vvEPA
            United States
            Environmental Protection
            Agency

            Research and Development
            Environmental Research
            Laboratory
            Athens GA 30605
 »„,«,, I/
'V 1978
Fate and Impact
of Pentachlorophenol
in a Freshwater Ecosystem

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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 fosler technology transfer and a maximum interface in related fields
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      1   Environmental  Health Effects Research
      2   Environmental  Protection Technology
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      8   "Special" Reports
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This report has been assigned to the ECOLOGICAL RESEARCH series Thissenes
describes research on the effects of pollution on humans, plant and animal spe-
cies, and materials Problems  are assessed  for their long- and short-term influ-
ences Investigations include formation, transport, and pathway studies to deter-
mine the fate ol pollutants and the*r effects  This work provides the technical basis
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This document is available to the public through the National Technical informa-
tion Service, Springfield, Virginia 22161

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                                                                       EPA-600/3-78-063
                                                                       July 1978
                              FATE AND IMPACT OF PENTACHLOROPHENOL

                                    IN A FRESHWATER ECOSYSTEM
                                               by

                                     Richard H. Pierce, Jr.
                               Institute of Environmental Science
                               University of Southern Mississippi
                                 Hattiesburg, Mississippi 39401
1
-S
s

\
0
                                   Grant Number R-803-82-0010

*
~j
i
                                         Project Officer

                                          N. Lee Wolfe
                                 Environmental Processes Branch
                                Environmental Research Laboratory
                                      Athens, Georgia 30605
                                U.S. Environmental Protection
                                Region 5, library tf»HZft
                                77 West befcsoft Boufwwj, 12th Flow
                                        l  60604-3590
                                ENVIRONMENTAL RESEARCH LABORATORY
                               OFFICE OF RESEARCH AND DEVELOPMENT
                              U.S. ENVIRONMENTAL PROTECTION AGENCY
                                      ATHENS, GEORGIA 30605

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                                 DISCLAIMER

     This report has been reviewed by the Environmental Research Laboratory,
U.S. Environmental Protection Agency, Athens,  Georgia,  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.
                                      ii

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                                  FOREWORD

     Environmental protection efforts are increasingly directed towards
prevention of adverse health and ecological effects associated with specific
compounds of natural or human origin.  As part of this Laboratory's research
on the occurrence, movement, transformation, impact,  and control of envi-
ronmental contaminants, the Environmental Processes Branch studies the
microbiological, chemical, and physico-chemical processes that control
the transport, transformation and impact of pollutants in soil and water.

     Human illness and death have occurred from exposure to pentachlorophenol
(PGP) in industrial and agricultural applications.   In 1974 and 1975,
accidental release of wood-treatment wastes containing PGP in fuel oil
caused extensive fish kills in a freshwater lake in Mississippi.  The study
reported here examines the persistence and distribution of PCP and PGP-
degradation products in this lake to provide information on the effects
of PCP contamination of aquatic systems.
                             David W.  Duttweiler
                             Director
                             Environmental Research Laboratory
                             Athens, Georgia
                                    iii

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                                  ABSTRACT

     This investigation was undertaken to determine the  fate of  pentachloro-
phenol (PCP) that caused extensive fish kills in a freshwater lake in December
1974 and again in December 1976.   The kills resulted from the accidental
release of wood-treating wastes containing PCP in fuel oil.   Samples  of water,
suspended particulates, sediment,  leaf litter and fish were  collected from
February 1975 through April 1977  in an attempt to determine  the  persistence
and distribution of PCP and PCP-degradation products in  the  aquatic environment,

     Food chain relationships were investigated in the lake  and  the
accumulation and elimination of sublethal concentrations of  dissolved PCP
were studied under laboratory conditions for the bluegill (Lepomis
macrochirus).   Also investigated  were the solubility of  PCP  in water
at various pH levels and the release of PCP from contaminated watershed
material.

     Concentrations of PCP well above background levels  were found in the
water and in fish for over six months following the first spill  with another
increase observed fourteen months after the spill (February  1976)  following
a period of heavy rain.  After the second spill, high PCP concentrations
were observed in samples collected in January 1977, and  samples  collected
in April 1977 showed that PCP still remained in water and fish four months
after the spill.  The highest concentrations in fish were observed in the
bile followed by liver, gills, and muscle.  Lake sediment and leaf litter
contained high concentrations of  PCP throughout the two-year study.  Studies
of leaf litter from the contaminated watershed area showed it to be a source
for chronic pollution of the aquatic ecosystem.

     The major degradation products observed were pentachloroanisole
(PCP-OCH3) and the 2,3,5,6- and 2,3,4,5-tetrachlorophenol (TCP)  isomers.
These products were found to persist in sediment and fish along with PCP.
The methyl ethers (anisoles) of both TCP isomers and 2,3,4,6-TCP isomer
were observed in some samples but the small amounts were difficult to
quantitate.  The results suggested that PCP-OCH,, was formed  within the
aquatic environment, whereas much of the TCP appeared to have been formed
before entering the lake, perhaps by photoreduction in the fuel oil solution.

     At the pH of the lake water, PCP existed primarily  as the phenate
anion and the distribution of PCP throughout the water column was enhanced
by the solubility.  The acute toxicity to fish observed  immediately after
each spill occurred by uptake of the phenate anion dissolved in water.
Food chain relationships within the lake showed that game fish populations
depended ultimately upon benthic organisms as a food source.  The accumula-
tion of PCP in sediments, therefore, provided a source for chronic pollution
of fish caught for human consumption.


                                      iv

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     This report was submitted in fulfillment of grant no.  R-803-82-0010
by the University of Southern Mississippi,  Institute of Environmental Science
under the sponsorship of the U.S. Environmental Protection Agency.   This
report covers a period from January 1975 to April 1977 and the work was
completed as of August 31, 1977.

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                                  CONTENTS
Foreword	ill
Abstract	    iv
Figures	viii
Tables	    ix
Acknowledgement	    xi

     1.  Introduction	     1
     2.  Conclusions 	     5
     3.  Recommendations 	     7
     4.  Materials and Methods 	     9
              Environmental samples	     9
              PCP release from contaminated leaf litter	    13
              Solubility of PCP in water	    13
              Accumulation and elimination of PCP in fish	    16
              Food chain study	    17
     5.  Results and Discussion	    19
              Environmental samples	    19
              PCP release from contaminated leaf litter	    34
              Solubility of PCP in water	    36
              Accumulation and elimination of PCP in fish	    42
              Food chain study	    47

References	    56
Appendix	    59
                                     vii

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                                   FIGURES

Dumber                                                                     Page

  1   Sample sites in contaminated stream and lake 	   2

  2   Extractipn of PCP and PGP-degradation products from environmental
        samples	12

  3   Titration of PCP in aqueous solution	38

  4   Ultraviolet spectra of PCP and SPCP in 0.1 M buffer	39

  5   Accumulation of PCP in tissue during exposure to 0.1 ppm PCP ....  44

  6   Elimination of PCP from Group 1 (after 4 days exposure)	45

  7   Elimination of PCP from Group II (after 16 days exposure)	46
                                     viii

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                                    TABLES

Number                                                                     Page

  1   PCP and PGP-Degradation Products in Control Samples 	   20

  2   PCP in Water Samples Collected February 1975 - May 1976 	   21

  3   PCP in Water Samples Collected August 1976 - April 1977 	   22

  4   PCP in Sediment Samples Collected February 1975 - May 1976	   24

  5   PCP in Sediment Samples Collected August 1976 - April 1977	   25

  6   PCP in Fish Collected February 1975 - May 1976	   25

  7   PCP in Fish Collected August 1976 - April 1977	   26

  8   PCP in Leaf Litter	   27

  9   PCP and Degradation Products in Technical Grade PCP, Industrial
        Waste Holding Pond and Oil Slick from Stream	   29

 10   PCP-Degradation Products in Lake Water (Dissolved) Collected
        August 1976 - April 1977	   30

 11   PCP-Degradation Products in Lake Sediment Collected August 1976 -
        April 1977	   31

 12   PCP-Degradation Products in Fish Collected August and October 1976.   32

 13   PCP-Degradation Products in Fish Collected January and April 1977  .   33

 14   PCP-Degradation Products in Leaf Litter Collected August 1976 -
        April 1977	   35

 15   PCP Release from Contaminated Leaf Litter	   36

 16   Dissociation of PCP in Water	   37

 17   Spectrophotometric Characteristics in the Ultraviolet of PCP and
        SPCP	   40

 18   Solubility of 26°C of PCP and SPCP at Three pH Values Using Two
        Analytical Methods	   41
                                       IX

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 19   LC-50 of PCP to Lepomis machrochirus	43

 20   Accumulation of PCP in Fish Tissue after Exposure to 0.1 mg
        PCP/1 Water	43

 21   Elimination of PCP from Group II Fish,  Placed in a Clean Environ-
        ment after Sixteen Days Exposure to PGP-Contaminated Water ....  47

 22   Benthic Organisms Collected During August and October 1976 	  49

 23   Benthic Organisms Collected During January and April 1977	50

 24   Stomach Contents of Sunfish Collected from August 1976 - April 1977.  52

 25   Stomach Contents of Catfish Collected from August 1976 - April 1977.  53

 26   Stomach Contents of Non-game Fish Collected from August 1976 -
        April 1977	54

A-l   Physical Parameters from Water Sampling Sites from February 1975
        to May 1976	59

A-2   Physical Parameters from Water Sampling Sites from August 1976
        to April 1977	61

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                              ACKNOWLEDGEMENTS

     Special acknowledgement is given to Dr,  C.  R.  Brent,  Institute of
Environmental Science, and Dr. H. P. Williams,  Department  of Chemistry,
University of Southern Mississippi, for their involvement  as coinvestigators
during the first year grant project and for their continued assistance.
throughout the project period.  Several people were involved with various
aspects of the investigation.  The major contributers were:  Dr. D. M.
Victor, postdoctoral research fellow, Institute of  Environmental Science,
analysis of PCP and degradation products in environmental  samples;
Dr. M. S. Torrey, chemical consultant, solubility and pH studies;
S. R. Reeves, graduate assistant in the Department  of Chemistry, analysis
of environmental samples; G. W. Pruitt, graduate assistant in the Department
of Biology, study of the accumulation and elimination of PCP in bluegills;
and T. C. Modde, graduate assistant in the Department of Biology, study
of food chain relationships in the contaminated lake.

     Fish used for the accumulation and elimination studies were supplied
by the Mississippi Game and Fish Commission Lyman Fish Hatchery, Lyman,
Mississippi.  The Department of Biology, University of Southern Mississippi,
provided boats and equipment for the collection of  environmental samples
and the gas chromatograph with accessories was supplied by the Department
of Chemistry.

     The cooperation of the project director, Dr. N.  L. Wolfe, of the U.S.
Environmental Protection Agency's Environmental Research Laboratory, Athens,
Georgia, throughout the investigation and in obtaining GC-MS analysis of
selected samples is gratefully acknowledged.   The GC-MS analysis of other
samples was performed by C. A. McDaniel of the U.S.  Department of Agriculture,
Gulfport, Mississippi.
                                     XI

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                                   SECTION 1




                                 INTRODUCTION






     In December 1974, an undetermined amount of wood-treating wastes contain-




ing pentachlorophenol (PCP) in fuel oil overflowed the banks of a wood-treat-




ment company's waste water holding pond and soaked into soil and leaf litter




throughout the spill area (Figure 1).   The oil and PCP waste entered a small




creek and traveled about one kilometer to a sixty-acre freshwater lake near




Hattiesburg, Mississippi where the resulting fish kill was described as




extensive to total (Mississippi Air and Water Pollution Control Commission,




1975).  In December 1976 another extensive fish kill was observed in the lake




and subsequent analyses showed that the fish died from acute PCP poisoning„




The investigation reported here was undertaken to study the persistence and




distribution of PCP and major PCP-degradation products and impurities in the




aquatic ecosystem.




     Pentachlorophenol (I) and the sodium salt, sodium pentachlorophenate  (II),




are pesticides that are used extensively for many industrial and agricultural




applications.  The most important uses include:  as a fungicide and bacteri-




cide in processing textiles, paints, rubber and food; as a  mulluscacide to




control snails; as a herbicide; and, most extensively, as a wood preservative




(Bevenue and Beckman, 1967).  It is highly toxic to fish and other aouatic




organisms with a median lethal concentration (LC-50) of 0.2 to 0U6 ppm (Cote",




1972; Cardwell et al., 1976) and accumulation also has been observed in live-




stock and in humans (Plimmer, 1973; Shafik, 1973; Dougherty and Pitrowska,

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1976).   Human illness and death have occurred from improper handling of PCP-




treated lumber, from breathing PCP-contaminated sawdust,  and from exposure




when spraying solutions of PCP in fuel oil as a herbicide (Bevenue and Beckman,




1967; Shafik, 1973; Arsenault, 1976)„
                   fl)



     In addition to acute PCP poisoning, there is concern for contamination




and biological magnification of PCP in aquatic organisms resulting from chronic




exposure (Rudling, 1970; Stark, 1969; Buhler et al., 1973; Zitko et al., 1974;




Kobayashi et al., 1976).  Although the photo- and microbial-degradation of PCP




has been observed to occur rapidly under controlled laboratory conditions




(Crosby and Wong, 1976; Kirsch and Etzel, 1973), the pesticide has been found




to persist in natural aquatic environments.  The problem is magnified by the




persistence of PCP-impurities and degradation products, many of which are also




highly toxic, such as tetrachlorophenol (TCP), tetrachlorobenzo-p-quinone




(chloranil), tetrachlororesorcinol, polychlorinated dibenzo-p-dioxins (PCDD)




and polychlorinated dibenzofurans (PCDF) (Munakata and Kuwahara, 1969; Crosby




et al., 1973; Crummett and Stehl, 1973; Rappe and Nilsson, 1972; Buser, 1976)„




     This two-year investigation has focused on the concentration of PCP and




major PCP-impurities and degradation products in water, sediment, and fish in




the contaminated ecosystem.  In addition to investigating the fate of PCP,




other studies have been performed to gain insight into the overall effect of




PCP contamination.  Food chain relationships were studied by observing benthic




invertebrate populations in sediment and the stomach content of fish caught

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in the lake.  The accumulation and elimination of PCP by one of the major



species of fish in the lake, the bluegill (Lepomis macrochirus),  was observed




under controlled laboratory conditions„   Leaf litter, contaminated with PCP-in-




oil, was washed in water to determine the rate at which PCP might be released




from a contaminated water shed area.  The solubility of PCP in water at various




pH levels was also observed.




     Routine collection of environmental samples was initiated in February




1975, two months after the PCP spill and fish kil!0  The project received




funding in July 1975 and analysis of the environmental samples was initiated




in November 1975.

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                                   SECTION 2



                                  CONCLUSIONS





     Pentachlorophenol concentrations in the water column and in fish remained



high for several months following each fish kill; leaf litter from the contam-



inated water shed area and lake sediment contained high concentrations through-



out the two-year study periodo



     The major degradation products observed were PCP-OCH   2,3,5,6-TCP, and



2,3,4,5-TCP,  The TCP isomers appeared to have been formed from PCP in the oil



solution, prior to entering the lake, whereas PCP-OCH  seemed to have been
                                                     o


formed within the aquatic ecosystem, and within leaf litter along the stream



bank.



     Fish rapidly accumulated PCP and PCP-degradation products from the contam-



inated  lake with the largest concentrations observed in bile, followed by



liver, gills, and muscle tissue.  Laboratory experiments showed that the LC-50



for the bluegill, Lepomis macrochirus, was 0.3 ppm.  Fish exposed to sublethal



concentrations rapidly accumulated PCP, but were abTe to elimirate most of it



within sixteen days when placed in a clean environment.  Thus, the persistence



of PCP in lake fish for several months following each spill indicates that the



fish were subjected to chronic PCP contamination over an extended period of time.



     At the pH observed for the lake water, PCP existed in the soluble phenate



anion form, thus it was readily available for uptake by aquatic organisms,  A



small amount was associated with particulate matter v/hich mav have provided an



important means for incorporation into sediments.



                                      5

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     Food chain studies showed that all gamefish depended upon benthic




organisms either as a direct or indirect food source.   Therefore,  PCP and




PCP-degradation product accumulation in sediments provided a continuous source




for contamination of fish caught for human consumption,,   Questions remain




regarding the persistence of PCP in sediment, since a continuous influx of PCP




from the contaminated water shed could have given the appearance of PCP per-




sistence in the sediment.  In either case the sediment received continuous




exposure to PCP and further study is needed to determine the long-term fate




of PCP in the sedimentary environment.




     In general, the results indicate that PCP released into the aquatic




ecosystem was not rapidly assimilated by photo- or microbial-degradation.




Acute toxicity to fish occurred by rapid uptake of the water soluble phenate




anion, whereas chronic exposure occurred by leaching of PCP from the contam-




inated water shed into the lake and by incorporation of PCP into the benthic




food chain.  Thus, once contaminated with PCP, the sediment and water shed




area provided a source for chronic PCP pollution of the aquatic ecosystem.

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                                   SECTION 3




                                RECOMMENDATIONS






     Having ascertained the persistence of PGP in various parts of the ecosystem




and observed major PCP-degradation products, it would now be advantageous to




study individual aspects of the project more intensely both in the contaminated




lake and under controlled laboratory conditions to gain a better understanding




of the factors involved in the accumulation and degradation of PCP in the aquatic




environments.




     Of primary concern would be the partitioning, of PCP between oil and water




and the adsorption of PCP to suspended participate matter.  The photodegrad-




ation of PCP in fuel oil and volatilization of resulting products would be of




concern to companies utilizing evaporation as their method of waste water




disposal.  The formation and persistence of minor degradation products which




have been reported from previous laboratory experiments (i.e. tetrachloro-




hydroxyquinone5 tetrachlororesorcinol, PCDD and PCDF) should be monitored in



the contaminated ecosystem and their accumulation in fish should be studied




to determine if they present a possible hazard to the ecosystem or to people




using the Iake0




     Further study is needed on the accumulation and metabolism of PCP in fish




including uptake via food as well as through the gills0  Associated with this




would be the accumulation of PCP in benthic organisms and their role in PCP




bioaccumulation0  The relatively high concentration of PCP-like compounds in




the liver of supposedly non-contaminated fish should also receive more





                                      7

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attention.   Additional study of PCP in fish should include the conjugated




forms of PCP that are known to exist in liver and bile,,




     Questions remain regarding the composition and amount of the original




spill and the frequency with which additional PCP-containing waste was released




from the holding pond,,  The apparent persistence of PCP in lake sediment




alternatively could have resulted from a continuous influx of PCP from the




timber-treating company's operation.  Frequent monitoring of the waste water




holding pond and of runoff from the holding pond area would have been necessary




to determine the extent of PCP influx to the lake.  Further study is needed of




the persistence of PCP in lake sediment, of degradation products, and of the




potential for continuous contamination of the aquatic ecosystem via the benthic




food chain, resuspension, and dissolution in the water.

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                                   SECTION 4




                             MATERIALS AND METHODS






ENVIRONMENTAL SAMPLES




     Samples of the oil slick and a few random environmental samples were




obtained immediately after the spill in December 1974.   Routine sampling was




initiated in February 1975 and samples were stored frozen until analysis




began in November 1975, after the necessary equipment had been received and




the reagent blanks and efficiency of the extraction and analysis procedures




had been established.  Extraction and analytical techniques were developed




and improved throughout the first year.  These procedural improvements along




with information about the major PCP-degradation products helped to develop an




improved study for the second year.  Analytical procedures were modifications




of those described by the U.S. Environmental Protection Agency (1974).




     During the first year of the study, samples of water and sediment were




obtained bi-monthly from six sites  (Figure 1).  Leaf litter was collected along



the stream bank at site 1 near the spill area and fish were collected by seine




along the lake shore near sites 3 and 5.  Water quality parameters observed




were temperature, hydrogen ion activity (pH), dissolved oxygen, turbidity,




and total organic carbon.




     Water samples were collected in 4-liter glass jugs with aluminum-lined




caps.  Dissolved and particulate PCP were separated by filtering the water




through Reeve Angel grade 934-AH glass-fiber filter pads.  Dissolved PCP was




recovered by acidifying 2 liters of the filtrate to pH 2 with HC1 and extract-

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ing with 2 x 50 ml of beizene.  Participate PCP was recovered from the filter
pads by washing with 0.1 N HC1, extracting the pads in benzene with ultra-
sonication for IS mi .lutes, followed by rinsing the pads with hexane.  The
benzene and hexane -;nlutions were then combined.  Sediment samples were
collected with three ^rabs using an  Eckman dredge to provide at least 1 kg
of wet sediment from each site.  The samples were stored frozen in aluminum-
lined freezer containers, 'xtracted by ultrasonication in benzene, and analyzed
as described above for particulatc PCP.  Leaf litter was air-dried, blended to
small pieces, and analyzed as described above for sediment„
     Fish collected by seine from the two sites were combined, chopped into
small pieces, and air-J-'ied.  A 25-g sample of air-dried, chopped fish was
blended with 25 g Na_SO., extracted into 100 ml benzene with ultrasonication,
and filtered.  The benzene extraction was repeated, the filtered residue washed
with hexane, and the benzene and hexane solutions were combined.
     The resulting benzene and hexane solution from each of the above sample
extractions was washed with 0..1 N_ NaOH to separate phenolic compounds from
base-insoluble components.  The aqueous solution was then acidified to pH 2
with HC1 and the phenols  were extracted into hexane.  The PCP content of the
resulting hexane solution was determined by gas chromatographic analysis
utilizing electron capture  (EC-GC) detectors.  Samples were analyzed before
and after methylation with diazomethane according to the procedure  of Schlenk
and Gellerman  (I960).
     During the second year of the study  (July  1976 to July 1977),  improved
sample  collection and analysis techniques were utilized allowing more involved
analyses to be performed  on the samples.  Second-year samples were  collected
from four sites on a quarterly basis  (Figure  1)„  Fish were collected near
site B  by gill net to obtain  large specimens  so that various organs of  the  fish
                                      10

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could be analyzed separately.  Fish tissue was analyzed by lysing 1 g (wet




weight) in 2 ml of 50% H?SO., adding 2 ml acetonitrile, and extracting with




2 x 5 ml hexane.  The hexane solution (hexane-I) was then washed with dis-




tilled water and the base-soluble components (phenols) were extracted with




2 x 5 ml of 0.1 N^NaOH, the aqueous HaOH solution was then acidified to pH




2 with HC1 and the phenols were extracted with 2 x 5 ml hexane (hexane II)„




Both hexane-I (containing base-insoluble components) and hexane-II (con-




taining base-soluble components) were then analyzed by GC-EC before and




after methylation with diazomethane.  The basic extraction procedure used




during the second year of the study is shown in Figure 2.




     Water samples were analyzed in triplicate by acidifying filtered




1-liter samples to pH 2 and extracting with 2 x 25 ml hexane.  The hexane




extract was separated into hexane-I and hexane-II and analyzed as described




above for fish samples.  Sediment samples were air-dried, washed with 0.1 N_




HC1 and extracted with a solution of acetone/hexane (60/40, v/v) under




reflux for 20 hours.  The acetone was removed by washing with water and the




hexane solution recovered and treated as described above,,  Particulate




matter, collected on filter pads, and leaf litter were analyzed by the same




method as sediments.




     The base-insoluble components  (hexane-I solution) from selected samples




were further fractionated by elution through an alumina micro-column (Buser,




1975) in an attempt to isolate and identify dioxins and dibenzofurans.  Control




samples of water, sediment, leaf litter, and fish were concurrently collected




from an isolated 5-acre pond which received no industrial or agricultural




drainage.  Levels of PCP and PCP-degradation products in the control pond




are considered to represent background concentrations in this area.  Efficiency
                                      11

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of the extraction procedures was determined by the addition of known amounts

of PCP to clean samples and subjecting the "spiked" samples to the extraction

and analysis procedures.

     Samples were analyzed with a Varian model 2700 gas chromatograph with

Sc H electron capture detectors.  Two 3 mm x 2 m stainless steel columns were

used for identification:  a non-polar 3% SP-2100 on 80/100 Supelcoport and

a polar 10% SP-1000 on 80/1000 chromosorb W.A.W.  Injector temperature was
        HEXANE-I
      BASE-INSOLUBLE
        COMPOUNDS
                              SAMPLE
                         HEXANE EXTRACT
  0.1 N NaOH
BASE-SOLUBLE
 COMPOUNDS
                                        Acidify
            pH 2
                                             HEXANE EXTRACT
                             HEXANE-II
         AQUEOUS SOLUTION
             (Discard)
                        METHYLATE,  CH  =N=N
                          ANALYZE,  GC-EC
                           VERIFY,  GC-MS
       Figure  2.   Extraction  of  PCP  and  PCP-degradation products
                    from  environmental samples0
                                      12

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175°C, column 200°C, and detector 250°C.  The carrier was N  at a flow rate of




25 ml/min.  Compound identity was verified from representative samples utiliz-




ing a Hewlett-Packard 5933 gas chromatography-mass spectrometry (GC-MS)  data




system.  All solvents were reagent grade, redistilled in a glass distillation




apparatus and tested for purity by concentrating 100 fold, methylating and




analyzing by GC-EC.






PCP RELEASE FROM CONTAMINATED LEAF LITTER




     Leaf litter collected from the stream bank at site 1 on February 27, 1975,




was used to study the release of PCP from contaminated leaf litter into water.




Three replicate experiments were performed in which 1 g of air-dried leaf




litter was placed in 100 ml of distilled water and shaken at 60 rpm for 24




hourso  The water was then decanted through medium-porosity glass fiber filter




pads and saved for PCP analysis.




     The filter pad was then back-washed with 100 ml of distilled water and




the water added to the leaf litter for an additional 24-hour period of shaking.




The process was repeated and after the third 24-hour equilibrium period, the




three separate water samples and the leaf litter were analyzed for PCP content




according to the procedures described above for the first year study of




environmental samples.





SOLUBILITY OF PCP IN WATER




Solubility in Distilled Water




     The solubility of PCP in distilled water was determined by adding excess




reagent grade PCP to 250 ml distilled water and enhancing dissolution by ultra-




sonication or stirring up to 62 hours„  The concentration of the molecular




(phenol) and ionic (phenate) forms of PCP in aqueous solution was determined
                                      13

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by titrating a solution of PCP with HC1 and obtaining the spectrophotometric




curve of the solution from 400 to 200 nm as increments of HC1 were added.  To




calculate the concentration of the above forms at equilibrium, the absorbance




maxima at 219 nm was observed after the addition of 0.09 M HC1.   Assuming that




the concentration of the phenate anion is represented by the absorbance maximum




(A         at pH 12, then the quantity of phenol may be represented by




(A        - A   ) where A_,g is the absorbance at a lower pH.  The dissociation




constant is then calculated according to equation (1).




                            Ka  =        A319	             (!)







The pH was monitored with a Corning Model 12 pH meter with glass vs. calomel




electrodes, and spectral data was obtained with a Gary 17 spectrophotometer




utilizing 1-cm and 10-cm cells.,




Solubility in Buffered Solutions




     Since natural aquatic systems usually have some buffer capacity (i.e.




alkalinity), the study was expanded to determine the solubility of PCP in buf-




fered solutions at pH 2.2, 606, and 10.1.  The pH 2.2 buffer  solution was




prepared by mixing 0.1 M H PO. and 0.1 M KH-PO. until the desired pH was




obtained.  Buffer solutions at pH 606 were prepared from 0.1  f4 KH_PO. and 0.1




M NaOH, whereas pH 10.1 buffers were made from 0.1 M NaOH and 0.1 M H-BO,,.




     To determine absorption maxima in the ultra-violet  (u.v.), buffered




samples were prepared in pH 2.2 buffer for PCP and in pH 10.1 buffer for




sodium pentachlorophenate (SPCP).  Spectrophotometric curves  from 200 to 360 nm




were determined using a Bausch § Lomb Spectronic 710.




     Two methods were used to prepare PCP solutions for solubility studies.  In




the first, a quantity of PCP was weighed out; to this was added a known volume
                                      14

-------
of prepared buffer.  Each flask, including blanks and standard recoveries, was




then closed with an aluminum-foil covered stopper; wrapped with foil to exclude




light; and shaken for 18 hours or more at 120 rpm and 25-28°C on a New Brunswick




Scienctific Controlled Environment Incubator (New Brunswick, N.J.).




     In the second method, 0.1, N^NaOH was added to dissolve a known quantity




of PCP.  Acid was then added to the SPCP solution to bring the pH to the desired




level.  Flasks were then covered with aluminum foil and treated as in the first




method.




     Flasks were removed from the shaker, and aliquots transferred to glass




centrifuge tubes to be spun down in either a Model CL International Clinical




Centrifuge for 10 minutes or a Sorvall General Laboratory Centrifuge at 4700




rpm for 10 minutes.  Unwetted, floating PCP was removed from the solution sur-




face and sample aliquots were then taken from beneath the surface.




     Sample aliquots of 50 ml each were extracted using 125-ml separatory




funnels, and 1 ml aliquots were extracted in 15 x 150 mm test tubes using a




vortex mixer.  Sulfuric acid was added to each sample, where necessary, to




bring the pH to 2.  Samples were then extracted with two aliquots of hexane,




and the aqueous phase was discarded.  The combined hexane portions were then




washed with distilled water, and the water was discarded.  Then the hexane




phase was washed with two aliquots of 0.1 N_ NaOH and the hexane was set aside




as hexane-I.  The combined basic solutions were then acidified to pH 2 with




sulfuric acid and extracted with two aliquots of hexane.  These two aiiquots




were  combined and  set aside as hexane-II„




      For gas chromatographic analysis, samples containing phenols were




concentrated to about 5 ml under a stream of N  and then subjected  to methyl-




ation according to the method of Schlenk and Gellerman  (1960).  Samples were






                                      15

-------
allowed about 5 minutes to react and then were brought to an appropriate volume




for gas chromatographic analysis as described above for environmental samples.






ACCUMULATION AND ELIMINATION OF PCP IN FISH




     Six-month-old bluegill, Lepomis machrochirus, were obtained from the




Lyman Fish Hatchery, Lyman, Mississippi,  The fish were acclimated to laboratory




conditions for a two-week period, randomly divided into test groups of ten to




thirty in 30-liter glass aquaria and re-acclimated for 24 hours with no feeding




before initiating toxicity and exposure studies„




     The studies were performed as static bioassays in dechlorinated tap water.




Each aquaria was monitored at the beginning and end of each 24-hour period for




pH, temperature, conductivity, and dissolved oxygen.  The PCP content was mea-




sured in each aquarium after the initial 24-hour period to verify the desired




exposure level„  The test solutions were changed every 24 hours thereafter to




compensate for PCP loss by evaporation, adsorption, and decomposition,,  Control




aquaria were treated in the same manner, without PCP.




     Standard stock solutions of PCP were prepared by two procedures.  A PCP




standard was made by dissolving 1 g reagent grade PCP in 1 liter of acetone.




An  SPCP standard  (for sodium pentachlorophenate) was prepared by dissolving



1 g PCP in an aqueous NaOH solution at pH 12 and bringing the pH to 7.4 with




the addition of 0.1 M H PO..  All exposure studies were performed with the




PCP standard solution.




     Before  initiating exposure studies, the toxicity of PCP for L_^ machrochirus




was verified using  96-hour median  lethal concentration  (LC-50)  static bio-




assays  according  to the procedure  in Standard Methods  (American Public Health




Association,  1971).  Ten  fish were placed in each test  aquaria  and ten for




control„  Percent survival  was  observed at the end of each 24-hour period.





                                      16

-------
     Accumulation studies were performed in three replicate aquaria containing




thirty fish each along with a control aquaria.  The fish were exposed to a




sublethal concentration of 0.1 ppm PCP and two fish from each aquarium were




removed for analysis on day 1, 2, 4, 8, and 16 of the exposure period.  A 1-g




sample of muscle tissue and the combined gills, liver, and digestive tract




were analyzed for PCP content for each fish.  On days 4, 8, and 16, three




additional fish were killed for separate analysis of gills, liver, and digestive




tract.




     Elimination studies were initiated by placing fish exposed to 0.1 ppm PCP




in clean water, which was changed every 24 hours.  These studies were performed




in triplicate aquaria versus control for each of two groups of fish.  Group-I




fish (short-term exposure) were placed in clean water after 4 days exposure




and group-II fish (long-term exposure) were placed in clean water after 16




days exposure.




     Group-I fish were collected on day 1, 2, 4, 8, and 16 and the muscle and




combined gills, liver, and digestive tract were analyzed.  Group-II fish were




collected on day 2, 4, 8, and 16 for muscle and combined tissue analysis of




the muscle, gills, liver, and digestive tract„




     Fish Collected for PCP analysis were weighed and measured prior to dis-




section.  Tissues to be analyzed were weighed and placed in 30-ml vials.  The




PCP content was determined in a manner similar to that described above for




fish tissue analysis of environmental samples.




FOOD CHAIN STUDY




     Benthic collections were taken quarterly  at four stations during the




second year of  the project«  Collections  consisted of three  (15,5 cm  x 15.5  cm)




samples  from an Eckman dredge at each station.  Samples were placed in plastic






                                     17

-------
bags and packed in ice.  After returning to the laboratory, samples were fixed




in a ten percent formalin solution.  Organisms were separated from the substrate




by passing samples through a wire sieve (U.S. Standard No. 50).  Benthic



invertebrates were then separated from the strained material, identified and




volume determined.




     Fish analyzed in food habit studies were captured by both trawl and gill




net..  Immediately after capture fish were placed on ice and returned to the




laboratory.  Stomachs were removed and the species and length of fish recorded.




Stomachs were then placed in ten percent formalin until examination.  Food




items were identified in the same manner as the benthic samples.  Analysis of




the stomach contents includes the determination of the number, volume and




frequency of occurrence of each food item.
                                      18

-------
                                   SECTION 5




                            RESULTS AND DISCUSSION






ENVIRONMENTAL SAMPLES




     Low levels of PCP and PCP-degradation products were observed in the con-




trol pond samples (TABLE 1) exhibiting concentrations of 0.3 ppb in water, 3




ppb in sediment, 7 ppb in fish muscle, and 70 ppb in fish liver.  Reagent




blanks were well below the PCP concentration observed in control samples




indicating that a slight background concentration of PCP did exist in the




supposedly non-contaminated environment samples.  This background contamination




could be due to atmospheric transport of PCP from treatment sites.  It has




also been suggested (Arsenault, 1976), that a naturally occurring fungal




metabolite, p-methoxytetrachlorophenol could be mistaken for low levels of




PCP in some samples.




     Procedures utilized during the first year study provided the following




percent recoveries ± one standard deviation:  water, 90 ± 15; sediment, 90 ± 40;




fish, 62 ± 14 0  Second-year procedures provided the following extraction




efficiencies:  water, 95 ± 10; sediment 110 ± 25; fish, 90 + 8.




PCP Persistence and Distribution




     The investigation during the first year of sampling, concerned primarily




with the distribution and persistence of PCP in the lake, has been discussed




by Pierce et al. (1977) and will be summarized here in relation to the rest




of the study.  Within two months after the spill, PCP was uniformly distrib-




uted throughout the lake at a concentration of 10 ppb in February 1975





                                      19

-------
                       TABLE 1.  PCP AND PCP-DEGRADATION

                         PRODUCTS IN CONTROL SAMPLESOa
Sample
Waterb
Dissolved
Particulate
Sediment
PCP

003±001
001±0005
3.0±0_4
PCP-OCH3 2,3,5,6-TCP 2,3,4,5-TCP

<0001C O.liO.Ol <0001
<0.1 <0.1 <0.1
<0.1 1.010.2 <0.1
Fish6


   Muscle             7.0±3         <1             <1                 <1


   Liver             7000±40        <1             <1                 <1



Leaf Litter£          500±1          5.0±2          700±2              300±1



 Average of duplicate analyses ± % the range,,


 Concentrations reported as ug/liter0

£
 Lower limit of detection,,


 Concentrations reported as pg/kg air-dry sediment.


Concentrations reported as ug/kg wet-weight tissue,,

f
 Concentrations reported as yg/kg air-dry leaf  litter,,
(TABLE 2)o   The concentration decreased to background levels (<1 ppb) by


October 1975, increased again to about 15 ppb in February 1976, and steadily


declined through May 1976.  Pentachlorophenol associated with particulate


matter usually represented less than ten percent of the dissolved PCP (TABLE 2)


Water samples collected during the second year (TABLE 3) showed background



                                      20

-------
                 TABLE 2.   PCP CONCENTRATION IN WATER SAMPLES
                  COLLECTED FEBRUARY 1975 THROUGH MAY 1976.
Date Sample
Feb. 27, 1975
Dissolved
Particulate
Apr. 24, 1975
Dissolved
Particulate
June 28, 1975
Dissolved
Particulate
Aug. 5, 1975
Dissolved
Particulate
Oct. 11, 1975
Dissolved
Particulate
Dec. 6, 1975
Dissolved
Particulate
Feb. 7, 1976
Dissolved
May 3, 1976
Dissolved
1

9
0.2

11
3

13
2

N.A.
N.A.

10
2

76
5

29

18
2 3
Pg

11 6
0.4 0.

6 8
NaA0a 0.

8 2
0.2 1

N.A. 3
N.A. 0.

5 0.
0.3 <0.

25 1
0.4 <0.

N0A0 15

N.A. 2
Site
4
PCP/ liter

9
3 0.4

8
2 0.1

3
2

2
3 0,4

8 0.1
lb <0.1

2
I <0.1

10

N.A.
5 6

9 8
0.6 0.2

9 15
0.2 N.A.

2 82
0.2 0.4

3 1
0.2 N.A.

1.0 0.2
0.1 <0.1

2 N.A.
<0.1 N.A.

10 26

2 2
,N0A0 = Not Analyzed,
 Lower limit of detection.
                                      21

-------
levels in lake water in August and October 1976,  high concentrations in January

and February 1977, and decreasing somewhat,  yet still well above background in

April 1977.  Although suspended particulate matter contained less than ten

percent of the PCP in the water column throughout the study, it may be important

as a transport mechanism from the water column to sediment.
                   TABLE 3.  PCP IN WATER SAMPLES COLLECTED
                        AUGUST 1976 THROUGH APRIL 1977,
Date    Sample
       Site
B               C
   yg PCP/liter
Aug, 11, 1976
Dissolved3
Parti culate
Oct., 22, 1976
Dissolved
Part icu late
Jan, 5, 1977
Dissolved
Particulate
Feb. 22, 1977
Dissolved
Particulate
Apr. 27, 1977
Dissolved
Particulate

11.0±0.4
0,2

N,A.C
N.A,

82.0±32
0,4

146,0 7
0,18

16oO±0.4
0,33

0,1+0,02
0006

0,1+0,03
0,04

24,0±13
N.A,

N.A.
N.A.

5,0±0,5
0,29

0,110,03
0,05

0,2±0,05
0,04

25,0±7
0.2

29,0±2
0,14

5.0+0,7
0,35

0.1±0.
0,06

1,0±0,
0.2

16.0+6
0.2

N.A.
N.A.

5,0±0,
0,29

01


1








2

 wean  of  triplicate  analyses  ± sandard deviation.

 Composite  of  all  filter pads from three one-liter samples,
 Q
 N,A0  = Not Analyzed,
                                      22

-------
     Water quality parameters monitored for February 1975, through May 1976,




(TABLE A-l) show that the pH remained slightly acidic in the lake, generally




between pH 6.0 to 6.8 but was more acidic in the shallow stream (4.2 to 6.2).




Near-surface water was well oxygenated, except in the shallow stream when the




water was stationary and varied seasonally with temperature.  Total organic




carbon (TOC) remained fairly constant throughout the study period except for




anomolously low concentrations observed in April 1975.




     During the second year of the study, dissolved oxygen (D.O.)  and tempera-




ture were monitored near the surface and near the bottom at each site, but pH




was recorded for surface samples only (TABLE A-2).  Surface samples exhibited




conditions similar to the previous year, but the bottom samples revealed




anoxic conditions existing at the bottom of site C for the summer, fall, and




spring sample periods.




     Sediment samples retained PCP concentrations well above background




throughout the first year of the study  (TABLE 4).  The variability observed




among these samples may be attributed to the inefficiency of the sonication




extraction procedure, compounded by variation in the environmental samples.





The second-year sediment samples (TABLE 5) show that large concentrations of




PCP remained in sediments throughout the study period.




     Sediment contained high PCP concentrations in August and October 1976




(500 ppb average) and exhibited a slight decrease in January 1977 (200 ppb),




after the second fish kill, indicating a residence time of over a week in the




water column before incorporation into sediment.  Lake sediment showed an




increase near the mouth of the stream in February 1977 (1,500 ppb) but in




April 1977 the concentration returned to the January levels (250 ppb).
                                      23

-------
                TABLE 4»  PCP CONCENTRATION IN SEDIMENT SAMPLES
                 COLLECTED FEBRUARY 1975 THROUGH MAY 1976.a
Date
Feb.
Apr,
June
Aug.
Ont.
Dec,
Feb.
May

27, 1975
24, 1975
28, 1975
5, 1975
11, 1975
6, 1975
7, 1976
3} 1976
1
800
1,160
1,300
N.A,C
927
163
100
96
Site
2 345
yg PCP/kg air-dry sediment
lb 22
36 21
1 1.4
Nr,A0 10
471 48
900 11
N.A. 313
NoA. 20
26
98
583
205
91
97
10
N.A.
119
180
860
207
56
97
84
21
6
2
34
92
45
24
N.A.
81
7
o
 Composite of three grab samples„


 Lower limit of detection,.

£
 Not analyzed.




     Small fish collected by seine during the first year showed high whole-


body PCP concentrations in February (2,500 ppb dry-weight) and April 1975


(TABLE 6),  The concentration was diminished yet still above background in


June 1975, increased some in December 1975 and February 1976, and then decreased


again to background by May 1976 (TABLE 6).  Improved sampling and analytical


procedures used for the second year of the study provided a more complete


description of the accumulation of PCP in fish.  These results (TABLE 7) show


that fish contained only background levels of PCP in October 1976 but rapidly


accumulated very high concentrations in January 1977 immediately after the


                                      24

-------
                 TABLE 5.  PCP  IN SEDIMENT SAMPLES COLLECTED
                      AUGUST  1976 THROUGH APRIL  1977.

Date A

Augo 11, 1976 857±57
Oct. 22, 1976 166+38
Jan. 5, 1977 277153
Feb. 22, 1977 N.A0b
Apr, 27, 1977 4+1
0
Average of duplicate analyses 1
Not analyzed.
TABLE 60
FEBRUARY
Collection Date
Feb. 27, 1975
Apr, 24, 1975
June 23, 1975
Oct. 11, 1975
Deco 6, 1975
Feb. 2, 1976
May 3, 1976
Site
B C a D
ug/kg air-dry sediment
429+169 520+151 142144
9941394 389+12 212+8
239175 150±13 170178
1, 518187 NoAo N.A.
250114 238+3 132121
^ range0

PCP IN FISH COLLECTED
1975 THROUGH MAY 1976.
ng PCP/g air-
dry fish tissue
2,500+200
1,380120
130+70
<50b
651+650
87122
<50
Average of replicate analyses 1 % the range.
Lower limit of detection.
                                     25

-------
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-------
spill.  Concentrations decreased somewhat by April 1977 but were still well

above background levels.  Bass collected freshly dead or dying in January 1977

shortly after the spill, contained PCP in concentration of 2,100,000 ppb in

bile; 230,000 ppb in liver tissue; 42,000 ppb in gills; and 13,000 ppb in

muscle.  These values represent concentration factors over the PCP content in

water of 500 for muscle; 1,500 for gills; 8,000 for liver; and 80,000 for bile.

     Leaf litter collected near the spill site contained very high concentrations

of PCP throughout the investigation (TABLE 8).  The variability observed between

sampling dates probably reflects the heterogeneous nature of the collection

area, but the large concentrations observed overall indicate that contaminated


                          TABLE 8.  PCP IN LEAF LITTER.
                     Date
         PCP
ng/g air-dry leavesc
                 Feb. 27, 1975

                 Apr. 24, 1975

                 June 23, 1975

                 Aug. 11, 1975

                 Dec. 6, 1975

                 Feb. 10, 1976

                 May 3, 1976

                 Aug. 11, 1976

                 Oct. 22, 1976

                 Jan. 5, 1977

                 Apr. 27, 1977
     6,4001250

     2,5501650

     5,2001300

     5,800+1,200

     3,470

     1,680+12

     6,00011,000

    10,300+1,000

     3,1491380

    15,900+180

     2,9701800
  Average of duplicate analyses 1 % the range.
                                      27

-------
leaf litter provided a potential for long-term pollution of the aquatic




ecosystem.




PGP Degradation Products




     Since the source of PCP contamination was the oil and water from the




industrial waste water holding pond, samples of oil and water from the pond




and oil from the surface of the stream near the spill site were collected and




analyzed for PCP and PCP-degradation products.  The results (TABLE 9) show that




the PCP concentration was 617,000 ppb in the oil slick from the stream;




220,000 ppb in holding pond oil; and 8,700 ppb in holding pond water.  The




major degradation products observed in the oil slick were the 2,3,4,5- and




2,3,5,6-TCP isomers, each approximately 13% of the PCP concentrate (TABLE 9)=




These percentages far exceeded the percent TCP observed in a sample of technical




grade PCP  (1 to 2%) suggesting that both isomers of TCP were formed from PCP in




the oil solution, probably by photodegradation as suggested by Crosby  (1972).




     The major degradation products observed in the contaminated lake were




pentachloroanisole  (PCP-OCH ) and the two isomers of TCP.  Varying quantities




of the methyl ether (anisole) of both TCP isomers were also observed but




proved difficult to quantitate, due to low concentrations and interference




from naturally occurring substances.  The 2,3,4,6-TCP isomer was not observed




but may have been present in small quantities.  Trichlorophenol eluted with the




solvent front under the chromatographic conditions used, thus its concentration




was not determined.  The presence of chloranil, PCDD, and PCDF were  indicated




in sediment and holding pond oil samples in ug/kg quantities, utilizing the




procedure  described by Buser  (1975), but our analytical system did not provide




adequate  quantitation.  The gas chromatographic retention of the methylated




TCP isomers relative to methylated PCP was observed to be 0.5 for 2,3,5,6-TCP






                                      28

-------
             TABLE 9.  PCP AND DEGRADATION PRODUCTS IN TECHNICAL GRADE

             PCP, INDUSTRY WASTE-HOLDING POND AND OIL SLICK FROM STREAM.
                                   PCPa	2,3,5,6-TCPb	2,5,4,5-TCPb
Technical-Grade PCP Solution       1,000          1.2%               <0001%



Holding Pond
Oil Slick
Water
Stream Oil Slick6
220,000
8,700
617,000
13%
9%
12%
N.A.
N.A.
13%
ang PCP/ml solution (ppb).


 Reported as percentage relative to PCP concentration.

Q
 Not analyzed.


 Collected from industrial  waste holding pond, September 8, 1975.

g
 Colelcted from spill area, December 18, 1974.
and 0.80 for 2,3,4,5-TCP on 3% SP-2100, and  0.46  for  2,3,5,6-TCP  and 1.21  for


2,3,4,5-TCP on 10% SP-1000o  The relative response  factor  for  peak  height  was


1.0 for 2,3,5,6-TCP and 0.25 for 2,3,4,5-TCP on 3%  SP-2100;  and  1.5 for 2,3,5,6-


TCP and 0.25 for 2,3,4,5-TCP on 10% SP-1000.


     Degradation products in control pond samples are given  in TABLE 1.  The


concentrations were found to be essentially  at reagent blank lavels in all


samples except leaf litter, which exhibited  background levels  of  all products


in the 3-7 ug/kg range.
                                      29

-------
     The concentration of degradation products dissolved in the water column



are shown in TABLE 10.  The PCP-OCH_ remained at background levels throughout,



reflecting the low solubility in water.  The 2,3,5,6-TCP was below background



in August and October, but increased to almost 1 ppb in January 1977 and re-



mained above background through April 1977.  The 2,3,4,5-TCP isomer remained



below or near background throughout the sampling period.



     Sediment retained high concentrations of all the degradation products



throughout the August 1976 through April 1977 study period (TABLE 11).  The



TCP isomers were both more concentrated than PCP-OCH  from August through
                                                    o


February, but the latter increased in April.  This observation, along with



the absence of PCP-OCH3 in technical PCP or the oil slick suggests that PCP-



OCH  was formed in the aquatic environment, probably by microbial action on



PCP as reported by Cserjesi and Johnson  (1972).  The changes in TCP con-



centration followed  a pattern similar to that for PCP, suggesting that TCP



was formed before it reached the sedimentary environment„
               TABLE  10.   PCP-DEGRADATION  PRODUCTS  IN LAKE WATER

        (DISSOLVED) SAMPLES  COLLECTED AUGUST   1976  THROUGH APRIL   1977.
Date
Aug.
Oct.
Jan.
Feb.
Apr.
PCP-OCH
•J
11,
22,
5,
22,
27,
1976
1976
1977
1977
1977
0.
0.
0.
0.
0.
06±0
04±0
08±0
07±0
03±0
.01
.01
.02
.03
.01
2,3
ug
0.
Oo
0.
0.
0.
,5,6-TCP
PCP/liter
08±0.02
06±0.02
9+0.1
3±0.02
9±0.1
2,
0
0
0
0
0
3,4,5-TCP
005±0
.03+0
.07±0
.05±0
.3±0.
.04
.01
.02
.02
1
aAverage of sites B,  C, and D ± standard deviation,
                                      30

-------
               TABLE  11.   PCP-DEGRADATION  PRODUCTS  IN LAKE SEDIMENT
                   COLLECTED AUGUST   1976  THROUGH APRIL   1977.
Date
Aug.
Oct.
Jan.
Feb.
Apr.
PCP-OCH3a
ug
11,
22,
5,
22,
27,
1976
1976
1977
1977
1977
18.
6.
16.
1.
60.
0±5
0±6
Oil
5±0.2
0±20
2,3,5,6-TCPa 2,3,4,5-TCPb
PCP/kg air-dried sediment
120±60
62±5
50±20
340115
53±25
129
63
24
N.A.C
15+3
 o
 Average  o£ values  for  sites  B,  C,  and  D  ±  standard  deviation.


 Site B only.

 c
 N.A. = not analyzed.
     The concentrations of PCP-degradation products in various fish tissues


are shown in TABLE 12 for samples collected in August and October 1976, and


in TABLE 13 for fish collected in January and April 1977.  Fish collected in


August and October contained low concentrations.  Samples collected in January


1977, shortly after the second fish kill, showed very high concentrations

indicating that fish rapidly accumulated all products from the environment.


The TCP isomers were found in increasing concentration in muscle, gills, liver,


and bile, in the same manner as was observed for PCP.  The PCP-OCH  was general-


ly less concentrated than TCP and showed a marked reduction in bile, probably


as a result of the insolubility in aqueous solution.  The high concentration


of PCP-OCH_ in fish obtained from water containing very  low concentrations


indicates a very high partition coefficient for PCP-OCH  from water to fish.


It is also possible that the fish received some of the PCP-OCH  in their diet.


                                      31

-------
The persistence of PCP and PCP-degradation products observed in fish indicate

that the fish were exposed to high levels over an extended period of time and

that the toxic chemicals were not rapidly eliminated but were retained, perhaps

in a conjugated form, as reported by Kobayashi, et a!0 (1976).
                  TABLE 12.  PCP-DEGRADATION PRODUCTS IN FISH
                      COLLECTED AUGUST AND OCTOBER  1976.
Fish
        (No.)
                  Size
                   cm
  PCP-OCH3       2,3,5,6-TCP       2 3,4,5-TCP
 	ng PCP/g wet-weight tissue	
Sunfish   (2)
                   5-10
                     muscle
                     i •    b
                     liver
August 11, 1976


    41±20
   600
                                                     5±2
                                                    92
                                                                     130
                               October 22, 1976
Sunfish (2)


Catfish (2)


Sucker (1)
12-15
muscle 3±1 <1
liver 11±1 40±10
25-26
muscle <1 1±0.6
liver 17+5 50±15
20
muscle N.A. <1
liverb 30 260

<1
5±1

<1
150±100
285
 Average of replicate samples ± % the range.

 Analysis of single, composite sample.
 'Lower limit of detection.
 Not analyzed.
                                      32

-------
                  TABLE 13.   PCP-DEGRADATION PRODUCTS IN
                  FISH COLLECTED JANUARY AND APRIL  1977.
Fish (No.)

Sunfish6 (2)



e
Bass (3)




Catfish6 (1)


Suckerf (1)




f
Sunfish (2)


£
Catfish (2)



Size
cm

15-20
muscle
gills*
liver

36-44
muscle
gills
liver
bile
25 b
muscle
liver
22
muscle
gills'
liver


14-20
muscle
liver

40
muscle
liver
bile
PCP-OCH3
January 6,

60130
230
560


170 80
60+8
600+200
208±8

164
1,200

84
90
490
April 27,


29±1
155±35


140±35
350+200
210+20
2,3,5,6-TCP
ng PCP/g wet-weight
1977

75±15
360
950


230 96
335±35
5,600+2,000
114,000±10,000

219
8,500

45
450
11,360
1977


20±2
200±50


60±20
720±60
1,000±500
2.3,4,5-TCP
tissue

/•»

-------
     Since leaf litter contained very high concentrations of PCP,  some of the




minor degradation products (i.e., TCP-OCH )  were observed which were not dis-




tinguishable in other environmental samples.  The large concentration of the




anisoles of PCP and both TCP isomers (TABLE  14) throughout the study period




indicates that the process by which anisoles are formed occurred within the




dried grass and leaf litter along the banks  of the stream0  The persistence of




all products throughout the study period showed that the leaf litter was a




source for continuous environmental pollution.






PCP RELEASE FROM CONTAMINATED LEAF LITTER




     This experiment was devised to determine the extent to which contaminated




leaf litter might release PCP to the water,  thus providing a source for con-




tinuous pollution of the aquatic ecosystem.   The results (TABLE 15) show that




approximately ten percent of the PCP in the leaf litter was leached out over




each 24-hour peiod of shaking in water.  The original concentration of PCP




in the leaf litter was 6.4 Mg/g and that in the water after equilibrium




was about 0.5 yg/g.  Since the reported solubility of PCP in water is 15 ppm




(Bevenue and Beckman, 1967), solubility would not have been a limiting factor.




A mass balance  (TABLE 15) shows that all of the PCP was accounted for in the



experiment.




     These data indicate that PCP associated with leaf litter and vegetation




along the bank of a stream would be released slowly over a period of time.




Therefore, contaminated leaf litter serves as a source for chronic PCP contami-




nation of the aquatic environment.  This finding is supported by the persistence




of PCP in leaf  litter throughout the study.
                                      34

-------












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35

-------
             TABLE 15.   PCP RELEASE FROM CONTAMINATED LEAF LITTER
Sample
1
2
3
Average
Original
Day 1
0.9
0,6
0,3
0,6
leaf litter
Water
Day 2 Day 3
mg PCP /liter
003 0,3
0.3 0.2
0.8 1.1
0.5 0,5
sample
Leaf Residue
mg PCP/k?
4.9
3,9
5.9
408

Total
6.2
5oO
8.1
6,4±1
6.4±0,3
SOLUBILITY OF PCP IN WATER




     The solubility of PCP in unbuffered, distilled water was found to be in




the range of 10 to 14 mg/1 (ppm) at 23°C with a resulting pH of 5.1.  These




values are similar to those (14-19 mg/1 in water) reported by Bevenue and



Beckman C1967).  Curves representing the titration of a solution of 9.2 ppm




PCP in distilled water with 0,09 M HC1 along with the back titration of the




acidified solution with 0<,1 M NaOH are shown in Figure 3.  Concentrations of




the phenate and phenol forms calculated for various pH values are given in




TABLE 16 along with the pKa values which were found to be an average of 4.5.




     The fact that the curves in Figure 3 are not congruent indicates that a




nonreversible process occurred upond acidification of PCP and that  the solu-




bility of PCP was suppressed.  This nonreversible process could result from




difficulty in dissolving  and dissociating the solid phenol before equilibrium




could be attained.





                                      36

-------
           TABLE  16.  PCP DISSOCIATION  IN WATER AT VARIOUS pH LEVELS
A" a
0,77
0.716
0.605
0.514
Oo444
0.390
HA
1.08
Iol34
1,245
1.34
1.41
1.46
pH
5.06
4.61
4.32
4.41
3.40
3.39
pKa
5.17
4.80
4.63
4.30
4.50
4.46
  Phenate  concentration  (dissociated form).


  Phenol concentration (undissociated  form),

 £
  pKa  calculated from equation  (1), p.  14.
     Ultraviolet scans of PCP and SPCP in buffer solutions are presented in

Figure 4 and summarized in TABLE 17.  The absorbance maxima for SPCP agree

with the maxima (218.5, 248, and 319 nm) presented in Sadtler (1972), although

conditions of analysis, such as pH or ionic strength, were not indicated in

Sadtler.  However, the molar absorptivities calculated from Sadtler  (218.5 nm,

1.3 x 106; 248 nm, 4.4 x lO4; 319 nm, 2.7 x lO1*) are much higher than those in

TABLE 1.  Without a description of conditions under which the Sadtler data

were obtained, it is not possible to speculate on the causes of these dif-

ferences.  The molar absorptivity of pentachlorophenate ion at 319 nm agrees


well with that reported above from the data for distilled water.

     Absorbance was linear with concentration in the mg/1 range at 320 nm for

SPCP in 0.1 M borate buffer at pH 10.1 and in 0.1 M phosphate buffer at pH 6.6.


                                      37

-------
For PCP, absorbance was also linear at pH 2.2 at 2.4 nm in 0.1  M phosphate
buffer.
     A preliminary study indicated that solubility, as determined by adding
prepared buffer to known amounts of PCP, was complete within one day.  All
subsequent samples were shaken overnight before centrifugation  and analysis.
                                    A Titration of PCP with 0.09 M HC1
                                    O Back titration with 0.1 M NaOH
                0    10    20    30   40   50  60    70   80  90  100  110  120  130
                                           ul HC1
               140   130   120  110   100   90  80    70   60  50   40   30   20   10
                                           ul NaOH
 Figure 3.   Titration of PCP  in aqueous solution.
                                      38

-------
     All samples analyzed by gas chromatography were prepared by adding



buffer solutions to known quantities of crystalline PCP.  This method was



plagued by PCP crystals floating on the surface tension of the solution.



Transfer of floating PCP during sample preparation of sample aliquots for


extraction may account for at least part of the great variability (i.e.,



large standard deviations) in solubilities determined by this method (TABLE 18)
   w
   ca
   oi
   o
                219
                    SPCP
         200   220   240   260   280   300   320


                               WAVELENGTH (nm)
340   360   380
     Figure 4.  Ultraviolet spectra of pentachlorophenol (PCP) and sodium-

     pentachlorophenate (SPCP) in 0.1 M buffer.
                                     39

-------
        TABLE 17.   SPECTROPHOTOMETRIC  CHARACTERISTICS  IN THE  ULTRAVIOLET
               OF  PENTACHLOROPHENOL AND  SODIUM PENTACHLOROPHENATE
                                IN  0.1 M BUFFER
    X max(nm->                                    Molar Absorptivity
 Pentachlorophenol

      214                                            7.5  x  104

      229 (shoulder)                                  1.7  x  104
 Sodium Pentachlorophenate

      219                                            4.6  x 104

      249                                            1.0  x 104

      320                                            5.0  x 103
Another factor contributing to this variability could be dilution errors,

especially in light of the fact that samples had to be diluted as much as

250,000-500,000 times to get them within the working range of the instrument.

     At the dilutions needed to use the gas chromatograph, there were no

evidences of contaminants in either the hexane-I fraction or the hexane-II

fraction prior to methylation0  Blanks at pH 2.2 and 6.6 were less than 10 ug/1,

and at pH  10.1 less  than  200 yg/1.  Recoveries  ranged from 80%  to  130%.

     Samples analyzed by  absorption in  the  u.v. were prepared by dissolving

PCP in base and acidifying  the SPCP solutions to the desired pH.   With  this

method,  the problem  of  PCP  floating on  the  surface  tension was  considerably

reduced,  although  not entirely eliminated.  The higher  values for  solubilities

at pH  2.2  and  6«6  (TABLE  18)  for  spectrophotometry  compared with gas  chroma-

tography may indicate that  true saturation  had  not  been achieved in  samples

                                      40

-------
analyzed by gas chromatography.  Another possibility is that the high dilution

ratios needed for samples prepared for gas chromatography consistently

produced lower concentrations than samples analyzed spectrophotometrically;

for example, pH 10.1 samples were diluted at most only 1000 times before

spectrophometric analysis.,  Or, the difference may indicate that samples

analyzed spectrophotometrically were supersaturated, although this possiblity

seems remote since there were copious amounts of PCP and SPCP precipitated

in the pH 2.2 and 6.6 sample flasks.  A further check on this question is

needed.  In the case of pH 10»1, reproducibility within individual experiments

was fairly good, but reproducibility between runs was poor.  Apparently, PCP

at high pH's readily forms SPCP by reacting with the NaOH in the buffer.  Thus,

a crude titration was effected by adding PCP to a 0.1 M NaOH-H_B03 buffer.

Evidences of this titration effect were found in the marked drops in pH, to as

low as 8.5, in solutions of 0.1 M basic buffer to which PCP had been added in

what was thought initially to be excess.  As a rough estimate from data devel-

oped in this study, it seems possible that the solubility of SPCP at pH 10.1
            TABLE  18.   SOLUBILITY AT  26 C OF PENTACHLOROPHENOL AND
                SODIUM PENTACHLOROPHENATE AT THREE pH VALUES
                        USING TWO ANALYTICAL METHODS
pH mg
Determination by
Gas Chromatography
2.2 300±200
6.6 550 ±240
10.1 17,400 ±800
PCP/litera
Determination by
Spectrophotometry
7.2
660
11.900 ±900
  o
  ±  one  standard  deviation.

-------
exceeds 0.05 M»  A more valid estimate could be obtained using 1 M buffer;




however, such a concentrated buffer is outside the realm of what can be found




in all but the most extraordinary aquatic environments.  Thus, it is perhaps




best, albeit vague, to say that SPCP is freely soluble at pH 10.1.




     The pKa of PCP is variously reported to be 4.8 (Blackman et al., 1955),




4.82 (Robinson and Bates, 1966), 502 (Dyer,  1959), 5.26 (Tiessens, 1929),  and




5.3 (Griffith et a!0,  1938)  and 4.5 (above)  for distilled water.  Even allowing




for the variation in reported pKa values, all PCP in solution at pH 2,5 or less




is present in the acidic, non-dissociated form.  Taking the solubility of PCP




at pH 2.2 to be 5,3 mg/1 (TABLE 18), one can calculate a Ksp for PCP ranging




from 1.0 x 10~10 (for pKa = 5»3) to 6.3 x 10~10 (for pKa = 4.5).






ACCUMULATION AND ELIMINATION OF PCP IN FISH




     These results have been reported previously by Pruitt et al. (1977),  and




are summarized here.




     The 96-hour LC-50 value for the PCP Standard was 0.26 ± 0.01 mg/1 and




that for the SPCP Standard was 0.33 ± 0.01 mg/1 (TABLE 19).  These values agree




with those reported for various aquatic organisms by Goodnight  (1942) , Holmbert




et al.  (1972), and Cardwell et al.  (1976).  The pH of the test solutions




ranged  from 7.2 to 7.7, indicating  that the active form of either standard




was the phenate anion.




     Exposure of six-month old bluegill sunfish (Lepomis macrochirus) to a




sublethal concentration of PCP  (0.1 mg/1) resulted in the accumulation of PCP in




various tissues.  The liver was found to concentrate the largest amount (35,000




ng/g) followed by the digestive tract (21,000 ng/g), gills  (6,000 ng/g), and
                                      42

-------
               TABLE 19.  LC-50 OF PCP TO LEPOMIS MACROCHIRUS.


Time
(hours)
24
48
72
96
PCP LC'5°a SPCP
mg/liter
0.42 ± .02 0.33
0.32 ± .02 0.32 ± .02
0.28 ± .03 0.35 ± .01
0.26 ± 0.1 0.33 ± .01
aAverage of three replicate samples ± one-half the range.



muscle  (1,000 ng/g)  (TABLE 20).  Pentachlorophenol was rapidly accumulated by

all tissues with equilibrium apparently being established by day 8 (Figure 5).

     The efficiency of the extraction procedure was determined to be 93 percent

with a  standard deviation of 6 percent by the addition of standard PCP to fish


                 TABLE 20.   ACCUMULATION OF PCP IN FISH TISSUE
                     AFTER  EXPOSURE TO 0.1  mg PCP/1 WATER.
Tissue
Muscle
Gills
Digestive
Tract
Liver
4
0.5±0.1
2.6+0.5
9 ±2
35 ±20
Days
yg PCP/g wet
1.
6
21
25
ft
Exposure
8
weight tissue
3+0.2
±2
±4
±20
16
0.4±002
5 ±3
13 ±5
23 ±13
Q
 Average of triplicate samples ± standard deviation.


                                      43

-------
tissue and subjecting these "spiked" tissues to the extraction procedures in

six replicate analyses.  Reagent blanks were obtained by subjecting control

fish from PCP-free water to the above extraction and analysis procedure and

the PCP content was less than 0.01 ppm in all control samples.

     The elimination of PCP from muscle and combined gills, liver, and intesti-

nal tract from Group I fish (4 days exposure) is shown in Figure 6.  Similar

data for fish from Group II (16 days exposure) are shown in Figure 7.  The

elimination of PCP from the individual organ tissues from Group II fish is

shown in TABLE 21.

               16
                      Q  Combined  tissues

                      O  Muscle tissue
   Figure  5.
                                2         4
                                Days  of Exposure
Accumulation of PCP in tissue during exposure to 0.1 ppm PCP.
Average of six replicate samples ± standard deviation.
                                      44

-------
     A comparison of Group I with Group II elimination data (Figures 6 and 7)


reveals a lag period of 4 days in Group I that was not observed in Group II,


indicating that it took the fish about 8 days to develop a mechanisms for PCP


elimination.  This supports the results of the accumulation study which showed


a leveling off and apparent decrease in PCP concentration in tissue after 8


days of continued exposure, possibly representing the time necessary for the


fish to develop an enzyme system capable of eliminating PCP.  Kobayashi and
            bo

            t»
            Cu
            u
            CL,
                3 •
                2 •
                                              D  Combined tissue


                                              O  Muscle tissue
Figure 6.
                                2        4         8        16

                            Days of Elimination - Group I
Elimination of PCP from Group I (after 4 days exposure)
of six replicate samples ± standard deviation.
Average
                                     45

-------
Akitake (1975) reported that loss of PCP in goldfish (Carassius auratus) was



caused by the metabolic transformation of PCP to pentachlorophenylsulfate.



This was identical to the conjugate form found in the shortnecked clam by



Kobayashi et al. (1970).  It has also been reported that fish dispose of such



lipid-soluble substances by passive diffusion through the gills (Brodie et al.,



1962).
                           (8.1)
             W)



             I?
             a,
             u
                 2  -
                                             O Combined tissue



                                             O Muscle tissue
                                2          4         8          16


                          Days  of  Elimination -  Group  II




Figure 7.  Elimination of PCP from Group II  (after 16 days exposure)

           of six replicate samples ± standard deviation.
Average
                                      46

-------
               TABLE 21o  ELIMINATION OF PCP FROM GROUP II FISH,
                   PLACED INTO A CLEAN ENVIRONMENT AFTER
               SIXTEEN DAYS EXPOSURE TO PCP-CONTAMINATED WATER.
Tissue
Muscle
Gills
Digestive Tract
Liver
4
0.06±0002
0.16±0007
2 ±0.9
0.7 ±005
r\
Days Exposure
8
yg PCP/g wet weight tissue
0.03±0.01
0.13±0.09
0,3 ±0.1
4 ±5
16
0.03+0.01
0.08±0003
0.13±0.02
0.6 ±0.5
o
 Average of triplicate samples ± standard deviation.
     After 16 days of elimination in PCP-free water, the fish still contained

PCP residues (TABLE 21).  The liver contained the greatest amount (600 ng/g)

followed by the digestive tract (130 ng/g), gills (80 ng/g), and muscle (30

ng/g)•   By the end of the 16-day elimination study, both Group I fish and

Group II fish had eliminated PCP to about the same level (Figures 6 and 7).

Thus, after the initial 8-day lag period, the fish were able to eliminate PCP

to the same degree regardless of exposure time, yet a longer period would be

required for complete depuration.


FOOD CHAIN STUDY

Benthic Organisms

     Station A, nearest the spill area, was represented by a slow stream

environment with a bottom chracterized by gravel, coarse sand, and sediment.

However, stations B, C, and D were lentic habitats characterized by soft, silty,

clay substrates.  Benthic invertebrates at all four stations were dominated by

                                      47

-------
the larvae of the two insect families,  Chironomidae and Culicidae,  and




Oligochaeta (TABLE 22 and TABLE 23).




     Chironomid larvae appeared as the  dominant benthic organisms within inter-




mediate depths of the lake (stations  B  and D).   The dominant chironomid




collected was the genus Chironomus.   Other genera present were Harnischia,




Coelotanypus, and Tanypus.  Chironomids were least abundant both near the spill




area and in the deepest area of the lake.  Undesirable sediment at station A




in August and low oxygen levels produced by thermal stratification during




August and April at station C may have  affected chironomid abundance„




     Culicidae, exclusively Chaoborus,  present in consistent numbers within




the intermediate depths of the lake but were most abundant at the deepest




station, C.  Due to its tolerance to low levels of oxygen, Chaoborus was the




only benthic invertebrate collected at  station C during August.  Numerically,




Chaoborus larvae were dominant at station C throughout the study.  Oligochates,




primarily tubeficidae, were common only at station B in the upper region of




the lake, nearest the head waters.




     Diversity of the benthos appeared low throughout the lake.  Little seasonal




change in the composition of the benthos within each station was observed.




     Following the pentachlorophenol spill occurring in December 1976, no




organisms were observed in the sample collected from station A nearest the




spill area.  Absence of organisms may be attributed to the dry conditions pre-




ceding the sampling period.  Although an unusually large number of chironomid




head capsules were collected at station B, its benthic composition following




the spill did not appear  adversely altered.  Subsequent collections in April




1977 did not reflect a numerical decrease among the dominant invertebrates




present.






                                      48

-------
                    TABLE 22.  BENTHIC ORGANISMS COLLECTED
                       DURING AUGUST AND OCTOBER  1976.
Organisms
    Stations
B              C
Diptera
Chironomidae
                                    August
L"
Pd
Culicidae
Chaoborus L
Ceratopogonidae L
Oligocheata
Nematoda
Gastropoda

Chironomidae
L
P
Chaoborus
L
P
Oligocheata
Nematoda
Copepoda
15 290
5

87
1
30 87
1
1
October

62


222

72
1

204
6

787 90
1
2




8 215
3

1350 359
12 1

11
2
 Total number of organisms<• from three (15.5 cm x 15.5 cm) Eckman dredge samples.
 Stream was dry in October.
 Larvae.
 Pupae.
                                      49

-------
                    TABLE 23.   BENTHIC ORGANISMS COLLECTED
                       DURING  JANUARY AND APRIL  1977.a
                                                Stations
Organisms
Chironomidae
  Lc
  Pd
Ceratopogonidae L
Cuclicidae
Chaoborus L
Oligocheata
                                    January
                                             65

                                              1
                                            170

                                            132
                                     April
  56
   1

3024
158

  1
286
Chironomidae
L
P
Chaoborus
L
P
Ceratopogonidae L
Dytiscidae L
Nematoda
Oligocheata

379
2

15
2
1
1
1
4

271
1

298 238
6 15
1 3

2 4
1
       number of organisms from three  (15.5 cm x  15.5 cm) Eckman dredge  samples,
 No invertegrates were observed at site A.
 "Larvae.
 Pupae.
                                       50

-------
Food Habits




     Results indicate that small sunfish (Lepomis spp.) and intermediate sized




bluegill (L_._ macrochirus) fed predominantly on small bottom organisms, primarily




chironomid larvae (TABLE 24).  Benthic oraganisms together consitute 77.3% of




the diet of the smaller sunfish (<50 mm) collected.  Larger sunfish also




appeared to utilize benthic prey, largely in the form of chironomid larvae.




In addition to insect larvae, larger warmouth (JU_ gulosus) also utilized smaller




fish as foods




     Larger game fish, collected with the aid of a gill net were observed to




feed on fewer numbers of larger food items (TABLE 25).  Crayfish constituted




the bulk of the observed channel catfish (Ictalurus punctatus) ration, however,




large numbers of chironomid larvae and the presence of a smaller fish within




the stomachs suggests a diverse dieto  The black bullhead  (!„ melas) and yellow




bullhead (I0 natal is) appeared to feed on a wide range of  food items indicated




by both insect larvae, vegetation, and fish scales found in the gut.




     Rough fish, golden shiner  (Notemigonus crysoleucas) and  sharpfin chub-




sucker  (Erimyzon tenuis), appeared to be grazers with their respective rations




consisting primarily of filamentous algae and microcrustaceans (TABLE 26).




     Among the three dominant benthic groups, chironomid larvae, Chaoborus




larvae, and Oligochaetes, chironomids appeared as the most utilized food  source




by fishes„  Although chironomid  larvae were represented in the stomachs of




most fish  species, they comprised the dominant food  source of small and inter-




mediate length sunfish  (Lepomis  spp.)0  Larger sunfish, particularly warmouth




(L, gulosus) and green sunfish  (L. cyanellus), also  appeared  to prey on smaller




fish (Calhoun, 1966)„  Although no largemouth bass  (Micropterus salmoides) were




collected  with identifiable  stomach contents, Snow  (1971)  and Bennett  (1962)







                                     51

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contend that fish and larger invertebrates constitute the major portion of




their diet.




     The black bullhead (Ictalurus melas), yellow bullhead (I0  natalis) and




channel catfish (I0 punctatus)  appeared as omnivorous feeders in which much




of their ration was also derived either directly or indirectly from the benthos.




Bullheads appeared to feed on both aquatic dipteran larvae and smaller fishes




with aquatic vegetation also utilized by black bullhead.  Crayfish appeared to




constitute the bulk of the channel catfish ration with chrionomid larvae and




smaller fish also present.




     Both non-game species collected, golden shiner (Notemigonous crysoleucas)




and sharpfin chubsucker (Erimyzon tenuis)  appeared as discriminant grazers




upon non-benthic bood items.  Filamentous algae appeared to constitute the




major component of the larger golden shiner ration with chironomid larvae




representing a minor portion.  Sharpfin chubsucker appeared to graze primarily




upon microcrustaceans with chironomid larvae also constituting a secondary




importance.




     In general it appears that the basis of the food chain within Country




Club Estates Lake is channeled through the benthic invertebrate community,




particulary in regard to game fish species,  The benthic food source is of




immediate significance to the younger components of both the sunfish and




catfish populations  (Calhoun, 1966)0  Smaller sunfish in turn furnish forage to




larger predaceous game species (i<>e., larger sunfish, largemouth bass, catfish).




Non-game species appear less dependent upond a benthic food source, utilizing




prey items suspended in the water column.
                                      55

-------
                                    REFERENCES
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 2.   Arsenault, R.  D.   Pentachlorophenol  and  Contained Chlorinated Dibenzo-
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 3.   Bennett,  G.  W.  Management of Artifial Lakes and Ponds„   Reinhold Pub-
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 40   Bevenue,  A.,  and  H. Beckman.   Pentachlorophenol:  A Discussion of Its
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 50   Blackman, G.  E.,  M. H. Parker,  and  G. Carton,   The  Physiological  Activity
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 6.   Brodie, B. B.  and R. P. Maickel.  Mode of Action of Drugs0  Proco Inst.
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 7.   Buhler, D. R0, M. E. Rasmusson,  and H. S. Nakave.   Occurrence of  Hexachlo-
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 8.   Buser,  H. R.   Analysis of Polychlorinated dibenzo-p-dioxins and Dibenzo-
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 9.   Buser,  H. R.   High-Resolution Gas Chromatography of Polychlorinated Dibenzo-
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12.   Cote,  Ro  P,   A Literature Review of the  Toxicity of Pentachlorophenol  and
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                                      56

-------
13.   Crosby,  D.  G.   Photodegradation of Pesticides in Water.   Amer.  Chem.  Soc.,
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14.   Crosby,  D.  G.,  K0  W0  Moilanen, and A0  S0 Wong.  Environmental Generation
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15.   Crosby,  D.  G,,  and A. So  Wong.  Photochemical Generation of Chlorinated
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17.   Cserjesi, A. J.,  and E. L. Johnson.  Methylation of Pentachlorophenol by
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17(a)Dougherty,  R.C.,  and K. Pitrowska.  Screening by Negative Chemical loni-
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18.   Dyer, D. L.  The Effect of pH on Solubilization of Weak Acids and Bases.
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19.   Goodnight,  C. J.   Toxicity of Solium Pentachlorophenate and Pentachloro-
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20.   Griffith, R. ()„,  A. McKeown, and W. J. Shutt.  Annual Tables of Constants
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22.   Kirsch, E.  J. and J. E. Etzel.  Microbial Decomposition of PCP.  Journal
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23.   Kobayashi,  K.,  H.  Akitake, and T. Tomiyama.  Studies on the Metabolism
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24.   Kobayashi, K. and H. Akitake.  Studies on the Metabolism of Chlorophenols
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                                      57

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27.   Munakata, K.  and M.  Kuwahara.   Photochemical Degradation Products of
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28.   Pierce,  R.  H.,  Jr0,  C.  R.  Brent, H.  P.  Williams, and S.  G.  Reeves.   Penta-
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29.   Plimmer,  J.  R.    Technical Pentachlorophenol:  Origin and Analysis of
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30.   Pruitt,  G.  W.,  B. J.  Grantham, and R0  H.  Pierce, Jr.  Accumulation and
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32.   Robinson, R.  A., and R0 G0 Bates.   Dissociation of Some Substituted
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34.   Sadtler Research Laboratories, Inc.  The Sadtler Standard Spectra, UV-
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35.   Schlenk, H.,  and J.  Gellerman.  Esterification of Fatty Acids with Diazo-
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36.   Shafik, T.  M.   Determination of PCP and Hexachlorophene in Human Adipose
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37.   Snow, H.  Harvest and Feeding Habits of Largemouth in Murphy Flowage,
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38.   Stark, A.  Analysis of Pentachlorophenol in Soil, Water, and Fish.  J.
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39.   Tiessens, G.  J.  Trichloro- and the Higher Chlorophenols and Their
     Electrical Conductivity in Water.   Rec. Trav. Chem., 48, 1929.  pp. 1066-
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40.   U. S. Environmental Protection Agency.   Manual of Analytical Methods for
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     Carolina, 1974.

41.   Zitko, V., 0. Hutzinger, and P.M.K. Choi.  Determination of Pentachloro-
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     Toxicol., 12, 1974.  pp. 649-653.
                                      58

-------
TABLE.A-l  PHYSICAL PARAMETERS FROM WATER SAMPLING SITES
               FROM FEBRUARY  1975 TO MAY  1976

Date Station
2-27-75 1
2
3
4
5
6
4-24-75 1
2
3
4
5
6
6-28-75 1
2
3
4
5
6
8-2-75 1
2
3
4
5
6
Temp
°C
15
16
15
16
16
16
19
19
22
22
22
22
23
23
30
30
30
30
NA
NA
28
29
29
29
Do00
pH mg/1
8,8
8,4
906
904
8.6
9.4
6.4
6.0
9o8
9,5
9.5
9.3
0,6
4.3
9,0
9.8
906
9o4
NA
NA
6,2 7,8
6.3 6.6
6.3 702
5.8 6.6
TOC
mg/1
12o6
14,2
12.4
NA&
14.0
17.6
6.3
6,2
7.9
7.9
7.9
704
NA
2009
17.5
17.4
NA
16o2
NA
NA
16,9
18.1
17.2
15.5
                                              (continued)
                           59

-------
                           TABLE A-l.   (CONTINUED)

Date
10-11-75





12-6-75





2-7-76





5-3-76





Station
1
2
3
4
5
6
1
2
3
4
5
6
1
2
3
4
5
6
1
2
3
4
5
6
Temp
°C
20
20
22
23
24
24
12
10
15
15
15

14
NA
11
12
11
11
18
NA
22
NA
23
22
pH
5.1
5o2
NA
NA
6,2
5.0
4.8
4o6
5,1
6.5
606

6,0
NA
6.4
6.5
6,5
6,3
6.2
NA
6,8
NA
6.7
6.6
D000
mg/1
8.0
6,0
4.0
8.0
9,0
8.8
5.9
6.6
10.2
10.4
10.6

8.2
NA
8.9
9.7
9.7
10.0
5,9
NA
8.0
NA
8.7
8.2
TOC
mg/1
24.9
24.5
18o5
17.2
19.6
17.7
24 .1
NA
16.6
16.7
16.9

20.0
NA
15.8
19.8
19.8
22.2
21.7
NA
15.6
NA
15.4
17.9
TMot analyzed.
                                      60

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        TABLE A-2  PHYSICAL PARAMETERS FROM WATER SAMPLING SITES
                      FROM AUGUST  1976 -  APRIL  1977

Date
August, 1976






October, 1976






January, 1977






April, 1977






Station
A
B

C

D

A
B

C

D

A
B

C

D

A
B

C

D

(depth)
meters
0.3
0.3
2.0
0,3
5.0
0.3
2.0
Dry
0.3
108
0.3
4.0
Oo3
1.5
0.3
0.3
1.8
0.3
6.0
0.3
2.6
0.3
0.3
2,0
0.3
5.0
0.3
1.5
Temp
°C
27
26
26
26
20
27
25
N0A.
16
12
15
12
17
12
12
12
7
12
6
12
7
25
24
18
26
15
24
20
D.O.
mg/1
N.A.a
8.0
7.4
8.7
0.2
7.5
5.0
N.A.
10.4
10.2
10.6
2,7
10.5
10o6
N.A.
11.8
9.5
12.2
6.2
12.8
6.0
N.A.
6.5
5.0
6.7
0.3
6.6
3.0
pH
5.8
5,7

6.1

6oO

NoA.
6.6

6.5

6.5

6.8
6.5

6.5

6.5

6.5
6.5

6.6

6.6

Not analyzed.
                                   61

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                             TECHNICAL REPORT DATA
                       (Please read Instructions on the reverse before completing)
1 REPORTNO.
EPA-600/3-78-063
                                                 3. RECIPIENT'S ACCESSION NO.
4. TITLE AND SUBTITLE
 Fate and Impact of Pentachlorophenol in a
 Freshwater Ecosystem
           5. REPORT DATE
             July 1978 issuing date
           6. PERFORMING ORGANIZATION CODE
7. AUTHOR(S)
 Richard H. Pierce, Jr.
                                                 8. PERFORMING ORGANIZATION REPORT NO.
9. PERFORMING ORGANIZATION NAME AND ADDRESS
 Institute of Environmental  Science
 University of Southern Mississippi
 Hattiesburg, MS   39401
           10. PROGRAM ELEMENT NO.

             1HE775
           11. CONTRACT/GRANT NO.
            R-803820
12. SPONSORING AGENCY NAME AND ADDRESS
Environmental Research  Laboratory - ATHENS
Office of Research and  Development         '
U.S.  Environmental Protection Agency
Athens,  GA  30605
        GA
           13. TYPE OF REPORT AND PERIOD COVERED
           Final  7/75-11/77
           14. SPONSORING AGENCY CODE
             EPA/600/01
15. SUPPLEMENTARY NOTES
16. ABSTRACT
 This investigation  was  undertaken to determine the fate of  pentachloro-
 phenol (PCP) that caused extensive fish  kills in a freshwater  lake in
 December 1974 and again in December 1976.  The kills resulted from the
 accidental release  of wood-treating wastes containing PCP in fuel oil.
 Food chain relationships were investigated in the lake and  the accumu-
 lation and elimination  of sublethal concentrations of dissolved PCP
 was studied under laboratory conditions  for the bluegill  (Lepomis
 macrpchirus).  The  highest concentrations  of PCP in fish were  observed
 in the bile followed by liver, gills,  and  muscle.

 Lake sediment and leaf  litter contained  high concentrations of PCP
 throughout the two-year study. Studies of  leaf litter from  the contami-
 nated water shed area showed it to be  a  source for chronic  pollution
 of the aquatic ecosystem. The major degradation products observed were
 pentachloroanisole  (PCP-OCH3) and the  2,3,5,6- and 2,3,4,5-tetrachloro-
 phenol (TCP) isomers. These products were  found to persist  in  sediment
 and fish along with PCP. The methyl ethers (anisoles) of both  TCP iso-
 mers and the 2,3,4,6-TCP isomer were observed in some samples  but the
 small amounts were  difficult to quantitate.
17.
                          KEY WORDS AND DOCUMENT ANALYSIS
               DESCRIPTORS
                                      b.IDENTIFIERS/OPEN ENDED TERMS
                       c.  COSATI Field/Group
 Phenol
 Toxicology
 Degradation
 Water pollution
Chlorinated  phenols
Bioaccumulation
Environmental  fate
Aquatic degradation
Environmental  per-
  sistence
06F
06T
68D
13. DISTRIBUTION STATEMENT

 Release to Public
19. SECURITY CLASS (This Report}
 Unclassified
21. NO. OF PAGES

    74
                                       20. SECURITY CLASS (Thispage)
                                       Unclassified
                                                             22. PRICE
EPA Form 22?0.'i 15-73}
                                     62
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