903R94026
CBP/TRS 130/94
       The Effect of Salinity on the Acute Toxicity
      of Total Dissolved and Free Cadmium to the
          Copepod Eurytemora affinis and the
          Larval Fish Cyprinodon variegatus
                           ,
                         ;^:;'ul Street
TD
225
.C54
C125
1994
           Chesapeake Bay Program

-------
The Effect of Salinity on the Acute Toxicity of Total
   Dissolved and Free Cadmium to the Copepod
             Eurytemora affinis and the
         Larval Fish Cyprinodon variegatus
                     October 1994
                        U S. F.u:..cnmital Pcalecfeon ftgency
                        iu.,,,ofl ill iiUOiiJiaUea Resource
                        Cwlar (1PM52)
                        841 Chestnut Street
             MDE
     Printed by the U.S. Environmental Protection Agency for the Chesapeake Bay Program

-------

-------
                October 1994
                   Report
The Effect of Salinity on the Acute Toxicity
      %
 of Total Dissolved and Free Cadmium to the

     Copepod Eurytemora affinis and the

      Larval  Fish Cyprinodon variegatus
            Lenwood W. Hall, Jr.
            Michael  C.  Ziegenfuss
             Ronald D. Anderson

           University of Maryland
  Maryland Agricultural Experiment Station
     Wye Research and Education Center
                P.O. Box 169
         Queenstown, Maryland 21658
                     and
               Brent L. Lewis

           University of Delaware
          College of Marine Studies
            Lewes,  Delaware 19958

-------
                             ABSTRACT



     The objective of this study was to determine the influence of



a range of salinities  (5, 15 and 25 ppt) on the acute toxicity of



total dissolved and free cadmium to sheepshead minnow, Cyprinodon



variegatus  larvae and  the  copepod, Eurytemora  affinis nauplii.

                                                s

Data were analyzed to determine if the  acute toxicity  (96 h LC50s)
                      -*.


was  different  among  salinities  for  the  test  species.    Total



dissolved cadmium was measured in selected  test conditions and the



proportion of total cadmium  as Cd+2 (free ion or toxic form) was



determined at each salinity.   Ninety six hour LC50 values for C.



variegatus were 180.3, 312.4 and 495.5  Mg/L total cadmium at 5, 15



and 25 ppt,  respectively.   A significant increase in LC50 values



with salinity was likely related to a decrease in the free ion as



salinity  increased.   Ninety-six hour LC50 values  for E.  affinis



were 51.6, 213.2 and 82.9 liqfL  total cadmium at 5, 15 and 25 ppt,



respectively.  A comparison of LC50 values  for the copepod between



salinities showed a significant difference between 5 and 15 ppt and



between 15  and  25 ppt.   There was no  difference  in  LC50 values



between  5 and  25 ppt. The physiological  characteristics of  E.



affinis were likely  responsible for the higher  tolerance at the



middle salinity. Cadmium speciation in  the  various test salinities



was  dominated  by association  with  inorganic binding  ligands;



organic  complexation  was  negligible.    The  speciation  at  all



salinities  was  dominated  by   CdCl* and  CdCl2°.    The free  ion



accounted for 20, 8 and 4.5 % of the total  cadmium at 5, 15 and 25



ppt,  respectively.    As  current  water  quality  criteria do  not

-------
distinguish  among  individual  cadmium  species  these  data  have



important implications for estuaries such as Chesapeake Bay because



the presence of the  toxic form of cadmium will increase as salinity



decreases.
                                11

-------
                        TABLE OF CONTENTS


                                                             Page

ABSTRACT	' . . i

INTRODUCTION  	 1

METHODS 	 5
     Test Organisms	5
     Test Procedures	5
     Cadmium Analysis 	 8
          General Procedures  	 8
          Total Dissolved Cadmium Analysis  	 9
          Organic Complexation  	  10
          Cadmium Speciation Calculations 	  13
     Statistical Analysis 	  15

RESULTS	16
     Water Quality and Cadmium Chemistry	16
          Toxicity Data	22

DISCUSSION	28

ACKNOWLDEGEMENTS	33

REFERENCES	34

APPENDIX A -   Raw data from the Eurytemora and Cyprinodon
               96 h toxicity tests at three salinities
                             .  iii

-------

-------
                          INTRODUCTION

     One commitment  of  the  1988 Chesapeake Bay  Basinwide Toxics
Reduction Strategy was to give contaminants on the Toxics of
Concern List priority in the development of water quality criteria
(U.S.  EPA,  1991a).   Presently the  United States  Environmental
Protection  Agency  develops  water  quality  criteria  for  both
freshwater and marine systems.  Estuarine organisms are supposed to
be  protected under  the marine criteria.    There are  ,however,
compelling  biological  and  chemical  factors  that  may  prevent
estuarine biota  from being protected  under marine  criteria and
these  factors justify the need for specific  estuarine criteria.
Estuarine  organisms,  because of  their  inherent  physiological
differences  from  freshwater  and  marine   organisms,  may  differ
substantially in  sensitivity to some toxic substances. For example,
recent toxicity  studies with an  estuarine zooplankter  and fish
showed  that salinity ranging  from  5  to  25  ppt  significantly
influenced the toxicity of atrazine (Hall et al.,  in press).  . The
unique  water chemistry  of  estuarine  environments  may also  be
responsible  for   differences  in  bioavailability of  some  toxic
substances, thus  affecting their toxicities.
     Four  metals  listed on  the  Toxics  of  Concern  list  for
Chesapeake Bay were potential  candidates for assessing the effects
of salinity on their toxicity (cadmium,  chromium,  copper and lead).
We  eliminated chromium  and  copper because  of  potential problems
with  the  speciation  chemistry.   Lead  was  eliminated  due  to

-------
solubility problems at various salinities and possible differential
precipitation rates at various salinities. Cadmium was, therefore,
selected  for this  study  due  to  less  projected  problems  with
speciation  chemistry.   The toxicity  data base for  cadmium with
Chesapeake Bay species was also more extensive when compared with
the other metals considered for this project (Hall  et al.,, 1994).
     The  environmental  impact  of  cadmium in aquatic  systems is
determined  by  its  total  concentration,  by. partitioning between
dissolved and particulate phases, and  by its "chemical speciation"
(i.e. by the physicochemical forms  in  which the element is found).
The toxicity and/or bioavailability of a trace metal  to aquatic
organisms has in most instances been  found to correlate with the
activity  of the  free metal ion rather than with the total metal
concentration (e.g. Brand et al.,  1983, 1986;  Sunda et al., 1987,
1990) .  The concentration of the free ion may be much lower than
the  total metal  concentration due to  complexation by various
inorganic and  organic  ligands in  solution.   The  association of
metals  with natural complexing  ligands  may  therefore  serve to
buffer the system with respect  to the  toxicity of a given metal.
     The  inorganic  speciation  of  cadmium in natural waters  is a
function  of pH,  temperature, the ionic strength of the solution,
and the relative concentrations of potential binding ligands.  In
seawater, the inorganic speciation  of cadmium  is predicted to be
dominated by association with the chloride ion, while in freshwater
total cadmium will be dominated by the free  hydrated ion (Cd2*) at
pH 6 and  partitioned between the free ion and carbonate complexes

-------
at higher pH (Turner et al., 1981; Byrne et al., 1988).  Byrne et
al.  (1988)  estimated  that 97.2%  of dissolved inorganic  Cd in
seawater  exists  as  chloride  complexes,  predominantly CdCl* and
CdCl2°.  In an estuarine environment,  where freshwater and seawater
mix  and  chemical  reactions  can occur,  the  change  in  cadmium
speciation from the free ion and carbonate species to predominately
chloride complexes occurs  at  low salinities  (< 5 ppt).  Chloride
complexes will therefore dominate the cadmium speciation over most
of the estuary.
     In contrast to  its we 11-characterized  inorganic speciation,
the speciation of dissolved cadmium with respect to natural organic
ligands is poorly  known.   In the central North Pacific,  cadmium
appears to be 60-70% complexed by strong, relatively Cd-specific,
organic ligands.   The  latter are present,  however, at  very low
concentrations (approx. 0.1 nM)  (Bruland,  1992).  Similar behavior
has been observed  for  cadmium in coastal waters of the northwest
Atlantic,  with complexing ligand concentrations on the order  of 0.3
nM (Lewis and Luther, unpublished data).
     The study described in this  report was conducted to determine
the influence of salinity  on  the toxicity of  total dissolved and
free cadmium to  estuarine  species.   Specific  objectives  were to
determine  the  acute  toxicity  (96  h LCSOs)  of cadmium to  two
Chesapeake Bay resident species,  the  sheepshead minnow, Cyprinodon
variegatus  larvae and copepod  Eurytemora  affinis nauplii,  at
salinities of  5,   15  and  25  ppt.    These data  were  analyzed to
determine if acute toxicity (96 h LC50 values) was different among

-------
salinities for each species.  Total dissolved cadmium was measured
in selected test conditions.   The solution speciation of cadmium
with respect to free hydrated ions and inorganic complexes in the
sample solution was also determined using MINEQL+,  an interactive
PC version  of the  original  MINEQL equilibrium modeling program
(Schecher  and  McAvoy,  1991).    MINEQL+  utilizes  equilibrium
constants to  solve mass  balance expressions,  using a  modified
Newton-Raphson iterative procedure.

-------
                             METHODS

Test Organisms
     Eurytemora affinis cultures were maintained at 8, 15, 'and 22
ppt salinity and 23-25 C  in our laboratory.  Copepods were reared
in autoclaved estuarine water  (14 ppt) obtained from the Choptank
River at Horn Point Center for Environmental and Estuarine Studies
(GEES).   Salinity  was  adjusted with H-W  Marinemix  or deionized
water.  Copepods were fed a diet consisting of equal volumes of two
phytoplankton  species,  Thalassiosira fluviatilis  and Isochrysis
galbana, each maintained in log-phase growth.   The phytoplankton
were also cultured in autoclaved estuarine  water supplemented with
F/2 media  (Guillard,  1975).
     Cyprinodon  variegatus  larvae  were  obtained from  Aquatic
Biosystems, Inc.  (Fort  Collins, CO).  Larvae  were <24-h old and
shipped  at three salinities  (8,  15, and  24 ppt).   Larvae were
placed in aquaria containing salinity adjusted (5,  15, and 25 ppt)
Choptank  River  water  and  fed Artemia  nauplii  for  overnight
acclimation.

Test Procedures
     Cadmium  chloride   (lot   number  50H-0879)   used  in  these
experiments was  obtained from Sigma Chemical Company (St. Louis,
MO) .  Autoclaved estuarine water from the Choptank River (10 ppt)
was used as control water and  diluent  for all  toxicity tests.
Salinity adjustments to the desired test  salinities (5, 15, and 25

-------
ppt) were made with HW Marinemix or deionized water. Acute toxicity
tests  (96 h) with Eurytemora and sheepshead  larvae were conducted
as static non-renewal.   All  tests  were conducted in a biological
incubator  to  maintain   a  constant  temperature of  25  C and  a
photoperiod  of  16-h light:8-h  dark.    Standard  water  quality
parameters  (temperature, dissolved oxygen, pH, and salinity)  were
recorded initially and at the end of the exposure period for each
test condition.   Selected  test  conditions were sampled initially
and at 96 h for total cadmium analysis and speciation.
     The Eurytemora experiment at 5 ppt salinity was conducted at
the following nominal cadmium concentrations:  0, 32, 56, 100, and
180  jig/L.    The test at 15  ppt  salinity  was conducted  at the
following nominal concentrations:  0,  32,  56,  100,  180,  320, and
560 M9/L cadmium.  Nominal  concentrations  of cadmium in the 25 ppt
salinity test were:  0,  56, 100, 180,  320,  and 560 ngfL.  Each test
concentration  was  prepared by diluting a  stock solution  (100 ug
cadmium/L)  of cadmium  chloride  with salinity  adjusted  Choptank
River water.  The salinity  adjusted diluent for  all conditions was
prepared by diluting the estuarine water  to 5 ppt  with deionized
water and adding synthetic  seasalt  to the desired salinity.  Stock
solutions were prepared 1-2  days prior to testing  by dissolving
40.77  mg of  anhydrous  cadmium  chloride  in 250 mL of  deionized
water.
     Toxicity  tests  were  initiated  with  copepodids  (48  to  72-h
old). Copepodids were obtained by isolating adult gravid copepods
in polycarbonate jars containing salinity adjusted estuarine water

-------
for '24-h and collecting the  recently  hatched neonates.   Neonates
were held for 48-h prior to  starting  each  test.   Three replicate
150 mL glass beakers containing 100 mL of test solution were used
for  each  condition.    A  test chamber  was  suspended within each
beaker to contain the  organisms.   Chambers were constructed from
3.8 cm diameter rigid polycarbonate tubing cut to a length of 5.0
cm to provide a  40  mL volume when suspended  in  the  beaker.  The
bottom of the chamber  was  covered with 53 urn mesh Nitex screen.
Copepodids were counted by drawing small aliquots of copepods and
water into a wide-bore glass pipet and  examining under a dissecting
microscope  (15x  magnification).   The initial  number  of copepods
(10-15)   and  the  corresponding   test   chamber  were  recorded.
Eurytemora  were  fed  daily  with  1.0  mL   of  a  two-species
phytoplankton mixture  (50/50;  v/v).   Algal  densities  within the
test chamber were generally  1-2 x  104  Isochrysis cells/mL and 2-3
x 103 Thalassiosira cells/ml.   Algal  cell counts  were conducted
with  a  Spencer  improved  Neubauer corpuscle counting  chamber.
Survival was evaluated in  each condition after  a  96  h exposure.
Copepods were counted by first lowering the volume of solution in
the test chamber, then removing the remaining copepods and water in
small aliguots with a  pipet.  Each aliquot within the pipet was
examined with the aid of a dissecting microscope for the presence
of live copepods.
     Cyprinodon  acute  toxicity  tests  (96  h)  were  conducted
following U.S.  EPA protocol (U.S. EPA.,  1991b).   For  the test
conducted at 5 ppt salinity, larvae were exposed to the following

-------
nominal cadmium  concentrations:   0,  56, 100,  180,  320,  560, and
1000  /ig/L.    The  15  ppt salinity  test was  conducted with the
following nominal concentrations:  0, 100, 180,  320,  560, 1000, and
1800  /xg/L.    The  25  ppt salinity  test was  conducted with the
following nominal  concentrations:  0,  180,  320,  560,  1000, 1800,
and 3200 Mg/L- Each concentration was prepared  by diluting a stock
solution of  cadmium (1000 Mg/L)  with the appropriate volume of
salinity adjusted  diluent.   Tests were initiated with 48-h old
larvae following a 24-h acclimation period.  The maximum salinity
change was » 5ppt.  Three replicate 600 mL glass beakers containing
400  mL of  test  solution were  used  for each  condition.    Each
replicate  received ten  larvae  by  transferring them  from  the
acclimation water to a test beaker with a fire-polished, wide-bore
glass pipet.  Larvae were fed at :48 h with 100 uL of concentrated
Artemia  nauplii.   At  that time,  dead  larvae  were counted and
removed from  each  beaker.  Larval survival  was evaluated  in each
condition after 96 hours of exposure.

Cadmium Analysis
     General  Procedures
     Total dissolved cadmium and  cadmium speciation measurements
were  conducted  by the College  of Marine Studies,  University of
Delaware  (Lewes,  DE).    Samples  for  total dissolved cadmium and
speciation analyses were filtered (0.4 um polycarbonate membrane)
and  collected  in  precleaned  polyethylene  containers.    Total
dissolved  cadmium  samples  were preserved with  Seastar ultrapure

                                8

-------
nitric  acid  (Seastar  Chemicals,   Inc.,  Seattle,  WA) .   Samples
collected in polyethylene bottles for speciation measurements were
immediately frozen and shipped to the University of Delaware on dry
ice  by Federal  Express  courier   service.    The  following  test
conditions were sampled  initially  and  at  96h for total dissolved
cadmium and speciation measurements:  Eurytemora test at 5 ppt (32,
100, 180,  and 560 Mg/L) /  Eurytemora test at 15 ppt  (32, 100, and
560 M9/L) ;   Zurytemora  test at 25 ppt (56, 180,  and 560 pq/L) ;
Cyprinodon test at 5 ppt  (56, 180,  and 1000 M9/L) ;  Cyprinodon test
at  15  ppt (100,  320,  and  1800  jxg/L) ;  Cyprinodon test  at 25 ppt
(180, 560, and 3200
Total Dissolved Cadmiu^ Analyses
     Total  dissolved  cadmium  concentrations  were  measured  by
Inductively Coupled  Plasma  - Atomic Emission  Spectroscopy  (ICP-
AES) .   Concentrations were  determined by  comparison  of sample
emission values with  a linear calibration curve.  Working standards
were prepared  by serial  dilution of a  1000 ppm  commercial ICP
cadmium  standard  (Inorganic Ventures,   Inc.,  Toms  River  NJ) .
Standards were prepared in an  organic-free  (ultraviolet-irradiated)
natural seawater  matrix, diluted to the appropriate salinity (5, 15
or 25 ppt) and acidified to 0.1 N with high purity quartz-distilled
nitric acid.  Thus the matrix of  the standards was equivalent to
that of the samples,  correcting for any signal suppression due to
seasalts  in the  samples.    Analytical  sensitivity was  1.46±0.1
emission units/jig/L-Cd, with a detection  limit of approximately 3

-------
Mg/L.
Organic Complexation
     Voltammetric measurements of cadmium were conducted using an
EG&G Princeton Applied Research  (PAR)  Model 384B-4 polarographic
analyzer with a PAR  Model  303A mercury drop electrode.  Analyses
were performed  in the square  wave anodic  stripping voltammetry
(SWASV) mode with  a hanging mercury drop electrode (HMDE) .  Cadmium
was reduced and deposited in the mercury drop for one minute at a
deposition  potential  of  -1.0 V.    Instrumental parameters for
reoxidation  and stripping of  the  cadmium from  the mercury drop
were:  scan  rate  - 200 mV sec'1,  pulse amplitude = 20 mV, pulse
frequency - 100 Hz, scan range - -1.0 to -0.4 V.
     The form  of  the  metal  deposited  at a  mercury electrode is
dependent upon both  the thermodynamic  stability and the kinetic
lability  of the  complexes,  as  well   as  the  thickness  of  the
diffusion layer at the electrode  surface and  the  diffusion rate of
a complex through this layer.   For a  metal-ligand complex, the
dissociation of the complex, and subsequent reduction of the metal
to form the mercury amalgam can be represented as:
                             *d
                       MLpn+ <==>  M"+ + p L
                              *i
                       M"+ + n e'	> M°(Hg)
where M and  L are the metal and complexing ligand  respectively, and
k  is  the  rate of  reaction for  the   dissociation (kd)   or the
formation of (kf)  of  the metal-ligand complex ML.

                               10

-------
     For  a  given deposition  potential a  stripping voltammetric
method will detect only the free ionic form of the metal plus those
complex  species  which dissociate  to  the free  ion within  the
timespan required for diffusion of the complex into  and out of the
electrode diffusion  layer.  This  is illustrated schematically in
Figure  l.    Such complexes can  be defined  as electrochemically
active  or  "labile"  in  the  context  of  detection  by  stripping
voltammetry.  All other complexes  (e.g. strong organic complexes)
will be electrochemically inert, or "non-labile", passing through
the  electrode  diffusion  layer  without  dissociation and  hence
yielding no measurable current.
     Assuming  that  there  are no  electroactive organic  cadmium
complexes  in  solution,  the  measured  current  will  be  directly
proportional to the  concentration of Cd', where [Cd']  is the total
concentration of dissolved inorganic cadmium  species present (i.e.
free hydrated Cd2* plus inorganic complexes)  (Bruland, 1992).  Cd'
is related  to the concentration  of the  free ion,   [Cd2+],  by an
inorganic  side  reaction  coefficient,  such   that   [Cd'] = [Cd2*]acd.
(Ringbom and Still,  1972).
     In the absence of electrochemically inert cadmium complexes,
titration   of   the   samples   with  cadmium   should   yield  Cd'
concentrations   equivalent   to   the    total   dissolved   cadmium
concentration measured by ICP-AES.  For the purposes  of this study,
the  extent  of  cadmium complexation by natural organics  in  the
source water should  be negligible.  Even if  we assume an initial
binding ligand concentration in the diluted source water of 10 nM

                                11

-------
                        Hg Electrode
                       * + ne'-> M°(Hg)
+ pL
                                        Diffusion
                                        Layer
                                        Bulk
                                        Solution
Figure  1.   Dissociation and reduction of a  metal  complex at a
         mercury electrode  (after Florence,  1986).   (M and L  are
         the metal and complexing ligand  respectively,  and fc is
         the rate of reaction for the dissociation  (kj  or the
         formation (k{) of the netal-ligand complex ML.
                             12

-------
(an'order of magnitude  above reported values for seawater),  this
represents  less  than  4%  of  the total  cadmium  in the  lowest
concentration sample  (32 ppb). The organic complexation of cadmium
will  be unimportant  assuming that  the test  organisms did not
produce prodigious amounts of complexing material over the course
of the experiment.

Cadmium Speciation Calculations
     The  solution speciation of  cadmium  with  respect to  free
hydrated ions and inorganic complexes in the sample solutions was
estimated using MINEQI/  (Schecher and McAvoy,  1991), an interactive
PC version  of  the original  MINEQL equilibrium modeling program.
MINEQL  (Westall et al.,  1976),  and its predecessor REDEQL (Morel
and Morgan,  1972),  utilizes equilibrium constants to  solve  mass
balance  expressions,  using  a modified  Newton-Raphson  iterative
procedure.
     The  input  for  MINEQL*  consists  of  the  total  solution
concentrations of  all components to be modeled  and  an extensive
data base of equilibrium constants for the formation of solution
species and solid  phases consisting  of combinations  of the basic
components.    For  the  purposes  of  this  study, the  components
consisted of the cadmium ion, the major and minor seawater cations
and anions, and H* (Table 1).
     The concentrations of the seawater ions were calculated based
upon the sample salinity and the relative proportions of each ion
in natural seawater.  Based on information supplied by the

                                13

-------
Table 1.  Dissolved solution  components  for  MINEQL  equilibrium
          modeling program.
                                         Anions
                  Na*                       Cl"
                   K*                       Br~
                  Ca2*                       F-
                  Mg2*                      C032~
                  Sr2+                      S042'
                  Cd2*
                                 14

-------
manufacturer, the major ion composition of the "MarineMix" used to


amend sample salinities to 15 and 25 ppt is equivalent to that of


natural seawater.  Therefore, no correction was necessary for the


use of commercial salts rather than natural seawater.  The hydrogen


ion concentration (pH)  was considered as a fixed parameter, set to
                                                t
the pH measured in each sample.   In the  absence of total inorganic
                     -•*.

carbon or alkalinity measurements, the samples were assumed to be


in equilibrium with the atmosphere with respect  to the carbonate


system  (pC02  =  10'3 5  atm).    It  was  further  assumed that  no


precipitation of  the mineral phase  otavite  (CdC03)  occurred over


the course of the 96 h experiments.   Total cadmium concentrations


were within  8%  and 16% of the nominal  concentrations  added for


Cyprinodon  and  Eurytemora  tests,   respectively,  indicating  no


significant removal of cadmium due to precipitation reactions.





Statistical Analysis


     The 96h LC50 values with 95% confidence limits were generated


from the mortality data using the Trimmed Spearman-Karber method


(Hamilton, et al., 1978).  The LC50 values from adjacent salinities


were  compared  by standard  error  of  means   (USEPA,   1985a)  to


determine significant effect  (p<0.05).
                                15

-------
                             RESULTS
Water Quality and Cadmium Chemistry
     Water quality conditions measured every other day during the
six 96 h toxicity tests are presented in Table 2.   All conditions
appeared  adequate  for  survival  of  test species.   Nominal  and
measured concentrations of total cadmium  on day 0 and 4 during the
acute  tests  are  shown  in  Table  3  and  Figure  2.    Measured
concentrations were very similar to the nominal concentrations in
all tests as the relative standard deviation ranged from  0.42 to
6.89 %.   In most instances, the relative standard  deviation was
less than 3%. All  three saline controls contained  no detectable
cadmium at a detection limit of 3  M9/L-
     Four samples were selected for  voltammetric  analysis (Table
4) .  The resulting titration curve in Figure 3 was linear in each
instance thus suggesting no significant organic complexation  (r2 >
0.997).  The presence of strong, electrochemically inert complexes
would  result  in a  significant deviation from  linearity at  low
cadmium concentrations  (Bruland, 1992).  The electroactive cadmium
concentrations agreed  within  2.5  to 5  % with the  total cadmium
values determined by  ICP-AES,  indicating that the  speciation of
cadmium  in  the  test solutions is  dominated  by the free  ion  and
inorganic complexes  (Table 4).  Voltammetric analysis  therefore
yeilded  no   additional  information  beyond  the  total  dissolved
cadmium  concentrations,  rendering  it unnecessary to  perform ASV
measurements  with  every  sample.    Note that  the  voltammetric
analyses also serves as an independent  check upon the accuracy of

                               16

-------




•
o
4J
O
O
4J
IT
•H
O
•H
X
o
•P

9
*^
1
o
£
1
«o
O\
3
4J
O»
•H
t.
1
ID
0
•H
*J
•H
•o
§
o
>,
4J
•H
iH
(0
&
• .
fe
4J
«
3
C
•H
•
1
3
•
(M
9
iH
A
£



dS"
Q^



M§
a a
to ^





••4
i






a
« o"
H ~



>•
P
j i _^j -
4J •« »•»
a c 4*
«^j a
l^j ^j n
C^ r+ Gt
0 *-»
(0



•
•H
O
i
^ o\ C4
• • t
c r^ r>-
1 l
n in «*
• • •
*» r» «o



>o « r-
H M
1 1 1

m •* *
r4 CM

* co m
r* «o *
• • •
CO CO CO
1 1 1
n en ot
m o co
• • •
i- co r*



in in
CM CM
*•
1 CM 1

* «*
«M CM



m m in
H CM




«
•*j
q
s
«J
•
M
r» ^- a»
• • •
r* r- vo
l i l
f- O ^
• • •
•c «o in



\o to  t^
* t-> o»
t- r- r*



in in in
CM CM CM
i i i

^ ^ ^"
CM CM CM



in in in
H CM



10
s
&
•
1
^
•
o
17

-------
Table s .  Total cadmium concentrations as determined by  ICP-AES.
          Nominal cadmium values represent the original  cadmium
          concentrations added to the samples at the beginning
          of each experiment.  (Analytical precision is  reported
          as the standard deviation and the coefficient  of variation
          (C.V.) based upon replicate analyses (n-5) of  the same sampli
Nominal Measured
Organism Time Salinity
Cyprinodon
Cyprinodon
Cyprinodon
Cyprinodon
Cyprinodon
Cyprinodon
Cyprinodon
Cyprinodon
Cyprinodon
Cyprinodon
Cyprinodon
Cyprinodon
Cyprinodon
Cyprinodon
Cyprinodon
Cyprinodon
Cyprinodon
Cyprinodon
Eurytemora
Eurytemora
Eurytemora
Eurytemora
Eurytemora
Eurytemora
Eurytemora
Eurytemora
Eurytemora
Eurytemora
Eurytemora
Eurytemora
Eurytemora
Eurytemora
Eurytemora
Eurytemora
Eurytemora
Eurytemora
DO
DO
DO
D4
D4
D4
DO
DO
DO
D4
D4
D4
DO
DO
DO
D4
D4
D4
DO
DO
DO
D4
D4
D4
DO
DO
DO
D4
D4
D4
DO
DO
DO
D4
D4
D4
5
5
5
5
5
5
15
15
14
15
15
16
25
25
25
26
26
26
5
5
5
6
6
6
14
14
14
14
15
14
24
24
24
26
27
26
[Cd]
56
180
1000
56
180
1000
100
320
1800
100
320
1800
180
560
3200
180
560
3200
32
100
560
32
100
180
32
100
560
32
100
560
56
180
560
56
180
560
[Cd]
52.98
166.10
963.01
55.88
177.09
994.23
97.53
312.99
1736.46
99.81
318.12
1893.76
175.01
559.11
3274.89
183.77
561.38
3252.98
27.01
93.17
550.10
28.16
92.27
168.86
30.21
100.19
535.90
28.16
88.29
501.66
50.51
176.37
523.50
49.44
160.28
518.72
Std.
Dev.
1.12
2.04
24.78
0.74
1.88
18 . 69
2.66
6.89
19.47
3.25
6.15
8.64
1.84
15.81
125.69
6.02
2.36
101.08
0.87
0.97
15.67
1.94
1.11
3.65
1.10
1.47
7.96
1.30
1.98
17.70
0.52
5.. 90
4.95
2.80
1.99
13.29

C.V.
2.12
1.23
2.57
1.33
1.06
1.88
2.73
2.20
1.12
3.25
1.93
0.46
1.05
2.83
3.84
3.28
0.42
3.11
3.23
1.04
2.85
6.89
1.21
2.16
3.64
1.47
1.49
4.61
2.24
3.53
1.03
3.34
0.94
5.66
1.24
2.56
                                18

-------
      3500
            0    500  1000  1500  2000 2500  3000  3500
         600
                                       (b) Eurytemora
                                        i	i
             0     100    200   300    400    500   600

                Nominal Cadmium Concentration (//.g/L)

Figure 2. Total cadmium as determined by ICP-AES versus the
          nominal cadmium concentrations added to samples at the
          beginning of the experiments.   The  solid lines represent
          the expected 1:1 lines for  perfect  agreement between the
          data sets.           19

-------
Table 4.  Voltammetric   analysis   of  selected   samples.   [Cd']
          represents the sum of all electroactive cadmium species.
          [Cd] is the value from ICP-AES analysis.
Organism
Time
ICP-AES
 Salinity
[Cd]
[Cd']
Cyprinodon
Cyprinodon
Eurytemora
Eurytemora
     D4
     D4
     D4
     D4
    15
    26
     6
    14
 99.81     95.10
183.77    179.81
 28.16     27.49
 28.16     28.92
                               20

-------
      <
      c
      c
      £
      3
      o
      jse
      o
      «
      0.
20.59 X + 56.48
                         2345

                       Cadmium added (/xg/L)
Figure 3. Titration curve for the voltaametric analysis  of
          Eurvtemora. 5 ppt salinity,  32 M9/L Cd, t-4.   The solid
          and  dotted  lines  represent the linear regression  and
          95%  confidence intervals,  respectively,  through the
          data.
                                21

-------
the ICP-AES results for total dissolved cadmium.
     The inorganic cadmium  speciation  as  predicted by MINEQL+ is
present in Table 5 and  6.   The predicted  concentrations for each
dissolved species in terms of concentration is presented in Table
5 while Table  6 lists  the  species  as  a percentage  of the total
cadmium in solution.   Seven  species were identified as significant
(>1%) : the free hydrated ion (Cd2*); carbonate and sulfate complexes
(CdCO3 and CdS04)  and the four  chloride complexes (CdCl*,  CdCl2°,
CdCl3~, and CdOHCL0.  The speciation was  dominated at all salinities
by CdCl* and  CdCl2°.   The free ion accounted for 20, 8 and 4.5% of
the total  dissolved  cadmium at  5,  15  and  25  ppt,  respectively.
Small variations between  tests were due to small differences in
sample pH and salinity.

     Toxicity Data
     Ninety-six hour LC50 values for E. affinis and C. variegatus
are presented in Table 7 (See Appendix A for raw data) . The copepod
values were 51.6, 213.2  and  82.9 M9/L total cadmium at 5,  15 and 25
ppt,  respectively.    Acute  toxicity values for  Cyprinodon  were
180.3, 312.4 and  495.5 nq/L total cadmium at 5,  15  and 25 ppt,
respectively.  A comparison of LC50 values for E.  affinis between
various salinities showed  a  significant difference  between 5 and 15
ppt and between 15  and 25  ppt (Table 8).  There was no significant
difference in  LC50  values  between  5 and  25  ppt.   A comparison
between the various LC50 values for Cyprinodon showed a significant
increase with salinity  (Table 8).   The LC50 at 5 ppt was

                                22

-------
Table  5 .  Thermodynamic equilibrium model results as a function of species
           concentration.  Equilibrium modeling was done using the MINBQL+
           interactive personal computer program.


Org. Time
Cyp.
Cyp.
Cyp.
Cyp.
Cyp.
Cyp.
Cyp.
Cyp.
Cyp.
Cyp.
Cyp.
Cyp.
Cyp.
Cyp.
Cyp.
Cyp.
Cyp.
Cyp.
Eur.
Eur.
Eur.
Eur.
Eur.
Eur.
Eur.
Eur.
Eur.
Eur.
Eur.
Eur.
Eur.
Eur.
Eur.
Eur.
Eur.
Eur.
DO
DO
DO
D4
D4
D4
DO
DO
DO
D4
D4
D4
DO
DO
DO
D4
D4
D4
DO
DO
DO
D4
D4
D4
DO
DO
DO
D4
D4
D4
DO
DO
DO
D4
D4
D4

Sal
5
5
5
5
5
5
15
15
14
15
15
16
25
25
25
26
26
26
5
5
5
6
6
6
14
14
14
14
15
14
24
24
24
26
27
26

pH
7.63
7.62
7.56
7.5
7.46
7.57
8.03
8.06
8.06
7.75
7.73
7.87
8.21
8.21
8.22
7.93
7.91
8.01
7.62
7.60
7.63
8.09
8.11
8.1
8.09
8.13
8.13
8.32
8.38
8.37
8.18
8.16
8.23
8.24
8.15
8.45
Total
[Cd]

52.98
166.10
963.01
55.88
177.09
994.23
97.53
312.99
1736.46
99.81
318.12
1893.76
175.01
559.11
3274.89
183.77
561.38
3252.98
27.01
93.17
550.10
28.16
92.27
168.86
30.21
100.19
535.90
28.16
88.29
501.66
50.51
176.37
523.50
49.44
160.28
518.72
Predicted Cone, of
Cd(2+) CdOHCl
10.33
32.48
188.83
10.99
35.07
194.45
7.81
24.84
146.12
8.27
26.41
146.12
7.74
24.62
143.87
8.26
25.40
145.00
5.26
18.21
107.23
4.42
14.27
26.30
2.54
8.31
44.51
2.09
5.91
35.74
2.37
8.37
24.05
2.06
6.62
19.78
0.57
1.74
8.85
0.45
1.30
9.34
2.26
7.72
43.39
1.26
3.83
30.46
5.02
15.96
95.65
2.83
8.28
59.80
0.28
0.94
5.90
0.79
2.69
4.82
0.81
2.90
15.51
1.16
4.00
22.59
1.38
4.64
15.85
1.48
3.93
23.27
CdCl +
32.26
101.38
590.10
34.28
109.37
608.08
51.14
162.98
916.06
54.06
173.10
996.99
74.97
239.41
1393.76
80.48
247.28
1416.24
16.41
56.87
334.95
15.62
50.58
92.84
15.85
52.04
278.75
13.49
40.35
232.67
22.14
77.78
225.92
20.57
67.33
200.07
Dissolved Complexes (ug/L)
CdC13 -
0.35
1.08
6.31
0.37
1.17
6.51
4.11
13.04
64.74
4.34
13.83
90.03
15.85
50.36
294.49
18.10
55.30
318.09
0.18
0.61
3.57
0.23
0.76
1.39
1.12
3.69
19.67
0.97
3.32
16.75
4.30
15.06
44.29
4.69
16.30
45.75
CdC12.
6.87
21.58
125.89
7.31
23.27
129.26
27.31
87.00
460.84
28.89
92.06
560.88
62.83
200.07
1168.96
69.01
211.31
1213.92
3.50
12.14
71.26
3.87
12.59
23.04
8.00
26.19
140.50
6.89
22.03
119.14
17.87
62.61
183.21
17.98
60.13
175.34
CdCO3
0.66
1.98
8.74
0.39
1.02
9.44
2.63
9.62
57.32
0.77
2.24
23.27
5.63
17.98
109.59
1.63
4.55
41.36
0.32
1.01
6.85
2.28
8.09
14.16
1.15
4.50
24.05
2.75
10.21
59.57
1.51
4.83
19.33
1.71
3.60
43.50
CdS
1.
5.
29.
1.
5.
30.
1.
5.
31.
1,
5,
31.
2.
7,
43
2
6
38
0
2
16
0
2
4
0
1
9
0
1
9
0
2
7
0
1
6
                                       23

-------
Table  6.   Thermodynamic equilibrium model  results as a percentage of the
           total  cadmium concentration.   Equilibrium modeling was done using
           the MINEQL+  interactive personal computer program.


Org. Time
Cyp.
Cyp.
Cyp.
Cyp.
Cyp.
Cyp.
Cyp.
Cyp.
Cyp.
Cyp.
Cyp.
Cyp.
Cyp.
Cyp.
Cyp.
Cyp.
Cyp.
Cyp.
Eur.
Eur.
Eur.
Eur.
Eur.
Eur.
Eur.
Eur.
Eur.
Eur.
Eur.
Eur.
Eur.
Eur.
Eur.
Eur.
Eur.
Eur.
DO
DO
DO
D4
D4
D4
DO
DO
DO
D4
D4
D4
DO
DO
DO
D4
D4
D4
DO
DO
DO
D4
D4
D4
DO
DO
DO
D4
D4
D4
DO
DO
DO
D4
D4
D4

Sal
5
5
5
5
5
5
15
15
14
15
15
16
25
25
25
26
26
26
5
5
5
6
6
6
14
14
14
14
15
14
24
24
24
26
27
26

PH
7.63
7.62
7.56
7.5
7.46
7.57
8.03
8.06
8.06
7.75
7.73
7.87
8.21
8.21
8.22
7.93
7.91
8.01
7.62
7.60
7.63
8.09
8.11
8.1
8.09
8.13
8.13
8.32
8.38
8.37
8.18
8.16
8.23
8.24
8.15
8.45
Total
[Cd]
Predicted Cadmium Speciation
As A Percentage of Total [Cd]
(Mg/L) c<*(2+) CdOHCl CdCl + CdC13 -
52.98
166.10
963.01
55.88
177.09
994.23
97.53
312.99
1736.46
99.81
318.12
1893.76
175.01
559.11
3274.89
183.77
561.38
3252.98
27.01
93.17
550.10
28.16
92.27
168.86
30.21
100.19
535.90
28.16
88.29
501.66
50.51
176.37
523.50
49.44
160.28
518.72
19.5
19.5
19.6
19.7
19.7
19.6
8.0
7.9
8.5
8.3
8.3
7.7
4.4
4.4
4.4
4.5
4.5
4.5
19.5
19.6
19.5
15.7
15.5
15.6
8.4
8.3
8.3
7.4
6.7
7.1
.7
.7
.6
.2
.1
3.8
1.1
1.0
0
0
0
0
2.3
2.5
2.5
1.3
1.2
1.6
2.9
2.9
2.9
1.5
1.5
1.8
1.0
1.0
1.1
2.8
2.9
2.9
2.7
2.9
2.9
4.1
4.5
4.5
2.7
2.6
3.0
3.0
2.4
4.5
60.9
60.9
61.2
61.5
61.6
61.2
52.4
52.1
52.9
54.2
54.3
52.8
42.8
42.8
42.6
43.9
44.0
43.6
60.9
61.0
60.9
55.3
54.8
55.0
52.5
52.0
52.0
47.9
45.8
46.5
43.8
44.1
43.2
41.7
41.9
38.6
0
0
0
0
0
0
.2
.2
.7
.3
.4
.8
9.0
9.0
9.0
9.8
9.9
9.8
0
0
0
0
0
0
3.7
3.7
3.7
3.4
3.8
3.4
8.5
8.5
8.4
9.5
10.2
8.8
CdC12
13.0
13.0
13.0
13.1
13.1
13.0
28.0
27.8
26.6
28.9
28.9
29.7
35.9
35.9
35.8
37.7
37.7
.37.4
13.0
13.0
13.0
13.7
13.6
13.7
26.5
26.2
26.2
24.5
25.0
23.9
35.4
35.5
35.0
36.3
37.4
33.8
CdC03
1.2
1.2
0
0
0
0
2.7
3.1
3.3
0.0
0.0
1.2
3.2
3.2
3.3
0
0
1.3
1.2
1.1
1.2
8.1
8.8
8.4
3.8
4.5
4.5
9.8
11.6
11.9
3.0
2.7
3.7
3.5
2.2
8.4
CdS(
3,
3,
3,
3,
3,
3,
1,
1.
1.
1,
1,
1,
1,
1,
1,
1
1
1
3
3.
3
2,
2
2
1
1
1,
1
1
1
1
1
1,
1,
1.
1,
* 0 - less than 1Z
                                       24

-------
Tabje 7.  Ninety-six  h LC50  values (M9/L)  (with 95%  confidence
          limits) and mean control  survival  for  E. affinis and C.
          variegatus tested at three salinities.
Species        Test           Mean            96-H LC50
               Salinity       Control         (95% C.L.)
               (ppt)          Survival
                              %  (S.E.)
E. affinis        5           91.7 :(8.3)       51.6  (36.2-73.5)

                 15           97.0 (3.0)      213.2  (182-249.7)

                 25           80.0 (5.8)       82.9  (51.1-134.3)


C. variegatus     5          100              180.3  (151.5-214.5)

                 15           93.3 (3.3)      312.4  (275.1-354.7)

                 25          100           .   495.5  (420.9-583.2)
                               25

-------
Table 8.  A comparison of LC50 values between adjacent salinities
          using the standard Error of Means Method.
Species
Salinity
 (PPt)
Z Value
H Value
Significant
  (P<-05)
S. affinls      5-15

               15-25

                5-25

C. variegatus   5-15

               15-25

                5-25
4.1348
2.5729
1.6071
1.7222
1.6129
2.7778
1.4736
1.6614
1.8192
1.2166
1.2112
1.2384
*
*

*
*
*
                                26

-------
          significantly  lower  than  15  ppt and  the value at  15 ppt  was
          significantly  lower  than  25  ppt.  The value  at 5  ppt was  also
          significantly lower than at 25 ppt.
I
                                         27

-------
                            DISCUSSION
     Voltamroetric analysis  of  selected  samples  were in excellent
agreement with the ICP-AES measurements.  Standard addition curves
were linear, indicating no significant organic complexation.  The
"cadmium complexing capacity" of the experimental sample matrix was
therefore  negligible.    Furthermore,  there  was  no  significant
production of cadmium binding  ligands by  the test organisms over
the course  of the  experiments.   The  data presented above were
important for these  experiments because it was  demonstrated that
cadmium  speciation  was dominated  by association with  inorganic
binding ligands.
     In freshwater at pH of  6,  Turner et al.  (1981) predicted that
the  inorganic  cadmium  would  be  approximately  96%  free  with
carbonate complexes becoming important at higher pH.  In seawater
at 35 ppt and a pH of  8.2, the chloride complexes were predicted to
account  for  approximately 97%  of the inorganic species  with the
free ion responsible for less than  3% of the total (Turner et al.,
1981; Bryne et al.,  1988). Assuming that only chemical factors are
important  and the  organic  ligands  are  negligible, the  cadmium
toxicity  due  to  Cd*2  would  be  expected  to decrease  significantly
over the  course of an entire estuary (i.e., Chesapeake Bay) where
salinity may range from 1  to greater than 26 ppt. At natural total
cadmium  concentrations,  binding  of  cadmium  by  strong  complexing
ligands may reduce toxicity even further.
     The  inorganic complexation of  cadmium in the sample solutions
was estimated by the  use  of the MINEQL+ thermodynamic equilibrium

                               28

-------
model.   Model results indicated that the  cadmium speciation was
largely dominated by complexation with the chloride ion, with small
contributions by  the free  ion and  carbonate and sulfate species.
The free ion decreased from 20% of the total dissolved cadmium at
5 ppt to less than  5%  of the of  the  total at  25  ppt salinity.
Similar data have been reported by other investigators as more free
cadmium was present at low salinities varing in logarithmic fashion
from  about 23% of total as free cadmium at 5 ppt to only about 4%
at 32 ppt  (Sunda  et al.,  1978;  Engle and Fowler, 1979).  Our data
would suggest a  four fold decrease in toxicity  from 5 to 25 ppt
assuming that the free  ion is bioactive form of the  element and
physiological factors of the test  species are  negligible.   The
toxicity data with Cyprinodon  generally support this prediction as
there is approximately a three fold decrease in toxicity from 5 to
25 ppt.   The Eurytemora data however do not  support this prediction
as the 96 h LC50  values  at both 5  and  25 ppt were similar.  This
species was most  resistant to cadmium  at the middle salinity (15
ppt) .   The  physiological characteristics  of Eurytemora  may have
been  responsible for higher  tolerance  at the  middle  salinity.
Sprague  (1985)  has  suggested that  euryhaline  species are  most
resistent  to toxic  conditions at isosmotic  salinities due  to
minimization  of  osmotic stress.   Other investigators have  also
reported there  is   decreased osmotic  stress in various  aquatic
species as salinity  increases toward the isosmotic point,  with a
decreased  inward  flow  of  water,  which  presumably  would  be
accompanied by reduced intake  of toxic ions (Herbert and Wakefield,

                                29

-------
1964; Herbert and Shurben, 1965).
     The 96 h LC50 values for E.  affinis reported from the three
cadmium toxicity tests at the various salinities ranged from 51.6
to 213.2 M9/L total  cadmium.   Sullivan et al.  (1983)  reported a
similar 96 h LC50 of  147.7 ng/L total cadmium for E. af finis at 10
ppt.  Another  investigator  reported a substantially higher 96 h
LC50 of 1,080 M9/L total cadmium for Eurytemora (Gentile, 1982).
Acute toxicity values ranging from 90 to 337 /ig/L total cadmium at
30 ppt  for a similar copepod species,  Acartia tonsa  were also
similar to our  Eurytemora  data (Gentile,  1982; Sosnowski  and
Gentile, 1978).   The  lowest LC50  value  (51.6 M9/L) reported for E.
af finis in our experiments was only slightly higher than the U.S.
EPA acute  marine water quality  criterion  of 43  pg/L  (U.S.  EPA,
1987).  The range of  acute cadmium  values  reported for saltwater
invertebrate species  in the U.S.  EPA cadmium water quality criteria
document was 41.29 to  135,000 M9/L total cadmium  (U.S. EPA, 1985b).
These data  suggest that  Eurytemora is very  sensitive  to cadmium
when compared with other estuarine aquatic biota.
     The 96 h LC50 values for Cyprinodon larvae ranged from 180.3
to 495.5 M9/L total cadmium at the  three test  salinities. Cardin
(1982) reported  acute  toxicity values  of 577 to 602  Mg/L for the
larval stages of the Atlantic silverside and the winter flounder,
respectively at  20  ppt.   These  values are similar to  the acute
LCSOs we reported for Cyprinodon.  Other  investigators have reported
higher acute values for other larval estuarine fish.  Middaugh and
Dean (1977) reported 48 h LC50s of 9,000 and 32,000 /ig/L for 7 and

                               30

-------
14  .day  larval  mummichogs,  respectively  at  20  ppt.    These
investigators also reported 48 h LC50s of 3,800, and 2,200 nqfL for
1 and 14 day old Atlantic silverside larvae at 20 ppt.
     In a recent review synthesizing the influence of salinity on
the toxicity of various classes of chemicals, it was reported from
33  cadmium  toxicity  studies  that  cadmium  toxicity  generally
increased with decreasing salinity (Hall and Anderson, 1994). The
Cyprinodon data from the experiments follow this trend as 96 h LC50
values were significantly lower at lower  salinities thus suggesting
that cadmium bioavailablity  (chemical factors) were the predominant
mechanism for  toxicity.   The Eurytemora data do not follow this
trend due to the  physiological factors  previously  discussed. One
important aspect  of this study was  the calculation  of the free
cadmium  along  with  the  total  cadmium  concentration  in  the
experiments.   The free cadmium ion  (Cd*2) is generally considered
to be  the toxic  form  of  cadmium to  aquatic  biota  in  the water
column  and  it  is virtually inversely  proportional  to salinity
(Sunda et al., 1978; Engle and Fowler, 1979).  A calculation of 96
h LC50s for free  cadmium for Eurytemora  based  on using 20,  8 and
4.5% of the total  cadmium at 5,  15 and 25 ppt, respectively, showed
that free  cadmium was  still  less toxic  at the middle salinity
(Figure 4) .  The calculated free cadmium  LC50 values for Cyprinodon
were similar at both 15 and 25 ppt but  were somewhat higher at 5
ppt  (Figure 4).
                                31

-------
 CO
 «
•H
 §
i
is
 «^
 * «
 14
 O
 CD
 Q>
O

10
  s
I
•H
Pk
 (0
 0
'o
 0)
 a
to
'c
(C
O)
0)
jj:   ro
 to   >

LU   (J
                                                                 LO
                                                                 CM
                                                                 IT)
                                                                      CO
            o
            in
                 O
                 CO
                      O
                      CM
                                    32

-------
                         ACKNOWLEDGEMENTS







     We are grateful to  the  U.S.  Environmental Protection Agency



Chesapeake  Bay  Program  and  the  Maryland  Department  of  the



Environment for funding  this  research.   Special consideration is
                                                •


extended to Mr. Richard Batiuk, Ms. Deirdre Murphy and Mrs. Mary Jo



Garreis  for  comments  on  the  study design.    Mary Hancock  is



acknowledged for typing.
                                33

-------
                            REFERENCES

Brand, L.E., Sunda, W.G., and Guillard, R.R.L.  1983.  Limitation
     of marine phytoplankton reproductive rates by zinc, manganese
     and iron.  Linnol. Oceanogr., 28:1182-1198.
Brand, L.E.., Sunda, W.G., and Guillard, R.R.L.  1986.  Reduction
     of  marine phytoplankton  reproduction  rates  by  copper and
     cadmium.  J. Exp. Mar. Biol. Ecol., 96:225-250.
Bruland, K.W.   1992.   Complexation of cadmium by natural organic
     ligands  in the central  North Pacific.   Limnol. Oceanogr.,
     37:1008-1017.
Byrne, R.H., Kump, L.R., and Cantrell, K.J.  1988.  The influence
     of temperature and pH on trace metal speciation in seawater.
     Mar. Chem., 25:163-181.
Cardin, J.A.   1982.   Memorandum to J.H.  Gentile.   United States
     Enivronmental Protection Agency, Narragansett, RI.
Engel, D.W., and Fowler,  B.A.   1979.   Copper and cadmium induced
     changes  in the metabolism  and structure  of  molluscan gill
     tissue.  In Marine Pollution: Functional Responses, Vernberg,
     W.B.,  Thurberg,   F.P.,  Calabrese,  A.,  and  Vernberg,  F.J.
     (eds.). Academic Press, New York, NY, pp. 239-256.
Florence, T.M.  1986.   Electrochemical approaches to trace element
     speciation in waters - a review.  Analyst, 111:489-505.
Gentile, S.H.  1982.   Memorandum to John H. Gentile. United States
     Environmental Protection Agency, Narragansett, RI.
Guillard,  R.R.L.    1975.    Culture  of phytoplankton  for feeding

                                34

-------
     marine  invertebrates.   In  Culture of  Marine  Invertebrate
     Animals,  Smith,  W.L.,  and  Chanley,  M.H.   (eds.).   Pleum
     Publishing, New York, pp.  29-60.
Hall,  L.W. Jr.,  and Anderson,  R.D.    1994.   The  influence of
     salinity  on the toxicity of various classes of  chemicals to
     aquatic biota.  Report.  Maryland Department of  Environment,
     Baltimore, MD.
Hall, L.W. Jr., Ziegenfuss, M.C., Anderson, R.D., Spittler,  T.D.,
     and  Leichtveis, H.C.   in  press.    Influence  of salinity on
     atrazine  toxicity  to  a Chesapeake  Bay  Copepod  (.Eurytejnora
     affinis)  and fish (Cyprinodon  variegatus; . Estuaries.
Hamilton,  M.A., Russo,  R.C., and Thurston, R.V.   1978.  Trimmed
     Spearman-Karber   method   for   estimating  median  lethal
     concentrations in toxicity bioassays.  Environ.  Sci. Technol.,
     11:714-719.
Herbert,  D.W.M., and Shurben,  D.S.   1965.  The susceptibility of
     salmonid  fish to poisons under  estuarine conditions  - II
     ammonium  chloride. Jnt. J. Air Wat. Poll., 9:89-91.
Herbert,  D.W.M., and Wakeford, A.C.  1964.  The susceptibility of
     salmonid  fish to poisons under estuarine  conditions - I zinc
     sulphate.  Int. J. Air Wat.  Poll.,  8:251-256.
Middaugh,  D.D., and Dean,  J.M.   1977.   Comparison sensitivity of
     eggs, larvae  and adults of the estuarine teleosts, Fundulus
     heteroc.Zitus and Menidia menidia to cadmium.  Bull. Environ.
     Contain. Toxicol.,  17:645-652.  .
Morel,  F., and  Morgan,  J.J.    1972.   A  numerical  method for

                                35

-------
     computing equilibria  in aqueous  chemical  systems. Environ.
     Sci. Tech.,  6:58-67.
Ringbom, A., and  Still,  E.  1972.  The calculation and use of alpha
     coefficients.  Anal. Chim. Acta., 59:143-146.
Schecher,  W.D.,  and  McAvoy,  D.C.    1991.   MINEQL*:  A Chemical
     Equilibrium Program for Personal Computers,  User's Manual,
     Version 2.22.  Environmetal Research Software, Hallowell, ME.
Sosnovski, S., and Gentile, J.H.  1978.  Toxicological comparison
     of  natural  and  cultural  populations of  Acartia tonsa  to
     cadmium,  copper and  mercury.  J.  Fish.   Res.  Board  Can.,
     35:1366-1369.
Sprague,  J.B.    1985.     Factors  that  modify  toxicity.    In
     Fundamentals  of  Aquatic   Toxicology,   Rand,   G.M.,   and
     Petrocelli,   S.R.   (eds.).     Hemisphere   Publishing  Co.,
     Washington,  DC,  pp. 124-163.
Sullivan, B.K.,   Buskey,  E., Miller, O.C., and Ritacco,  P.J.  1983.
     Effects of copper and cadmium on growth,  swimming and predator
     avoidance  in £uryte;nora  affinis  (Copepoda).  Mar.  Biol.,
     77:299-306.
Sunda,  W.G.,  Engel,   D.W.,  and  Thuotte,  R.M.   1978.    Effect  of
     chemical speciation on toxicity  of  cadmium to grass shrimp,
     Palaemonetes pugio: Importance of free cadmium ion. Environ.
     Sci. Technol.,  12:409-413.
Sunda, W.G., Tester,  P.A., and  Huntsman,  S.A.   1987*  Effects of
     cupric  and  zinc   ion  activities   on  the  survival  and
     reproduction of marine copepods. Mar. Biol., 94:203-210.

                                36

-------
Sunda, W.G., Tester, P.A., and Huntsman, S.A.  1990.  Toxicity of
     trace  metals to  Acartia  tonsa in  the Elizabeth  River and
     southern Chesapeake Bay.  Estuar. Coast. Shelf Sci., 30:207-
     221.
Turner,  D.R.,   Whitfield,  M.,  and  Dickson,  A.G.    1981.    The
     equilibrium  speciation of dissolved components in freshwater
     and seawater at 25°C and 1 atm pressure.  Geochim. Cosmochim.
     Acta., 45:855-881.
U.S. EPA  (United States Environmental Protection Agency).  1985.
     Ambient water quality criteria for cadmium -  1984.  U.S. EPA,
     Office  of  Water  Regulations  and  Standards,  Criteria  and
     Standards Division, Washington, DC.
U.S. EPA (United  States Environmental Protection Agency).  1985b.
     Methods  for measuring the  acute toxicity  of effluents  to
     freshwater and marine organisms.   3rd ed.  EPA 600/4-85-013.
     Environmental  Monitoring  and  Support Laboratory,  U.S.  EPA
     Cincinnati,  OH.
U.S. EPA  (United  States Environmental  Protection  Agency).   1987.
     Water  quality  criteria  summary.  U.S. EPA  Office  of  Water
     Regulations  and Standards,  Criteria and Standards Division,
     Washington,  DC.
U.S. EPA  (United  State Environmental Protection Agency).  199la.
     Chesapeake  Bay toxics of  concern list  information sheets.
     Report.  U.S. EPA Chesapeake Bay Program, Annapolis, MD.
U.S. EPA  (United States Environmental Protection  Agency).  1991b.
     Methods  for measuring the  acute  toxicity of  effluents and

                                37

-------
     receiving waters to freshwater and marine organisms, 4th ed.
     Weber, C.I. (ed.).  EPA/600/4-90/027.   U.S.; EPA, Cincinnati,
     OH, pp. 66-67.
Westall, J.C., Zachary, J.L.,  and Morel, F.M.M.  1976.  MINEQL, A
     Computer Program for the Calculation of Chemcial Equilibrium
     Composition of Aqueous  Systems.  Technical Note 18, Department
     of    Civil    Engineering,    Massachusetts   Institute   of
     Technolnology.,  Cambridge,  MA.         :
                                38

-------
                APPENDIX A







Raw data from the Eurytemora and Cyprinodon



  96 h toxicity tests at three salinities

-------

-------
96 h Eurytemora Tests
                              #  Alive/Total per Rep     x % Survival
Salinity  Cd cone  (mg/L)      A         B         c
5 ppt 0
.032
.056
.100
.180
15 ppt 0
.032
.056
.100
.180
.320
.560
25 ppt 0
.056
.100
.180
.320
.560
8/8
2/8
3/8
4/7
0/7
10/10
8/10
8/11
10/11
9/10
1/11
0/11
9/10
7/10
0/10
5/10
1/11
0/12
8/8
6/8
4/8
0/7
0/7
10/10
12/12
11/13
10/10
8/11
1/10
0/10
7/10
6/10
3/10
5/12
0/11
0/10
6/8
6/8
5/9
1/8
0/7
10/11
9/10
9/10
il/12
8/10
0/11
0/12
8/10
6/10
8/11
4/10
0/11
0/10
91.7
66.7
47.7
23.2
0
97
90
83
94
81
6
0
80
63.3
35.5
43.8
3
0
                               A-l

-------
96 h Cyprinodon Tests
Salinity
5 ppt






15 ppt






25 ppt






Cd cone (mg/L)
0
.056
.10
.18
.32
.56
1.00
0
.10
.18
.32
.56
1.00
1.80
0
.18
.32
.56
1.00
1.80
3.20
# Dead/ 10
A
0
1
1
8
9
10
10
1
0
2
4
10
10
10
0
1
2
6
9
10
10
per Rep
B
0
0
1
4
8
10
9
0
0
1
8
10
10
10
0
0
3
5
9
10
10
X %
C
0
2
1
7
5
9
10
1
0
0
2
9
10
10
0
0 .
3
5
9
10
10
Mortality
0
10
10
63
73.3
96.7
96.7
6.7
0
10
46.7
96.7
100
100
0
3.3
26.7
53.3
90
100
100
                               A-2

-------