-0\\
                                                        Draft
                                                        9/24/87
AMBIENT AQUATIC LIFE WATER QUALITY CRITERIA- FOR

                      SILVER
      U.S.  ENVIRONMENTAL PROTECTION AGENCY
        OFFICE OF RESEARCH AND  DEVELOPMENT
       ENVIRONMENTAL RESEARCH LABORATORIES
                 DULUTH,  MINNESOTA
            NARRAGANSETT, RHODE ISLAND
                                              Recycled/Recyclable
                                              Printed on paper that co
                                              50% post-consumer recycled fiber
r\  
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                                    NOTICES
This document has been reviewed by the Criteria and Standards Division, Office
of Water Regulations and Standards, U.S. Environmental Protection Agency, and
approved for publication.

Mention of trade names or commercial products does not constitute endorsement
or recommendation for use.

This document is available to the public through the National Technical
Information Service (NTIS), 5285 Port Royal Road, Springfield, VA  22161.
                                        11
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"V       '

                                            FOREWORD


                Section 304(a)(l)  of  the Clean Water Act  requires  the Administrator of
          the  Environmental  Protection Agency to publish  water quality criteria that
          accurately reflect the  latest scientific knowledge on  the kind and extent of
          all  identifiable effects on health and welfare  that might be expected from the
          presence of pollutants  in any body of water.  Pursuant to that end, this
          document proposes  water  quality criteria for  the protection of aquatic  life.
          These criteria do  not involve consideration of  effects on human health.

                This document is  a draft, distributed for public review and comment.
          After considering  all public comments and making any needed changes, EPA will
          issue the criteria in final form, at which time they will replace any
          previously published EPA aquatic  life criteria  for the same pollutant.

                The term "water quality criteria" is used in two sections of the  Clean
          Water Act,  section 304(a)(l) and  section 303(c)(2).  In  section 304, the term
          represents a non-regulatory, scientific assessment of  effects.  Criteria
          presented in this  document  are such scientific  assessments.  If water quality
          criteria associated with specific stream uses are adopted by a State as water
          quality standards  under  section 303, then they  become  maximum acceptable
          pollutant concentrations that can be used to  derive enforceable permit  limits
          for  discharges to  such waters.

                Water quality criteria adopted in State water quality standards could
          have the same numerical  values as criteria developed under section 304.
          However,  in many situations States might want to adjust  water quality criteria
          developed under section  304 to reflect local  environmental conditions before
          incorporation into water quality  standards.   Guidance  is available from EPA to
          assist States in the modification of section  304(a)(l) criteria, and in the
          development of water quality standards.  It is  not until their adoption as
          part of State water quality standards that the  criteria  become regulatory.
                                             Martha G. Prothro
                                             Director
                                             Office of Water Regulations and Standards
                                               iii
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                                ACKNOWLEDGMENTS
Loren J. Larson
Larry T. Brooke
(freshwater authors)
University of Wisconsin-Superior
Superior, Wisconsin
Jeffrey L. Hyland
Robert S. Carr
(saltwater authors)
Battelie New England Laboratory
Duzbury, Massachusetts
Charles E. Stephan
(document coordinator)
Environmental Research Laboratory
Duluth, Minnesota
David J. Hansen
(saltwater coordinator)
Environmental Research Laboratory
Narragansett, Rhode Island
                                       IV
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                                    CONTENTS








                                                                         Page




Notices.		   i»



Foreword	  i i i



Acknowl edgments	   i v



Tables	'•	   vi







Introduction	>	    1



Acute Toxicity to Aquatic Animals	    3



Chronic Toxicity to Aquatic Animals	    5



Toiicity to Aquatic Plants	    8



Bioaccumulation	     9



Other Data	    10



Unused Data	   13



Summary	*'.	   15



National Criteria.,	   16



Implementation	   17








References	   77
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                                     TABLES
                                                                         Page
1.  Acute Toxicity of Silver to Aquatic Animals		  22
2.  Chronic Toxicity of Silver to Aquktic Animals	.	  43
3.  Ranked Genus Mean Acute Values wiith Species Mean Acute-Chronic
      Ratios	s	•	•••	  46
4.  Toxicity of Silver to Aquatic Plahts	'..	  51
5.  Bioaccumulation of Silver by Aquatic Organisms	  52
6.  Other Data on Effects of Silver on Aquatic Organisms...	  54
                                       VI
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 Introduction



     Primary sources of anthropogenic silver in surface  waters  include



 industrial and smelting wastes,  wastes in jewelry manufacture,  or  electrical



 supply, and most importantly,  in the production and disposal of photographic



 materials.  In a study of six water treatment facilities,  however,  Lytle



 (1984) found the highest influent concentrations of silver in  plants



 receiving no known photoprocessing or industrial silver wastes. Silver,  as



 silver iodide, is used in cloud seeding operations, and atmospheric transport



 can result in silver in precipitation great distances from target  areas.



 Freeman (1979) suggested that influent ground water might also be  an



 important source of silver in surface waters.



     Silver cycling studies by Freeman (1979) showed a strong affinity of



 silver for aquatic sediments.  Sediments contained approximately 1000 times



 the silver concentrations occurring in overlying waters.  Organic  sediments



 (silt, clay) contained two to three times more silver than inorganic



 sediments (sand, pebble).  Dependent on the specific conditions (e.g., redox



.potential, pH, dissolved oxygen, organic content, etc.) in sediments, silver



 might be associated with materials such as manganese dioxide,   clay minerals,



 organic ligands, sulfate, sulfite, or occur as elemental silver.  Although



 silver can exist in the 0,' +1, +2, and +3 oxidation states, only the 0 and +1



 states occur to any great extent in the environment.  The +1 state is the



 only one that occurs in substantial concentrations  in natural  waters.  Due to



 the low solubility product constant (Ksp = 1.8 x  10"  ) of silver chloride,



 chloride has a strong influence on the concentration of free ionic silver



 (Callahan et al. 1979).  Free silver  ions are photoreduced to  elemental



 silver by natural sunlight at a rate  that is dependent  on such factors as the



 degree of radiation, water clarity, and differential penetration  of



 photoreactive wavelengths.



                                        1
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    Chambers and Proctor (1960) found that the germicidal  action  of  silver  in

distilled water was related to the concentration of  silver ions,  rather than

to the physical nature of the silver!from which the  ions  were  derived.

Studies with saltwater species have shown that toxicity of silver is related

to the concentration of the free +1 ion;  however,  chlorocomplexes appear  to
                                     I
play an important role in the accumulation of silver by saltwater organisms

(Engel et al. 1981).

    Symptoms of silver intoxication in aquatic organisms  appear to be similar

to those caused by other heavy metals.  Separation and disruption of the  gill

epithelium is frequently observed, resulting in esphisia.  Damage may be  the

result of silver ions reacting directly at the gill  membrane,  or as an

indirect result of hematological osmotic imbalances  (Katz 1979).   Although

working with a limited data set, Campbell and Stokes (1985) stated that

biological responses to silver are generally pH independent.

    Unless otherwise noted, all concentrations reported herein are expected

to be essentially equivalent to acid^-soluble silver concentrations.  All

concentrations are expressed as silvjsr, not as the chemical tested.  A
     "                               I
comprehension of the "Guidelines for! Deriving Numerical National Water
                                     I
Quality Criteria for the Protection  of Aquatic Organisms  and Their  Uses"

{Stephan et al. 1985), hereinafter referred to as the  Guidelines, and the

response to public comment (U.S. EPAj 1985a)  is necessary  in order to

understand the following text, tables, and calculations.  Results of such

intermediate calculations as recalculated LCSOs and Sp'ecies Mean Acute Values

are given to four significant  figurejs  to prevent  round-off  error in

subsequent calculations, not to reflect the precision, of  the  value.  The
                                     i
criteria presented herein supersede  previous  national  aquatic  life  water

quality criteria for silver  (U.S.  EPA 1976,1980a) because these  new criteria
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 were derived using  improved  procedures  and additional  information.  The

 latest comprehensive  literature  search  for information for this document was

 conducted in July,  1986;  some more  recent information might have been

 included.




 Acute Toxicitv  to Aouatic Animals

     Acceptable  data on the acute effects of silver in fresh water are

 available  for twelve  species of  invertebrates and seven species of fish

 (Table 1).   Although  water hardness or  associated factors probably influence

 silver toxicity and the previous freshwater criterion (U.S. EPA 1980) was

 based on  hardness,  it has been determined that insufficient data are

 available  at medium and high hardnesses (> 75 mg/L as CaCOo) upon which to

 derive national  freshwater criterion based upon hardness.  The lack of data

 on  silver  toxicity at higher hardnesses and the poor agreement between the

 few data  that are available  results in  poor agreement between species on the

 regression slopes which were calculated but not presented.  Because the

 freshwater criterion  derived herein is  weighted by toxicity data from soft

 waters, criterion concentrations might  be overly protective of aquatic

 organisms  in hard waters.
                                                            t
     Freshwater  Species Mean Acute Values (SMAV) for silver range from

 0.9 ng/L for  a  cladoceran (Daphnia magna) to 560 \ig/l> for a crayfish

 fOrconectes  immunis)  (Table 1).   Genus Mean Acute Values (GMAV) for the 15

most  sensitive  genera occur within a small range, 2.155 to 29 /ig/L (Table

3).   Although the five most sensitive genera are arthropods, freshwater

fishes do not appear to be greatly more resistant to silver intoxication with

SMAVs ranging from 8.163 ^g/L for Rhinichthvs osculus to 13 ng/L for

Lepomis macrochirus.   The Final  Acute Value (FAV) in fresh water is

1.833 Mg/L.  This value exceeds  the SMAV for Daphnia magna (0.9

                                       3
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    The  acute  toxicity of  silver to resident North American saltwater animals

has been determined with ten  species of  invertebrates, including five

molluscs,  four crustaceans and a polychaete, and eleven species of fish

(Table 1).  The acute values  range from  3 pg/L for the Eastern oyster,

Crassostrea virginica (Zaroogian, Manuscript) to > 1,000,000 fig/L for the

raummichog, & value in excess  of silver's solubility (Dorfman 1977).  Of the

nine most  resistant species,  eight were  fishes.  The four most sensitive

species  include a fish, the summer fljounder Paral ichthvs dentatus. and three

bivalve  molluscs, including the Eastern  oyster; Pacific oyster, Crassostrea

gjgas and  quahog, Mercenaria  mercenaria.
                                     i
    The  toxicity of silver to several! saltwater species has been tested more

than once  in the same or different laboratories with generally reasonable

agreement  in acute values.  Values ranged from 145 to > 357 pg/L for the

polychaete, Neanthes arenaceodentata i(Peach and Hoffman 1983); from 3 to

37 WJ/L  for the Eastern and Pacific oysters (Calabrese et al.  1973;

Coglianese 1982; Coglianese and Martin 1981; Dinnel et al. 1983; Maclnnes and

Calabrese  1978; Zaroogian, Manuscript');  from 23.5 to 66 ng/L for the

copepod  Acartia tonsa (Lussier and Cardin 1985; Schimmel 1981); from 74.3 to

300 ng/L for static tests and from 65, to 313 ng/L for flow-through

testa for  the  mysid Mysidopsis bahia [(Schimmel 1981); from 640 to

58,000 ng/L for static tests  and from 441 to 1,876 ng/L for flow-

through  tests  with the sheepshead minnow, Cyprinodon variegatus (Heitmuller

et al. 1981; Schimmel 1981);  from 4.7 to 47.7 ng/L for summer  flounder,
                                     f
Paralichthvs dentatus (Cardin 1986); land from 196 /ug/L to 503  ng/L for

winter flounder Pseudopleuronectes americanus (Cardin 1986).

    Data on the relative sensitivities of early life stages of summer and

winter flounder to silver are contradictory.  Acute values were similar,
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 196.3 to 503 ng/L,  in tests which began with embryos just after fertili-




 zation, in early clevage, at blastula and one-day-old larvae of the winter




 flounder (Cardin 1986).  In contrast, acute values from flow-through tests




 that began with embryos  in early clevage were 15.5 and 47.7 jug/L.  Acute



 values were 8 ng/L  in tests that began with embryos at gastrulation and



 4.7 pg/L with the larvae (Cardin 1986).



    Of the 19 genera for which saltwater Genus Mean Acute Values are



 available (Table 3), the most sensitive genus, Crassostrea.- is about 190



 times more sensitive than the most resistant, Fundulus.  Molluscs, including




 oysters, quahogs, scallops, and squid are particularly sensitive to silver.




 Certain crustaceans and  fishes are similarly sensitive.  Acute values are .




 available for more  than  one species for two genera; the maximum difference in




 Species Mean Acute  Values is a factor of 2.74.  The saltwater Final Acute




 Value for silver was calculated to be 14.50 ng/L.  This value is slightly




 higher than Species Mean Acute Values for the Eastern and Pacific oysters,



 and the copepod Acartia  clausi and greater than acute values from nine




 individual tests with these three species and the summer flounder,



 Paralichthvs dentatus.








 Chronic Toxicity to Aquatic Animals




    Acceptable data on chronic toxicity of silver to freshwater organisms are



 available for a cladoceran and two species of fish (Table 2).  Elnabarawy et




 al. (1986) conducted life-cycle tests with three cladoceran species,




 Ceriodaphnia reticulata. Daphnia magna. and J). pulex. but did not measure




 silver concentrations in test chambers.  They reported chronic values of



 1.3,  < 0.56,  and < 0.56 ng/L,  respectively.




    The chronic values for the two cladoceran species reported are close  to




or greater than 48-hr LCSOs.   Based on these values, most acute-chronic




                                       5
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  ratios for the cladocerans are less t'han 1.0.   This is probably due to



  mitigating influence of the presenceiof food in the chronic tests.   Chapman



  (1980) reported the 48-hr EC50 for Da!phnia magna increased by a factor of  40



  when organisms were fed.   The mean 21-day LC50  for D.  magna of



  3.4 vg/L reported by Nebeker (1982)  is  greater  than its  Species Mean Acute



  Value,  2.557  ng/L.   All  studies  reported high mortalities  in chronic



  exposures  in  the  first  24-hr period.  Although  having  high acute  toxicity  in



  aquatic macroinvertebrates,  silver does  not  appear to  have significant



  cumulative effect  in chronic  exposures.   Nebeker (1982)  and co-workers (1983)



  reported chronic values for  D. magna ranging from 2.6  to 28.6  fig/L,



  resulting in  acute-chronic ratios  from 0.3911 to 0.7507.



     The effects of  chronic exposure to silver have  been  studied with two



  fishes, the rainbow trout and  fathead minnow.  Nebeker et  al.  (1983)



  conducted a 60-day  early life-stage test  with rainbow  trout  (Salmo



 gairdneri); growth  was reduced at  a silver concentration of  1.06 /zg/L.



 Although small, but statistically  significant,  growth  reductions were



 observed at the lowest concentrationsjtested, intermediate  concentrations did



 not produce growth reductions compared to the control.   The most sensitive



 parameter appeared to be survival,  whjch was reduced at 0.51 pg/L, but not



 at  0.36 fig/l.   The  chronic- value  for this study was 0.43 jug/L.  Davies



 et  al.  (1978)  reported a similar  effect  of silver on survival of rainbow



 trout.   In an  18-month exposure,  survival was reduced at 0.17 /zg/L,  but.



 was  not  affected at  0.09 jtg/L.  Growth was affected in  18 months at



 0.34 fig/L.  The chronic  value  for this study  was 0.12 ng/L.




    Holcombe and co-workers  (1983)  conducted  an  early life-stage exposure  *



with the fathead minnow, Pimephales promelas.  Growth was reduced at a silver
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 concentration of  1.07  pg/L,  although  no  effects on growth were observed at



 0.65  pg/L.   Survival of  fry  was  reduced  at 0.65 /xg/L, but not at



 0.37  f*g/L.   The chronic  value  for  the  fathead minnow was 0.49 ng/L. ,



 The acute-chronic  ratio  was  13.66.



    Theoretically,  acute-chronic ratios  should not be less than 1.0.  The



 chronic  value in any test must be  equal  to or less than the acute value.



 Although the  Species Mean Acute-Chronic  Ratio for Daphnia magna was



 calculated to be 0.4994, considering  the mitigating influence of food, as



 reported by  Chapman (I960) and Nebeker et al. (1983), this value might be



 artificially  low.   The Acute-Chronic  Ratio (ACR) for this species may more



 realistically be in the  range of 15 to 20, which is in general agreement with



 ACRs  for other species tested.  Therefore, the ACRs for Daphnia magna were



 omitted  from  the calculation of the Final Acute-Chronic Ratio.



    The  chronic toxicity of  silver has been determined in five life-cycle



 toxicity tests with the  saltwater  mysid, Mvsidopsis bahia (Table 2).  Chronic



 values from these tests  conducted  at  five laboratories ranged from  15.00 to



 87.75 tig/L (McKenney 1982).  Reproduction was reduced at 15, 19, and



 53 ng/L  in three tests,  and  both reproduction and survival were reduced at



 16 ng/L  in one test.   For three of the tests, 96-hr LCSOs from



 flow-through  tests  using the same  dilution water are available.



 Acute-chronic  ratios for these tests  ranged from 5.273 to 13.29.  The Species



 Mean Acute-Chronic  Ratio for this  mysid  is 8.512.



    The  three  useful Species Mean  Acute-Chronic Ratios are 33.29, 13.66, and



 8.512 (Table  3).  The  geometric mean  of  these values is 15.70, which  is the



 Final  Acute-Chronic Ratio.   Division  of  the freshwater and saltwater  Final



Acute  Values  by 15.70  results in freshwater and saltwater Final Chronic



Values of 0.1168 and 0.9236 pg/L,  respectively, which are lower than  the



 lowest available chronic values.




                                       7
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TOT!city  to  Aquatic  Plants           ;


    Three  acceptable tests are available with freshwater species exposed to


silver  (Table 4).  The most  sensitive  species was the alga Selenastrum


capricornutum for which  the  96-hr EC50, based on chlorophyll a, production,
                                     I
was 2.8 ng/L (U.S. EPA 1978).  Brown and Rattigan (1979) exposed two


freshwater vascular  plants to silver for 28 days.  ECSOs for El odea


canadensis and Lemna minor were 7,500  and 270 jug/L, respectively.


    Toxicity tests on silver have been conducted with eight species of


saltwater  plants (Tables 4 and 6).  The 96-hr EC50 for the diatom,


Skeletonema  costatum. was 130 fig/L based on cell counts and 170 /Jg/L


based on chlorophyll  a. (U.S. EPA 1978).  Chlorophyll a. was reduced after two


days exposure to 5 /Jg/L  for  the dinoflagellate, Glenodinium hal1i (Wilson


and Freeberg 1980).   Formation of cystocarps, sexual fusion, in the red alga
                                     i

Champia paryula was  reduced  by 1.9 pg/L (Steele and Thursley 1983).,


    The effect of temperature and salinity on the toxicity of silver has been


studied with three phytoplankton species (Wilson and Freeberg 1980).


Salinity did not significantly affect  the toxicity of silver to the diatom


Thalassiosira pseudonana. whereas the  dinoflagellate Gymnodinium  splendens


appeared to  be more  resistant at higher salinities (Table 6).  T. pseudonana


was most resistant at temperatures between 16 and 20°C, whereas G. splendens


was most resistant at temperatures between 20 and 30°C.  Chlorophyll a. was


reduced about 65% after  two  days exposure to from 15 to 110 jtxg/L  for


Isochrysis galbana for 13 temperature  - salinity combinations; from  13 to


84 tig/L for T.  pseudonana for 25 temperature -  salinity combinations;  and


from 1.3 to  18 /zg/L  for  G. splendens ifor 15 temperature - salinity


combinations.                       >
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    A Final Plant Value,  as defined in the Guidelines,  cannot  be  obtained


because no test in which the concentrations of silver were  measured has  been


conducted with any aquatic plant species..






Bioaccumulation


    Two studies reported on silver uptake  by freshwater fish (Table 5).


Largemouth bass fMicropterus salmoides) muscle tissue had bioconcentration


factors (BCF) of 11 and 19 after a 120-day exposure to 1 and 10 //g/L,


respectively.  Bluegills (Lepornis macrochirus) exposed for 180 days had whole


body BCFs of 15 and 150 at water concentrations of 10 and 100 /ig/L,


respectively (Cearley 1971).  Both species demonstrated a concentration-


dependent BCF.  In contrast, Barrows et al. (1980) reported no significant


uptake of silver by bluegills in a 28-day exposure.  No water concentration


was given.


    Bioconcentration tests have been conducted on silver with one  saltwater


species, the blue mussel, Mvtilus edulis.  (Table 5).  The mussels  were


exposed to three concentrations of silver for 12 to 21 months (Calabrese et


al. 1984).  The highest BCF observed was 6,500.  The BCF decreased with


increasing concentration of silver in water and reached a maximum  value after


12 months of exposure.  Fisher et al. (1984)  reported a BCF of 34,000 for the


diatom Thalassiosira pseudonana. and 13,000 for the green alga Dunaliella


tertiolecta exposed to silver cyanide for 12  hours (Table 6).              «
                                                                          ;»••

    No U.S. FDA action level or other maximum acceptable concentration  in


tissue, as defined in the Guidelines, is available for  silver; therefore, no


F-inal Residue Value can be calculated.
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 Other Data


     Other data on the lethal and subjlethal effects of silver on aquatic


 organisms are found in Table 6.   Two; algal species were tested for onset of


 inhibition of cell multiplication (Bringman and Kuhn 1977a,197Sa,b,1980b).


'The blue-green alga,  Microcvstis aeruginosa.  was about 14 times more


 sensitive to silver than the green alga,  Scenedestnus quadricauda.   The


 blue-green alga was affected at  0.7 ng/L,  whereas the green alga was not


 affected at concentrations less  than 9.5  ^g/L.   Other tests- on green algal


 species produced ECSOs or reduced griowth  effects in 6- to 21-day exposures


 ranging from 6.4 to 100 fzg/L.   In general, bacteria were about as


 sensitive as algae to silver.   However,  the duration of exposures was much.


 shorter (0.5 to 16 hr) for the bacteria tests than for the algal tests (6-21


 day).


     Bringmann and Kuhn (1959a, 1980a,'b,c)  tested three species of protozoans


 for incipient inhibition.   Results ranged from 2.6 /ig/L for a 48-hr


 exposure of Chilomonas paramaecium to 580 /ig/L for a 72-hr exposure of


 .Ento.s.iphon sulcatum.                                         /


     Nehring (1976) ran 14-day  exposures to silver with two species of  •


 immature insects.   A  mayfly nymph,  Ephernerel la grandis. was the most


 sensitive  with a 14-day,LC50 of  < 1 /ug/L  and a stonefly naiad, Pteronarcys


 californica.  was nearly as sensitive! with a 14-day LC50 of 4 to 9 /Ltg/L.


 Bioconcentration factors  (BCF) were determined for each species at death in
 •»'                                  I
 exposures  of  1  to 14  days.   BCFs varied inversely with exposure


 concentration.   This  may  have  been tfie result of increased bioconcentration


 with lower exposure levels or  due to'early deaths at the higher exposure
                                     !                          •*'"

 concentrations.   Mean BCFs of  37 to 84 were reported in the stonefly and


 mayfly,  respectively.  •             ;
                                       10
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     Davies  et  al.  (1978)  exposed  rainbow trout embryos and  larvae for 5 and



 22  weeks.   They  observed  premature hatching at concentrations as low as



 2.2 p,g/L.   Rombough  (1985)  exposed rainbow trout embryos to silver and



 reported median  time  to death  (LT50).  He also exposed a group of embryos



 with the zonae radiatae (egg capsule)  removed.  Median time to death was



 inversely related  to  exposure  concentration for all embryos.  Embryos without



 the zonae radiatae were more sensitive to silver.



     Birge (1978) and  Birge  et  al. (1978) exposed two species of fish and two



 species  of  amphibians to  silver during early  life stages.   ECSOs (dead and



 deformed larvae) ranged from 10 to 240 /ig/L for 7 to 8-day  exposures.



 These  results  are  greater than most of the Species Mean Acute Values for



 fishes found in  Table 1.




     LaPoint et al. (1984) related silver concentrations in  a Texas stream to



 benthic  invertebrate  community dynamics.  Although silver levels were high,



 attaining a maximum of 79.9 ng/L, other factors, such as extreme nutrient



 loading,  appeared  to  obscure any effects caused solely by silver.



     Wilson and Freeberg (1980) studied the effects of temperature and



 salinity  on the  toxicity  of silver to  several species of saltwater



 unicellular algae.   For the most extensively  studied species, the diatom



 Thalassiosira  pseudonana.  'silver was more toxic at temperatures above and



 below 20°C.   For a particular  temperature, the toxicity tended to decrease



with increasing  salinity,  except for the combination of 20°C and 3 g/kg



 salinity, which was the least  toxic combination tested.  The dinoflagellate



Gvmnodinium splendens also was more resistant to silver at  higher salinities.



    Several  studies have been  conducted with macroalgae (Boney et al. 1959;



Steele and Thursby 1983).   A significant decrease in the growth of female



gametophytes of the red alga Champia parvula was observed after two days of
                                       11
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 exposure to 3.2 pg/L.  No cystocarp formation occurred at  concentrations



 above 1.2 pg/L.                         .



     An interlaboratory comparison was performed with the polychaete  Neanthes



 arenaceodentata (Pesch and Hoffman 1983).   Ability to burrow was  the effect



 tested.   The geometric mean values for the  96-hr and 28-day  ECSOs were  158.6



 and 158.7 pg/L, respectively,  which indicates that no additional  toxicity



 occurred during the last 24 days of the test.  Windom et al.  (1982)  studied



 the uptake of silver from food by a polychaete.    *



     A number of studies of physiological  or biochemical effects have been



 conducted with polychaetes (Pereira and Kanungo 1981),  snails (Maclnnes and
                                 » .


'Thurberg 1973), bivalves (Calabrese et al.  1977a,1984;  Thurberg et al.



 1974,1975),  crustaceans (Calabrese et al.  1977b) and fish  (Calabrese et al.



 1977b;  Gould and Maclnnes 1977;  Jackim 1974;  Jackim et al.  1970;  Thurberg  and



 Collier  1977).   Ionic imbalances in the coelomic fluid and a significant
                                     i


 decrease in respiration were observed with  the blue mussel,  Mvtilus  edulis.



 the Eastern oyster,  Crassostrea  virginica.  the surf clam,  Spisula solidissima.
                                     I •                          i   «------


 the quahog,  Mercenaria mercenaria.  and the  soft-shell clam,  Mva arenaria.



 after 96-hr exposures to silver  concentrations of 50 to



 100 fig/L.



     Dinnel  et al.  (1982,1983)  conducted tests with gametes and embryos  of  many
                                     i              •»

 species  of  echinoderms.   The ECSOs,  based on sperm cell fertilization success



 after 60-rain exposures,  ranged from 29.8  to 115.3 ng/L for the four  species



 tested.  The most  sensitive effect observed was the percentage of larvae



 developing  to the  pluteus stage  after 5 days  of exposure.   The lowest EC50



 based on this effect  was  14.9  /zg/L for  the  sea urchin Strongvlocentrotus



 droebachiensis.



    The effeet  of  silver  on the  early life  stages of winter  flounder,



 Pseudopleuronectes americanus. was  investigated by Klein-MacPhee  et  al.  (1984)



                                        12
-------
and Voyer et al. (1982).  A significant increase in larval  mortality was



observed after 18 days of exposure to 92 ng/L.   Growth was  significantly



reduced by 180
Unused Data



    Some data on the effects of silver on aquatic organisms were not used



because the studies were conducted with species that are not resident in



North America (e.g., Khangarot and Ray 1987a; Khangarot et al.  1985; Laroze



1955).  McFeters et al. (1983) tested a brine alga, which is too atypical to



be used in deriving national criteria.  Doudoroff and Katz (1953), Engel et



al. (1981). Ganther (1980), Goettl et al. (1976), Jenne et al.  (Manuscript),



Kay (1984), LeBlanc (1984), Lockhart (Manuscript), Phillips and Russo (1978),



Whitton (1970), and the International Joint Commission (1976) compiled data



from other sources.



    Results were not used when the test procedures were not adequately



described (Ding et al. 1982; Fitzgerald 1987; Goettl et al. 1974,1978;



Hassell 1962;  Ishizake et al. 1966; Palmer and Maloney 1955; Tanaka and



Cleland 1978).  Acute and chronic tests with fathead minnows from Davies



(1976), Davies and Goettl (1978), LeBlanc et al. (1984) and EG & G, Bionomics



(1979) were not used because silver concentrations were measured using a



silver electrode (Chudd 1983), and it is expected that results would have



been substantially different had they been reported in terms of acid-soluble



silver.



    Data were not used when silver was a component of an effluent or mixture



(Bryan et al.  1983; Doudoroff et al. 1966; Greig 1979; Lewis 1986;



Lopez-Avila et al. 1985; Luoma and Jenne 1975; Malins et al. 1984;  Martin  et



al. 1984;  McDermott et al. 1976; Parsons et  al.  1973; Reynolds  1979;



Roesijadi  et al. 1984; Terhaar et al. 1972;  Young  and Lisk  1972).   Data  were



                                       13
-------
not used when the organisms were exposed to silver by injection or  gavage



(Hibiya and Orguri 1981; Storebakken et al. 1981).   Christensen (1971),



Christensen and Tucker (1978), and Dalraon and Bayen (1976)  only exposed



enzymes, excised or homogenized tissue, or cell  cultures.



    Tests conducted without controls (Albright and Wilson 1974;  Coleman  and



Clearley 1974) were not used.  Data from Buikema et al.  (1973,  197ta,b)  were



not used due to possible reproductive interactions.  High control mortalities



occurred in a life-cycle test reported by McKenney (1982).   Data from Hale



(1977) was not used because dilution water contained high concentrations of



other heavy metals.             ,.   .       .



    Results of some laboratory tests! were not used because the tests were •

         a*                           |

conducted in distilled or deionized water without addition of appropriate



salts (Chambers and Proctor 1960; Jones 1939,1940; Mukai 1977; Shaw and



Groshkin 1957; Shaw and Lowrance 1958).  ffatanabe and Takiraoto (1977) tested



silver toxicity in duckweed at a pH below 6.5.  Dilution waters used by
                                    i


Hannan and Patouillet (1972) contained high organic  levels.  Results from



Bringmann and Kuhn (1977b) were not used because organisms werfe cultured and



tested in different waters.



    Results of laboratory bioconcentration tests were not used when the



concentration of silver in the test solution  was not adequately measured



(Goettl and Davies 1978).  Reports of  the  concentrations of  silver  in wild



aquatic organisms  (Araiard 1978a,b,1979; Bryan et al. 1983; Eisler  et  al.



1978; Estabrook et ai.  1985;  Feldt and Melzer 1978;  Hall et  al.  1978; Jones
                                    I


et al. 1985; Lucas and  Edgington  1970; Martin,  Manuscript; Martin  and Flegal
                                    I


1975; Martin and Knauer 1972; Martin  et al.  1984;  Nelson et  al.  1983;



Reynolds 1979; Strong and Luoma  198L;  Telitchenko  et al.  1970;  long  et  al.



1972; Van Coillie  and Rousseau  1974)  were  not used to calculate
                                       14
-------
 bioaccumulation factors  due  to  an  insufficient  number  of measurements of the



 concentration of silver  in water.   BCFs  obtained  from  microcosm or model



 ecosystem studies were not used when  the concentration of  silver  in water



 decreased with time  (Terhaar et al. 1977).








 Summary



    The toxicity of  silver is probably influenced by water hardness or



 related factors,  although  insufficient data are available on which to base



 national  freshwater  criteria upon  hardness.  Silver is highly toxic to both



 freshwater macroinvertebrates and  fishes  in acute exposures.  Acute values



 ranged  from 0.9  /jg/L to  29 pg/L for the  15 most sensitive species.  A



 crayfish, Orconectes immunis. was  the most resistant species to silver with a



 98-hr LC50 of  560 pg/L.  The  six most sensitive species were arthropods.



    Data  are  available for a  cladoceran  and two species of fish in chronic



 exposures.  Chronic  values for  cladocerans were above  acute values that were



 obtained  in acute tests  in which the organisms were not fed, but  were below



 acute values  obtained in acute  tests  in  which the organisms \yere  fed.  Mean



 chronic values were  0.2272 and  0.49 /ig/L  for rainbow trout and fathead



 minnows,  respectively.  Their respective  acute-chronic ratios were 33.29 and



 13.66.  Freshwater vascular  plants appeared to be relatively insensitive to



 silver,  although algae and other microorganisms were reported to  be very



 sensitive.  Uptake of silver was reported for several  organisms.



 Bioconcentration factors ranged  from  less than detectable to 150.



    Acute toxicity values  for silver are  available for 21 species of



 saltwater animals including  ten''species of invertebrates and eleven species



of fish.  Acute values range from 3 /ug/L  for the Eastern oyster to
                                       15
-------
> 1,000.000 for the mummichog.  Fishes are generally resistant except for


sensitive early life stages.  The four most sensitive species include embryo


and larval stages of the summer flounder, Eastern oyster,  Pacific oyster,  and



quahog.


    The chronic toxicity of silver has been determined in five life-cycle


toxicity tests with the saltwater mysid, Mvsidopsis bahia.  Chronic values


ranged from 15.00 to 87.75 fig/L based primarily on decreases in


reproduction.  Acute-chronic ratios for the three tests for which 96-hr LCSOs


were available ranged from 5.273 to 13.29.  The toxicity of silver has been


determined with eight species of saltwater plants.  Four species,


Thalassiosi ra pseudonana. Glenodinium halli.  Gymnodinium splendens. and
                                     [

Champia parvula were affected in one or more tests at concentrations below


the acute value for the most sensitive saltwater animal.  The blue mussel can


bioconcentrate silver from 1,056 to 6,500 times the concentration  in water.


Embryonic development of sea urchins and surf clam embryos was affected and


physiological or histological changes occurred in American lobsters, surf


clams, and blue mussels at concentrations below the acute value  for  the most


sensitive saltwater animal.






National Criteria         •


    The procedures described  in the "Guidelines for Deriving  Numerical


National Water Quality Criteria for the  Protection of Aquatic  Organisms, and


Their Uses" indicate that, except possibly where  a locally  important species
                                     i

is very sensitive, freshwater aquatic organisms and their uses  should  not be


affected unacceptably if the  four-day average concentration  of  silver  does


not exceed 0.12 jug/L more than once every  three years on  the  average and


if the one-hour average concentration does not exceed 0.92 /xg/L more than

                                     r
once every three years on the average.


                                       16
-------
     The procedures described in the  "Guidelines  for  Deriving Numerical



 National Water Quality Criteria for  the  Protection of Aquatic Organisms and



 Their Uses" indicate that,  except  possibly  where  a locally  important species



, is very sensitive, saltwater aquatic organisms and their uses should not be



 affected unacceptably if  the four-day average concentration of silver does



 not exceed 0.92 pg/L more than once  every three years on the average and



 if -the one-hour average concentration does  not exceed 7.2 ng/L more than



 once every three years on the average.








 Implementation



     Because of the variety of forms  of silver in  ambient water and the  lack



 of definitive  information about their relative toxicities to aquatic species,



 no available analytical measurement  is known to  be ideal for expressing



 aquatic life criteria for silver.  Previous aquatic  life criteria  for metals



 and metalloids (U.S.  EPA  1980b) were expressed  in terms of  the total



 recoverable measurement (U.S. EPA  1983a), but newer  criteria for metals  and



 metalloids have been expressed in  terms  of  the  acid-soluble measurement  (U.S.



 EPA 1985b).  Acid-soluble silver (operationally  defined as  the silver that



 passes through a 0.45 pta  membrane  filter after  the sample has  been



 acidified to a pH between 1.5.and  2.0 with  nitric acid)  is  probably  the  best



 measurement at the present for the following reasons:



  1.   This measurement is  compatible  with nearly  all  available  data concerning



      toxicity  of silver to,  and bioaccumulation  of silver  by,  aquatic



      organisms.   It is expected that the results  of  tests  used in  the



      derivation of the criteria would not have  been  substantially  different



      if they had been reported in  terms  of  acid-soluble  silver.



  2.   On samples  of ambient water,  measurement of  acid-soluble  silver will



      probably  measure all forms of silver that  are toxic  to aquatic  life or



                                       17
-------
     can be  readily converted to toxic forms under natural conditions.  In

     addition, this measurement probably will not measure several forms,  such
                                   I
     as silver that is occluded in minerals, clays, and sand or is strongly

     sorbed  to particulate matter, that are not toxic and are not likely to

     become  toxic under natural conditions.  Although this measurement (and

     many others) will measure soluble complexed forms of silver, such as the

     EDTA complex of silver, that probably have low toxicities to aquatic

     life, concentrations of these forms probably are negligible in most

     ambient water.                        '

3.   Although water quality criteria apply to ambient water, the measurement

     used to express criteria is likely to be used to measure silver  in

     aqueous effluents.  Measurement of acid-soluble silver is expected to be

     applicable to effluents because it will measure precipitates, such as
                                   i
     carbonate and hydroxide precipitates of silver, that might exist  in an

     effluent and dissolve when the effluent is diluted with receiving

     water.  If desired, dilution of effluent with receiving water before
                                   i
     measurement of acid-soluble silver might be used to determine whether

     the receiving water can decreasje the concentration of acid-soluble

     silver because of sorption.

4.  The acid-soluble measurement isi expected to be useful for most metals

    and metalloids, thus minimizing! the number of samples and procedures

    that are necessary.            j
                                   i
5.  The acid-soluble measurement does not require filtration of the  sample
                                   i
                                   I
    at the time of collection, as does the dissolved measurement.
                                   I
6.  The only treatment required at ^he time of collection  is preservation  by

    acidification to a pH between 1.5 and 2.0, similar to that  required  for

    the total recoverable measurement.
                                      IS
-------
 7.  Durations of 10 minutes to 24 hours between acidification and filtration



     of most samples of ambient water probably will not affect the result



     substantially.



 8.  Ambient waters have much higher buffer intensities at a pH between 1.5



     and 2.0 than they do at a pH between 4 and 9 (Stumm and Morgan 1981).



 9.  Differences in pH within the range of 1.5 to 2.0 probably will not



     affect the result substantially.



 10.  The acid-soluble measurement does not require a digestion step,  as does



     the total recoverable measurement.



 11.  After acidification and filtration of the sample to isolate the acid-



     soluble silver, the analysis can be performed using either atomic



     absorption spectrophotometric or ICP-atomic emission spectrometric



     analysis (U.S. EPA 1983a), as with the total recoverable measurement.



 Thus, expressing aquatic life criteria for silver in terms of the acid-



 soluble measurement has both tozicological and practical advantages.  The



 U.S. EPA is considering development and approval of a method for a



 measurement such as acid-soluble.                             .*



     Metals and metalloids might be measured using the total recoverable



 method (U.S. EPA 1983a).  This would have two major impacts because this



 method includes a digestion procedure.  First, certain species of  some metals



 and metalloids cannot be measured because the total recoverable method cannot



 distinguish between individual oxidation states.  Second, in some  cases  these



 criteria would be overly protective when based on the total recoverable



 method because the digestion procedure will dissolve silver that  is not  toxic



 and cannot be converted to a toxic form under natural conditions.  Because  no



measurement is known to be ideal for expressing.aquatic  life criteria  for



 silver or for measuring silver in ambient water or aqueous effluents,



measurement of both acid-soluble silver and total recoverable silver  in



                                       19
-------
ambient water or effluent or both might  be  useful.   For  example, there might

be cause for concern when total  recoverable silver  is  much  above am

applicable limit, even though acid-soluble  silver is below  the  limit.

     In addition, metals and metalloids  might be  measured using the dissolved

method, but this would also have several impacts.  First,  in many  toxicity

tests on silver the test organisms were  exposed to both dissolved  and

undissolved silver.  If only the dissolved silver had  been measured,  the

acute and chronic values would be lower than if acid-soluble or total

recoverable silver had been measured.  Therefore, water quality criteria
                                     I
expressed as dissolved silver would be  lower than criteria expressed as acid-

soluble or total recoverable silver.  Second, not enough data are available

concerning the toxicity of dissolved silver to allow derivation of a

criterion based  on dissolved silver.  Third, whatever analytical method is

specified for measuring silver  in ambient  surface water will probably also be

used to monitor  effluents.   If  effluents are monitored by  measuring only the

dissolved metals and metalloids, carbonate  and hydroxide precipitates of

metals would not be measured.   Such  precipitates might  dissolve,  diue to

dilution.or change  in  pH  or  both, whfcn  the effluent is  mixed with receiving

water.  Fourth,  measurement  of  dissolved  silver  requires filtration  of the

sample at the time  of  collection.   For  these  reasons,  it is recommended  that

aquatic  life criteria  for silver not; be expressed as  dissolved silver.

     As discussed  in the  Water  Quality  Standards Regulation (U.S. EPA 1983b)

and the Foreword to this document,  a water quality criterion for aquatic life

has regulatory  impact only after it ihas been adopted  in a state water quality

 standard.   Such a  standard specifies a criterion for  a pollutant that is

 consistent  with a  particular designated use.  With the concurrence of the

 U.S.  EPA,  states designate one or more uses for each body of  water or segment

 thereof  and adopt  criteria that are'consistent  with the use(s) (U.S. EPA

                                     ;   20
-------
1983c,1987).  In each standard a state may adopt the national criterion,  if
       •
one exists, or, if adequately justified, a site-specific criterion..

     Site-specific criteria may include not only site-specific criterion

concentrations (U.S. EPA 1983c), but also site-specific, and possibly

pollutant-specific, durations of averaging periods and frequencies of allowed

excursions (U.S. EPA 198Sc).  The averaging periods of "one hour" and "four

days" were selected by the U.S. EPA on the basis of data concerning how

rapidly,some aquatic species react to increases in the concentrations of some

pollutants, and "three years" is the Agency's best scientific judgment of the

average amount of time aquatic ecosystems should be provided between

excursions (Stephan et al. 1985; U.S. EPA 1985c).  However, various species

and ecosystems react and recover at greatly differing rates.  Therefore, if


adequate justification is provided, site-specific and/or pollutant-specific

concentrations, durations, and frequencies may be higher or lower than those

given in national water quality criteria for aquatic life.

     Use of criteria, which have been adopted in state water quality

standards, for developing water quality-based permit limits and  for designing

waste treatment facilities requires selection of an appropriate  waste load

allocation model.  Although dynamic models are preferred for the application

of these criteria (U.S. EPA 1985c), limited data or other  considerations
       •
might require the use of a steady-state model (U.S. EPA 1988).   Guidance on

mixing zones and the design of monitoring programs  is also  available  (U.S.

EPA 1985c,1987).
                                       21
-------
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