
pale green
2
13 7
6
Value after treatment by process of*:
LO-CLF
<1
39
367
9.4 x103
10



<2
5

LSPF LWS-CL
<1 <1
20 187
1 1 2,250
5.3 x103 11x103
5 192



<2 5
3 4

LWS-CLF
<1
17
169
3.5 x103
8



<2
3

 *Process code:  LO = lime only; LSPF = lime, sulfide polished and filtered; LWS = lime with sulfide;
                CL = clarified; CLF = clarified and filtered
t Volume per volume, percentage after 1 hr settling
t/zmho/cm at 21 °C

-------
                                               TEST RUN 7
                    Description of wastewater:  Rinse from anodizing and electroplating
                    Source area:  Kent, Washington
 Treatment process details*
 Precipitation pH for lime-
 only and lime-with-sulfide
 processes
Sludge volume t
                               Process consumables (mg/L)
9.25
Chemical analysis
Measurement
Cd
Cr (total)
Cu
Ni
Zn
pH
Conductivity *
Color
Hg
Pb
Ag
Sn

(all values except
Before-
raw feed
76
8.5 x103
1.3 x103
944
131
10.6
4,400
yellow
<10
45
44
460
H2S04 for Cr6+ reduction : 972
L0"- 14 Na2S03 for Cr6+ reduction: 211
LWS. 14 CaO for LO process: 389
S for LWS process: 1
S for LSPF process: 1
conductivity and pH in /ug/L)
Value after treatment by process of*:
LO-CL LO-CLF LSPF LWS-CL LWS-CLF
27 16 22 25 20
318 65 139 295 239
244 236 143 212 166
80 49 49 349 250
46 42 40 35 24




15 14 43 23 13
19 11 9 9 8
<10 <10 <10 <10 <10
 *Process code:  LO = lime only; LSPF = lime, sulfide polished and filtered; LWS = lime with sulfide;
               CL = clarified; CLF = clarified and filtered
f Volume per volume, percentage after 1 hr settling
tjumho/cmat 22°C

-------
                                              TEST RUN 8
                    Description of wastewater: From a nonferrous metal  smelter settling pond fed by water
                                             from a flue gas zinc extractor and by scrubber water from
                                             copper-phosphorus process
                    Source arear Perth Amboy, New Jersey
 Treatment process details'*
Precipitation pH for lime-
only and lime-with-sulfide Sludge volume
processes
8.5


Chemical analysis
Measurement
Cd
Cr (total)
Cu
Ni
Zn
pH
Conductivity
Color
As
Cr6+
Hg
Pb
Ag
Sn
Se

LO: 41
LWS: 29

(all values except conductivity and pH
Before-
raw teed
LO-CL
15x103 80
1 00 1 00
7x103 39
123 40
114x103 511
2.2
4,700
colorless
1.4 x103 54
<4
<1
5x103 38
1
5x 103
<1x103 44
Process consumables (mg/L)

H2SO4 for Cr6+ reduction:
Na2SO3 for Cr6+ reduction:
CaO for LO process:
S for LWS process:
Sfor LSPF process:
in M9/L)
Value after treatment by process of*:
LO-CLF LSPF LWS-CL
7 4 50
23 5 3
0.14 14 38
26 106 108
30 36 309



38 40 44


3 3 27


40 36 44

0
0
1,004
60
4


LWS-CLF
2
2
6
115
15



49


2


44
 *Process code:  LO = lime only; LSPF = lime, sulfide polished and filtered; LWS = lime with sulfide;
               CL = clarified; CLF = clarified and filtered
t Volume per volume, percentage after 1 hr settling
t Atmho/cmat19°C
                                                   50

-------
                                               TEST RUN 9
                   Description of wastewater:  Rinse from electroplating
                   Source area: Los Angeles, California
 Treatment process details'
 Precipitation pH for lime-
 only and lime-with-sulfide
 processes
Sludge volume'''
Process consumables (mg/L)
H2S04 for Cr6+ reduction:
LO : < 2 Na2SO3 for Cr6+ reduction :
8-75 CaO for LO process:
LWS: <2 c, .....
S for LWS process:
Sfor LSPF process:
2,420
97
515
190
65
Chemical analysis (all values except conductivity and pH in /ug/L)
Measurement
Cd
Cr (total)
Cu
Ni
Zn
pH
Conductivity*
Color
Hg
Ag
CN
_ , Value after treatment by process of*:
Before-
raw feed LO-CL LO-CLF LSPF LWS-CL LWS-CLF
<100 97 71 3 12 8
310 40 25 33 90 48
24x103 10x103 8x103 73 2.6 x103 400
99x103 16x103 12x103 1.2 x103 7.0 x103 4.2 x103
253 x 103 400 295 8 567 9
11.4
5,500
yellow
<0.1
4
31 x 103
 *Process code:  LO = lime only; LSPF = lime, sulfide polished and filtered; LWS = lime with sulfide;
                CL = clarified; CLF = clarified and filtered
t Volume per volume, percentage after 1 hr settling
tjum ho/cm at 19°C
                                                    51

-------
                                              TEST RUN 10
                    Description of wastewater:   Rinse from electroplating
                    Source area:  Chicago, Illinois
 Treatment process details*
Precipitation pH for
lime-only and lime- Sludge volume*
with-sulfide processes
10.0

Chemical analysis
Measurement
Cd
Cr (total)
Cu
Ni
Zn
PH
Conductivity
Color
Fe
Hg
Ag
Sn
LO: 43
LWS: 37

(all values except conductivity and pH in p.g/L)
Before- Value after
raw feed
LO-CL LO-CLF
58x103 1,130 923
5x103 138 103
2x103 909 943
3x103 2.2 x 103 2.3 x103
290 x103 1.2 x103 510
2.4
5,600
colorless
740 x103 2x103 334
<0.3 <0.3 <0.3
14 14 10
5x103 129 81
Process consumables (mg/L)
H2SO4 for Cr6+ reduction:
Na2S03 for Cr6+ reduction:
CaO for LO process:
S for LWS process:
Sfor LSPF process:

treatment by process of*:
LSPF LWS-CL
<10 26
37 49
929 60
2.6 x103 1.8 x103
12 216



305 563
<0.3 <0.3
8 7
71 71
0
41
2,680
400
141


LWS-CLF
<10
50
160
1.9 x103
38



229
<0.3
7
71
*Process code:  LO = lime only; LSPF = lime, sulfide polished and filtered; LWS = lime with sulfide;
               CL = clarified; CLF = clarified and filtered
t Volume per volume, percentage after 1 hr settling
           at 19°C
                                                   52

-------
                                               TEST RUN  11


                    Description of wastewater:   Rinse from aluminum cleaning, anodizing, and electroplating


                    Source area:  Auburn, Washington
Treatment process details*
 Precipitation pH for lime-
 only and lime-with-sulfide
 processes
Sludge volume
Process consumables (mg/L)
8.5
Chemical analysis
Measurement
Cd
Cr (total)
Cu
Ni
Zn
PH
Conductivity
Color
Pb
LO: 18
LWS: 16
H2SO4 for Cr6+ reduction : 0
Na2SO3 for Cr6+ reduction : 226
CaO lor LO process: 1 ,530
S for LWS process: 8
S for LSPF process: 1
(all values except conductivity and pH in pig/L)
Before-
raw feed inn
45 15
163x103 3,660
4.7 x103 135
185 30
2.8 x103 44
1.7
10,600
yellow
119 119
Value after treatment by process of*:
LO-CLF LSPF LWS-CL LWS-CLF
8 20 11 7
250 159 1,660 68
0.33 3 82 18
38 18 33 31
10 11 26 2



88 120 104 59
 *Process code:  LO = lime only; LSPF = lime, sulfide polished and filtered; LWS = lime with sulfide;
                CL = clarified ;CLF = clarified and filtered
 t Volume per volume, percentage after 1 hr settling
 * Mm ho/cm at 22°C
                                                   53

-------
 Treatment process details
                                             TEST RUN 12*

                    Description of wastewater:   Rinse from electroplating

                    Source area:  Chicago, Illinois

                        t
Precipitation pH for
lime-only and lime- Sludge volume* Process consumables (mg/L)
with-sulfide processes
8.5
Chemical analysis
Measurement
Cd
Cr (total)
Cu
Ni
Zn
pH
Conductivity**
Color
Hg
Pb
Ag
Sn
NH4
LO: 20 H2S04 for Cr6+ reduction: 0
Na2S03 for Cr6+ reduction : 0
LWS: 10 CaO for LO process: 760
LSPF: 2 S f or LWS process: 260
S f or LSPF process: 108
(all values except conductivity and pH in /ug/L)
_, , Value after treatment by process of *:
Pf.fnre— 	
raw feed L0.CL LO-CLF LSPF LWS-CL LWS-CLF
34 20 20 1 1 1
3
20 8 0.8 3 1 1
64 42 42 42 34 50
440 x103 75x103 71x103 4.7 x 103 2.5 x103 4.6 x 103
6.4
12,100
colorless
<10
45 15 17 17 22 15
61 4 4555
200 <10 <10 <10 <10 <10
tt
 * Test runs 12 and 13 were made with the same raw feed wastewater: run 12 at pH = 8.5 and run 13 at pH = 9.0
 t Process code:  LO = lime only; LSPF = lime, sulfide polished and filtered;  LWS = lime with sulfide;
                CL = clarified;  CLF = clarified and filtered
 + Volume per volume, percentage after 1 hr settling
** Aimho/cm at 25°C
tt Qualitative tests indicated the  presence of significant amounts of ammonium


                                                   54

-------
                                             TEST RUN 13*

                    Description of wastewater:  Rinse from electroplating

                    Source area:  Chicago, Illinois
 Treatment process details|t
Precipitation pH for lime-
only and lime-with-sulfide sludge volume * Process consumables (mg/L)
processes
9.0

Chemical analysis (all
Measurement
Cd
Cr (total)
Cu
Ni
Zn
PH
Conductivity**
Color
Hg
Pb
Ag
Sn
IMH4
LO:
LWS:

values except conductivity and
Before—
raw feed LO_C|_
34 21
3
20 7
64 29
440 x 103 37x103
6.4
12,100
colorless
<10
45 13
61 4
200 <10
tt
H2S04 for Cr6+Veduction:
Na^SOg for Cr reduction :
*CaO for LO process:
~~ S for LWS process:
Sfor LSPF process:
pH in jug/L)
Value after treatment by process of .
LO-CLF LSPF LWS-CL
21 1 1

842
29 31 72
29x103 2x103 730


-

14 13 9
4 4 1
<10 <10 <10

0
0
911
-


LWS-CLF
1

1
34
600




11
3
<10

 * Test runs 12 and 13 were made with the same raw feed wastewater:  run 12 at pH = 8.5 and run 13 at pH - 9.0
 t Process code:  LO = lime only; LSPF = lime, sulfide polished and filtered; LWS = lime with sulfide;
                CL = clarified;  CLF = clarified and filtered
 * Volume per volume, percentage after 1 hr settling
**jumho/cm at 25°C
tt Qualitative tests indicated the presence of significant amounts of ammonium


                                                  55

-------
                                             TEST RUN  14"
                   Description of wastewater:   Rinse from electroplating
                   Source area:   Atlanta, Georgia
 Treatment process details
     Precipitation pH for
     lime-only and lime-
     with-sulfide processes
Sludge volume'
 Process consumables (mg/L)
             8.5
     LO:     59

     LWS:   53
H2SO4 for Cr6+reduction:      0
Na2SO3 for Cr6+ reduction:   156
CaO for LO process:        5,009
S for LWS process:            995
S for LSPF process:            16
Chemical analysis
Measurement
Cd
Cr (total)
Cu
Ni
Zn
pH
Conductivity
Color
Fe
Hg
Pb
Ag
(all values except
Before-
raw feed
1.4 x103
10.3 x103
900
35x103
930 x 103
1.2
75,000
brown
415x 103
1
500
64
conductivity and

LO-CL
432
34
28
1,000
9.6 x 103

19 x 103

16
<2
pH in jug/L)
Value after
LO-CLF
360
5
28
750
1.4 x 103

1.5 x 103

17
<2

treatment by
LSPF
70
9
7
96
340

1.5 x 103

16
<2

process of ^:
LWS-CL LWS-CLF




No tests run. The extremely
high sulfide demand would
make a full-scale process
uneconomical.



'

* Test runs 14 and 15 were made with the same raw feed wastewater:  run 14 at pH = 8.5 and run 15 at pH = 10.0
t Process code:  LO = lime only;  LSPF = lime, sulfide polished and filtered;  LWS = lime with sulfide;
               CL = clarified; CLF = clarified and filtered
£ Volume per volume, percentage after 1 hr settling
*;umho/cm at 23°C
                                                 56

-------
                                               TEST RUN 15 *
                     Description of wastewater:   Rinse from electroplating
                    Source area:   Atlanta, Georgia
  Treatment process details
                         t
      Precipitation pH for
      lime-only and lime-
      with-sulfide processes
Sludge volume
Process consumables (mg/L)
H2SO4 for Cr6+ reduction:
LO: 62 Na2S03 for Cr6+ reduction:
10.0 LWg. 4g CaO for LO process:
S for LWS process:
Sfor LSPF process:
0
156
5,428
1,400
8
  Chemical analysis (all values except conductivity and pH in
Measurement
Cd
Cr (total)
Cu
Ni
Zn
PH
Conductivity**
Color
Fe
Hg
Pb
Ag
Before-
raw feed
1.4 x103
10.3 x103
900
35x103
930 x 103
1.2
75,000
brown
415 x 103
1
500
64

LO-CL
73
19
10
35
3.3 x103

2.0 x 103

17
<2
Value after treatment by
LO-CLF LSPF
66
22
8
21
1.0 x 103

1.6 x 103

15
<2
process of ' :
LWS-CL LWS-CLF




No tests run. The extremely
high sulfide demand would
make a full-scale process
uneconomical.





 *Test runs 14 and 15 were made with the same raw feed wastewater: run 14 at pH = 8.5 and run 15 at pH - 10.0
 Process code:  LO = lime only; LSPF = lime, sulfide polished and filtered; LWS = lime with sulfide;
               CL = clarified; CLF = clarified and filtered
  Volume per volume, percentage after 1 hr settling
*>mho/cm at 23°C

-------
                                               TEST RUN  16
                     Description of wastewater:  Rinse from electroplating
                     Source area:  Glendale, California
  Treatment process details*
Precipitation pH for lime-
only and lime-with-sulfide Sludge volume t
processes
1st stage*: 6.2
2d stage*: 9.0
Chemical analysis
Measurement
Cd
Cr (total)
Cu
Ni
Zn
PH
Conductivity**
Color
Cr6+
Hg
Ag
. . 78
(LO: 23
LWS: 13
(all values except conductivity and pH in /ug/L)
Before- Value after
raw feed LQ Cj_ LQC]_f
58 7 12
6.3 xlO3 4 2
1.1x103 860 848
160 30 34
650 x103 2.8 x103 2.3 x103
1.2
149,000
colorless
<5 <1 <1
<1
16
Process consumables (mg/L)
H0SOA for Cr6+ reduction:
6+
Na2S03forCr reduction:
CaO for LO process:
Sfor LWS process:
Sfor LSPF process:

treatment by process of*:
LSPF LWS-CL
<5 <5
3 5
132 13
34 33
242 104



<1 <1



0
31
14,380
381


LWS-CLF
<5
7
13
23
19



<1


 *Process code:  LO = lime only; LSPF = lime, sulfide polished and filtered; LWS = lime with sulfide;
                CL = clarified; CLF = clarified and filtered
 tVolume per volume, percentage after 1 hr settling
 t Because of the exceptionally large volume of sludge generated by this wastewater,
  precipitation was carried out in two stages
* Vn ho/cm at 20°C
                                                     58

-------
                                  APPENDIX B

                             ANALYTICAL METHODS

    Chemical analyses  were made for  the  following elements, compounds, and values
using the following methods:

    a.   Arsenic and selenium—Furnace atomic absorption spectroscopy, Some Applica-
         tions of  the IL 751  Atomic Absorption  Spectrophotometer, Engineering and
         Applications Staff, Instrumentation Laboratory Inc., Wilmington, Maine 01887

    b.   Cadmium, total chromium, copper, nickel, zinc, lead, silver, tin, iron:

         1.   For levels >50 jug/L:  Flame atomic absorption method on samples concen-
             trated by boiling, Methods for Chemical Analysis of Water and Waste, U.S.
             Environmental Protection Agency

         2.   For levels <50 jug/L: Flameless  atomic absorption method, Instrumenta-
             tion  Laboratory  Inc.,  Analytical  Instrument Division,  3onspin  Road,
             Wilmington, Maine 01887

    c.   Conductivity—Conductivity meter,  YSI Model 33 S-C-T, Yellow Springs Instru-
         ment Co.  Inc., Yellow Springs, Ohio  45387

    d.   Cyanide—Measurement by specific ion electrode,  Orion  Research Analytical
         Methods Guide, 7th Edition, May 1975

    e.   Hexavalent chromium—Diphenylcarbazide  colorimetric  procedure,  Standard
         Methods,  13th Edition, p. 426

    f.   Mercury—Manual  cold vapor  technique, Methods  for  Chemical  Analysis of
         Water and Waste, U.S. Environmental Protection Agency

    g.   Sludge  volume determination—Visual measurement  of   treated  sample in
         graduated cylinder after 1 hour settling. Sludge volumes are expressed in terms
         of the volume occupied  by  the sludge  as  a percentage  of  the  total volume
         treated.
                                        59

-------
                                  APPENDIX C

                      COMPARISON PLOTS OF FIVE METAL
                     CONCENTRATIONS FOR ALL SAMPLES

    The  comparison plots  show results from five  processes  using  cadmium,  copper,
chromium, nickel, and zinc effluent metal concentrations for all wastewater samples.

    Each point plotted in the diagrams has two  coordinates:   the  concentration  of a
metal in  the process A effluent (x-axis) and  the concentration of the same metal in the
process B effluent (y-axis).  A point below  the 45-deg line results when there is a higher
concentration  of the metal in process  A effluent; if all the points are below  the  line,
process A is clearly less effective in removing that metal than process B.  For example,
the copper diagram in Figure C-l  shows that  the  LO-CL process is less effective in
removing copper than the LSPF process  for all I** wastewaters except one.  The cadmium
diagram in Figure C-l shows no obvious advantage for either the LO-CL or LSPF process
for removing cadmium.
                                       60

-------
lee ,
                                                  1888
   CONCENTRATION OF CADMIUM
   FOR LO-CL PROCESS
CONCENTRATION OF COPPER
FOR LO-CL PROCESS (ng/L)
                     5
                     O
                          iee
                     Oco

                     OQ
                     1-0

                     DC0-
                     t-u.
                     Zfc
                     UjtO
                     o-1
                     zee
                     oo
                     Ou-
                             CHROMIUM
                                     10      lae      1880

                                 CONCENTRATION OF CHROMIUM
                                 FOR LO-CL PROCESS (ng/D
       CONCENTRATION OF NICKEL
       FOR LO-CL PROCESS (/jg/L)
   CONCENTRATION OF ZINC
   FOR LO-CL PROCESS
           C-1.  Comparison of LO-CL process and LSPFprocess using Cd, Cu  Cr, Ni,
                and Zn effluent metal concentrations for all wastewater samples.
                                         61

-------
 I 0000
                                                              10000
                 100    1000
CONCENTRATION OF CADMIUM
FOR LO-CLF PROCESS (fig/L)
i     10     100    1000    10000
 CONCENTRATION OF COPPER
 FOR LO-CLF PROCESS (Mg/L)
                                   10000 .
                                 —; 1000
                                ,[2  100
                                        CHROMIUM
                                       1      10     100    1000
                                  CONCENTRATION OF CHROMIUM
                                  FOR LO-CLF PROCESS 0*g/L)
                                                            100000
     1     10   100   1000  10000
   CONCENTRATION OF NICKEL
   FOR LO-CLF PROCESS (jiig/L)
1     10   100   1900  10000  100000
  CONCENTRATION OF ZINC
  FOR LO-CLF PROCESS (Mg/L)
      Figure C-2.  Comparison of LO-CLF process and LO-CL process using Cd, Cu, Cr,
                  Ni, and Zn effluent metal concentrations for all wastewater samples.
                                           62

-------
     tee
2



Is
O o»
u.3
O w

zffi
Oo
H O

<£
EC Q-
I- u.
Z 0-
ui«g
O -1
z cc
OO
O il-
         CADMIUM
        i            ie            lee

        CONCENTRATION OF CADMIUM

        FOR LWS-CL PROCESS (jug/D
   ie       lee      leee


CONCENTRATION OF COPPER

FOR LWS-CL PROCESS (/jg/L)
                                lee
                           O  i

                           u.3
                           HO


                           
-------
  g
I- Q.
§0
o -1
Z DC
O O
OU.    i
         CADMIUM  -
        CONCENTRATION OF CADMIUM
        FOR LWS-CL PROCESS
   i      ie    lee    teee
    CONCENTRATION OF COPPER
    FOR LWS-CL PROCESS i
                         03
                         13
                         "-S8
                         Ouj
                         O -1
                         z tn
                         O O
                         O U-    !
                                  CHROMIUM
                                 i        te       lee      teee
                                     CONCENTRATION OF CHROMIUM
                                     FOR LWS-CL PROCESS (jig/L)
O D>
  ~
O in
z o
lg
I- Q-
o -
Z (T
O O
O u.
         NICKEL
        i      ie    168    leee
            CONCENTRATION OF NICKEL
            FOR LWS-CL PROCESS
N ~
O LU
Z O
lg
H Q.
te
}- O
U
Z DC
O O
O u-
         ZINC
      CONCENTRATION OF ZINC
      FOR LWS-CL PROCESS (/ug/D
       Figure C-4.  Comparison of L WS-CL process and LO-CLFprocess using Cd, Cu, Cr,
                   Ni, and Zn effluent metal concentrations for all waste water samples.

-------
08
I- 0
go
o -1
z cc
o o
O u.
     100
       1
         CADMIUM-
        i        10       tee
 CONCENTRATION OF CADMIUM
 FOR LWS-CLF PROCESS (jig/L)
    i      ta     leo     ieea
CONCENTRATION OF COPPER
FOR LWS-CLF PROCESS
                                      i        10       ie>8
                                      CONCENTRATION OF CHROMIUM
                                      FOR LWS-CLF PROCESS Ijig/L)
              10     iee    1000    10000
          CONCENTRATION OF NICKEL
          FOR LWS-CLF PROCESS (M9/D
  1     10    100   1000  10000
CONCENTRATION OF ZINC
FOR LWS-CLF PROCESS (M9/L)
        Figure C-5.  Comparison of LO-CLF process and LWS-CLF process using Cd, Cu, Cr,
                    Ni, and Zn effluent metal concentrations for all wastewater samples.
                                               65

-------
     190 ,
U. uj
O O   19
        CADMIUM
o -
z cc
00
O u.
  ie        100       leee

CONCENTRATION OF CADMIUM
FOR LO-CL PROCESS 
-------
    1000
o —
ii f>
": t/>
O LLJ

Z O
O -
z cc
o o
(J LL
      10
         CADMIUM
        1        19        100

 CONCENTRATION OF CADMIUM

 FOR LSPF PROCESS (M9/L)
    1      10     166    1000

CONCENTRATION OF COPPER

FOR LSPF PROCESS
                                   1000 .
                              O _i


                              X ™
                              O ~  100


                              O uj



                              lg
                              h- 0.

                              < IL   10
                              o -1
                              Z DC
                              O O
                              O u.   1
                                       CHROMIUM
                                      1        10        180       1000

                                      CONCENTRATION OF CHROMIUM

                                      FOR LSPF PROCESS
   100002
                                                                    100000
                                                                 N ~


                                                                 S«
                                                                 O tu
                                                                     1000 (
                                                                 o -
                                                                 z cc
                                                                 o o
                                                                 O u.
       1     10     100    1000   10600


         CONCENTRATION OF NICKEL

         FOR LSPF PROCESS (fig/L)
                                                                          ZINC
  1    10   100   1000  10000

  CONCENTRATION OF ZINC

  FOR LSPF PROCESS (»ig/L)
       Figure C-7.  Comparison of LSPF process and LO-CLF process using Cd, Cu, Cr, Ni,

                   and Zn effluent metal concentrations for all wastewater samples.
                                              67

-------
                                                           iooo
  CONCENTRATION OF CADMIUM

  FOR LWS-CLF PROCESS (/ig/L)
    i         10       100

      CONCENTRATION OF COPPER

      FOR LWS-CLF PROCESS (/ufl/L)
                            1000
                               i        10       100       1000

                               CONCENTRATION OF CHROMIUM

                               FOR LWS-CLF PROCESS
                                                         10000
                                                      o
                                                      ^
                                                      N "
                                                      u.
                                                      O m
                                                      7 03
                                                      ^ "J
                                                      o o
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-------
5

53

9 »
< a.
U. C/J
O ui

U
z cc
00
O u.
         CADMIUM
CONCENTRATION OF CADMIUM

FOR LWS-CLF PROCESS
                                                                      CONCENTRATION OF COPPER

                                                                      FOR LWS-CLF PROCESS (Mg/L)
                                         i      10     100    iiioc1

                                  CONCENTRATION OF CHROMIUM

                                  FOR LWS-CLF PROCESS (»ig/U
                                                               10000
                                                           5 3
                                                           N —
                                                           I- Q.
                                                           < _1
                                                           F9
                                                           Z IT
                                                           O O
                                                           O u.
    CONCENTRATION OF NICKEL

    FOR LWS-CLF PROCESS
                                                                     ZINC
                                                                        10     109    1'XX'    10000

                                                                    CONCENTRATION OF ZINC

                                                                    FOR LWS-CLF PROCESS
             C-S.  Comparison of L WS-CLF process and L WS-CL process using Cd, Cu, Cr,
                   Ni, and Zn effluent metal concentrations for all wastewater samples.
                                             69

-------
S3
51
Si
z
     '«•
  o  ,M
o -1
z cc
o o
O U.
                   iee
  CONCENTRATION OF CADMIUM
  FOR LWS-CL PROCESS (/ug/L)
                                                                              iee    ieee   leeee
                                                                    CONCENTRATION OF COPPER
                                                                    FOR LWS-CL PROCESS (/jg/L)
                                  ime
                              o_
                              EC -I
                              5s
                              28
                              DC-J
                              Z DC
                              00
                              O u.
                                   iee
                                       CHROMIUM
                                                 iee
                                     CONCENTRATION OF CHROMIUM
                                     FOR LWS-CL PROCESS (ng/L)
w
oc_i  IM
o-1
Z DC
8S
          NICKEL i
        i    IB    iee  leee
         CONCENTRATION OF NICKEL
         FOR LWS-CL PROCESS
                                                                o -1
                                                                Z DC
                                                                o o
                                                                o u.
                                                                          ZINC
                                                                        i    le    iee  leee
                                                                      CONCENTRATION OF ZINC
                                                                      FOR LWS-CL PROCESS (jug/L)
            C-10.   Comparison of LWS-CL process and LO-CL process using Cd, Cu, Cr,
                   Ni, and Zn effluent metal concentrations for all wastewater samples.
                                             70

-------
                                    APPENDIX D

                        SIGN TEST STATISTICAL ANALYSIS

    Sign test statistical analyses were performed to establish a hierarchy (charted in
Figure D-l) to rank the five wastewater treatment processes.  The hierarchy was based
on cadmium, copper, chromium, nickel, and zinc effluent concentration data from the 16
test runs.

    The hierarchy was established  by  successively selecting and comparing two proc-
esses  to determine if the  pair gave  significantly different results and then ranking  the
processes accordingly.   For example, the LSPF  process was compared to the  LWS-CL
process. For each of the  16 test runs, a set of  five matched pairs  was established by
pairing the  Cd  effluent  concentration  of the  LSPF  process  with  the Cd  effluent
concentration  of  the LWS-CL  process;  the Cu  effluent concentration  of  the LSPF
process with the Cu effluent concentration of the LWS-CL process; and similarly, for  Cr,
Ni, and Zn.  Thus, a set of about 80 matched pairs was established for  the sign test.
They  were  used  to determine  which  two processes  produce  significantly  different
effluent concentration  levels.  Successive pairs  of  processes were  compared until  the
hierarchy chart (Figure D-l) was completely established.

    The results of the  sign test analyses on sets of  matched pairs are shown in Figures
D-2 through D-l 1.
          LARGEST REDUCTION
          IN HEAVY METALS
                            UJ
                             e> <
                             Z tL
                             UJ
  111
u- 2

— O
                                      LSPF * LWS-CLF
                                      LO-CLF * LWS-CL
                            Based on Cd, Cu, Cr, Ni,
                            and Zn effluent concen-
                            tration data and analyzed
                            at 75-percent confidence
                            level
                                        LO-CL
          SMALLEST REDUCTION
          IN HEAVY METALS
           Figure D-1.  Hierarchy of wastewater treatment processes established from
                      sign test statistical analysis.
                                          71

-------
PAIRED DIFFERENCES
(LO-CL FROM LO-CLF)*
1 O +
.
; - i>g y| 1
i i
"IHUUU
r
i _j
                                                           • Number of positive differences:
                                                           • Number of negative differences:
                                                           • Computed Z-statistic:
                                                           • Tabled Z-value:
                                            7
                                           59
                                            6.278
                                            1.150
               20        40        60
                    MATCHED-PAIR NUMBER
80
100
             Figure D-2.  Agreement between LO-CLF and LO-CL not significant
                         at 75-percent confidence level.
PAIRED DIFFERENCES
(LO-CL FROM LSPF)*
I O +
-
- - -y — - u|| - -- -
1 1 1
\
1 1
                                                          • Number of positive differences:
                                                          • Number of negative differences:
                                                          • Computed Z-statistic:
                                                          • Tabled Z-value:
                                            6
                                           63
                                            6.742
                                            1.150
               20        40        60
                    MATCHED-PAIR NUMBER
80
100
             Figure D-3.  Agreement between LSPF and LO-CL not significant
                          at 75-percent confidence level.
coo
si*
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mO n
££ °
OIL
Q_l
Sv
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i i
                                                          • Number of positive differences:
                                                          • Number of negative differences:
                                                          • Computed Z-statistic:
                                                          • Tabled Z-value:
                                           10
                                           47
                                            4.768
                                            1.150
               20         40         60
                    MATCHED-PAIR NUMBER
80
100
          Figure D-4.  Agreement between L WS-CL and L WS-CL F not significant
                       at 75-percent confidence level.
' Differences between effluent concentrations (Cd, Cu, Cr, Ni, and Zn) of paired processes
                                             72

-------
Si
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OU-
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                                                             Number of positive differences:
                                                             Number of negative differences:
                                                             Computed Z-statistic:
                                                             Tabled Z-value:
                20         40         60
                     MATCHED-PAIR NUMBER
                                             80
                                                      100
              Figure D-5.  Agreement between LO-CLF and LWS-CL significant
                           at 75-percent confidence level.
l_l_ *;£ A
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                                                           • Number of positive differences:
                                                           • Number of negative differences:
                                                           • Computed Z-statistic:
                                                           • Tabled Z-value:
                20         40        60
                     MATCHED-PAIR NUMBER
                                              80
                                                       100
              Figure D-6. Agreement between LSPF and LWS-CL not significant
                          at 75-percent confidence level.
                                                                                        29
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f£CO

II
                20         40         60
                     MATCHED-PAIR NUMBER
                                              80
                                                           • Number of positive differences:    52
                                                           • Number of negative differences:    13
                                                           • Computed Z-statistic:            4.713
                                                           • Tabled Z-value:                 1.150
                                                       100
             Figure D-7. Agreement between LO-CL and LWS-CL not significant
                         at 75-percent confidence level.
  Differences between effluent concentrations (Cd, Cu, Cr, Ni, and Zn) of paired processes
                                              73

-------
C/JU.
LU _|
00
ito

             • Number of positive differences:
             • Number of negative differences:
             • Computed Z-statistic:
             • Tabled Z-value:
                                   7
                                  58
                                   6.202
                                   1.150
                20        40        60
                     MATCHED-PAIR NUMBER
80
100
            Figure D-8. Agreement between LWS-CLF and LO-CL not significant
                        at 75-percent confidence level.
Ou-
"DC
Qu-
                                             I
             • Number of positive differences:
             • Number of negative differences:
             • Computed Z-statistic:
             • Tabled Z-value:
                                 45
                                 18
                                  3.276
                                  1.150
                20        40         60
                     MATCHED-PAIR NUMBER
80
         100
             Figure D-9. Agreement between LO-CLF and LSPF not significant
                         at 75-percent confidence level.
*
t/5 	 )
LU O
IFFERENC
FROM LO-
o +
Qu.
Q-i -
QjO
DCW
<§
Q 	


~
. n nil


L







i i i i i
0 20 40 60 80 1C
                                                          •  Number of positive differences:
                                                          •  Number of negative differences:
                                                          •  Computed Z-statistic:
                                                          •  Tabled Z-value:
                                          45
                                          19
                                            3.125
                                            1.150
                     MATCHED-PAIR NUMBER
          Figure D-10.  Agreement between LO-CLF and LWS-CLF not significant
                        at 75-percent confidence level.
* Differences between effluent concentrations (Cd, Cu, Cr, Ni, and Zn) of paired processes

-------
col-
tu u.
UJ -1
CCS

tl  0
Qu.
DC W
si
                20         40        60
                      MATCHED-PAIR NUMBER
                                               80
                                                             • Number of positive differences:    30
                                                             • Number of negative differences:    31
                                                             • Computed Z-statistic:             0.000
                                                             • Tabled Z-value:                 1.150
                                                        100
              Figure D-11.  Agreement between LSPF and L WS-CLF significant
                             at 75-percent confidence level.
* Differences between effluent concentrations (Cd, Cu, Cr, Ni, and Zn) of paired processes

-------
                                  APPENDIX E

       WILCOXON MATCHED-PAIR, SIGNED-RANK STATISTICAL ANALYSIS

    The  Wilcoxon matched-pair, signed-rank statistical method (13)  was used to estab-
lish the hierarchy chart (Figure E-l) to rank the five wastewater  treatment processes.
The  hierarchy  was  based on  cadmium, copper,  chromium,  nickel, and  zinc effluent
concentration data from the  16 test runs.

    The  hierarchy was established  by  determining if  a  pair of processes gave signif-
icantly different results.  The  processes were ranked accordingly.  For  example, the
LSPF process was compared  to the LWS-CL  process. For each of the 16 test runs, a set
of five matched pairs  was established  by pairing the Cd effluent  concentration of the
LSPF process  with  the Cd effluent concentration of the  LWS-CL  process; the Cu
effluent  concentration of the LSPF process with the Cu effluent  concentration of the
LWS-CL  process; and similarly, for Cr, Ni, and Zn.  Thus, a set of about 80 matched
pairs was established for the Wilcoxon method.  They were used to determine which two
processes produced  significantly different  effluent concentration levels,  based on the
T-value reported in Table E-l.

    The  signed ranks indicated that the LSPF process produced lower effluent concen-
tration levels than those of  the LWS-CL process.  Thus, the LSPF process  was ranked
above the LWS-CL process on the hierarchy  chart. If the two processes did not produce
significantly different results,  the  processes would have  had the  same rank  on the
hierarchy chart, as  in the comparison of the LSPF process  to  the  LWS-CLF process.
Successive pairs of processes were compared until the hierarchy  chart  (Figure E-l) was
completely established.
                                        76

-------
         LARGEST REDUCTION IN
         HEAVY METALS
                                LU t/J
                                D 2
                                -I O
                                to w
                                < u
                                HI Z
                                DC O
                                O U
         SMALLEST REDUCTION IN
         HEAVY METALS
LSPF = LWS-CL
                                          LO-CLF = LWS-CL
                                              LO-CL
                    Based on Cd, Cu, Cr, Ni,
                    and Zn effluent concen-
                    tration data and analyzed
                    at 95-percent confidence
                    level
         Figure E-1.  Hierarchy of wastewater treatment processes established from
                      Wilcoxon matched-pair, signed-rank statistical analysis (ref.  13).
         TABLE E- 7.  T VALUES OF WILCOXON MA TCHED-PAIR, SIGNED-RANK
                      STATISTICAL ANALYSIS
T-value calculated from
Comparison experimental data (smaller
pair sum of like-signed ranks) •*
LO-CL and LO-CLF
LSPF and LWS-CL
LO-CL and LWS-CL
LSPF and LWS-CLF
LWS-CL and LWS-CLF
LO-CLF and LSPF
LO-CLF and LWS-CL
LO-CLF and LWS-CLF
108
411
401
868
195
385
848
495
Tn^g-value required for a
significant difference at
95% confidence level t
848
717
821
717
620
643
794
794
Significant difference
at 95% confidence level
Yes
Yes
Yes
No
Yes
Yes
No
Yes
* Includes data for only cadmium, copper, chromium, nickel, and zinc heavy metals,
t When the T-value calculated from the experimental data exceeds the Tg^-value, the
  two processes are not significantly different at the 95% confidence level,
                                             77

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                                 APPENDIX F

                    CAPITAL COST OF FULL-SCALE PLANTS

    The  full-scale plants outlined in this appendix  were used  to provide the  basis for
capital equipment  cost comparisons.  The plants do not include cyanide destruction
systems  or hexavalent chromium  reduction systems; such processes would be  a  cost
burden on all  five processes.  This appendix includes plant schematics, layout drawings,
and construction details.

LIST OF FIGURES

F-l      Small LO-CL and LO-CLF plant schematic
F-2      Small LSPF, LWS-CL, and LWS-CLF plant schematic
F-3      Medium-sized LO-CL and LO-CLF plant schematic
F-4      Medium-sized LSPF plant schematic
F-5      Medium-sized LWS-CL and LWS-CLF plant schematic
F-6      Large LO-CL and LO-CLF plant schematic
F-7      Large LSPF plant schematic
F-8      Large LWS-CL and LWS-CLF plant schematic
F-9      Small plant layout-all processes (LO-CL, LO-CLF, LSPF, LWS-CL,
         and LWS-CLF)
F-10     Medium-sized LO-CL and LO-CLF plant layout
F-ll     Medium-sized LSPF plant layout
F-12     Medium-sized LWS-CL and LWS-CLF plant layout
F-13     Large LO-CL and LO-CLF plant layout
F-l4     Large LSPF plant layout
F-15     Large LWS-CL and LWS-CLF plant layout
F-16     Cross section of medium-sized and large plants—all processes (LO-CL,  LO-CLF,
         LSPF, LWS-CL, and LWS-CLF)


ENGINEERING SPECIFICATIONS  FOR SMALL PLANTS
(Figures F-l, F-2, and F-9)

A.  The leveling storage tank will hold a minimum of one day's effluent and will be acid-
    resistant.  This provides for batch processing, which is the most economical method
    for this flow rate.

B.  The mixer-clarifier tank will  hold the same amount of effluent as tank A.  Tank B is
    to be acid-resistant lined and will also contain an acid-resistant coated mixer.  For
    convenient sludge removal, this  tank must have a tapered  bottom with a view-port
    for observation of the sludge  bed level.  Manually controlled pH levels are tested in
    the lab.   Sulfide and H2S  levels  are  controlled manually as determined by an
    automatic H2S gas detector.  Upon completion of sludge removal to the filter press,
    item  C, the effluent is discharged  in the  following manner:  to the  sewer (LO-CL

                                       78

-------
    process);  to  the  filter (LO-CLF process); to the aerator (LWS-CL process); and to
    the filter and aerator (LSPF and LWS-CLF processes).

C.  The filter press  dewaters  the  sludge to 60-percent  moisture content.  Means for
    sludge removal are to be provided.

D.  The aerator is used to  oxygenate the effluent before  discharge; the  rate  depends
    upon system size.

E.  The filter is a manifold type for small particulate removal.

F-  An automatic audible alarm must  be installed in the process area to signal when
    tank levels are too high and to detect H2S gas.

G.  Flow control should be kept to specifications for efficient operation.

H.  An instrument control panel must be easily  accessible to the operator  and centrally
    located to the treatment area.  Instruments installed  on the panel must include the
    following:
    H.I.  On-off control of all pumps.
    H-2.  Indicators  of  water levels  in  each tank, including a  yellow light for above-
          normal levels  and a red emergency light for critical water levels.
    H.3.  A  flow diagram of  the  treatment plant  process with lights that  indicate
          equipment  operation status:   green  for  equipment operating and valves in
          normal position,  red for equipment  "off"  and  valves redirecting flow, plus
          flashing red for automatic pump switchover.

I.  For the lab, sufficient  equipment  must be provided to perform  pH titrations  and
    sulfide and H2S detection.

J.  Adequate storage space (to be as safe as reasonable) must be provided for all needed
    process chemicals.

K.  For emergency and safety  provisions, a sump should be provided, with the tank farm
    curbed off in case of accident.  Emergency lights must be provided for the control
    panel and for the process area.

L.  Automatic  switchover must be provided for all pumps in case of failure. The pump
    between tanks A and B should be acid-resistant.

M.  All valves are manual, with one acid-resistant valve before tank A.

N.  Acid-resistant pipe  is to be provided wherever it may contact untreated wastewater.

    Flow rate is assumed to be as indicated in system specifications.  An allowance for
equipment for double-pump automatic switchover was not  taken into account. All pumps
have been located in  the storage area to avoid exposure to weather,  thus contributing to
ease of  maintenance and increased reliability.  Because  of the low flow rate, this is a
batch process. The lab is to be used to determine the pH level and the amount ot sullide
needed.   The amount  of polymer  needed  can also be  determined;  for  this, proper
equipment should be provided.


                                         79

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ENGINEERING SPECIFICATIONS FOR MEDIUM-SIZED AND LARGE PLANTS
(Figures F-3 through F-8 and F-10 through F-16)

A.  The lagoon is based on a 2.13m (7-ft) depth because of elevation and tidal conditions
    at a proposed site. An acid-resistant coating is to be installed to protect the lagoon
    in case of treatment plant breakdown.  The use of support pilings around and within
    the lagoon is suggested.  This provides for the construction of  a deck covering the
    lagoon, except for a grate that surrounds the treatment plant proper.

B.  The deck should be constructed to support the weight  of the treatment  plant. The
    area directly under  the plant should be  constructed  to withstand  at least  4,880
    kg/m2  (1,000 lb/ft2), and the remaining area, at least 488 kg/m2 (100 lb/ft2).

C.  The treatment plant includes the following:

    C.I  The leveling tank is to be lined with an acid-resistant coating. This is the first
         stop for the plant wastewater, unless the wastewater is directed to the lagoon.

    C.2  The flash mixer is to be lined with an acid-resistant coating; the mixing blade
         is to be coated also.  A roof,  having H2S  detectors, should be provided for the
         flash mixer.

    C.3  The lime store area is an  elevated tank for unslaked lime; the raised position
         provides for easy transport to the C-2 area.  The tank is to be attached to the
         control room building for added support.
         C.3.1   The lime slaker mixes  fresh, slaked lime and  water and  passes this
                 lime slurry to a  slurry  tank.   (The  manufacturer-supplied system
                 includes pumps, pipes, and slaker.)
         C.3.2   The lime slurry  tank is used for continuous flow to either tank B or
                 recycle.  (The manufacturer-supplied system includes pumps, tank, and
                 piping up to, and including, the valve.)  The valve must be electrically
                 operated for control by the pH system.
         C.3.3   The pH control area is to contain the pH control machinery (automatic
                 and manual). This includes pH level monitors, controllers, and record-
                 ers.  The pH sensors are to be located on the  pipe leading to tank B
                 from tank A and on the line leaving tank B.

    C.4  The polymer feed area includes the mixer, tank, and pipes up to and including
         the pumps; this is a continuous process at a designated flow.

    C.5  The flocculating  tank  receives flow from tank B and the polymer feed system.
         The tank located on top  of  the clarifier, is arranged  so that  overflow will
         cascade into the clarifier.

    C.6  The clarifier  is  furnished by the  manufacturer  and  receives  flow from the
         flocculator and the filter press.  The sludge contracted at the clarifier bottom
         flows to the sludge storage tank (tank H) by a pump.   The clarifier  overflow
         drains into the sewer.
         C.6.1   Clarifier  overflow goes  to  the aerator, tank K,  by  gravity feed (for
                 sulfide treatment system only).
         C.6.2   Clarifier  overflow goes to the aerator, tank 3-3,  by gravity feed (for
                 sulfide polish system only).


                                        80

-------
    C-7  The sludge storage  tank is designed to hold  a day-to-day supply of sludge for
         batch processing by the filter press, according to the recommended procedure.

    C.8  The filter press is  a manufactured item  that can process a 2-day supply of
         sludge in 12 hr. Means for sludge removal are to be provided.  Removed water
         is recirculated to the clarifier; this flow can also be directed to the lagoon for
         dilution or complete reprocessing. Sludge is dewatered to 60-percent moisture
         content.

    C.9  The sulfide feed system is  supplied  by  the manufacturer; it  includes tank,
         motors,  pumps,  and pipe up  to and including  the  valve (to  be electrically
         operated).  (The system is for sulfide treatment  and sulfide polish  systems
         only.)
         C.9.1   The sulfide  control area is to contain  the sulfide  control machinery
                 (automatic   and manual);  this  includes  monitors,  controllers, and
                 recorders. Free-sulfide and H2S level sensors should be installed:
                 C.9.1.a   On the pipe between tanks A and B, and between  tanks B
                           and C (for sulfide treatment system only);
                 C.9.1.b   On the line between tanks G and 3-3, and between tanks 3-3
                           and L (for sulfide polish system only).
         C.9.2   The sulfide slurry tank is a mixer and should have H2 S gas detection
                 equipment  installed  around it.    The  tank receives flow  from the
                 clarifier and sulfide feed tank, which feeds to a filter (manifold type).
                 (The tank is for the sulfide polish system only.)

    C.10 The aerator oxygenates the  effluent before discharge.  The rate depends on
         system size.  (For sulfide treatment and sulfide polish systems only.)

    C.ll The filter is  a manifold type for small particulate removal to be discharged
         into the aerator.  (For the sulfide polish system only.)

D.  An audible  alarm and an automatic process water detour are needed.  An audible
    signal  must be installed in the process area to  sound when the water in the tanks
    reaches  critical levels, when the pH level is too acid for the process, or when H2 S
    gas is detected.  The main valve at the plant process water inlet must automatically
    detour process water to the lagoon.

E.  The flow control should be kept to specifications for efficient operations.

F.  An instrument control panel  must  be easily  accessible to the operator and centrally
    located  to  the treatment equipment.   Instruments  installed on the panel must
    include the following:
    F.I  On-off control of all pumps.
    F.2  Indicators of water levels in each tank,  including a  yellow light for above-
         normal levels and a red emergency light for critical water levels.
    F.3  A  flow  diagram of  the  treatment plant process with lights  that  indicate
         equipment operating status:   green  for  equipment  operating  and valves in
         normal  position, red for equipment "off" and  valves redirecting  flow, plus
         flashing red  for  automatic  pump  switchover.   Remote  indicators must  be
         provided for all pH  and sulfide readings and for H2S gas monitors.
                                         81

-------
G.  Adequate storage space is to be allotted for all chemical storage in safe, controlled
    areas as near as practical to the location of use.

H.  For emergency and safety provisions, the plant must contain the following:
    H.I  Backup dust  equipment  must  be  provided,  including  switching,  valves,  and
          controls to operate properly.
    H.2  Emergency  lights must be  displayed on the control panel and  in the manu-
          facturing process area as described under indicators (F.2).

I.   For pumps, automatic switchover must be provided in case of failure.  Some pumps
    should be as acid-resistant as possible, depending on their location in the  system.

J.  All necessary safety valves  should be included. The valve  on the effluent receiving
    side of tank A  should be  electrically operated and as acid-resistant as  possible, or
    coated; the same  holds true for the valve on the outlet side of tank A.

K.  All pipe that will contact  untreated wastewater  is to have  an acid-resistant liner
    and, in the case of lagoon pipes, an acid-resistant coating.

    Flow rate is assumed to be as indicated in system  specifications.  Allowance  for
equipment for double-pump automatic switchover was not taken into account. All pumps
have been located in the storage area to avoid exposure to weather, thus contributing to
ease of maintenance and increased reliability.
 INFLUENT,
 37.85 m3
 (10,000 gal)
 PER DAY
 (NONCHROMATE,
 NONCYANIDE)
  TANK,
  45.42 m3
  (12,000 gal)
TANK,
45.42 m3
(12,000 gal)
           PUMP,
           0.15 m3/min
           (40 gal/min)
             PUMP,
             0.38 m3/min
             (100 gal/min)
SLUDGE
FILTER
                PUMP,
                0.38 m3/min
                (100 gal/min)  (CLF SYSTEM ONLY)
                                                                              PUMP,
                                                                              0.15 m3/min
                                                                              (40 gal/min)
   Plant capacity = 37.85 m3 (10,000 gal) per day
                                                            FILTER
                                                                          SLUDGE
                                                  TO SEWER


                       Figure F-1. Small LO-CL and LO-CLF plant schematic.
                                          82

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INFLUENT,
37.85 m3
(10,000 gal)
PER DAY
(NONCHROMATE,
NONCYAIMIDE)
   TANK,
   45.42 m3
   (12,000 gal)
                                 (12,000 gal)
PUMP
0.15m3/min
(40 gal /mini
                PUMP,
                0.38 m3/min
                (100 gal/min)
  • Plant capacity = 37.85 m3 (10,000 gal) per day
      PUMP,
      0.38 m3/min
      (100 gal/mini
                                              PUMP,
                                              0.15m3/min
                                              (40 gal/mini
                                                                                       SLUDGE
                                                                               Omit filter for
                                                                               LWS-CL system
                 Figure F-2.  Small LSPF, L WS-CL, and L WS-CLF plant schematic.
                                                 83

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     Plant capacity = 757 m3 (200,000 gal) per day
     Lagoon
     Leveling tank
     Lime feed
     Flash mixer
     Polymer feed
     Flocculating tank
     Clarifier
     Sludge filter press
763 m3 (201,600 gal)
31.8m3 (8,400 gal)
0.95 L/min (0.25 gal/min)
5.3 m3( 1,400 gal)
5.3 L/min (1.4 gal/min)
2.65 m3 (700 gal)
72.5 m2 (780 ft2)
0.3 m3 (10.8 ft3) per day,
60% moisture
INFLUENT,
757m3
(200,000 gal)
PER DAY
(NONCHROMATE,
NONCYANIDE)
                                             LAGOON
                                 LU
                                                                LEVELING TANK
LIME FEED SYSTEM
                                                        ~l
           i-1       	 RECYCLE
             U     I—I C2?;5°l
           itj—M> m     .  TTT "~i
           nwn      !        iBiSg/
           kh      !:          T
                                                  pH CONTROL
           POLYMER FEED
                    n i             SCUM
                      FLOCCULATING TANK
                                                                              FILTER
                                                                         (CLF SYSTEM ONLY)
                       CLARIFIER
             CONTINUOUS FLOW RECORDER ft SAMPLER
                      TO SEWER OR STREAM
                                       EAR EFFLUENT           |
                                          HEAVY 5LU06E  FILTER PRESS

                                                          SLUDGE STORAGE
                                                                          D
                                                                            I
                                                                        TRUCK OR PUMP TO LAGOON
                Figure F-3.  Medium-sized LO-CL and LO-CLF plant schematic.

-------
  Plant capacity = 757 m3 (200,000 gal) per day
  Lagoon
  Leveling tank
  Lime feed
  Flash mixer
  Polymer feed
  Flocculating tank
  Clarifier
  Sludge filter press

  Aerator
-  763 m3 (201,600 gal)
-  31.8 m3 (8,400 gal)
-  0.95 L/min (0.25 gal/min)
-  5.3 m3( 1,400 gal)
-  5.3 L/min (1.4 gal/min)
-  2.65 m3 (700 gal)
-  72.5 m2 (780 ft2)
-  0.3 m3 (10.8 ft3) per day,
   60% moisture
-  0.9g (0.002 Ib)  per minute
   of 02
INFLUENT,
757m3
(200,000 gal)
PER DAY
(NONCHROMATE
NONCYANIDE)
                                                                                  SULFIDE FEED SYSTEM
                                                                                  0.3 L/min (0.08 gal/min)
LIME FEED
 SYSTEM
AERATOR
   POLYMER FEED
       CONTINUOUS HOW RECORDER I SAMPLER
              TO SEWER OR STREAM
                                                  FILTER PRESS

                                                      SLUDGE STORAGE

                                           TRUCK OR PUMP TO LAGOON
                        Figure F-4. Medium-sized LSPF plant schematic.
                                               85

-------
Plant capacity = 757 m3 (200,000 gal) per day
 Lagoon
 Leveling tank
 Lime feed
 Flash mixer
 Polymer feed
 Flocculating tank
 Clarifier
 Sludge filter press

 Aerator
763 m3 (201,600 gal)
31.8m3 (8,400 gal)
0.95 L/min (0.25 gal/min)
5.3 m3< 1,400 gal)
5.3 L/min (1.4 gal/min)
2.65m3 (700 gal)
72.5 m2 (780 ft2)
0.3 m3 (10.8ft3) per day,
60% moisture
0.9g (0.002 Ib) per minute of C>2
INFLUENT,
757m3
(200,000 gal)
PER DAY
(NONCHROMATE,
NONCYANIDE)
                                                                        SULFIDE FEED
                                                                        SYSTEM, 1.25
                                                                        L/min (0.33 gal/min)
  LINEFEED
   SYSTEM
                                     a                 LI
                        CLARIFIERj	UBHTSLUBBgW-^  J
                                                                              FILTER
                                                                         (CLF SYSTEM ONLY)
AERATOR
                                                                               SLUDGE STORAGE
                 TO SEWER OR STREAM
                                                                     TRUCK OR PUMP TO LAGOON
            Figure F-5. Medium-sized LWS-CL and LWS-CLFplant schematic.
                                            86

-------
 Plant capacity = 1,893 m3 (500,000 gal) per day
 Lagoon
 Leveling tank
 Lime feed
 Flash mixer
 Polymer feed
 Flocculating tank
 Clarifier
 Sludge filter press
1,908 m3 (504,000 gal)
79.5 m3 (21,000 gal)
2.5 L/min  (0.66gal/min)
13.25 rr>3 (3,500 gal)
13.25 L/min (3.5gal/min)
6.6 m3 (1,750 gal)
182m2(l,960ft2)
0.8m3(27ft3)perday,
60% moisture
LIME FEED SYSTEM
                             INFLUENT,
                             1,893 m3
                             (500,000 gal)
                             PER DAY
                             (NONCHROMATE,
                             NONCYANIDE)
                                                                    LEVELING TANK
            POLYMER FEED
          |f             turn
          FLOCCULATING TANK 1
                         CLARIFIER
[CLEAR EFFLUENT            \   |
I    I     I  SETTLING TANK
                                                           FILTER
                                                      (CLF SYSTEM ONLY)
                       TO SEWER OR STREAM
                                                                       HEAVY SLU06E FILTER PRESS

                                                                          I   II      SLUDGE STORAGE
                                                                                |
                                                                           TRUCK OR PUMP TO LAGOON
                  Figure F-6.  Large LO-CL and LO-CLF plant schematic.
                                               87

-------
    Plant capacity = 1,893 m3 (500,000 gal) per day
    Lagoon
    Leveling tank
    Lime feed
    Flash mixer
    Polymer feed
    Flocculating tank
    Clarifier
    Sludge filter press

    Aerator
1,908 m3 (504,000 gal)
79.5m3 (21,000 gal)
2.5 L/min  (0.66 gal/min)
13.25m3 (3,500 gal)
13.25 L/min (3.5 gal/min)
6.6 m3( 1,750 gal)
182m2(1,960ft2)
0.8 m3 (27 ft3)  per day,
60% moisture
2.7g (0.006 Ib) per minute
of 02
                                     LAGOON
INFLUENT,
1,893 m3
(500,000 gal)
PER DAY
(NONCHROMATE,
NONCYANIDE)
LINEFEED
 SYSTEM
                                                        LEVELING TANK
                                                                         SULFIDE FEED SYSTEM.
                                                                         0.8 L/min (0.21 gal/min)
AERATOR
             TO SEWER OR STREAM
                                                                      FILTER PRESS

                                                                          SLUDGE STORAGE

                                                                TRUCK OR PUMP TO LAGOON
                             Figure F-7.  Large LSPF plant schematic.
                                                 88

-------
       Plant capacity = 1,893 fr»3 (500,000 gal) per day
       Lagoon
       Leveling tank
       Lime feed
       Flash mixer
       Polymer feed
       Flocculating tank
       Clarifier
       Sludge filter press
    •  Aerator
 1,908 m3 (504,000 gal)
 79.5 m3 (21,000 gal)
 2.5 L/min (0.66 gal/min)
 13.25 m3 (3,500 gal)
 13.25 L/min (3.5 gal/min)
 6.6 m3( 1,750 gal)
 182m2(1,960ft2)
 0.8 m3 (27 ft3) per day,
 60% moisture
 2.7g (0.006 Ib) per minute
of O2
INFLUENT,
1,893 m3
(500,000 gal)
PER DAY
(NONCHROMATE,
NONCYANIDE)
  LIME FEED
   SYSTEM
                                                            SULFIDE FEED
                                                            SYSTEM, 3.2 L/min
                                                            (0.84 gal/min)
     POLYMER FEED
               1 [             MUM

                FLOCCULATING TANK
AERATOR
                                  EFFLUENT
                            I,  I
                        CLARIFIER!	I       LIGHT SLUDGEN-r-^
          CONTINUOUS FLOW RECORDER t SAMPLER
                  FILTER
              (CLF SYSTEM ONLY)
                 TO SEWER OR STREAM
                                               .FILTER PRESS
                                                     SLUDGE STORAGE

                                          TRUCK OR PUMP TO LAGOON
                     Figure F-8.  Large LWS-CL and LWS-CLF plant schematic.
                                                  89

-------
INFLUENT,
37.85 m3
110,000 gal)
PER DAY
                                                                                           SLUDGE
                                                                                           REMOVAL
                      LAB,
                      CONTROL,
                      AND
                      STORAGE ROOM
     • Scale 1 in = 10ft
     • Plant capacity = 37.85 m3 (10,000 gal) per day

     •Aerator used in  LSPF, LWS-CL,and LWS-CLF plants only
     tFilter bank used in LO-CLF, LSPF, and LWS-CLF plants only
                                                                        LEGEND:
A   Stoiage tank
B   Mjxer-clarifier tank
C   Filter press
&   Pump
®   Valve
D   Aeiator*
E   Filter bankt
 Figure F-9. Small plant layout-all processes (LO-CL, LO-CLF, LSPF, LWS-CL, and LWS-CLF).
                                                90

-------
   20ft
                DISCHARGE
G 0-

¥


E
C+
o
C-3
CD 9
o ig
IP--B

C-2
60ft
                                                    SLUDGE
                                                    REMOVAL
                                       LJ
                                           u
                       LEGEND:
                      A
                      8
                      C-1
                      C-2
                      C-3
                      C-4
                      D
Leveling tank
Flash mixer
Lime store
Lime slaker
Lime slurry
pH control
Polymer feed
E   Flocculating tank
G   Clarifier
H   Sludge storage
I    Filter press
L   Filter (CLF system only)
63   Pump
Ig)  Valve
INFLUENT, •
0.53 m3
(140 gal)
PER
MINUTE
                                i Plant capacity = 757 m3 (200,000 gal) per day
                     Figure F-10.  Medium-sized LO-CL and LO-CLF plant layout.
                                                    91

-------
                  65ft
••
-L
o
CM
0
co
L
-r.
3m °1 fi7 ft ml
• ~1.b7tt •)
i n



_

G
J'1 E
rO« 6* > -
D C"3 C-2
-H V JSLsu,
r


C-1
| 	 fj I I I I * I -¥l \J= t & ~ I I

L---~.*~ ..«_^[
j-3 «f — r '
" j -USr


L
T
— K *
DISCHARGE
o
H
^^H^J^
9
CONTROL
AND
STORAGE
ROOM


	 10- | -4
1
[ 	
r 99
3 i
B
L ^ 	 •
"—*"^T
nH
ALP
SYS
A
i
C-l-O-f-" 	 '
2KB
kRM
TEM
fiti
!
* SLUDGE
REMOVAL

nu u u
LEGEND:
A Leveling tank H Sludge storage
B Flash mixer | Filter press
C-1 Lime store H Pump
C-2 Lime slaker  Valve
C-3 Lime slurry j-1 Sulfide feed
C-4 pH control J-2 Sulfide control
D Polymer feed J-3 Sulfide slurry
E Flocculating tank K Aerator
G Clarifier L Filter


J
H
n
u
INFLUENT,
PER MINUTE
   • Plant capacity = 757 m3 (200,000 gal) per day
Figure F-11.  Medium-sized LSPF plant layout.
                      92

-------
        LEGEND
        A   Leveling tank
        B   Flash mixer
        C-1  Lime store
        C-2  Limeslaker
        C-3  Lime slurry
        C-4  pH control
        D   Polymer feed
        E   Flocculating tank
G   Clarifier
H   Sludge storage
I    Filter press
B   Pump
®   Valve
J-1  Sulfide feed
J-2  Sulfide control
K   Aerator
L   Filter (LWS-CLF system only)
INFLUENT,—
0.53 m3
(140 gal I
PER MINUTE
         • Plant capacity = 757 m3 (200,000 gal) per day

Figure F-12.   Medium-sized LWS-CL and LWS-CLF plant layout.
                                  93

-------
LEGEND:
A   Leveling tank
B   Flash mixer
C-1  Lime store
C-2  Lime slaker
C-3  Lime slurry
C-4  pH control
D   Polymer feed
E    Flocculating tank
G    Clarifier
H    Sludge storage
I     Filter press
E3    Pump
®    Valve
L    Filter (LO-CLF system only)
INFLUENT,—I
1.32 m3
(350 gal)
PER MINUTE
    Plant capacity = 1,893 m  (500,000 gal) per day
     Figure F-13.   Large LO-CL and LO-CLF plant layout.

-------
23.3 ft
                                                                     CONTROL
                                                                     AND
                                                                     STORAGE
                                                                     ROOM
                                                        DISCHARGE
                            LEGEND:
                            A   Leveling tank
                            B   Flash mixer
                            C-1  Lime store
                            C-2  Limeslaker
                            C-3  Lime slurry
                            C-4  rjH control
                            D   Polymer feed
                            E   Flocculating tank
                            G   Clarifier
H
I
J-1
J-2
J-3
K
L
Sludge storage
Filter press
Pump
Valve
Sulfide feed
Sulfide control
Sulfide slurry
Aerator
Filter
                                INFLUENT.	1
                                1.32m3
                                (350 gal)
                                PER MINUTE
                               > Plant capacity = 1,893 m3 (500,000 gal) per day
                                    Figure F-14.  Large LSPF plant layout.
                                                         95

-------
 LEGEND:
A
B
C-1
C-2
C-3
C-4
D
E
G
 Leveling tank
 Flash mixer
 Lime store
 Lime slaker
 Lime slurry
 pH control
 Polymer feed
 Flocculating tank
Clarifier
H   Sludge storage
I-   Filter press
B   Pump
®   Valve
J-1  Sulfide feed
J-2  Sulfide control
K   Aerator
L   Filter (LWS-CLF system only)
                                                                        INFLUE
                                                                        1.32m3
                                                                        (350 gal)
                                                                        PER MINUTE
                 • Plant capacity = 1,893 m3 (500,000 gal) per day
         Figure F-15,   Large L WS-CL and L WS-CLF plant layout.
                                  96

-------
CLARIFIER
                 o
                              |CQNTROL[
                              AND
                              ISTORAGEJ
                              ROOM
SLUDGE
STORAGE
                                         60 to 70 ft
             NOTE
             Treatment plant is above the lagoon on a deck
             that covers the entire lagoon.  Deck bracing
             piles are'not shown; area under plant should
             withstand 4,880 kg/m2 (1,000 Ib/ft2), other
             areas, 488 kg/m2 (100 Ib/ft2).
                                                                      FILTER PRESS
                                  DECK


                                  '« 1 ft
                                                                                 7ft
                                 -WALL
                                  BRACE
                                  PILING
                 LAGOON WITH ACID-
                 RESISTANT COATING
                 (~ 200,000 gal,
                  757 m3/day PLANT)
       Figure F-16. Cross section of medium-sized and large plants-all processes
                     (LO-CL, LO-CLF, LSPF, LWS-CL, and LWS-CL F).
                                            97

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                                  APPENDIX G

                     GRAPHIC PRESENTATION OF RESULTS

    Figures G-1 through G-5 graphically compare the raw feed and effluent concentra-
tions  of  cadmium,  copper,  chromium,  nickel, and  zinc heavy  metals  for  the five
precipitation processes:

    a.  Lime only, clarified (LO-CL)
    b.  Lirne orily, clarified and filtered (LO-CLF)
    c.  Lime, sulfide polished and filtered (LSPF)
    d.  Lime with sulfide, clarified (LWS-CL)
    e.  Lime with sulfide, clarified and filtered (LWS-CLF)

    Figure G-l shows the relationship of LO-CL process effluent concentrations for the
16 test runs.  Similar bar graphs in groups of five each (Figures G-2 through G-5) show
the same type  of data for the other four processes.
                                       98

-------
                                         DC
                                         LU
                                         Q.
                                         O.
                                         O


                                         O
                                         H
                                         <
                                         IT

                                         Z
                                         III
                                         8J
                                               le
                                                 COPPER
       4 567 8  9 101112 13141516
         TEST RUN NUMBER
        1234
                 5  6  7  8 9 1011 12 13141516
                 TEST RUN NUMBER
                                                               Raw feed
                                                               LO-CL process effluent
                2 3 4 5  6  7  8 9 1011

                      TEST RUN NUMBER
14 1516
                                         o

                                         N
                                         o
                                         I-
                                         LU
                                         8J
                                              18
                                                 ZINC
12345678 910111213141516

        TEST RUN NUMBER
                                                 1234
                5 6 7  8  9 1011 12 13141516

                TEST RUN NUMBER
  Figure G-1. Relationship of LO-CL process effluent concentration to raw feed
             concentration for Cd, Cu, Cr, Ni, and Zn.
                                     99

-------
Q

O
LL
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Z
g

H

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        CADMIUM
                                                 DC
                                                 HI
                                                 a.
                                                 a.
                                                 O
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                                                 LL
                                                 O

                                                 Z
                                                 O


                                                 <
                                                 DC

                                                 Z
                                                 LU

                                                 2
         1 2
               4 5 6 7 8 9 10 11 121314 1516

                TEST RUN NUMBER
                                                         COPPER
1234
                                                                  5678 910111213141516

                                                                  TEST RUN NUMBER
             o
             cc
             i   leeee
             o
             g


             <
             DC


             01
             8-1
                  lee
                      CHROMIUM
                      123456789 10 11

                               TEST RUN NUMBER
                                                 14 1516
                                                                        Raw feed
               LO-CLF process effluent
ai
^
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<
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81
         NICKEL
        123456789 101 1213141516

                TEST RUN NUMBER
                                                 O


                                                 N

                                                 LU

                                                 O
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                                                 CC
                                                 LU

                                                 23

                                                 8J
                                                      tee
                                                          ZINC
                                                         12345678 910111213141516

                                                                  TEST RUN NUMBER
         Figure G-2.  Relationship of LO-CLF process effluent concentration to raw feed

                     concentration for Cd, Cu, Cr, Ni, andZn.
                                            100

-------
—   10888
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o
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O    180
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         CADMIUM
         12    4 5 6 7  8  9 1011 12 1314
                 TEST RUN NUMBER
                                        16
                                                 CC
                                                 LU
                                                 a.
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                                                 O
                                                 LL
                                                 o

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                                                  81
                                                      180
                                                         COPPER
                                                            2  3  4 5 6 7 8 9 10 11 121314   16
                                                                  TEST RUN NUMBER
5
— 100000
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                      1  23456789 1011
                               TEST RUN NUMBER
                                                 14   16
Raw feed


I.SPF process effluent
UJ
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81
    \vvvv
         NICKEL
         1  2 3 4  5  6  7  8 9 10 11 12 1314
                 TEST RUN NUMBER
                                         16
                                                 81
                                                              3 4
                                                                  5 6 7 8  9 1011 12 1314
                                                                   TEST RUN NUMBER
                                                                                         16
          Figure G-3. Relationship of LSPF process effluent concentration to raw feed
                      concentration for Cd, Cu, Cr, Ni, andZn.
                                             101

-------
Q

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O
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g


cc
i-
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     IBB
         CADMIUM
         12    4 5 6 7 8  9 10 11 12 13

                 TEST RUN NUMBER
                  16
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                            oc

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                                                          COPPER
                                      2 3 4  5 6 7 8 9 1011 12 13

                                             TEST RUN NUMBER
                                                                                          16
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                      CHROMIUM
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         TEST RUN NUMBER
                                                     16
                                                                          Raw feed
                                                    LWS-CL process effluent
    leeeee
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81
          NICKEL
         1  2 3 4  5  6 7 8 9 10 11 12 13
                 TEST RUN NUMBER
                   16
                          o
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                          N
                          LL
                          O
                          z
                          o
                          DC
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                          Z
                          HI
                                                81
                                                      tee
                                                       ie
                                    ZINC
                                                         1 2 3  4  5 6 7 8 9 10 11 12 13
                                                                  TEST RUN NUMBER
                                                                   16
         Figure G-4.  Relationship of L WS-CL process effluent concentration to raw feed
                     concentration for Cd, Cu, Cr. Ni, andZn.
                                             102

-------
Q
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         CADMIUM
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                 TEST RUN NUMBER
                                   16
                                           cc
                                           LU
                                           Q.
                                           Q.

                                           O
                                           O

                                           U.

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                                           Z

                                           o

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                                                1008
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                                                         COPPER
                                                    1  2 3 4 5 6 7 8  9 10 11 12 13

                                                            TEST RUN NUMBER
                                                                                  16
            O
            cc
            I
            o
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            o
            z
            o

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            cc

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             188
             i«
                     CHROMIUM
                123456789 10 11

                       TEST RUN NUMBER
                                                16
                                                                   Raw feed
LWS-CLF process
         1 2 3
          4 5 6  7  8 9 10 11 12 13

            TEST RUN NUMBER
                                                O


                                                N
                                                LL
                                                o

                                                z
                                                g

                                                N

                                                oc
                                                81
                                                         ZINC
                                                    1  2 3 4  567  8  9 10 11 12 13

                                                             TEST RUN NUMBER
                                                                                        16
         Figure G-5.  Relationship of LWS-CLF process effluent concentration to raw feed

                     concentration for Cd, Cu, Cr, Ni, and Zn.
                                             103

-------
                                  APPENDIX H

           CRITERIA FOR SELECTING pH VALUE FOR PRECIPITATION
    Figure H-l, which indicates theoretical  hydroxide solubilities (14), shows  that the
optimum pH for maximum precipitation  varies for different metals.  Consequently, a
treatment plant that receives a mixed heavy metal load must adopt a compromise pH.
The value will depend on  the desired reduction levels for specific heavy metals.  Two
other factors are also usually taken into account.  First, an unnecessarily high pH results
in unnecessarily high lime costs.  Second, subsequent acidification may be  required, if
the local discharge permit requires a maximum pH of 9.0, as many permits do.
                  -J
                  CD
                  O
                  c/i
                    0.01  —
                   0.001  —
            Figure H-1.  Effect of pH on effluent concentration of heavy metals.
                                       104

-------
SELECTION OF pH VALUE
     For this work,  the preferred pH value was one that would reduce the heavy metal
theoretical  solubility levels below the EPA "1978  Proposed Effluent Limitation Guide-
lines" (1«0.  The limits are listed in Table H-l.


     Combination of the solubilities of Figure< H-l with the EPA guidelines generates
Table H-2.  Bold numbers in the table are levels below guideline limits.
                        TABLE H-1. PROPOSED EPA GUIDELINE
                                   LEVELS
Heavy metal
Cr6+
Ag
Pb
Cd
Zn
Cr (total)
Ni
Cu
Proposed 30-day
• average efficient
level Uig/L)
90
340
400
i 500
1,500
1,600
1,800
2,000
  TABLE H-2. EFFLUENT CONCENTRATION RELATED TO EPA PROPOSED LIMITATIONS


                             Concentration (jug/U* at pH values of:
  Heavy	———————	
  metal   8.00     8.25    8.50   8.75    9.00    9.25    9.50    9.75  10.00  10.25  10.50

    Cd   >1,300 >1,300  >1,300  >1,300 >1,300 >1,300 >1,300  1,300   230     38     11

    Cr       30     24      20      21      29     50    100   200   500    850   2,000

    Cu        5      2     < 1     < 1    <1    <1    <1   <1    1.5      3      5
Ni
Zn
2,800
8,000 1,400
1,000
300
350
75
120
60
38
75
9
110
4
190
1.5
330
1
550
1
850
  'Boldface values are below EPA guideline levels.
                                         105

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                                            TECHNICAL REPORT DATA
                                   (Please read Instructions on the reverse before completing)
1. REPORT NO.
  EPA-600/2-80-139
                                                                           3. RECIPIENT'S ACCESSION NO.
4. TITLE AND SUBTITLE
    Sulfide Precipitation of Heavy Metals
                 5. REPORT DATE
                        JUNE  1980 issuing  date.
                                                                           6. PERFORMING ORGANIZATION CODE
7. AUTHOR(S)

    A. K. Robinson and 3. C. Sum
                 8. PERFORMING ORGANIZATION REPORT NO,

                    D6-42205-5
9. PERFORMING ORGANIZATION NAME AND ADDRESS

    Boeing Commercial  Airplane Company
    P.O.  Box 3707
    Seattle, Washington  98124
                                                                           10. PROGRAM ELEMENT NO.
                    1 BB 610
                 11. CONTRACT/GRANT NO.

                    S805413
 12. SPONSORING AGENCY NAME AND ADDRESS
    Industrial Environmental Research Laboratory—Cin., OH
    Office of Research and Development
    U.S. Environmental Protection Agency
    Cincinnati, Ohio  45268
                 13. TYPE OF REPORT AND PERIOD COVERED
                    Final, Oct. 77-July '79
                 14. SPONSORING AGENCY CODE
                    EPA/600/12
 15. SUPPLEMENTARY NOTES
 16. ABSTRACT

        This research program was initiated with the objective
    of  evaluating  a new  process,  the  sulfide precipitation  of
    heavy metals from industrial wastewaters.  The process was
    expected to effect a more complete removal of heavy metals
    than conventional lime processing because of the much lower
    solubilities of metal sulfides than hydroxides.

        Five  processes were  compared in bench-scale, con-
    tinuous-flow equipment:  conventional lime processing, con-
    ventional lime  processing plus filtration, lime with a sulfide
    polishing and  filtration, lime with sulfide,  and  lime with
    sulfide'plus filtration.

        Samples of actual wastewaters from 14 metal  working
    industries (including  Boeing) were  processed through the
    bench-scale equipment using all five processes.  Reductions
    in the concentrations of cadmium, chromium, copper, nickel,
    and zinc, plus selected other metals,  were measured  by
    atomic absorption chemical analysis.

       Capital and operating costs for the five  processes were
    compared for  three  plant  sizes:    37.85  m3/day  (10,000
    gal/day), 757  mVday  (200,000  gal/day), and 1,893  nWday
    (500,000 gal/day).
     The report  recommends that,  to  reduce the levels of
 cadmium, copper, nickel, or zinc from a wastewater treat-
 ment plant using conventional lime processing, the addition
 of a final filtration should be  considered first.  If filtration
 does  not achieve  the desired  low  levels,  then  a sulfide
 polishing process with added filtration is recommended.  If
 reduction of  the levels of chromium, lead, silver, or tin is
 required,  the conventional  lime process  plus filtration is
 recommended.   The  sulfide  process did not significantly
 reduce the levels of these metals.

     Details  are  included on the use of a specific ion elec-
 trode for the control  of sulfide  additions.  The report does
 not  include   comparison testing of  the  commercial  Sulfex
 process.

     This  report  was  submitted  in  fulfillment  of  Grant
 S805413 by Boeing  under the sponsorship of the U.S. Environ-
 mental  Protection  Agency.  This report covers a period from
 October 1977 to July  1979; work was completed as of 3uly
 1979.
 7.
                                        KEY WORDS AND DOCUMENT ANALYSIS
                       DESCRIPTORS
b.lDENTIFIERS/OPEN ENDED TERMS  C.  COSATI Field/Group
   water treatment
   wastewater
   electroplating
   waste treatment
   precipitation
   sulfides
   heavy metals
   toxic metals
   68D
 8. DISTRIBUTION STATEMENT

   Release to public
19. SECURITY CLASS (ThisReport)
   unclassified
21. NO. OF PAGES
  118
                                                          20. SECURITY CLASS (Thispage)
                                                             unclassified
                                  22. PRICE
EPA Form 2220-1 (Rev. 4-77)    PREVIOUS  EDITION is OBSOLETE
                                                                            U.S. GOVERNMENT PRINTING OFFICE:  1980--657-165/0025
                                                        106

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