United States
Environmental Protection
Agency
Office of
Radiation Programs
Washington, D.C. 20460
EPA-520/1-86-017
October 1986
Radiation
xvEPA
Fate and Bioaccumulation
of Soil-Associated Low-Level
Naturally Occurring
Radioactivity Following
Disposal into a Marine
Ecosystem
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FATE AND BIOACCUMULATION OF SOIL-ASSOCIATED LOW-LEVEL NATURALLY
OCCURRING RADIOACTIVITY FOLLOWING DISPOSAL INTO A MARINE ECOSYSTEM
CARLTON D. HUNT9
MARINE ECOSYSTEMS RESEARCH LABOROATORY
GRADUATE SCHOOL OF OCEANOGRAPHY
UNIVERSITY OF RHODE ISLAND
NARRAGANSETT, RI
02882
PROJECT OFFICER
MARILYN VARELA
OFFICE OF RADIATION PROGRAMS
US EPA
WASHINGTON, D.C.
20460
OCTOBER 1, 1986
FINAL REPORT FOR
COOPERATIVE AGREEMENT CR-810265-02 (In part)
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FOREWORD
In response to the mandate of Public Law 92-532, the Marine
Protection, Research, and Sanctuaries Act (MPRSA) of 1972, as
amended, the Environmental Protection Agency (EPA) has developed
a program to promulgate regulations and criteria to control
the ocean disposal of radioactive wastes. Interest expressed
by other Government agencies has led EPA to consider the
environmental fate of soils, containing very low levels of
naturally occurring radioactivity, after disposal at a deep-sea
site. An important technical factor in any environmental
assessment of this disposal alternative for dry soils is the
potential for biological uptake of radionuc lides as they pass
through the water column and at the ocean bottom following
initial disposal at the ocean surface.
This report summarizes the biological data obtained
through laboratory experiments using large experimental tanks
to simulate such a disposal operation. The material being
investigated LS soil from a Middlesex, New Jersey site which
contains low levels of naturally occurring radioactivity,
primarily radium, thorium, and uranium. The experimental
methods and results are described, and conclusions drawn
regarding behavior, biological effects, and biological uptake of
radioisotopes associated with soil using controlled marine
ecosystems to simulate fate of the soils if they were to be
disposed of in the ocean. Another EPA Office of Radiation
Programs (ORP) report (Bonner, et al., 1985) describes the
physical and chemical characteristics of the Middlesex soil and
predicts, through a modeling effort, the transport rates and
behavior of the soil at a deep ocean disposal site. Both
studies were carried out in a manner consistent with the Hazard
Assessment Strategy developed by the EPA Office of Water. The
Hazard Assessment Strategy contains the scientific framework
under which potential ocean disposal permit requests may be
evaluated.
The Office of Radiation Programs will use this report as
an information base for any future inquiries regarding the ocean
disposal of soils containing low levels of radioactivity. The
methodologies described may also be valuable for the environ-
mental assessments of other kinds of pollutants proposed for
ocean disposal.
The Agency invites all readers of this report to send
any comments or suggestions to Mr. David E. Janes, Director,
Analysis and Support Division, Office of Radiation Programs
(ANR-461), Environmental Protection Agency, Washington, D.C.
20460.
Sheldon Meyers,Director
Office of Radiation Programs (ANR-458)
111
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ABSTRACT
The fate of Radium (Ra) and other naturally occurring Uranium series
isotopes associated with soils disposed in seawater was examined
using the Marine Ecosystem Research Laboratory (MERL) controlled
marine ecosystems. Thirty-seven kilograms of a soil containing
approximately 400 pCi Ra-226/g from an inactive uranium ore
processing plant site in Middlesex, N.J. were added to each of two
mesocosms over five days in mid-September 1984. Radionuclide
activity in these and two control mesocosms was observed for three
months after the soil additions. Radioactivity in the soil
appeared to be confined to discrete soil particles rather than
being distributed equally on the soil particles, suggesting the
source of the radioactivity was remnant ore particles.
Immediately following the additions, 0.2 to 1.5 percent of the
added radioactivity (depending on nuclide) was found in plant
detritus that floated to the water surface. Ten percent of the
added Ra was found in the water column within three days of soil
additions and an additional five percent mobilized to the water
column during the subsequent 90 days. Longer term mobilization of
Ra from the sediments was confirmed by benthic flux chambers.
Uranium isotopes showed similar release on contact with seawater,
while less than 1 percent of the Lead (Pb)-210, Polonium (Po)-210,
and Thorium (Th) series isotopes were released immediately after
the additions. Long term release of nuclides other than Ra could
not be determined due to insufficient data from the water column
over the course of the experiment.
Of the Ra mobilized, more than 97 percent was found in the dissolved
phase. The log of the distribution coefficients (Kd) between
dissolved and particulate phase Ra in the water column of the soil
amended ecosystems averaged 3.5; this is two orders of magnitude
less than found in the control systems and in samples from the
Narragansett Bay water added to the mesocosms. The low Kd's
probably resulted because available adsorption sites on the ambient
particles were saturated by the high dissolved phase Ra concentrations
Insufficient data were collected for Kd determinations of other
nuclides to enable similar comparisons between treatments. Size
fractionated analysis of the particulate matter suggests the majority
of the particle-associated Ra was in the <25 urn size class as was the
total suspended load.
Increases in Ra and other isotope activity in the sediments were
confined to the surface 1 cm initially, and penetrated to
approximately 2 cm by the termination of the experiment as a result
of bioturbation and settling processes. Mass balance calculations
relating the total activity found in the sediments to that added
were not satisfactory, primarily due to poor quantification of the
sediment porosity.
Little effect on the ecosystem structure and function were found
from the soil additions. System respiration exceeded production
in the short term but not over the course of the experiment.
v
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Zooplankton biomass was within normal limits for all ecosystems.
Diatom growth may have been suppressed immediately after soil
additions but over the experiment plankton species composition did
not appear to be affected. The abundance and species assemblage
of the benthic community were within normal limits both before and
after soil additions. Some species may have been lost because of
the soil additions but this did not appear to influence the
overall function of the benthic community in the ecosystem. The
only major effect on system parameters was a reduction in the rate
of sediment resuspension in the soil amended systems. This
reduction was driven by mechanical burial of sediments available
for resuspension.
At the species level, bioaccumulation of Ra and other
radionuclides was observed in all species sampled, including
zooplankton and benthic species in direct contact with the soil.
Depending on species, benthic organisms experienced a 10 to 50
fold increase in Ra concentrations relative to organisms from the
control systems. Those organisms living closest to the soil or
with the highest turnover rate of body tissue accumulated the most
Ra per unit dry tissue. The total Ra-226 and Po-210 found in the
bivalve Pitar morrhuana could be linearly related to the shell
length. No significant difference in this relationship was found
between organisms from the two ecosystems receiving soil. The
slope of the relationship was significantly different than for
organisms from the control systems suggesting a possible
relationship for evaluating exposure fields of organisms to
contaminants.
The mussel, Mytilus edulis. exposed to effluents from the soil
amended ecosystems showed 2 to 3 fold increases in Ra activity in
their tissues relative to animals from the control systems.
Bioaccumulation was initially rapid with a slow, variable increase
over longer exposure periods. A two fold decrease in total Ra
activity did not alter the observed accumulation of Ra for 28 day
exposure periods. Thus, the bioaccumulation was independent of
the total Ra activity in the water column but could be related to
the particulate phase Ra concentrations since the activity in this
phase remained constant while the dissolved phase decreased.
Measures of food conversion and growth efficiency in M. edulis
suggest animals exposed to the effluent had reduced growth
efficiencies over a 28 day exposure period. The toxicological
agent responsible for this effect could not be determined as
elements and compounds other than radionuclides were not
quantified during the experiment.
The experimental design provided a unique capability to determine
Ra and other radionuclide bioaccumulation in a variety of marine
organisms under well defined and constrained natural ecological
conditions. The ability to quantify time varying changes in the
exposure field, resulting from natural geochemical processes
operating in the systems, enhanced the ability to interpret the
biological data while concurrently addressing fate and process
questions.
VI
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ACKNOWLEDGEMENTS
Many people contributed to the development and completion of this
project. Without their interest and efforts the project would not
have been completed. Fred Russel was instrumental in configuring
the siphon system and numerous other construction tasks. Eric
Klos managed tank maintenance and ensured that the flow of water
to the systems was within experimental specifications. Greg
Tracey provided enlightening discussions and valuable advice on
the mussel exposure units and experimental design for this part of
the project. Skip Nelson found the mussel bed and helped to
recover the organisms in addition to providing advice about
handling them. Jeff Frithsen oversaw the radiation health aspects
in a manner which balanced scientific objectives without
compromising safety aspects. Jeff and Jamie Maughen advised on
methods for benthic animal recovery and counted benthic animals in
a timely manner plus acting as editors for species names. Steve
Kelly and Glenn Almquist were responsible for collection and
processing of samples. Jon Boothroyd loaned research grade
sediment sieves and Rotap shaker. Percy Donaghay of the
University of Rhode Island provided lively discussions and insight
into ecosystem behavior. Radionuclide counting at EERF was
overseen by Mike Mardis and Gerry Luster. Without their efforts
and those of the EERF analytical staff no radionuclide results
would be available. The draft report was critically reviewed by
numerous people, including Marilyn Varela, Bill Curtis, James
Neiheisel and Fred Hodge of the Office of Radiation Programs, Stu
Kupferman and Leo Gomez, Sandia National Laboratories, Jan Prager
ERLN, Jim Bonner, Texas A and M University, and Candace Oviatt,
Jeff Frithsen, Barbara Sullivan and Peter Doering of MERL. Even
though I did not always agree with or incorporate all of their
suggestions, I thank them for giving their time and thoughts to
ensure a better quality final document. In additon to the EPA
Project Officer, general project direction and design were
assisted greatly by the interest and knowledge of Stu Kupferman,
Sandia National Laboratories and Vic Bierman, formerly with the
EPA, ERLN, now at the University of Notre Dame. This report does
not necessarily reflect the views and policies of the
Environmental Protection Agency, nor does mention of trade names
or commercial products constitute endorsement or recommendation
for their use. The research was supported by EPA grant #
CR-810265-02 (in part).
VI
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TABLE OF CONTENTS
Foreword i i i
Abstract v
Acknowledgements vi i
Table of contents ix
List of figures xi
List of tables xix
Executi ve summary xxi i i
Introduction 1
Methods 5
Source material 5
Soil samples 5
Soil characterization 5
Experimental design 7
Ecosystem response - methods 10
Bioaccumulation studies 15
Benthic organisms from the mesocosms 15
Benthic organisms external to the mesocosms 16
Kinetics of nuclide uptake 16
Results and discussion 22
Ecosystem response 22
Phytoplankton 22
Production 22
Zooplankton 29
Benthic community 38
Total suspended solids 43
Transport and mobilization of radionuclides from soils 47
Flotsam 47
Short term mobilization 47
Long term mobil ization 49
Sediment inventory 59
Mass balance summary 64
Partitioning of radionucl ides in the water column 64
Radium 64
Distribution coefficients of other nuclides 72
Nuclide distribution within particle size classes.......... 72
Sediment resuspension 75
ix
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Bioaccumulation studies. 79
Mytilus edulis. . 79
Growth parameters........................................ 79
Uptake of radium - Experiment 1. 79
Uptake of radium - Experiment 2......... 85
Radium in Mytilus edulis fecal matter 87
Effects on mussel growth parameters..... 95
Other nuclides........ 99
Zooplankton............ ........ 99
Benthic organisms. 107
Bioaccumulation in Pi tar morrhuana 107
Bioaccumulation in other benthic organisms Ill
Comparison of bioaccumulation in all organisms............. Ill
Conclusions. 114
Appendix A. Middlesex soil size and radioactivity distributions 117
Appendix B. Distribution of porosity and nuclides in sediment.. 126
Appendix C. Benthic flux of radionuclides. 129
Appendix D. Summary of nuclide activity in benthic organisms... 131
Appendix E. Summary of Mytilus edulis growth and nuclide data.. 133
Appendix F. Summary of water column radionuclide data 138
Appendix G. Summary of sediment radionucl ide results 147
References Cited 152
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LIST OF FIGURES
Fig. 1 Schematic representation of EPA Hazard assessment
methodology for ocean disposal of anthropogenic wastes
(Prager et al., 1984) 2
Fig. 2 THE MERL MESOCOSM
Natural pelagic and benthic communities are isolated in
unit experimental system - mesocosms. Seawater turnover,
mixing and temperature are scaled to simulate natural
conditions. Mesocosms are operated identically and
experimental control and replication is attained at the
ecosystem level 8
Fig. 3 Schematic of the apparatus used to deploy sediment
traps at various depths in the MERL ecosystem 14
Fig. 4 Diagram of units in which Myti1 us edulis were
exposed to constant volumes of effluent from the MERL
mesocosms 17
Fig. 5 Chlorophyll a versus time in soil amended (T-12 and 14)
and control mesocosms (T-13 and 15) 21
Fig. 6 Total DCMU fluorescence versus time in experimental and
control ecosystems 22
Fig. 7 Size fractionated DCMU (<25 urn particle size cutoff and
total) versus time in soil amended (A & C) and control
mesocosms (B & C) 23
Fig. 8 Dissolved Silica versus time in soil amended (T-12
and 14) and control (T-13 and 15) mesocosms 24
Fig. 9 Total DCMU and Fluorescence vs time in soil amended
(A & C) and control (B & C) mesocosms 25
Fig. 10 Net daytime production versus time in control (T-13
and 15) and soil amended (T-12 and 14) mesocosms 26
Fig. 11 Comparison of nightime respiration as a function of
time in control (T-13 and 15) and soil amended (T-12
and 14) mesocosms.. 27
Fig. 12 Net daily production versus time in control (T-13
and 15) and soil amended (T-12 and 14) mesocosms 28
Fig. 13 Changes in water column pH as a function of time in
control (T-13 and 15) and soil amended (T-12 and 14)
mesocosms 32
xi
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Fig. 14 Changes in dissolved oxygen concentrations as a
function of time in control (T-13 and 15) and soil
amended (T-12 and 14) mesocosms. Variability in
oxygen concentrations on any given day shows the
range experienced between dawn and dusk sample
periods. 33
Fig. 15 Water column temperature vs time in soil amended and
control mesocosms 34
Fig. 16 Changes in dissolved ammonia vs time in control and
soi 1 amended mesocosms 35
Fig. 17 Response of dissolved Phosphate as a function of time
in control and soil amended mesocosms. 36
Fig. 18 Comparison of zooplankton biomass as a function of
time in control (T-13 and 15) and soil amended (T-12
and 14) mesocosms... 37
Fig. 19 A. Total suspended load vs time in control and soil
amended mesocosms. B. Total suspended load in
Narragansett Bay water entering the mesocosms 44
Fig. 20 Comparison of the temporal response in total suspended
load vs mass of particles in the < 25 urn particle
size. A and C soil amended mesocosms, B and D control
mesocosms 45
Fig. 21 Sediment resuspension rate as a function of time in
control and soil amended mesocosms. Resuspension
rates determined with sediment traps positioned 0.3
meters above the sediment surface for 24 hours 46
Fig. 22 Total Ra activity in the water column vs time.
A. Control mesocosms and Narragansett Bay water
entering the ecosystems. B. Soil amended mesocosms.
Note scale change between A and B 53
Fig. 23 Comparison of total measured Ra (dissolved plus
particulate) in the water column to total water column
activity predicted if no remobilization or removal to
sediments occurred after soil additions.
A. Mesocosm 12. B. Mesocosm 14 54
Fig. 24 Changes in total Ra activity per sampling interval as
calculated from a simple mass balance equation (See
text). Ra added in the feed water (Input), change in
total activity in the water column (dM/dT), loss from
mesocosm by flushing (Flush loss) and exchange between
water column and sediments (Sed input, addition from
sediment is positive). A. Mesocosm 12. B. Mesocosm 14.. 56
XI
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Fig. 25 Calculated benthic flux of Ra into the water column
versus temperature. Results based on mass balance
calculations depicted in Fig 24. For comparison the
Ra flux measured on October 26, 1984 is shown by the
point labeled Chamber 303 57
Fig. 26 Comparison of measured benthic fluxes in control and
soil amended treatments October 26, 1984, 39 days
after soil was added to the mesocosms 58
Fig. 27 Porosity of sediments in soil amended mesocosms as a
function of depth before and after soil additions.
A. Mesocosm 12 B. Mesocosm 14 60
Fig. 28 Ra activity in sediments vs depth before and after
soil additions 61
Fig. 29 Ra distribution in top 5 cm of the sediment column
as a percentage of the total Ra in the upper 5 cm
prior to (A and C) and at the termination of the
experiment (B and D) in mesocosms 12 and 14,
respectively 63
Fig. 30 Partitioning of Ra between total, dissolved and
particulate phases in control mesocosms (A and B) and
Narragansett Bay feed water (C) as a function of time.
The percentage of the Ra in the dissolved phase of
each treatment is depicted in D 66
Fig. 31 Partitioning of Ra between total, dissolved and
particulate phases in soil amended mesocosms as a
function of time 67
Fig. 32 Calculated distribution coefficient for Ra as a
function of time for all mesocosms and lower
Narragansett Bay water 68
Fig. 33 Association of Ra with particles, total and <25 urn
size class, in the water column as a function of time.
Soil amended system A and B, control systems C and D.. 74
Fig. 34 Comparison of radionuclide activity in resuspended and
surface sediments (upper 0.5 cm) four days after soil
addition to the mesocosms 76
Fig. 35 Radium activity in resuspended particles versus time,
Control mesocosms T-13 and 15, soil amended mesocosms
T-12 and 14 77
Fig. 36 Comparison of radium activity in particles, sediment
and resuspended sediments as a function of time in
soi 1 amended mesocosms 78
XI
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Fig. 37 Final shell length of individual mussels held in
effluents from the mesocosms as a function of time
after exposure initiated. A. Individual organisms.
B. Mean final shell length of 5 animals per treatment
per time interval. Error bars for mean shell length
not shown to reduce confusion on graph. Standard
deviation of the lengths were similar and ranged
between 1 and 2 mm 80
Fig. 38 Increase in shell length of organisms vs time.
A. Individual mussels. B. Average growth increment vs
time. Error bars for mean growth increment not shown
to reduce confusion on graph..... 81
Fig. 39 Tissue dry weight of mussels as a function of time.
A. Individuals. B. Average 83
Fig. 40 Ra activity in Mytilus edulis tissue, pCi/g dry
weight, as a function of time in all mesocosms and in
control organisms held external to the exposure
systems. A. Individuals. B. Average Ra activity..... 84
Fig. 41 Total Ra in tissues of Mytilus edulis tissue,
pCi/animal, as a function of time in all mesocosms and
in control organisms held external to the exposure
systems. A. Individuals. B. Average total Ra per
animal 86
Fig. 42 Comparison of the shell length of mussels in control
and experimental mesocosms and external control
organisms (C-I and C-F, Initial and final) after
exposure for 28 days to two levels of Ra activity
(Exp. 1 at higher levels than Exp 2). A. Individual
organisms. B. Average length, standard deviation for
5 animals per treatment shown 89
Fig. 43 Comparison of the increase in shell length of mussels
from control, experimental mesocosms and external
controls (C-I and C-F, Initial and final) after
exposure for 28 days to two levels of Ra activity
(Exp. 1 at higher levels than Exp 2). A. Indivdual
organisms B. Average increase, standard deviation
for 5 animals per treatment shown 90
Fig. 44 Comparison of the tissue dry weight of mussels from
control, experimental mesocosms and external controls
(C-I and C-F, Initial and final) after exposure for
28 days to two levels of Ra activity (Exp. 1 at higher
levels than Exp 2). A. Indivdual organisms
B. Average increase, standard deviation for 5 animals
per treatment 91
xi v
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Fig. 45 Comparison of Ra activity, pCi/g dry weight, of
mussels from control, experimental mesocosms and
external controls (C-I and C-F, Initial and final)
after exposure for 28 days to two levels of Ra
activity (Exp. 1 at higher levels than Exp 2).
A. Indivdual organisms B. Average increase,
standard deviation for each treatment shown 92
Fig. 46 Comparison of total Ra activity, pCi/ animal, in
mussels from control, experimental mesocosms and
external controls (C-I and C-F, Initial and final)
after exposure for 28 days to two levels of Ra
activity (Exp. 1 at higher levels than Exp 2).
A. Indivdual organisms B. Average increase, standard
deviation for each treatment shown 93
Fig. 47 Comparison of changes in total suspended load (graph A)
and flux of fecal material from mussels (grapgh B)
as a function of time 94
Fig. 48 A. Radium activity in Mytilus edulis fecal matter
from soil amended mesocosms as a function of time.
B. Radium activity in Mytilus edulis fecal matter
from controls mesocosms as a function of time 96
Fig. 49 Average Ra activity in particulates (total and < 25
micron size class) and fecal matter from mussels
exposed to water from control and the soil amended
mesocosms 97
Fig. 50 Calculated flux of Ra passing through Mytilus
edul is as a function of time 98
Fig. 51 Comparison of Mytilus edulis growth efficiency (A)
and food conversion efficiency (B) in control and
soil amended mesocosms as a function of time 100
Fig, 52 A. Average Po-210 and Pb-210 activity in mussels
exposed 14 days to effluents from mesocosms.
B. Average U nuclide activities in mussels exposed for
14 days to effluents from mesocosms. C. Average Th
nuclide activities in mussels exposed for 14 days to
effluents from mesocosms 101
Fig. 53 Ra activity in zooplankton as a function of time 102
Fig. 54 Uranium 234 and 235 in zooplankton as a function time. 103
Fig. 55 Pb-210 and Po-210 in zooplankton as a function time... 104
Fig. 56 Uranium 238 and Th-230 in zooplankton as a function
of time 105
xv
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Fig. 57 Thorium 227 and 232 in zooplankton as a function of
time. 106
Fig. 58 A. Ra-226 activity, pCi/g dry weight, in Pi tar
morrhuana recovered from the sediments at the
termination of the experiment as function of shell
length. Controls T-13 and 15, soil amended mesocosms
T-12 and 14.
B. Po-210 activity, pCi/g dry weight, in Pi tar
morrhuana recovered from the sediments at the
termination of the experiment as function of shell
length. Po activities are not decay-corrected to day
of collection. Key as for A 108
Fig. 59 A. Total Ra-226 activity, pCi/animal, in Pitar
morrhuana recovered from the sediments at the
termination of the experiment as function of shell
length. Controls T-13 and 15, soil amended mesocosms
T-12 and 14.
B. Total Po-210 activity, pCi/animal, in Pitar
morrhuana recovered from the sediments at the
termination of the experiment as function of shell
length. Po activities are not decay-corrected to
day of collection. Key as for A 109
Fig. 60 A. Comparison of Ra activty in benthic animals
recovered at the termination of the experiment.
LEP= Leptocheirus pinquis; NEP= Nephtys incisa:
PIT= Pitar morrhuana: PHE= Pherusa affinis;
MOG = Molqula manhattensis
B. Ratio, experimental to controls, of Ra and Po-210
in benthic animals recovered at the termination of
the experiment 112
Fig. 61 Comparison of the ratio of Ra (experimental/control)
in all organisms recovered from the mesocosms during
and at the termination of the experiment 113
Appendix A.
Fig. A Distribution of soil grain size 118
Fig. B Cumulative distribution of soil grain size 119
Fig. C. Auto-radiography of soil particles .showing discrete
distribution of activity in soil particles 120
Fig. D. Distribution of Ra, Po, and U-238 as a function of
soil grain size in soil sample Bl 121
Fig. E. Distribution of U-238 abd Pb-210 as a function of soil
grain size in sample Bl. 122
XVI
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Fig. F. Mass weighted composition of Ra, U-238, and Po in soil
sample Bl 123
Fig. G. Comparison of mass weighted distribution of Ra to
grain size distribution in soil sample Bl 124
Fig. H. Comparison of mass weighted distribution of U-238 to
grain size distribution in soil sample Bl 125
xvi i
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LIST OF TABLES
Table 1. Total radionuclide activity associated with Middlesex
N.J. soil sample Bl 6
Table 2. Summary of soil and total radioactivity added to
mesocosms during September 1984 9
Table 3. Samples collected for radionuclide analysis during soil
study, September - December 1984. 11
Table 4. Summary of ecosystem and geochemical parameters examined
during soil disposal experiment September to December
1984 12
Table 5. Average daily production and respiration in control
mesocosms (13 and 15) and soil amended systems (12
and 14) during the fall of 1984. Units are in
g 02m-2d-l 30
Table 6. Benthic nutrient flux and respiration on Oct. 26, 1984,
35 days post soil additions. Negative values indicate
fluxes are into the sediment 31
Table 7. Macrobenthic animal densities prior to soil additions
(August). Densities are in animals per core. Data
based on 10 replicate 2.54 cm diameter cores collected
randomly from the mesocosms. Animals per cm2 can be
obtained by multiplying by 1973.5 39
Table 8. Macrobenthic animal densities at the termination of the
experiment (August). Densities are in animals per core.
Data based on 10 replicate 2.54 cm diameter cores
collected randomly from the mesocosms. Animals per
cm2 can be obtained by multiplying by 1973.5 40
Table 9. Comparison of macrobenthic animal densities prior to
soil additions (August) and at termination of the
experiment (December). Densities are in animals per
core. Data based on 10 replicate 2.54 cm diameter
cores collected randomly from the mesocosms. Animals
per cm2 can be obtained by multiplying by 1973.5 41
Table 10. Recovery of large animals from terminal sieving of
sediments. Screen size was 6.4 mm. Results are
representative, not absolute, as efforts to recover
all organisms were not made during collection of
animals for bioaccumulation studies. Population
reported as number per mesocosm 42
xi x
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Table 11.
Table 12,
Total radionuclide activity of organic detrital
flotsam recovered from the mesocosm surface after
soil was added to the mesocosms. „
48
Increase in water column radionuclide activity
resulting from addition of soil to mesocosms.
Results based on the concentrations observed with
the systems in batch mode and three days post
completion of soil additions. Units are in pCi/1.
In column 2 d, p, and t refer to dissolved,
particulate, and total radionuclide activity
50
Table 13. Release of radionuclides from soil within one week of
soil additions to mesocosms. Release based on the
increase in water column concentrations before and
after soil addition while mesocosms were on batch
mode
51
Table 14. Comparison of the percentage of soil associated nuclides
leached on contact with seawater during three studies of
different scale. Sample size, seawater volume, contact
times and temperature are: 0.0003 to 0.0012 kg, 11, 20
hrs, 20 OC; 4.4 kg, 13000 1, 4 h, 22 oc; and 37 kg,
13000 1, 72 to 168 h, 17 oc in the bench scale,
settling studies and mesocosm study, respectively 52
Table 15. A. Ra inventory in the sediments receiving soil in
nCi/mesocosm. Inventory calculated from
I = A x (1-P) x d x z x 2.5x104, where I is the
inventory in a given layer of sediment in Curies, A is
the activity in the sediment, P is porosity, d is the
dry density of the material , z is the depth interval
(cm) and 2.5x10^ is the area of the sediment surface
in cm2.
B. Mass balance comparison to known additions 62
Table 16. Summary of input, output and mobilization of Ra
associated with Middlesex soils added to seawater.
Table 17,
Summary of Ra activity in particles from experimental
and control mesocosms during experimental period.
Concentrations in pCi/g
Table 18. Ra distribution coefficients in the water column during
soil addition experiment. Presented as log Kd ,
65
70
71
Table 19. Distribution coefficients for nuclides other than Ra.
Distribution coefficients calculated only when activities
were detectable. Results are also compared with other
partitioning studies. ... 73
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Table 20. a) Average chlorophyll a concentrations (ug/1) in the
water column of the mesocosms during the Mytilus
edulis exposure experiments 1 and 2. b). Rank in
abundance of chlorophyll a or average change in shell
length after 28 and 56 days of exposure 82
Table 21. Average concentration of Ra-226 in dissolved and
particulate phases during mussel exposure experiments
1 and 2. Units are pCi/1 88
Table 22. Summary statistics for Ra in Pi tar morrhuana.
A. Length versus pCi/g dry tissue. B. Length versus
pCi Ra/ animal 110
Appendix B
Table A. Distribution of water content and porosity as a function
of depth in the sediment column. Mean of 2 pooled
samples (5 cores per sample depth) 127
Table B. Concentration of nuclides in sediments before and after
soil additions. Units are pCi/g dry weight. Other
nuclides show similar patterns 128
Appendix C
Table A. Ra benthic flux comparison by treatment. ORP project,
October 26, 1984 130
xxi
-------
EXECUTIVE SUMMARY
In 1983 the EPA Environmental Research Laboratory at Narragansett
(ERLN), in response to an EPA Office of Radiation Programs (ORP)
initiative, proposed that their generic hazard assessment
methodology be extended to specifically include disposal of low
level radioactive waste in the oceans, as a tool supporting
evaluation of potential permit applications to ORP- The principle
objective of this effort was to develop a useful, scientifically
credible framework within which the permitting process could be
undertaken. The methodology requires several levels of
information including waste characterization, site
characterization, determination of exposure fields and fate of
radionuclides plus determining potential biological effects at
several levels of testing and evaluation.
Data useful to the developemnt of the hazard assessment
methodology for radioactive waste disposal were limited.
Therefore, an experimental and a modeling effort were initiated to
obtain relevant and useful information for the development and
application of the hazard assessment methodology for this type of
material. These efforts focused on 1) the transport
characteristics of a waste soil and 2) fate and effects, at both
the ecosystem and species level of analysis, of radionuclides
associated with the soil. The availability of a soil contaminated
with low levels of naturally occurring radioactivity from a
Department of Energy designated Formerly Utilized Sites Remedial
Action Program (FUSRAP) site enabled application of a potential
candidate soil to the experimental and modelling efforts.
The focus of the experimental effort was on collection of
information relative to the geochemical behavior of radionuclides
found associated with the soil when disposed in sea water and on
bioaccumulation of the radionuclides in several marine organisms.
Controlled marine ecosystems of 13 m3 were employed to examine the
fate and effects questions over a 3 month period. These systems
provide the capability to simultaneously examine the behavior and
effects of contaminants using natural marine communities while
retaining a measure of control over experimental conditions.
Results
The data base from this experiment is sufficient in quantity and
quality to enable development and application of a hazard
assessment methodology for disposal of uncontained waste in
seawater. The results of the experiment indicate that:
1. A low but significant fraction of the radioactivity will be
released immediately on contact with seawater,
2. A small fraction of the Ra will continue to leach from the soil
once deposited,
xxi
-------
3. Uncontained disposal of the soil will result in plant detritus,
carrying elevated radionuclide activity, floating to the water's
surface where it is more available to organisms (birds and fish)
feeding there,
4. The Ra mobilized from the soil on disposal will remain in the
dissolved phase and be slowly dispersed by currents and mixing
processes until removed from the water column by natural
processes,
5. Bioaccumulation of the radionuclides from the soil will occur
in marine organisms exposed to the soil. The extent of
bioaccumulation depends on the type of organism and its habitat:
in relationship to the soil location,
6. Possible decreases in the growth efficiency of the blue mussel
Mytilus edulis were observed when exposed to effluents from the
soil amended ecosystems. The causative agent could not be
definitively determined since all potential agents were not
quantified during the experiment,
7. Long-term effects on ecosystem function were not observed.
Short term effects were not detectable two weeks after the soil
additions,
8. Distribution coefficients between dissolved and particulate
phases depended on the experimental technique employed and the
relative ratio between the mass of the particles and volume of
seawater.
Limitations
The results of this effort are limited in that horizontal
transport at a real disposal site is not considered. Such
considerations are beyond the capabilities of most experimental
systems and can most accurately be determined from in situ
studies. Our ability to predict the behavior of radionuclides
other than Ra was limited by the lack of funds to perform
appropriate analyses. Similarly, sediment interstitial water
chemistry and nuclide distributions were not available, reducing
the ability to predict vertical migration in sediments and
determine geochemical factors influencing mobilization. Comments
provided during the review process made clear the value of
obtaining mineralogical data as a means of monitoring soil
movement in post disposal monitoring programs. We were also
limited in our ability to examine possible mechanisms causing
reduced Ra flux after deposition. Such studies would be
enlightening relative to the length of time to expect the
mobilization process to continue. Interpretation of cause-effect
relationships would also have benefited if supporting data for
other possible toxic elements could have been generated. Finally,
this is but one type of waste which could be studied for ocean
disposal. Other wastes may have characteristics that are as
XXI V
-------
unique as this one, requiring continued assessment and refinement
of techniques for evaluating the waste.
Recommendations for future work
Several recommendations can be made regarding future studies of
this type and for the characterization of candidate wastes for
ocean disposal. First and foremost is the application of the data
from this experiment to the hazard assessment method such that
predictive models can be derived and tested. An effort in this
area will help determine where additional data is required. Based
on this study and review comments it is recommended that:
1. Grain size characterization should be routinely made, these are
necessary for determination of vertical transport rates and
horizontal dispersion,
2. Characterization should be made of the material for distinctive
mineralogical and chemical signatures (heavy metals or organic
compounds) which can be used to monitor movement of the material
once deposited in the sediments,
3. Leaching charateristics of the material should be determined to
estimate the degree to which the contaminants are released on
contact with seawater. Leaching rates are also neccessary in
order to determine how fast the material will lose the
contaminants during settling through the water,
4. The association of contaminants with specific grain size,
chemical phases or minerals should also be determined to aid in
the prediction of the extent and rate of mobilization,
5. The amount of detritus that may float to the ocean surface
should be quantified in addition to contaminant concentrations in
the material.
Future experimental studies are required to;
1. Determine if the observed decrease in the growth efficiency in
Mytilus edulis is real and the causative agent(s). In addition,
the effect should be evaluated for its significance in terms of
ecosystem effects and protection,
2. Identify and quantify the pathways, dissolved versus
particulate, by which the radionucl ides are taken up by filter
feeding organisms and the importance of this to disposal
strategies,
3. Quantify and evaluate the significance of the observed
bioaccumulation of radionuclides, including food availability on i
the uptake, at the species and ecosystem level,
4. Determine if the observed relationship between total
radionuclide activity in bivalves and shell length can be used as
XXV
-------
a means of determining and monitoring field animals for
contaminant levels to which the organisms are exposed,
5. Better quantify the dependence of elemental distribution
coefficients between dissolved and particulate phases on
radionuclide concentrations and experimental techniques.
These and other research areas will provide additional ability to
refine the hazard assessment methodology as it applies to ocean
disposal of materials containing low levels of radioactivity.
More pressing is the application of the information gathered in
this experiment to the hazard assessment model, so that testing
and validation can progress towards applying the concept as a tool
for evaluating ocean disposal permit applications.
XXVI
-------
INTRODUCTION
The Marine Protection, Research and Sanctuaries Act of 1972
authorizes the Environmental Protection Agency (EPA) to regulate
all ocean disposal activities in the United States of America
including disposal of radioactive wastes not specifically
prohibited by law. Under the provisions of this Act, EPA is also
required to establish and apply criteria for review and evaluation
of disposal permit applications. In 1981 Sandia National
Laboratories initiated an evaluation of potential disposal sites,
including the oceans, for soils contaminated with low but
significant levels of naturally occurring radionuclides under the
Department of Energy's Formerly Utilized Sites Remedial Action
Program (FUSRAP) which was designated to evaluate and clean up
numerous inactive industrial plant sites remaining from the
Manhattan Project (Kupferman et al., 1984). Sandia identified the
former sampling plant site at Middlesex N.J. as a potential
candidate for ocean disposal. Efforts were begun to document the
feasiblity and advantages of ocean disposal of soil and rubble
from this site in comparison to land disposal options and to
support potential permit applications to EPA.
In 1983 the EPA Environmental Research Laboratory at Narragansett
(ERLN), in response to an EPA Office of Radiation Programs (ORP)
initiative, proposed that their generic hazard assessment
methodology (Prager et al., 1984) be extended to specifically
include disposal of low-level radioactive waste in the oceans, as
a tool supporting evaluation of potential permit applications to
ORP. The principle objective of this effort was to develop a
useful, scientifically credible framework within which the
permitting process could be undertaken. The methodology requires
several levels of information including waste characterization,
site characterization, determination of exposure fields and
determination of potential biological effects at any of several
levels (tiers) of sophistication (Fig. 1). The availability of
soils contaminated with low levels of naturally occurring
radioactivity from a designated FUSRAP site enabled application of
a specific material to the development of the hazard assessment
methodology, providing a more generalized and valid tool for the
evaluation and decision process.
Preliminary characterization of the Middlesex site by Sandia
suggested several potential contaminants including naturally
occurring radionuclides, inorganic and organic toxics (Kupferman
et al., 1984). Of these, only radionuclides were at significant
levels above background. In addition Sandia identified DWD-106,
a previously designated site for industrial waste disposal in the
northwest Atlantic Ocean, as a candidate site to receive the soils
(Kupferman et al., 1984). The Sandia studies and results were
useful but were not designed to develop and test the EPA hazard
assessment methodology. This methodology specifically requires 1)
an understanding of transport mechanisms and exposure fields which
would result from disposal of this soil material and 2) measures
of biological effects under known exposure conditions. Since
-------
STRATEGY FOR OCEAN DISPOSAL
SITE
CHARACTERIZATION
WASTE
CHARACTERIZATION
JL
EXPOSURE
ASSESSMENT
LEVEL 1
#
•
LEVEL N
HAZARD
ASSESSMENT
1
DISPOSAL
DECISION
EFFECTS
ASSESSMENT
LEVEL 1
•
«
LEVEL N
I
[MONITORING
i
VALIDATE /REVISE
HAZARD ASSESSMENTS
Fig. 1 Schematic representation of EPA Hazard assessment
methodology for ocean disposal of anthropogenic wastes (Prager et
al., 1984).
-------
field measurements of transport at ocean disposal site are
difficult to obtain (Brown et al., 1983; Peroni and Hanson, 1981)
without "a priori" understanding of possible transport rates and
vectors, EPA determined that laboratory scale experiments and a
modeling effort should be combined to provide the necessary
transport information for a deep ocean disposal site.
The biological and exposure information, required for the
increasingly sophisticated levels of effects and exposure
assessment depicted in Figure 1, could be obtained from any of
several test procedures. These procedures could range from small
scale studies such as acute single species bioassay tests or
simple chemical partitioning studies to mesocosm scale (controlled
experimental ecosystems of >10 m3) studies with natural biological
communities. The characteristics of the Middlesex soil made
unlikely any acute lethal radiological or other toxic effects to
biological species. This was confirmed by acute solid phase
bioassay studies conducted for Sandia by Battelle New England
(Hillman et al., 1983). Thus, a more subtle, chronic assessment
was required to determine potential sublethal exposure effects for
this material.
The specific sublethal exposure effects which might be expected
from this type of material are not clearly defined. Ultimately
radiation protection requires dose-to-man estimates. These
estimates require bioaccumulation data for potentially harmful
radionuclides. There is a surprising paucity of data on tissue
residues of natural radionuclides of marine organisms (Jackson et
al., 1983) from which to make bioaccumulation estimates. It was,
therefore, determined that tissue residue data in several species
of marine organisms under known exposure fields were required as a
first order assessment of potential exposure effects. More
sophisticated effects such as growth and food chain conversion
efficiencies in specific species were also desirable. Since
biological communities within an ecosystem could be altered by the
addition of large quantities of soil and associated contaminants,
data to elucidate possible alterations in community structure were
required. At the ecosystem level, measures of possible alteration
in ecosystem function were desirable.
It was determined that the most effective method for providing
simultaneous information on exposure fields and biological effects
at the species, community and ecosystem level in addition to
testing and further developing the EPA hazard assessment strategy,
was a mesocosm study in which natural communities were exposed to
a known amount of the contaminated soil under controlled
conditions. Use of mesocosms had the added advantage of providing
geochemical information i.e., removal rates of dissolved
components, partitioning between dissolved and particulate phases
and post depositional mobilization of the nuclides with which to
link exposure fields and tissue residues to potential
post-depositional mobilization of nuclides. The EPA, through ORP
funding to ERLN and to the University of Rhode Island's Marine
Ecosystem Research Laboratory (MERL), proceeded to plan the study
-------
in May 1984. Radionuclide analyses were scheduled for the ORP,
Eastern Environmental Radiation Facility (EERF) in Montgomery,
Alabama.
The approach to the study involved three phases:
1. Description of the physical and chemical characteristics of
the Middlesex soil,
2. Estimation of transport rates and behavior of the soil
at a deep ocean disposal site through combined laboratory
and modeling studies, and
3. Examination of the behavior, effects and biological uptake
of radionuclides associated with the soil using controlled
marine ecosystems.
Results of phases 1 and 2 have been summarized by Bonner et al.,
1986. The following report describes results from phase 3, the
exposure assessment study in the controlled marine ecosystems at
the MERL.
This study phase had these specific objectives:
1. To determine the biogeochemical behavior of low-levels of the
naturally occurring radionuclides Ra-226; U-234, 235, 238;
Th-227, 228, 230, 232; Pb-210 and Po-210 associated with soil
from the Middlesex, N.J. FUSRAP site under controlled natural
ecosystem conditions,
2, To determine exposure concentrations of these radionuclides
in the water column and sediments as a function of time,
3. To determine net bioaccumulation of these radionuclides in
benthic and water column organisms contained within the
ecosystem,
4. To determine uptake rates and "equilibrium" net
bioaccumulation in the mussel Mytilus edulis maintained
in mesocosm effluents,
5. To determine if changes in growth and food chain conversion
efficiency on Mytilus edulis resulted from exposure to
the soils,
6. To determine if changes in phytoplankton, zooplankton and
benthic community structure or function resulted from the
soil additions.
7. To determine if alterations in ecosystem production and
respiration resulted from the addition of the soils.
-------
METHODS
Source Material
Soil samples
Soil samples were obtained from the Middlesex site in August 1982
by MERL and Sandia personnel. Soil samples were excavated from
several locations on the site, sieved through 6 mm screens, field
characterized for total radioactivity and combined into five
separate 100 kg subsamples having different total radioactivity.
Samples were homogenized at the site in a 0.15 m3 cement mixer and
divided into 50 kg replicate batches. The sample used in this
experiment (Bl) had the highest radioactivity of the five samples
collected.
Soil Characterization
Specific gravity was determined using standard pycnometric
procedures at 20 degrees centigrade. The average bulk specific
gravity was 2.31 g/cm3. Soil particle size distribution was
determined after quantitatively oven drying (70°C) 100 g soil
subsamples for percent moisture. The dried sample was then sieved
for 20 minutes with a Ro-tap particle sieve shaking system
(Carver, 1971) using 0.5 Phi size increments between 4.0 and - 1
Phi. The soil retained on each sieve was quantified in terms of
mass and the mass percent and a cumulative size distribution
calculated. Results are summarized in Appendix A.
Particles obtained from the dry size classification procedure were
analyzed for total radioactivity by two techniques. A gross
measure of total radioactivity was determined on each size class
by counting total Gamma-Beta and total alpha emanating from a
known mass with a Nuclear Measurements, Inc., PC-5 proportional
counting system. Results were calculated in terms of counts per
minute per gram dry sample (CPM/g) and corrected for incident
background radiation. These same samples were then sent to EERF
for quantification of the radionuclides Ra-226, Pb-210, Po-210,
U-234, 235, 238 and Th-227, 228, 230, 232.
Selected size classes were subjected to autoradiography to
determine whether the radioactivity was associated with discrete
particles within the soil matrix (possibly unadulterated ore from
the grinding procedures of the assay plant) or homogeneously
distributed on all particles (indicating weathering of the ores
originally used). Appendix A details these results.
The activity of specific radionucl ides associated with the bulk
soil was determined in 1982 by Sandia (Brush, personal
communication) and in 1984 by the Eastern Environmental Radiation
Facility (EERF) of EPA in Montgomery, Alabama (Table 1). Appendix
A summarizes size and radionuclide distribution characteristics.
-------
Table 1. Total radionuclide activity associated with the Middlesex N.J. soil
sample Bl in pCi/g dry weight.
Isotope
Ra-226
Pb-210
Po-210
U-238
U-235
U-234
Th-227
Th-228
Th-230
Th-232
Sample
#A
365
317
358
373
9
374
24
27
388
33
#B
358
387
10
387
25
33
462
47
#C
397
470
371
304
12
321
32
41
379
46
#CCa
359
515
388
373
26
377
54
73
404
76
#ia
460
400
NA
20
NA
NA
29
460
29
#2
530
480
NA
25
NA
NA
33
540
34
EERF
373
434
369
359
14
365
34
34C
408
42C
Average
20
103
14
37
8
30
14
7
37
8
ALL
422
436
17
33C
430
38C
•-sd--
72
79
8
6
61
8
a. Samples A, B, C, CC were analyzed at the Eastern Environmental Radiation
Facility of EPA. Sample CC was calculated from the mass weighed activity
of individual size classes obtained from dry seiving of the sample.
b. Samples 1 and 2 were analyzed for Sandia by Battelle Northwest.
c. The high value for CC was not used in the mean.
-------
Experimental Design
Four mesocosms at the MERL were initiated in September 1984 for
the ecosystem/ bioaccumulation phase of the experiment. The
mesocosms are 1.8 m diameter by 5 m high cylinders containing 13
m3 of water overlying a 2.5 m2 by 30 cm sediment column (Fig. 2).
The systems are outdoors and exposed to natural sunlight and
weather. Generally the systems are operated in a flow-through
mode with water from lower Narragansett Bay entering at 480 1/d in
four daily 10 minute pulses of 120 1 each. Turbulence is provided
with vertical plunger-like devices maintained in a 2-h-on, 4-h-off
cycle (Nixon et al., 1980). The mesocosms, their operation,
ability to replicate natural ecosystem processes and usefulness in
studying biogeochemical processes have been extensively described
elsewhere (Pilson et al., 1980; Oviatt et al., 1980; Hunt and
Smith, 1982; Santschi, 1982; Santschi et al., 1984).
During this experiment, water was added by the pulse feed mode at
an average 499 +- 14 1/d. However, water was removed from the
system with a siphon located 1 meter below the mesocosm surface.
The siphon drew water at a rate of 425 1/d. This water was routed
to exposure units containing the bivalve Mytilus edulis (see
below). Input volume in excess of that drained with the siphon
was removed from the mesocosms with the normal overflow system.
Sediments for this study were recovered from north of Conimicut
Island in Narragansett Bay in October 1983 using a 0.25 m2 Unsel
spade corer (Hunt and Smith, 1983). The systems were on
flow-through mode from October 1983 to April 1984 when the water
column was drained and refilled. From May to mid August 1984 the
mesocosms were operated in batch mode for an experiment studying
the effects of the clam Mercenaria mercenaria on ecosystem
response (Doering et al., In press). Upon termination of this
experiment, the Mercenaria were removed by hand from the
sediments. This disturbed and mixed the surface 2-4 cm of
sediment. Following this procedure the systems were operated on a
fast flow through mode (1 day water column turnover time) for
three weeks in order to insure that a normal Narragansett Bay
phytoplankton assemblage was present for the Middlesex soils
experiment and to allow the surface sediment layer to re-establish
itself. Benthic cores were collected from the mesocosms on Sep.
12, 1984 for background radionuclide counts and enumeration of
benthic organisms for comparison with terminal counts from the
previous Mercenaria experiment.
Between September 17 and 21, 1984 a composite soil sample
(designation BIB) from the Middlesex N.J. FUSRAP site was added to
each of two mesocosms (#'s 12 and 14). A known mass of soil (7.5
kg dry weight) was distributed by hand over the surface of the
mesocosm each day during the morning mixing cycle. A total of
37.2 kg of soil was added to each mesocosm (Table 2). It was
estimated that each soil addition would add 0.13 cm of soil to the
sediment, if evenly distributed over the surface. The total soil
addition was calculated to add 0.7 cm of sediment to the
-------
CONTROL
SEAWATEH TURNOVER
120 I/FEED (• L/min.13.3 L/fflln •• FEED)
4*0 L/0AY: 2T DAY REPLACEMENT TIME
MIXING
2 h ON - 4 ft Off
8 MPM
C TEMPERATURE
HEAT EXCHANGER ON/OFF
± 1 °C OF (AY TEMPERATURE
DIMENSIONS
DEPTH
(m)
AREA
VOLUME
TANK INSIDE DIAMETER 1.83 m
HEiQHT S.49 m
WATER
BENTHOS
S.O
0.38
2.63
2.S2
13.1
0.96
Figure 2 THE MERL MESOCOSM
Natural pelagic and benthic conmunities are isolated in
unit experimental systems - mesocosms. Seawater turnover,
mixing and temperature are scaled to simulate natural
conditions. Mesocosms are operated identically and
experimental control and replication is attained at the
ecosystem level.
-------
Table 2. Summary of soil and total activity added to mesocosms during
September 1984.
Parameter Average total
activity,
pCi/ g dry
Total mass added to each mesocosm
Kg/ mesocosm
12
14
Wet mass
Dry mass
Ra-226
Pb-210
Po-210
U-234
U-235
U-238
Th-227
Th-228
Th-230
TH-232
41.67
37.23
41.63
37.19
422
436
369
359
14
365
34
33
430
38
Total activity added to each mesocosm
uCi/mesocosm
15.7
16.7
13.7
13.4
0.5
13.6
1.3
1.2
16.0
1.4
-------
mesocosms. Aliquots of soil (300 ml) were taken each day to
determine moisture content. The mesocosms were maintained in
batch mode during soil additions. Two mesocosms (13 and 15)
served as controls.
The experiment was continued until mid December when water
temperatures reached 8 °C. During this period samples (Table 3)
were collected to assess both the response of the ecosystem to the
soil addition, to determine the geochemical behavior of selected
nuclides and to determine bioaccumulation of these nuclides in
both benthic and water column organisms (Table 3).
Ecosystem response - methods
Parameters used to assess the ecosystem response are shown in
table 4 along with appropriate references. Modifications to the
listed methods are described below.
Dissolved inorganic nutrients were filtered immediately after
collection and frozen until analyzed after the experiment was
terminated in December. Benthic nutrient flux was determined for
each mesocosm in mid October to establish whether benthic nutrient
remobilization was within normal limits. Samples for direct
measurement of radionuclide flux were also collected. Initial and
final dissolved samples were obtained as outlined below.
Total suspended matter (TSM) was determined with 47 mm, 0.45 urn
Gelman Metricel filters rather than Nuclepore filters to expedite
sample digestion and analysis at EERF. Tests of these filters
using 0.2 urn filtered seawater determined they could be used to
quantify TSM if copiously flushed with running deionized water for
10 minutes and dried prior to use. If the filters were not
washed, they exhibited a variable loss of weight when particle
free water was passed through them. Depending on the manner in
which the filters were loaded onto the filter support, between 100
and 1000 ml of seawater would pass through the filters before they
became blocked. After a sample had passed through a filter, it
was rinsed with 10 ml of deionized water to remove seasalt.
Several filters were used on each sample in order to obtain the
required volume of seawater for dissolved radionuclide analysis.
Tracking of sample volumes and weight for each filter determined
the replicability of the TSM with these filters and the vacuum
filtration technique to be <10 percent as a coefficient of
variation. When more than one filter was required to obtain 4 1
of filtered seawater, filters were combined after weighing and
sent to EERF for radionuclide analysis as a single sample. Total
sample mass for radionuclide determinations ranged from 2 to 10
mg.
Particles <25 urn in size were also collected to measure the
exposure field of organisms filtering particles in this size
range. These samples were collected by bonding a 25 urn mesh net to
an 8 cm diameter polycarbonate cylinder (1 m long) and submerging
the screened portion of the column in the water while the mixers
10
-------
Table 3. Samples collected for radionuclide analysis during soil study,
September December 1984.
Paramater
Frequency
Radionuclide behavior - Geochemical
Water column
dissolved
particulate,
<25 and Total
Sediments
Resuspended
Sediment
sections
(1 cm)
weekly
weekly
weekly
pre, 1, 6 and
13 weeks post
soil addition
Radionuclide bioaccumulation
Zooplankton weekly
Benthic organisms termination
Mytilus edulis variable
11
-------
Table 4. Summary of ecosystem and geochemical parameters examined
during soil disposal experiment September to December 1984.
Ecosystem response - Water Column
Parameter Frequency
Chlorophyll a weekly
Size fractionated weekly
Fluorescence (in vivo
and DCMU)
Zooplankton biomass weekly
Dissolved inorganic weekly
nutrients (NH3, N02+
N03, P04, Si)
Benthic nutrient
and nuclide flux
System production/ weekly
respiration, Oxygen
and pH
Suspended load: total, weekly
<25 and >25 urn
Temperature weekly
Water input rates weekly
Method
Yentsch and Menzel, 1963
Lorenzen, 1966
Donaghay, 1983
Sullivan, 1983
Solorzano, 1969; Beach, 1983;
Technicon Industrial Systems,
1973
Hunt, 1983; Kelly et al.,
1985
Oviatt et al., 1986;
Carritt and Carpenter, 1966;
Sampou, 1983
Hunt and Smith, 1983
Klos, 1983
Ecosystem Response
Sediments
Benthic abundance
pre and post
soil addition;
termination
Sediment resuspension weekly
Frithsen and Rudnick, 1983
Frithsen et al., 1983
Hunt, 1983
12
-------
were in operation. Water collected was returned to the
laboratory, filtered as above and the filters dried, weighed and
shipped for analysis. Size fractionated fluorescence and DCMU
[3-(3, 4-Dichlorophenyl)-l,l Dimethylurea] fluorescence (DCMU
fluorescence is directly proportional to the total energy absorbed
by photosystem 1 during photosynthesis) were determined on the
whole water and in subsamples of the 25 urn filtered water samples.
Total zooplankton biomass was determined by filtering organisms
collected from duplicate net tows in the mesocosms onto tarred
Metrical filters, oven drying at 50 oc, and reweighing the sample.
These samples were shipped to EERF for analysis. Samples were
enumerated for species composition on September 24 and October 22,
1984.
Sediment resuspension rates were determined weekly with
cylindrical traps (H/D ratio 2.4) located 0.3 m above the sediment
on ridged poles (Fig. 3). Traps were left in place for 24 hour
and located at a similar position in the tank relative to the
mixer action. Sediments were transferred onto 1.0 urn tarred
filters, dried at 50 °C, reweighed and shipped for analysis.
Sediment cores for benthic community analysis were collected in
all systems one week before soil additions and at termination in
the control mesocosms. Samples were also collected from the
experimental systems 1, 6 and 14 weeks after the soil additions.
Ten 2.5 cm diameter cores were randomly collected from each
mesocosm for benthic enumeration. The top 0 to 6 cm of each core
was sectioned and preserved for benthic species enumeration.
Cores were counted individually after sieving through a 300 mesh
sieve.
Sediment samples for total radionuclide distributions as a
function of depth were collected from each mesocosm prior to and
1, 6 and 14 weeks after soil additions. The latter cores were
used to determine the physical translocation of the soil by
gravitational and bioturbation processes. Ten 2.5 cm diameter by
10 cm cores were randomly collected before and immediately after
soil additions. These cores were sectioned into 1 cm intervals
and the sections combined into 2 pooled samples each containing
sediment from 5 cores. On subsequent coring dates 5, 5 cm
diameter cores were collected and sectioned in one cm intervals.
These sections were then subcored with a 2.5 cm cylinder to reduce
effects of particles being carried to deeper depths by friction
during coring. Coarse sand sediments, such as were added to the
mesocosms, were found to be particularly prone to such carry down
when using the larger diameter core barrels. If not controlled by
subcoring, surface sediments carried down along the core barrel
edge were transferred to deeper core sections, causing erroneous
results for the deeper sections. After subsampling, each pooled
section was placed in a tared storage bottle, weighed, dried at 60
oc until dry and reweighed. This data set was used to calculate
sediment water content and porosity. Selected sections from all
mesocosms were sent for total radionuclide analysis by EERF.
13
-------
D
E
P
T
H
00 -
05 -
! 0 -
I 5 -
2.0 -
2.5 -
3.0-
2.3 -
4.0 -
1
45 -
2.8 cm
Figure 3. Schematic of a apparatus used to deploy sediment traps at various
depths in the MERL ecosystem.
-------
Bioaccumulation Studies
Bioaccumulation was determined with two approaches; 1) organisms
collected from within the mesocosm and 2) filter feeding bivalves
maintained in effluent water from the mesocosms. The former were
intended to determine tissue residues in organisms experiencing
natural ecosystem processes and variability. Zooplankton in the
water column were sampled as a function of time while several
species of macrobenthic organisms having different feeding modes,
ie., filter versus deposit feeding, were collected at the
termination of the experiment. The second approach was intended
to obtain data on the kinetics and equilibrium activity of nuclide
uptake in an organism exposed to known particulate and dissolved
phase concentrations of radionuclides in the water column but
separated from the direct influence of the sediment.
Benthic organisms from the mesocosms
In mid December 1984 the water column was drained and sediment
trays removed to a platform for sieving. The surface 10 cm of
sediment was shoveled onto a quarter inch screen and organisms
washed free of mud. Organisms retained on the screen were hand
picked and placed in filtered, clean seawater for depuration (24
h). Soft tissue organisms were separated by species, counted and
subsets of equal number (depending on the availability and size
of the organisms) placed in tared storage vials. These samples
were then weighed, dried at 60 °C, reweighed for wet and dry mass
determinations. Following depuration bivalve shells were cleaned
of adhering mud and the axial shell length measured. The
organisms were then shucked and the wet and dry tissue weight of
individual animals determined as above. Tissues of very small
bivalves were pooled after length measurement to provide larger
sample sizes. Arthropods and other small species were separated
into pooled samples of known number, and wet and dry weights
determined. After all samples had been identified and processed,
a subset of those organisms which were common to all mesocosms
were selected for bioaccumulation determinations. Five species of
organisms were selected. Filter feeding organisms included the
bivalve Pi tar morrhuana, the arthropod Leptocheirus pinquis and
the sea squirt Molqula manhattensis; deposit feeders were Nephtys
insisa and Pherusa affinis. Individual samples of P. morrhuana
having lengths ranging between 1.5 and 5.4 cm were sent from both
the control and soil amended mesocosms to determine radionuclide
activity in the tissues. Remaining organisms were archived for
future analysis as necessary. For the remaining organisms, a
minimum of 2 pooled samples from the control and 2 from the
experimental treatments were each analyzed for bioaccumulation of
radionuclides.
15
-------
Benthic organisms external to mesocosms
Kinetics of nuclide uptake
One uncertainty in bioassay studies is whether or not
bioaccumulation has reached an equilibrium level. A second is the
rate at which equilibrium is achieved. Knowledge of the
"equilibrium" state is critical for dose to man estimates and
other extensions of the bioaccumulation information. These
questions were examined by placing the filtering bivalve Mytilus
edulis in the effluent from the mesocosms and observing the change
in tissue residue of selected nuclides as a function of time.
The exposure units (Fig. 4), used in this study were patterned
after the systems developed by Tracey (in preparation), to examine
the effects of Cu and of sewage sludge on the growth of Mytilus
edulis. An exposure system external to the mesocosms was employed
to minimize potential alteration of the ecosystem within the
mesocosm by the high water column filtering rates common to this
organism. The exposure units consisted of a plexiglass reservoir
to which water siphoned from the main mesocosm was fed by gravity.
The intake for the gravity siphons was located 1 m below the water
surface of the mesocosm. Delivery tubing was 1.3 cm i.d. diameter
polyethylene. Flow rates to the system were regulated with a
knife edge connected to a float.
One requirement of this study was to supply natural particles from
the mesocosms to these organisms in such a way that the
availability of particles to the organisms would not be changed
when animals were removed from the effluent stream as the
experiment progressed. This was achieved by providing small
siphon tubes from the reservoir to individual exposure units.
Animals were placed in 600 ml beakers and water from the small
siphon added at the surface. The excess water was allowed to flow
over the lip of the beakers into a containment trough. Organisms
under study could then be removed as necessary without altering
the supply of food and particles to the remaining animals. The
individual siphon flow rates were adjusted to supply water at a
known rate (50 ml/ min) to each exposure unit providing a 12
minute water turnover time in the beakers. A total of 6
individual siphons were used for each mesocosm with a combined
flow rate of 300 ml/ min of water siphoned from the mesocosm.
Flow rates were checked 3 times per week on the individual siphons
and adjusted as necessary to provide a constant flow of water
during the exposure period. The flow rates employed were
sufficiently fast to minimize loss of particles in the small
reservoir by settling.
The four exposure units were placed in a large tank to protect
against spillage of radionuclides in case any connection broke.
All overflow water from the exposure system was collected in the
bottom of this trough and shunted to the drain system serving the
radiation area of MERL. This entire system was housed in an
enclosed area beneath the catwalks of MERL. The area is equipped
16
-------
TO RAD
SUMP
NOTE' NOT DRAWN TO SCALE
- INTAKE FLOW (from rnesocosm)
GLASS TANK
INTAKE FLOAT
REGULATOR
-PLATFORM
ORGANISM EXPOSURE
VESSEL
OVERFLOW
TROUGH
Fig. 4 Diagram of units in which Mytllus edulis were exposed to constant
volumes of effluent from the MERL mesocosms.
-------
with fluorescent lights on timers which provide light-dark cycles
compatible with daylight periods for any given season of the year.
In addition, the area has a supply of running seawater and holding
tanks in which organisms or sediment cores can be maintained under
ambient water conditions. The temperature of the room can also be
controlled.
Individual organisms of the species Mytilus edulis were collected
with a scallop dredge on October~ll, 1984 from immediately west of
Fox Hill on Conanicut Island in Narragansett Bay. Organisms
ranging between 4 and 5 cm were returned to MERL. Animals between
4.4 and 4.7 cm length were selected, measured with a caliper to
the nearest 0.1 mm, numbered and placed in a holding tank
continuously receiving water from Narragansett Bay. The remaining
organisms were placed in a second large holding tank also
receiving running seawater. These organisms were removed and
exposed to the radionuclides in the effluents from the mesocosms
in a second experiment starting in November.
On October 15, 120 organisms were randomly selected. Five animals
were placed in each of 6 exposure beakers for each treatment and
control mesocosm. A total of 30 organisms were exposed per
treatment. Ten organisms were left in the tank with running Bay
water as external controls. All animals from a given beaker were
collected from each mesocosm in log time series 1, 3, 7, 14, 28,
and 56 days after initial exposure for this experiment (Experiment
#1). Individuals were measured for growth when collected,
shucked, and tissue and shells stored separately in individually
tared containers. Tissue samples were dried at 60 °C and both wet
and dry weight determined. This process was repeated for
experiment #2, starting on November 13, using the organisms held
in the second holding tank.
During this period beakers were cleaned regularly of fecal
deposits. On several occasions beakers were cleaned and the total
amount of fecal material deposited in a 24 h period was
determined. The deposited pellets were rinsed onto a filter,
water removed by vacuum, rinsed free of salt water, dried and
total mass determined. This data was used to examine the
efficiency of these organisms in removing particles by comparing
the mass of particles passing into a beaker (TSM x Volume) to the
total mass of particles retained. Some of these samples were sent
for radionuclide determination. Beakers without mussels did not
trap a significant mass of particulates over the collection
period.
A selected set of mussels were shipped to EERF for radionuclide
determination after two weeks of exposure. The results of this
analysis indicated that the variability between organisms would be
such that detection and quantification of increases in
radionuclide activity could be made with as few as three animals.
Accordingly, a selected subset of those organisms collected were
sent for individual analysis. Uptake rates were examined with
animals from the first exposure experiment, while bioaccumulation
18
-------
at different levels of exposure was determined by comparing
organisms exposed for 28 days in experiment 1 with those from
experiment 2.
19
-------
RESULTS AND DISCUSSION
Ecosystem response
Phytoplankton
Addition of the soil did not result in detectable short or long
term effects on the phytoplankton biomass as measured by
chlorophyll a (Fig. 5). Both of the control systems and
experimental system 12 had low and constant chlorophyll a
concentrations throughout the experimental period. Chlorophyll in
tank 14 was high initially and increased subsequent to the soil
additions. This increase can not be directly attributed to the
soil since a bloom may have been in progress prior to the soil
addition. Subsequent to this maximum, chlorophyll gradually
decreased becoming similar to the other treatments by early
November. Total DCMU fluorescence followed a similar pattern in
that tank 14 was higher than the other mesocosms from September
through early November (Fig. 6). DCMU fluorescence showed peaks
in activity in late September and late October and decreased
throughout the fall. Comparison of DCMU fluorescence in whole
water samples and the <25 urn size class indicates most of the
phytoplankton were less than 25 urn in size in all of the
ecosystems throughout the experiment (Fig. 7a-d). Thus, the
plankton community consisted primarily of flagellates or small
diatoms. In the soil treated systems the slow decrease in
dissolved silica (Si) over the experiment suggests limited uptake
by diatoms (Fig. 8). However, in the control systems the rapid 20
to 30 urn decrease in dissolved Si in late September suggests a
diatom bloom occurred. Since a commensurate decrease in the
experimental mesocosms was not observed it may be inferred that
the soil additions inhibited the ability of the diatoms to grow or
that an excess input of Si from the benthos masked Si uptake by a
diatom bloom.
Production
Comparison of total DCMU fluorescence to total fluorescence
indicates that all systems had active production in the
phytoplankton community throughout the experimental period (Fig
9). Estimates of net daily production based on changes in oxygen
concentration show similar levels of production in all treatments
throughout the experiment (Fig. 10). Negative net daytime
production was observed in the two soil amended mesocosms 10 days
after the soil was added but not in the controls. The decrease
was not observed one week later. Nighttime system respiration was
similar in each treatment throughout the experiment (Fig. 11).
Only tank 14 showed any increase in nighttime respiration and this
for only two sample periods, late September and mid December. The
net daily system production was generally positive throughout the
experiment in both control mesocosms (Fig. 12). The soil amended
tanks showed net respiration 10 days after the soil addition but
this was not sustained beyond this single sample period.
Comparison of the net daytime production and night respiration in
20
-------
28
en
D
CL
O
a:
o
u
14
0
+ T 12
x T 14
D T 13
o T 15
245 275 305
SEP OCT NOV
JULIAN DAY
335
DEC
Fig. 5 Chlorophyll a versus time in soil amended (T-12 and 14)
and control mesocosms (T-13 and 15).
-------
rv>
UJ
CJ
-z,
UJ
u
CO
UJ
QL
O
ID
U
a
o
80
60
40
20 •
0
D T 13
o T 15
245
275
305
335
SEP
OCT
JULIAN DAY
NOV
DEC
Fig. 6 Total DCMU fluorescence versus time in experimental and
control ecosystems.
-------
ro
CO
U
u
u
u
LO
LU
a:
o
u
a
LU
u
u
CO
Ld
a:
o
Z)
u
a
80
60
40
20
x TOTAL
o <25 urn
T 12
245
275
305
335
SEP
OCT
NOV
DEC
80
245
275
SEP
305
OCT NOV
JULIAN DAY
335
DEC
Ld
U
u
CO
LU
a;
o
U
a
UJ
u
u
en
LU
ce
o
n
u
a
80
60
40
20
B
x TOTAL
o <25 urn
T 13
245
SEP
275 305 335
OCT NOV DEC
80
60
40
20
D
x TOTAL
o <25 urn
T 15
245 275 305
SEP OCT NOV
JULIAN DAY
335
DEC
Fig. 7 Size fractionated DCMU (<25 urn particle size cutoff and total) versus
time in soil amended (A & C) and control mesocosms (B & C).
-------
E
D
tn
a
LU
o
in
t-t
a
50
40
30
20
10
245 275 305
SEP OCT
JULIAN DAY
335
NOV
DEC
Fig. 8 Dissolved Silica versus time in soil amended (T-12 and 14) and
control (T-13 and 15)mesocosms.
-------
ro
en
80
UJ 6°
UJ
u
uj 40
o
20
T 12
245
SEP
275
e DCMU
+ FLUOR.
305
335
OCT
NOV
DEC
80
60
40
20
B
T 13
245
SEP
9 DCMU
+ FLUOR.
275
305
335
OCT
NOV
DEC
80
uj 60
u
z
UJ
c_>
u 40
a:
o
20
T 14
DCMU
FLUOR.
245 275 305
SEP OCT NOV
JULIAN DAY
335
DEC
80
60
40
20
D
T 15
s> DCMU
+ FLUOR.
245 275 305
SEP OCT NOV
JULIAN DAY
335
DEC
Fig. 9 Total DCMU and Fluorescence vs time in soil amended (A & C) and
control (B & C) mesocosms.
-------
CTi
(NJ
E
X
C\J
o
0)
o
Q
O
0£
CL
U
>-
<
LU
245
SEP
DEC
JULIAN DAY
Fig. 10 Net daytime production versus time in control (T-13 and 15) and soil
amended (1-12 and 14) mesocosms.
-------
Tl
\
00
E
\
C\J
O
CO
a:
u
CL
cn
u
UJ
x
LD
-1 '
-3
-5
T
T
12
14
245 275 305
SEP OCT
JULIAN DAY
335
NOV
DEC
Fig. 11 Comparison of nightime respiration as a function of time in control
(T-13 and 15) and soil amended (T-12 and 14) mesocosms.
-------
IX)
CD
T)
N.
CM
E
\
CM
O
OT
O
u
Z)
a
o
a:
a.
UJ
2
335
OCT
JULIAN DAY
NOV
DEC
Fig. 12 Net daily production versus time in control (T-13 and 15) and soil
amended (T-12 and 14) mesocosms.
-------
the early phase of the experiment suggests the negative
respiration in tank 12 was due to reduction of water column
production while that in tank 14 was due to a decrease in daytime
production and an increase in nighttime respiration.
Average daily production and respiration during the experiment
show no detectable effects due to the soil addition (Table 5).
Benthic respiration determined 35 days after soil additions shows
a normal range in the respiratory demand by the benthos of all
mesocosms. However, the soil amended sediments show a distinct
trend of lower oxygen consumption (Table 6). Given that total
nighttime system respiration was only slightly depressed at this
time in the soil amended systems, one must conclude that the
respiratory demand of these treatments was shifted to the water
column. This is confirmed when the percentage of the nighttime
respiration due to benthic processes is estimated (Table 6). There
is a clear decrease in the contribution from the sediments which
averages about 30 percent less than in the controls.
Other measures of biological processes (pH and dissolved oxygen)
in the system were also within normal ranges (Figs. 13 and 14).
Oxygen concentrations were initially higher in the soil amended
systems but concentrations decreased within 3 weeks to that of the
control systems. In all treatments oxygen levels were within 1
mg/1 of saturation after October. An increase in 02 is expected
as temperature decreases (Fig. 15) during the fall while pH
increases can be expected as respiratory demands decrease in
response to decreasing temperatures.
Nutrient concentrations were similar in all treatments except for
mesocosm 14, which showed consistently higher Si and NH3 during
the first month of the experiment (Figs. 8, 16, 17). The
sustained high Si in this treatment along with the high
fluorescence suggests diatoms were not responsible for the
increased biomass and production in this system. Conversely, the
rapid drop in Si in the control mesocosms in late September
indicates a significant presence of diatoms in these systems.
Thus, it appears that the soil addition did not affect the
functional aspects of respiration and production but may have
influenced the community structure of the phytoplankton community.
Enumeration of the phytoplankton assemblage would have proven
valuable to this interpretation but was not available due to
fiscal constraints.
Zooplankton
Zooplankton biomass estimates show a continual decline from the
start of the experiment in all treatments (Fig.18). No obvious
change in zooplankton biomass was observed after the addition of
the soil. The decline through the early fall is as expected for
this period. However, the biomass estimates tend to be low
relative to previous mesocosm experiments. The average biomass
over the experiment was lowest in control tank 13 (11 mg/m3)
primarily due to low biomass at the start of the experiment. The
29
-------
Table 5. Average daily production and respiration in control mesocosms
(13 and 15) and soil amended systems (12 and 14) during the
fall of 1984. Units are in g 02nr2d-I.
Mesocosm
12 14 13 15
Net daytime production 1.43 2.43 2.04 1.89
Nighttime respiration -1.34 -1.77 -1.40 -1.38
Net system production 0.09 0.66 0.64 0.50
30
-------
Table 6. Benthic nutrient flux and respiration on Oct. 26, 1984, 35 days
post soil additions. Negative values indicate fluxes are into
the sediment.
Parameter
Mesocosm
Experimental
Temperature, °C
Phosphate, umol/m2/h
Ammonia, umol/m2/h
Silica, umol/m2/h
Oxygen, mg/m2/h
12
14
4.9
105
646
-32.8
14
14
5.5
101
-480
-43.7
Control
13
14.5
2.6
124
223
-69.2
14
14.5
5.2
117
241
-62.0
Night time system
respirationA, mg 02/m2/h -83
Percentage of nighttime
respiration attributable
to sediment
40
-96
46
-102
68
-110
56
A. Mean of night time respiration one week before and one week after the
benthic fluxes were determined.
31
-------
8. 4
8. 2
CO
rsj
I
CL
8.0
7. 8
+ T 12
x T 14
T 13
T 15
245 275 305
SEP OCT
JULIAN DAY
335
NOV
DEC
Fig. 13 Changes in water column pH as a function of time in control (T-13 and
15) and soil amended (T-12 and 14) mesocosms.
-------
GO
CO
245 275 305
SEP OCT
JULIAN DAY
335
NOV
DEC
Fig. 14 Changes in dissolved oxygen concentrations as a function of
time in control (T-13 and 15) and soil amended (T-12 and 14) mesocosms
Variability in oxygen concentrations on any given day shows the range
experienced between dawn and dusk sample periods.
-------
18
15
UJ
12 •
UJ
OL
S 9 1
B T 13
© T 15
* T 12
x T 14
245 275 305
SEP OCT NOV
JULIAN DAY
335
DEC
Fig. 15 Water column temperature vs time in soil amended and control
mesocosms.
-------
GO
on
O
E
D
a
LU
O
CO
CO
0
245 275 305
SEP OCT NOV
JULIAN DAY
335
DEC
Fig. 16 Changes In dissolved ammonia vs time in control and soil amended
mesocosms.
-------
O
E
D
O
CL
Q
UJ
O
CD
cn
»— «
a
1.2
. 6 •
.3
0
245 275 305
SEP OCT
JULIAN DAY
335
NOV
DEC
Fig 17 Response of dissolved Phosphate as a function of time in control and
soil amended mesocosms.
-------
150
245
275
SEP
305
OCT NOV
JULIAN DAY
335
DEC
Fig. 18 Comparison of zooplankton biomass as a function of time in control
(T-13 and 15) and soil amended (T-12 and 14) mesocosms.
-------
other treatments had similar average zooplankton biomass ranging
from 26 to 36 mg/m3.
Species composition of the zooplankton was not determined
routinely; however, examination of the community on September 24
(JD 268) showed polycheate larvae dominating the communities in
tanks 12 and 14 with a diverse mixture of animals in the two
controls. Pseudodjaptomus were notable in the control systems.
On October 22 (JD -96) Acartia tonsa dominated tanks 12 and 14
with Pseudodiaptomus coronatus and Oithona colcarva present in
abundant numbers. Harpactacoids were also present in these
treatments. The control treatments were dominated by
Pseudodiaptomus coronatus (T 13) and Oithona colcarva (T 15).
Each of these treatments had Acartia tonsa as secondary members of
the respective community. Other organisms, especially
harpactacoids and some polycheate larvae, were also present. Even
if some loss of zooplankton resulted from the soil additions the
effects did not appear to be detectable at the level of
measurement employed.
Benthic community
Macrobenthic invertebrate abundances obtained for all four
mesocosms prior to the soil additions showed similar communities
(Table 7) with the following exceptions:
1). Tank 12 had approximately 50% higher total abundance primarily
due to higher Streblospio benedicti and Chaetozone sp. population
densities,
2). Tank 14 supported lower total densities due to the virtual
absence of S. benedicti which was partially compensated for by a
similar species Polydora liqni.
3) Tank 12 had approximately twice the population of the amphipod
Ampelisca abdita than the other mesocosms.
Similarly, the macrobenthic community appeared similar in all
mesocosms at the end of the experiment (Table 8) except for a
factor of two lower total abundance in tank 14 due to absence of
S. benedicti. twice the density of Chaetozone sp. in tank 12 and a
similar density of amphipod species which changed from A. abdita
in 12 and 14 to Leptocheirus pinquis in 13 and 15.
Population densities in all mesocosms increased between August and
December, particularly in mesocosms 12, 13, and 15, where S.
benedicti increased markedly. In mesocosm 14 reduction in
Mediomastus ambiseta was offset by increases in other species
(Table 9) such that no overall change in population density was
observed. Densities of the large polychaete, Polycirrus sp. were
similar in all tanks in both August and December.
Large numbers of organisms greater than 6 mm were recovered when
the sediments were sieved (Table 10). Relatively larger numbers
38
-------
Table 7. Macrobenthic animal densities prior to soil addition (August).
Densities are in animals per core. Data based on 10 replicate 2.54
cm diameter cores collected randomly from the mesocosms. Animals
per m2 can be obtained by multiplying by 1973.5.
Organism
Streblospio benedicti
Mediomastus ambiseta
Nucula annulata
Chaetazone sp.
Polycirrus eximius
Polydora ligni
Ninio nigripes
Microphthalmus sczelkowii
Paranaitis
Asabel 1 ides
Clymenel 1 a
Nephtys insisa
Maldanidae
Asychis elongata
Pholoe minuta
Eteone heteropoda
Spiochaetopterus spp.
Ampharete
Phyllodoce arenae
Yoldia limatula
Lyonsia hyalina
Link, bivalve
Mulinia lateralis
Turboni 1 1 a
Cylichnella sp.
Cerianthiopsis americanus
01 igochaetes
Turbel larian
Molgula manhattensis
Phoronid
Corophium tuberculation
Leptocheirus pinguis
Ampelisca abdita
Ampelicsca spp.
TOTAL
1
X
9.7
14.8
2.5
10.8
0.3
0.1
0.1
0.2
1.2
0.2
2.5
42.4
L2
SD
3.9
5.0
2.4
3.9
0.7
0.3
0.3
0.4
1.2
0.4
2.8
1'
X
0.2
11.3
3.7
0.7
2.0
4.1
0.1
0.1
0.1
1.0
0.1
0.1
0.3
0.1
0.2
0.4
0.1
24.4
\
SD
0.4
7.9
5.5
0.8
2.2
3.2
0.3
0.3
0.3
2.2
0.3
0.3
0.7
0.3
0.6
0.7
0.3
1:
X
6.2
7.5
6.4
1.3
1.4
0.2
0.2
0.1
0.2
0.8
0.3
0.2
0.5
0.1
25.5
!
SD
4.1
6.8
5.6
0.9
0.8
0.4
0.6
0.3
0.4
1.3
0.7
0.4
1.1
0.3
15
X
4.3
12.9
4.4
1.5
1.7
2.1
0.1
0.2
0.1
0.3
1.4
0.3
0.5
0.1
29.9
SD
2.5
13.0
3.4
2.2
1.6
2.9
0.3
0.4
0.3
0.5
2.3
0.7
1.0
0.3
39
-------
Table 8. Macrobenthic animal densities at the termination of the experiment
(December). Densities are in animals per core. Data based on 10
replicate 2.54 cm diameter cores collected randomly from the
mesocosms. Animals per m2 can be obtained by multiplying by
1973.5.
Organism
Streblospio benedicti
Mediomastus ambiseta
Nucula annulata
Chaetazone sp.
Polycirrus ex i mi us
Polydora ligni
Ninio ni gripes
Microphthalmus sczelkowii
Paranaitis
Asabellides
Clymenella
Nephtys insisa
Maldanidae
Asychis elongata
Pholoe minuta
Eteone heteropoda
Spiochaetopterus spp.
Ampharete
Phyllodoce arenae
Yoldia limatula
Lyons i a hyalina
]
X
20.8
8.7
9.2
7.9
0.4
0.3
0.1
0.1
0.1
0.4
L2
0
4
5
5
0
0
0
0
0
0
SD
.7
.8
.0
.0
.7
.7
.3
.3
.3
.7
16
6
0
1
1
0
0
0
0
0
0
0
0
1<
X
.8
.7
.7
.3
.7
.1
.1
.1
.3
.1
.1
.1
.1
\
SD
7.6
8.1
0.9
1.2
1.7
0.3
0.3
0.3
0.7
0.3
0.3
0.3
0.3
i:
X
18.0
15.8
8.2
2.5
0.8
0.3
0.2
0.4
0.1
0.1
0.9
0.3
3
SD
9.5
9.0
4.9
3.3
0.6
0.7
0.4
0.7
0.3
0.3
1.3
0.7
X
22
16
9
4
1
1
0
0
0
15
.3
.4
.2
.0
.1
.6
.3
.1
.9
SD
1.8
7.7
5.5
2.5
1.3
0.9
0.3
0.3
0.9
Mulinia lateralis 1.7 3.7
Turboni11 a
Cylichnella sp.
Cerianthiopsis americanus
01 igochaetes
Turbel larian
Molgula manhattensis
Phoronid
Corophium tuberculation
Leptocheirus pinguis
Ampelisca abdita
Ampelicsca spp.
0
0
2
3
0
.2
.1
.2
.5
.1
0
0
2
2
0
.4
.3
.5
.7
.3
0
0
0
0
1
5.1 4.0 0
.1
.3
.1
.2
.7
.5
0
0
0
0
1
0
.3
.5
.3
.4
.9
.8
1
0
3
1
1
.0
.1
.1
.1
.7
1.5
0.3
3.3
1.3
3.3
TOTAL 54.7 23.3 50.5 65.0
40
-------
Table 9. Comparison of macrobenthic animal densities prior to soil additions
(August) and at termination of experiment (December). Densities are in
animals per core. Data based on 10 replicate 2.54 cm diameter cores
collected randomly from the mesocosms. Animals per m2 can be obtained by
multiplying by 1973.5.
Organism
Streblospio benedicti
Mediomastus ambiseta
Nucula annulata
Chaetazone sp.
Polycirrus eximius
Polydora ligni
Ninio ni gripes
Microphthalmus sczelkowii
Paranaitis
Asabellides
Clymenel 1 a
Nephtys insisa
Mai danidae
Asychis elongata
Pholoe minuta
Eteone heteropoda
Spiochaetopterus spp.
Ampharete
Phyllodoce arenae
Yoldia limatula
Lyonsia hyalina
Unk. Bivalve
Mulinia lateralis
Turbonil la
Cylichnella sp.
Cerianthiopsis americanus
Oligochaetes
Turbellarian
Molgula manhattensis
Phoronid
Corophium tuberculation
Leptocheirus pinguis
Ampelisca abdita
Ampelicsca spp.
PI
9
14
2
10
0
0
0
0
1
0
2
RE
.7
.8
.5
.8
.3
.1
.1
.2
.2
.2
.5
12
PI
20
8
9
7
0
0
0
0
0
0
0
0
2
3
0
DST
.8
.7
.2
.9
.4
.3
.1
.1
.1
.4
.2
.1
.2
.5
.1
PRE
0.2
11.3
3.7
0.7
2.0
4.1
0.1
0.1
0.1
1.0
0.1
0.1
0.3
0.2
0.4
14
Pi
6
6
0
1
1
0
0
0
0
0
0
0
OST
.8
.7
.7
.3
.7
.1
.1
.1
.3
.1
.1
.1
5.1
PRE
6.2
7.5
6.4
1.3
1.4
0.2
0.2
0.1
0.2
0.8
0.
0.2
0.5
0.1
0.1
13
POST
18.0
15.8
8.2
2.5
0.8
0.3
0.2
0.4
0.1
0.1
0.9
0.3
0.1
3 0.3
0.1
0.2
1.7
0.5
15
PRE
4.3
12.9
4.4
1.5
1.7
2.1
0.1
0.2
0.1
0.1
1.4
0.3
0.5
0.1
POST
22.2
16.4
9.2
4.0
1.1
1.6
0.1
0.1
0.9
0.4
1.7
1.0
0.1
3.1
1.1
1.7
TOTAL 42.4 54.7 24.4 23.3 25.5 50.5 29.9 65.0
41
-------
Table 10. Recovery of large animals from terminal sieving of sediments.
Screen size was 6.4 mm. Results are representative, not absolute, as efforts
to recover all organisms were not made during collection of animals for
bioaccumulation studies. Population reported as number per mesocosm.
Organism
Pitar morrhuana
Merceneria merceneria
Leptocheirus pinguis
Nephtys incisa
Pherusa affinis
Molgula manhattensis
Pagurus longicrapus
Crepidula
Crabs (various species)
Gastropodes
Cerabratulus sp.
Petricola pholadiformis
Harmonthoe imbricata
Mytilus edulis
TOTAL NUMBER
RECOVERED BIOMASS
Total, g/mesocosm
Pitar biomass
12
70
-
2
87
6
2
-
8
9
-
-
-
-
-
168
26.0
14.9
Mesocosm
14
44
1
37
15
10
5
-
-
-
9
-
1
-
1
125
18.0
7.3
13
21
5
90
22
15
50
3
2
1
2
1
1
1
-
214
34.7
10.2
15
32
-
90
46
9
20
-
-
2
-
-
-
-
-
199
29.1
17.9
42
-------
of the bivalve Pitar morrhuana were recovered in the soil addition
mesocosms while Leptocheirus pinquis and Molqula manhattensis were
more abundant in the control mesocosms. The terminal sieving
results are in general agreement with the results from the small
core analysis for the latter two organisms. Significant increases
of L. pinquis (Table 9) in the control mesocosms were not seen in
the soil amended systems even though similar numbers were found in
mesocosm 14 prior to the soil addition. The lower numbers in
mesocosm 14 suggest the soil had a significant impact on this
organism and clearly on the sessile M. manhattensis. Even though
L. pinquis appeared to be depleted by the soil addition in tank
14, there were significantly greater numbers than in 12.
The data suggest the addition of soil did not produce significant
change in the macrobenthic community during the experiment with
the exception of the species noted above. Therefore, it is
probable that all four mesocosms were functionally similar with
respect to sediment bioturbation and particle removal processes.
Total suspended loads
Total suspended loads (TSM) were similar throughout the experiment
(Fig. 19a). The same general temporal response was observed in
each mesocosm with high initial concentrations which decreased
through the fall. The TSM levels are within limits previously
found for the MERL mesocosms (Hunt and Smith, 1982). TSM in the
input water was typically higher than in the mesocosms by 30 to 50
percent (Fig 19b). During the initial 6 weeks of the experiment
mesocosm 13 exhibited consistently higher TSM (50 %) than observed
in the other systems. This most likely resulted from the presence
of M. mercenaria that resided in the very surface sediments during
the preceding experiment causing the sediment surface to be more
prone to resuspension.
Size fractionation data for the suspended particulates showed the
majority of the particles (80 to 90 %) were in the <25 micron size
class. The >25 urn size class was generally more constant in the
control treatments (0.7 mg/1) while the experimental treatments
were lower and more variable (Fig 20a-d). The experimental
systems tended to have >90 percent of the particles in the < 25 urn
class during the last month of the experiment. In contrast the
fluorescence data for all systems showed the phytoplankton biomass
to be present in the < 25 urn class throughout the experiment.
Thus, there appears to be a significant fraction of particulates
in the >25 urn size class early in the experiment which were not
directly associated with living phytoplankton. This material may
involve detritus from phytoplankton or be associated with sediment
resuspension processes.
Sediment resuspension rates in the soil amended treatments were
dramatically decreased on addition of the soil (Fig. 21).
Resuspension rates were decreased by 50 and 87 percent in
mesocosms 12 and 14, respectively immediately after soil
additions. Resuspension rates in mesocosm 12 continued to decline
43
-------
O)
E
Q
<
O
Q
UJ
Q
UJ
Q.
in
3
in
o
i-
e
6
245
275
305
335
SEP
OCT
NOV
DEC
Q
<.
O
a
UJ
a
UJ
a.
in
rj
in
o
12
10
8
6
B BAY
245
275
305
335
SEP
OCT
NOV
DEC
JULIAN DAY
Fig. 19 A. Total suspended load vs time in control and soil
amended mesocosms. B. Total suspended load in Narragansett Bay
water entering the mesocosms.
44
-------
en
en
E
O
_J
LU
Q.
to
to
m
E
a
o
a
LU
a
LU
a.
to
T 12
x TOTAL
o <25 urn
245
275
305
335
SEP
OCT
NOV
DEC
T 14
x TOTAL
o <25 urn
245
275
SEP
305
OCT
JULIAN DAY
335
NOV
DEC
B
245
T 13
x TOTAL
o <25 urn
275
305
335
SEP
OCT
NOV
DEC
T 15
x TOTAL
o <25 urn
245 275 305
SEP OCT NOV
JULIAN DAY
335
DEC
Fig. 20 Comparison of the temporal response in total suspended load vs mass
of particles in the < 25 urn particle size. A and C soil amended mesocosms, B
and D control mesocosms.
-------
-C
X
t\j
E
X.
07
C£
Z
a
•—i
tn
z
U
Q_
CO
UJ
o:
245 275 305
SEP OCT NOV
JULIAN DAY
335
DEC
Fig. 21 Sediment resuspension rate as a function of time in control and soil
amended mesocosms. Resuspension rates determined with sediment traps
positioned 0.3 meters above the sediment surface for 24 hours.
-------
until early October. Resuspension in the control treatments also
decreased but over a longer period and to a lesser extent.
Resuspension rates in the soil treatments remained constant and
low relative to the control treatments throughout the remainder of
the experiment. The lower resuspension rates do not appear to
result from changes in macrobenthic animal activity but result
because the soil added physically blocked resuspension of detritus
and sediments subject to resuspension.
Decreases in the resuspension rates and in the >25 urn TSM fraction
in the soil treatments imply that the reduction in sediment
resuspension rates resulted in a smaller contribution from larger
particles to the particulate concentration in the water column. In
addition, in late October a temporal correspondence between
increases in the >25 urn fraction of the TSM and an increase in the
resuspension rate in tank 14 was observed. Since phytoplankton
biomass did not increase at this time, the evidence suggests
sediment resuspension was contributing material to and influencing
the response of this particle size class.
Transport and mobilization of radionuclides
Flotsam
Following soil addition a substantial amount of flotsam remained
on the water surface. This material was primarily detritus from
terrestrial plants. Most of this material (Table 11) was removed
from the mesocosm with a screen (1/8 inch mesh) on September 21
after all soil had been added. This material was dried and total
mass determined. Samples sent to EERF for radionuclide
determinations showed this material had elevated radionuclide
activity relative to the bulk soil (Table 3). However, the total
radioactivity associated with the flotsam was much less than 1
percent of the total added to the tanks. The flotsam represents a
small but potentially significant source of radioactivity to
organisms that live at the ocean surface or actively scavenge
flotsam during dumping operations.
Short term mobilization
Prior laboratory scale studies had shown that a significant
fraction of the soil associated nuclides could be released on or
shortly after contact with sea water (Bonner et al. 1985). These
studies lacked in one of two areas, either the sample size was too
small or the contact time was too short to provide realistic
estimates of expected initial release of radioactivity from the
soils. The mesocosm scale studies were designed to alleviate
these shortcomings by maintaining the ecosystems in batch mode
during and for a short period after the soil was added. By
determining the increase in radioactivity after the additions, the
initial short term (3 to 7 days after additions due to the way
soils were added) mobilization of radionuclides could be
estimated. Longer term mobilization was determined by modeling
the loss of nuclides from the mesocosm as a function of time.
47
-------
Table 11. Total radionuclide activity of organic detrital flotsam recovered
from the mesocosm surface after soil was added to the mesocosms.
in
Ra-226
Pb-210
Po-210
U-234
U-235
U-238
Th-227
Th-228
Th-230
Th-232
Nuclide activity
flotsam, pCi/g dryb
12
1331
2293
6312
1253
35.3
1234
56.2
93.1
619
59.8
14
1228
2753
10520
1134
38.4
1114
51.7
77.1
492
44.2
Total , nCi % of total activitya
Mesocosm Mesocosm
12
32.9
56.6
155.9
30.9
0.87
30.5
1.4
2.3
15.3
1.5
14
25.7
57.5
220
23.7
0.80
23.3
1.1
1.6
10.3
0.93
12
0.21
0.34
1.1
0.23
0.17
0.22
0.11
0.19
0.095
0.11
14
0.16
0.34
1.6
0.18
0.16
0.17
0.08
0.13
0.064
0.066
a. Based on average activity as measured by EERF.
b. Mass removed from mesocosm 24.7 20.9 0.066 0.056
48
-------
Three days after soil additions stopped, the dissolved phase
concentration of all nuclides except polonium and thorium
increased from 5 to 1000 times depending on the nuclide (Table
12). The particulate phase of Po-210, Pb-210, and Th-230 also
increased following the soil addition. This increase was
generally comparable between the two mesocosms receiving the soil
except that Pb-210 had about 3 times higher initial release in
mesocosm 14 (Table 13). The proportion of each nuclide released
to the dissolved phase relative to the total added is consistent
with that observed during soil settling studies but not with bench
scale laboratory studies (Table 14).
The different amounts of radionuclides released under different
experimental conditions, i.e., bench (1 1) and mesocosm (13,000 1)
scales may result from using soils having different total nuclide
activity. Specifically, laboratory scale studies were conducted
using a sample with approximately 50 percent less total
radioactivity than that employed in the mesocosm studies. In
addition, the small sample size in the bench scale may have
resulted in heterogeneous soil samples or have affected the
desorption processes in ways different than experienced at the
mesocosm scale. Even though these differences are present, it is
clear that a small but significant fraction of the nuclides are
released upon initial disposal in seawater.
Long-term mobilization
Total Ra activity in the input water (0.235 +- 0.056 pCi/1, n = 7)
and rate of water additions (499 +- 14 1/d, n = 44) to the
mesocosms varied minimally during the experiment. Ra activity in
the control mesocosms was also constant during this period (Fig.
22a). Following initiation of flow to the mesocosms, total Ra in
the experimental systems decreased in a systematic manner (Fig.
22b) as expected if flushing or sedimentation were occurring.
Since Ra is thought to have a low affinity for particles it was
assumed that no sedimentation occurred. A simple conservative
flushing model, Ct = C0exp(-Qt) + C-j (l-exp(-Qt)), where Q is the
flushing rate of the system, t is time from start of flow and Co,
Ct and Ci are Ra concentrations at t = 0, a later time and in the
input water, respectively, was used to predict the expected total
water column radioactivity if Ra behaved conservatively. For this
experiment Ci was assumed to be constant during the experiment.
Comparison of the measured activities to those predicted under
conservative assumptions demonstrates that Ra was in fact
emanating from the sediments throughout the experimental period
(Fig. 23).
A simple mass balance model,
dM/dt = CiF - CaF - CaS
where dM/dT is the total change in the water column- CiF is the
feed water input (Ci = input concentration, F = flow rate (I/day )
to and from the mesocosm); CaF is the flushing loss (Ca = average
49
-------
Table 12,
Increase in water column activity resulting from addition of soil
to mesocosms. Results based on concentrations observed with
systems in batch mode and three days post completion of soil
additions. Units are in pCi/1. In column 2 d, p, and t refer
to dissolved, particulate, and total radionuclide activity.
# 12
# 14
Isotope/
Fraction
Ra-226
Pb-210
Po-210
U-234
U-235
U-238
Th-227
Th-228
Th-230
Th-232
d
P
t
d
P
t
d
P
t
d
P
t
d
P
t
d
P
t
d
P
t
d
P
t
d
P
t
d
P
t
Post
addition
118 +- 14
1.2
119.2
2.2 +-1.3
1.7
3.9
0.7 +- .2
1.62
2.3
146 +- 4
0.56
146.6
5.3 +- .7
0.041
5.34
156 +- 5
0.55
156.6
1.56 +- .4
0.022
1.58
ND
.006
ND
0.46 +- .3
1.92
2.4
0.08 +- .14
0.085
0.17
Pre
addition
0.12
0.085
0.205
0.41
ND
0.4
ND
0.06
0.06
1.3
0.07
1.4
0.07
0
0.07
0.92
0.048
0.97
0.6
ND
0.6
ND
0.005
ND
0.39
0.01
0.4
ND
ND
ND
Net
118
1.1
119
1.8
1.7
3.5
0.7
1.6
2.3
145
0.5
145
5.2
.04
5.3
155
0.5
156
1.0
.02
1.0
ND
0
ND
0.1
1.9
2.0
ND
ND
ND
Post
addition
118 +- 39
0.69
118.7
8.4 +- 3
2.2
10.6
1.1 +- .5
0.42
1.5
179 +- 5
0.19
179
6.2 +- 1.7
0.01
6.2
175 +- 6
0.2
175
0.4 +-.3
0.1
0.5
ND
ND
ND
1.2 +-.2
0.64
1.8
0.13 +-.07
ND
0.13
Pre
addition
0.13
0.11
0.24
0.34
0.3
0.6
0.13
ND
0.1
1.3
0.007
1.2
0.06
ND
0.06
1.2
ND
1.2
0.22
ND
0.2
ND
ND
ND
0.4
ND
0.4
0.01
ND
0.01
Net
118
0.6
118
8.1
1.9
10.0
1.0
0.4
1.4
178
0.2
178
6.1
0.0
6.1
174
0.2
174
0.2
0.1
0.3
ND
ND
ND
0.8
0.6
1.4
0.1
ND
0.1
50
-------
Table 13. Release of radionuclides within one week of soil additions
to mesocosms. Release based on the increase in water column
concentrations before and after soil addition while mesocosms
were on batch mode.
NUCLIDE
Ra-226
Pb-210
Po-210
U-234
U-235
U-238
Th-227
Th-228
Th-230
Th-232
INCREASE BASED ON
TOTAL a
12
uCi/tank
1.57
0.046
0.030
1.91
0.070
2.06
0.013
0
0.026
0
14
uCi/tank
1.56
0.13
0.018
2.35
0.081
2.30
0.004
0
0.018
0
INCREASE BASED ON
DISSOLVED
12
uCi/tank
1.56
0.024
0.009
1.91
0.069
2.05
0.013
0
0.0013
0
14
uCi/tank
1.56
0.11
0.013
2.35
0.081
2.30
0.0026
0
0.011
0.0013
a. Total equals dissolved plus particulate and assumes the particulate
nuclides measured were not original soil particles.
51
-------
Table 14. Comparison of percentage of soil associated nuclides leached
on contact with seawater during three studies of different
scale. Sample size, seawater volume, contact times and
temperature are: 0.0003 to 0.0012 kg, 1 1, 20 hrs, 20 OC;
4.4 kg, 13000 1, 4 hrs, 22 QQ; and 37 kg, 13000 1, 72 to
168 h, 17 °c in the bench scale, settling studies and
mesocosm study, respectively.
Range in percent released on contact with sea water
Isotope
Ra-226 2
Pb-210
Po-210
U-234
U-235
U-238 3
Th-227
Th~228
Th-230
Th-232
Bench scalel
20 to 80
5 to 28
12 to 26
13 to 33
7 to 26
11 to 32
45 to 53
7 to 32
13 to 33
20 to 31
Settling studies
7
1
1
9
14
9
<1
7
<0. 1
O.I
Mesocosm study
10
0.1 to 0 .7
0.06 to 0.01
14 to 17
14 to 16
15 to 17
< 2
« 1
« 1
« 1
1. Percent release depended on the ratio of particles to seawater volume.
2. H. Y. Li (LOGO) determined that about 15 percent of the Ra associated
with a sample having 50 percent of the total activity in the above
samples could be leached.
3. L. Brush, personnel communication, Sandia National Laboratory found
13 to 22 percent of the uranium remaining was leached during each step
of a sequential exposure of the soil sample Bl to new seawater solutions
Calculation of the total U released in his sequential extractions
suggests 6 to 10 percent of that originally present was released.
His data also suggest a time dependency for the release.
52
-------
WATER COLUMN RESPONSE
CONTROL MESOCOSMS AND BAY
.4-
O
cr
.1 •
13
15
BAY
245
275
305
335
365
125
SOIL AMENDED MESOCOSMS
12
14
245
305
Julian Day
335
365
Fig. 22 Total Ra activity in the water column vs time. A.
Control mesocosms and Narragansett Bay water entering the
ecosystems. B. Soil amended mesocosms. Note scale change between
A and B.
53
-------
WATER COLUMN RESPONSE IF NO BENTHIC FLU
PREDICTED VERSUS MEASURED - MESOCOSM 12
PREDICTED
MEASURED RA
DIFFERENCE
1252
10
50
00 70
WATER COLUMN RESPONSE - NO BENTHIC FLUX
PREDICTED VERSUS MEASURED - MESOCOSM 14
PREDICTED
MEASURED RA
DIFFERENCE
125
10
20 30 40 50
DAYS AFTER FLOW STARTED
70
Fig. 23 Comparison of total measured Ra (dissolved plus
particulate) in the water column to total water column activity
predicted if no remobilization or removal to sediments occured
after soil additions. A. Mesocosm 12. B. Mesocosm 14.
54
-------
concentration during time interval dt); and CgS is the
input/output from the sediment (S - flow rate to/from the
sediment), was used to estimate Ra flushing losses from the system
and to calculate the total sediment input over the time intervals
for which radionuclide activity data were available (Fig.24).
Summation over all intervals provides estimates of the total
mobilization and flushing loss over the experimental period.
The relatively constant difference between the measured and
predicted concentrations after 1 to 3 weeks of flushing (Fig.23)
suggests rates of Ra mobilization became relatively stable. The
total Ra mobilized over individual time intervals was also used to
calculate the rate at which Ra was fluxing from the sediment
(activity/time/area). Generally a higher flux was found at the
start of the experiment which decreased as temperature decreased
during the experiment (Fig. 25). Even so, the calculated rates
remained within a factor of 4 within a mesocosm during the course
of the experiment and are comparable between the two treatments.
Some of the noise in the calculated fluxes may be due to the
slight increase in the temperature experienced several weeks into
the experiment and possibly to periods of increasing phytoplankton
activity particularly in mesocosm 14. The ability of the mass
balance to predict the benthic Ra flux was confirmed by analysis
of samples from benthic chambers collected concurrently with
nutrient samples (Fig. 26). The fluxes determined directly in the
experimental systems are in excellent agreement with the mass
balance estimates considering time intervals involved in
developing the mass balance estimates. Comparison of the measured
benthic flux with those in the control systems further
demonstrates the soils provide a source of at least Ra to the
water column.
The decreasing benthic Ra flux with time may be attributed to
either decreasing temperature or to depletion of available Ra in
the sediments. It seems unlikely that the small temperature
decrease (from 14 down to 8 °C) could significantly affect
chemically driven mobilization processes (desorption, etc.) while
biological mechanisms which regulate the benthic mobilization of
many elements would respond strongly to changes in temperature.
The form of the Ra in the added soil (discrete minerals) was such
that its availability to organisms involved in benthic
remobi1ization must be limited. Thus, in the case of these soils,
the physical phase in which the radionuclides are found probably
constrains but does not eliminate the role of biologically
mediated mobilization. A lower flux could also result if burial
processes removed the contaminated soil from immediate
interactions with the water column, or more simply, if the supply
of readily mobilized Ra is slowly depleted from the soil. Lower
benthic flux may also be expected if the material were exposed to
colder temperature, regardless of mechanism(s) driving the
remobi1ization processes.
55
-------
ORP RA MASS BALANCE, MESOCOSM 12
dM/dT = Ci-F - C(1/2)»F -C(1/2>S
6«-7
O 3.-7H
I
V
!p
4J
D.
D
01
•o -3«-7 H
04
-e«-7
INPUT, FEED
dM/dT
FLUSH LOSS
SED INPUT
285
295
325
355
Be-7
Julian Day
ORP RA MASS BALANCE, MESOCOSM 14
dM/dT = Ci-F - C(1/2>F -C(1/2>S
—B— INPUT. FEED
—x- dM/dT
-^s^- FLUSH LOSS
-*-- SED INPUT
-7«-7
265
295 325
Julian Day
355
Fig. 24 Changes in total Ra activity per sampling interval as
calculated from a simple mass balance equation (See text). Ra
added in the feed water (Input), change in total activity in the
water column (dM/dT), loss from mesocosm by flushing (Flush loss)
and exchange between water column and sediments (Sed input,
addition from sediment is positive). A. Mesocosm 12. B. Mesocosm
14.
56
-------
BENTHIC FLUX, MESOCOSM 12
Determined from mass balance considerations.
7«-10
\
a
a
i
i—
ui
m
i-10-
i-10-
7.-12
Chamber, 303
X
297
278
338
9 11 13 15
TEMPERATURE, oC
BENTHIC FLUX, MESOCOSM 14
Determined from mass balance considerations.
.2«-9
te-10-
o
X
O
I
g
m
-2«-10-
B
338
11 13
TEMPERATURE, oC
is
17
17
Fig. 25 Calculated benthic flux of Ra into the water column
versus temperature. Results based on mass balance calculations
depicted in Fig 24. For comparison the Ra flux measured on
October 26, 1984 is shown by the point labeled Chamber 303.
57
-------
6a-10
RA BENTHIC FLUX BY TREATMENT
ORP PROJECT, OCTOBER 26, 1985
IN
o
u.
<
4e-10-
3e-10-
2e-11 -
12
—I t—
14 13
MESOCOSM
15
Fig. 26 Comparison of measured benthic fl
uxes in control and soil
'
58
-------
Examination of sediment Ra concentrations as a function of depth
during the experiment does not show significant movement of
soi1-associated radioactivity into the sediment. In addition,
soil additions caused the porosity in the surface 1 cm of the
sediment to decrease by 15 percent, primarily due to the sandy
nature of the soil (Fig. 27). The slight decrease in porosity
between 1 to 2 cm can be attributed to coring artifacts.
Subsequent cores did not show significant changes as a function of
depth in the post depositional profiles indicating little movement
of the soil into the sediment. The percent water in the sediments
was also consistent with this observation (see Appendix B for data
tables). Visual observation of the surface sediments prior to
sediment sieving at the termination of the experiment indicated
some dilution of the soil with marine sediment occurred and that
some of the soil was mixed downward slightly.
Post addition Ra concentrations in the surface sediment were
consistent with soil concentrations before additions and with
retention of the soil on the surface of the sediment column (Fig.
28). During the experiment, Ra concentrations in the surface
sediments appeared to decrease in mesocosm 14, possibly reflecting
dilution by lower lying sediments, but increased in mesocosm 12.
Chemical analysis confirmed limited migration of the soil into the
sediments during the experiment. Greater migration may have been
documented had pore water concentrations been measured. Analysis
of other less mobile elements confirmed limited migration into the
sediments for the solid phase of the soil (Appendix B).
Since extensive burial of the sediment did not occur it is
unlikely that Ra bearing particles were removed from interaction
with the overlying water column. Unfortunately, the experiment
was not designed to elucidate whether any or all of the possible
mechanisms contributing to the lower Ra flux at termination were
active. Thus, without further experimentation it is not possible
to determine if a finite reservoir of Ra is present which would
reduce the long term release rates should the material be disposed
of in the sea.
Sediment inventory
The total Ra inventory in each 1 cm sediment section (correcting
for changes in sediment porosity) showed a slight increase as a
function of depth prior to soil additions (Table 15a). The Ra
inventory at termination showed that the top 1 or 2 cm contained
93% of the total radioactivity found in the top 5 cm (Fig. 29).
Unfortunately the calculated Ra inventories, except at termination
in mesocosm 12, do not compare well with the known Ra addition
(Table 15b). In light of the low inventories obtained, the
agreement for mesocosm 12 at termination may be fortuitous,
resulting from the unexpectedly high Ra activity in the surface
sediment layer. The mismatch between post depositional
inventories and added Ra is not easily explained since Ra
concentrations are as expected if no dilution with underlying
sediments occurred. This makes the calculated porosity suspect
59
-------
80
SEDIMENT POROSITY
MESOCOSM 12
70-
o
us
D_
60-
50
Q
80
70-
O
0;
UJ
a.
00-
50
-a- PRE
-x- POST
—v- MID
-*- FIKAJ.
498
DEPTH, cm
SEDIMENT POROSITY
MESOCOSM U
10
,-a
—r-
2
—i—
8
- PRE
- POST
- UID
- FINAL
10
DEPTH, cm
Fig. 27 Porosity of sediments in soil amended mesocosms as a
function of depth before and after soil additions. A. Mesocosm 12
B. Mesocosm 14.
60
-------
700
RA CONTENT OF SEDIMENTS
WESOCOSW 12
800-
fsooH
400-
5 300 H
D
o: 200-
100-
700
e—r
2 4 ft 8
DEPTH, cm
RA CONTENT OF SEDIMENTS
MESOCOSM M
-a-- PRE
-A- POST
-*-- FINAL
4 6
DEPTH, cm
10
Fig. 28 Ra activity in sediments vs depth before and after soil additions,
61
-------
Table 15. A. Ra inventory in the sediments receiving soil in nCi/mesocosm.
Inventory calculated from I = A x (1-P) x d x z x 2.5x104, where I is the
inventory in a given layer of sediment in Curies, A is the activity in the
sediment, P is porosity, d is the dry density of the material , z is the
depth interval (cm) and 2.5xl04 is the area of the sediment surface in
CITK.
B. Mass balance comparison to known additions.
A. Inventory
12
14
Depth
0-.5
0-1
5-1
1-2
2-3
3-4
4-5
6-7
8-9
Total
0-5
Pre
13
14
15
20
20
16
15
81
Post
4,300
2,400
420
330
34
19
7,500
Final
15,000
870
150
94
31
19
16,000
Pre
9
13
13
14
14
13
63
Post
8,600
780
940
35
24
10,000
Mid
5,300
2,900
300
220
8,700
Final
2,400
3,900
370
8
150
63
8,500
B. Mass balance comparison; cummulative percentage of total Ra added.
Depth
Interval
0-1
0-2
0-3
0-5
12
Post
42.7
45.3
47.2
47.3
Final
96.9
102
103
104
Post
54.8
59.7
65.6
65.8
14
Mid
33.8
52.2
54
Final
25.9
50.7
53
54
62
-------
CTi
OO
Fig. 29 Ra distribution in top 5 cm of the sediment column as a percentage of
the total Ra in the upper 5 cm prior to (A and C) and at the termination of
the experiment (B and D) in mesocosms 12 and 14, respectively.
FRACTION OF RA IN TOP 5 CM BY SECTION
A MESOCOSM 12
r-.5(l755)
.75(19Z)
-.25(16%)
1.5(24%)—'
PRE
FRACTION OF RA IN TOP 5 CM BY SECTION
MESOCOSM 12
.25(93%)—/] | i |
FRACTION OF RA IN TOP 5 CM BY SECTION
WESOCOSM 14
C
4.5(22%)
3.5(22%)-'
PRE
FRACTION OF RA IN TOP 5 CM BY SECTION
MESOCOSM 14
FINAL
FINAL
-------
because other parameters entering the calculation are well
defined.
Water column and sediment data were insufficient to undertake a
similar mass balance and inventory comparison for other elements
associated with this soil.
Mass balance summary
Total input, loss, mobilization and calculated residual Ra
activity are summarized for both soil amended mesocosms in Table
(16). Clearly the dominant source of Ra to the water column was
the soil. A small but significant amount of Ra and other
nuclides, notably Po-210 (Table 11) were removed with organic
detritus which floated to the water surface after soil additions.
Ra was continuously mobilized during and after soil additions.
Approximately 15 percent of the added Ra was mobilized over 3
months. Between 60 and 70 percent of the total Ra mobilization
occurred during or immediately following (within 3 days) initial
contact with seawater. Sediment inventories throughout the
experiment were generally half of that expected and negate
verification of the observed mobilization and export from the
mesocosms from sediment analysis.
Partitioning of Nuclides in the water column
Radium
The distribution of Ra between dissolved and particulate phases
was similar in both control systems and the Bay feed water (Fig.30
a,b,c) during this experiment. In these waters, between 40 and 95
percent of the Ra was in the dissolved phase throughout the
experiment (Fig. 30d). Dissolved Ra was also the dominant form
after the addition of the Middlesex soil (Fig. 31). In contrast to
the controls, the fraction of dissolved Ra in the soil treatments
never fell below 97 percent of the total radium in the water
column.
Distribution coefficients for Ra (Kd = pCi Ra/Kg particles/ pCi
Ra/Kg seawater) were relatively constant throughout the experiment
in both controls and feed water (Fig. 32). The observed Kd's are
considerably higher than normally found for an element considered
to be non-particle reactive (Santschi et al., 1983; Amdurer et al.
1983). The experimental mesocosms had Kd's similar to those in
the controls and Bay water prior to addition of the soil.
Addition of the soil and subsequent release of Ra caused the
distribution coefficients to decrease by approximately 2 orders of
magnitude. Distribution coefficients tended to increase with time
but never returned to the pre-addition values.
The discrepancy between distribution coefficients is difficult to
explain. The cause may be approached from two directions. If
Kd's in the range of 102 to 103 are accepted as true reflections
of adsorptive equilibrium (Santschi et al., 1983), the higher Kd's
64
-------
Table 16. Summary of input, output and mobilization of Ra associated with
Middlesex soils added to seawater.
Compartment
INPUT
Soil
Feed
TOTAL
LOSS
Flotsam
Flushing
TOTAL
MOBILIZATION
Initial
Benthic
TOTAL
RESIDUAL
Calculated
Measured
Total ,
12
15,700
8
15.700
33
2,030
2,060
1,560
751
2,310
13,400
16,000
nCuries
14
15,700
8
15,700
26
2,210
2,240
1,510
1,070
2,580
13,100
8,500
Percentage of
12
99.9
0.1
100
0.21
12.9
13.1
9.9
4.8
14.7
85
102
added Ra
14
99.9
0.1
100
0.16
14.1
14.2
9.6
6.8
16.5
83
54
65
-------
.4-
RADIUM FRACTIONS, T-13
WATER COLUMN. SEPTEMBER TO DECEMBER 1984
A
.1 -
DB.
RADIUM FRACTIONS, T-15
WATER COLUMN. SEPTEMBER TO DECEMBER 1904
249
S7S
300
339
DS.
PART.
TOTAL
Z49
389
RADIUM FRACTIONS, BAY
WATER COLUMN. SEPTEMBER TO DECEMBER 1984
a-,
en
.1 -
DO.
PART.
TOTAl
100
fO'
80
70-
80
30
40
PERCENT DISSOLVED RA
WATER COLUMN. SEPTEMBER TO DECEMBER 1984
249
t7S
300
JULIAN DAY
339
369
30
D
T-13
T-18
SAY
249
ITS
309
JULIAN DAY
339
383
Fig. 30 Partitioning of Ra between total, dissolved and partlculate phases in
control mesocosms (A and B) and Narragansett Bay feed water (C) as a function
of time. The percentage of the Ra in the dissolved phase of each treatment is
depicted in D.
-------
150
100-
O
Q.
245
150
100-
O
a
245
RADIUM FRACTIONS, T-12
WATER COLUMN. SEPTEMBER TO DECEMBER I
275
305
JULIAN DAY
365
RADIUM FRACTIONS, T-14
WATER COLUMN. SEPTEMBER TO DECEMBER 1984
275 305
JULIAN DAY
335
365
Fig. 31 Partitioning of Ra between total, dissolved and
particulate phases in soil amended mesocosms as a function of
time.
67
-------
DISTRIBUTION COEFFICIENTS
Radium
3-
>4-
o
3-
T-12
T-14
T-13
T-15
BAY
249
275
305
DAY
335
365
Fig. 32 Calculated distribution coefficient for Ra as a function
of time for all mesocosms and lower Narragansett Bay water.
68
-------
in the control and Bay water must result from nonequilibrium
processes which increase the particulate phase concentrations,
e.g., active uptake by phytoplankton. Previous discussions of
ecosystem response suggested the control systems had a more active
diatom community than the experimental systems. If so, these
organisms may have played a role in determining the concentration
of particulate Ra to a greater extent than in the experimental
treatments.
On the other hand, in the experimental systems, the total number
of available adsorption sites for Ra uptake on the in situ
particles in the water column may not have been sufficient for an
equilibrium to develop in a large excess of dissolved Ra. Thus,
even though particulate Ra concentrations increased by 10 to 20
times over control systems (Table 17), a limited number of
adsorption sites in the presence of excess dissolved Ra would
cause saturation of those sites, resulting in low calculated
distribution coefficients. The low Kd's for the experimental
systems (Table 18) argue that dissolved and particulate phases in
these systems were out of equilibrium throughout the post soil
addition period. The systematic temporal increase in the
calculated Kj's as the experiment progressed (Fig. 32) suggests
the continuous decrease in dissolved Ra, when coupled with
constant particulate phase concentrations, resulted in slow
movement towards equilibrium conditions.
If either of the above discussions are valid, Ra removal from the
water column will become less efficient as a result of the soil
additions. In the first case loss of diatoms decreases the
ability of the system to cleanse itself due to removal of a
transport route. In the second case, flushing (in the real ocean
advection and dilution) from the system or uptake on newly formed
particles becomes the only major mechanisms acting to decrease the
Ra activity. Dilution only serves to decrease the radioactivity,
not remove the Ra from the water column. Removal of Ra from the
water column would depend on the ability of "new" particles,
undersaturated with Ra, to carry the excess Ra from the water
column. In normal oceanic systems these "new" particles would
include particles introduced via atmospheric transport and from
biological processes. Depending on the depth of the water column
lateral sediment transport coupled with resuspension could also
influence Ra removal.
69
-------
Table 17. Summary of Ra activity in particles from experimental and control
mesocosms during experimental period. Concentrations in pCi/g.
Julian
Day
261
269
272
276
290
297
312
325
338
Average
addition
Average
Average
Average
12
21.7
301
166
120
162
76
205
117
243
post
174
all controls and Bay
controls only
prespike
Ratio experimental to control
14
29.8
255
89
158
186
176
333
194
152
193
= 10.5
Tank
13
20.3
11.2
12.1
25.2
6.1
4.6
13.3
15
20.8
40.2
16.7
32.6
9.0
3.4
9.2
18.8
Bay
9.5
4.9
14.6
8.7
10.0
5.4
40.2
13.3
16.2
17.5
23.2
70
-------
Table 18. Ra distribution coefficients in the water column during
soil addition experiment. Presented as log Kd.
Radium
DAY
261
269
272
276
290
297
312
325
338
AVERAGE
SPIKE
AVERAGE
AVERAGE
AVERAGE
T-12
5.26
3.45
3.14
3.08
3.39
3.08
3.62
3.55
4.01
POST
3.53
ALL CONTROL
ALL CONTROL
PRESPIKE
T-
5
3
2
3
3
3
3
3
3
3
AND
14
.36
.35
.92
.12
.31
.49
.79
.9
.71
.56
BAY
T-
5
4
5
5
4
4
4
13
.32
.97
.04
.58
.46
.99
T-15
5
5
4
5
4
4
4
5
.14
.49
.06
.28
.61
.30
.68
.04
BAY
4.
4.
4.
4.
4.
4.
5.
4.
5.
5.
5.
83
49
78
79
7
56
46
93
03
07
28
71
-------
Distribution coefficients of other nuclides
A limited set of data was available to estimate distribution
coefficients for other nuclides. Available data suggest little
change in the distribution of the Pb, Po, and Th nuclides before
and after the soil was added (Table 19). The Kd's for these
nuclides are consistent with those report by Santschi et al.,
1983. However, uranium appears to have behaved similarly to the
Ra in that generally lower Kd's (about lOx) were found after the
soil addition. As with Ra, this probably reflects the very large
increase in dissolved Uranium nuclides after soil additions which
was not found for the other nuclides.
The Pb and Po distribution coefficients determined from small
scale bench studies and during the soil settling study (Bonner et
al., 1985) are similar to those found in the full scale mesocosm
study (Table 19). The Kd's for U and Th from both the bench and
settling studies appear to be larger than found in the control
systems and in the Narragansett Bay feed water while that for Ra
is smaller. These differences point strongly to nonequilibrium
conditions within the various experimental protocols measuring
distribution coefficients. Most likely, the limited availability
of particles in contact with the dissolved phases (Di Toro et
al., 1986) in the full scale mesocosm study caused the observed
differences. The more appropriate tool for assessing the behavior
of these nuclides appears to be the larger scale ecosystem since
partitioning coefficients different from bench scale laboratory
experiments were found under the more natural conditions of the
mesocosm. The results further point to the necessity for better
understanding where in the disposal process nonequilibrium and
equilibrium processes dominate the geochemical behavior of an
element.
Radionuclide distribution within particle size classes
Understanding the association of nuclides with various particle
sizes is important to determining exposure of various animals to
the nuclides. During this study the <25 urn particle size class
contributed greater than 80 percent of the total suspended load in
the mesocosms. The concentration of Ra in this size class was
generally greater per unit mass (Fig. 33) than found for the total
suspended load. Thus, particles greater than 25 urn appeared to
carry a relatively lower fraction of the particulate bound Ra than
did the smaller particles. As a result, those organisms feeding
selectively on the smaller size class are most likely to
experience greater exposure to the nuclides, depending on relative
rates of injestion and filtering of the water column. The higher
concentration in smaller particles is not unexpected due to the
higher surface area associated with these particles.
Quantitative estimates of size class associations of particulate
Ra on a per liter basis (pCi Ra / g TSM x g TSM / 1) were
inconclusive, primarily due to high counting errors associated
72
-------
Table 19. Distribution coefficients for nuclides other than Ra. Distribution
coefficients calculated only when activities were detectable.
Results are also compared with other partitioning studies.
TANK DAY
DISTRIBUTION COEFFICIENT (log)
Ra-226 Pb-210 Po-210 U-234 U-235 U-238 Th-227 Th-230 Th-232
• — — — — — — — — — — -._____ _ _ ______ _ _ _ _ _ _ _ ____________________ __________._ — _—._.___ — _ — _ — — -
Pre addition, Bay and controls
BAY
12
14
13
13
15
15
297
261
261
261
290
261
290
N
N
5.39
N
NR
5.33
NR
N
N
N
N
NR
5.82
NR
3.62
4.14
3.19
3.74
3.62
3.58
4.08
3.33
N
N
N
5.11
4.31
4.95
3.08
4.12
3.38
3.62
3.57
3.4
3.72
N
N
1.79
N
4.7
3.08
N
.45
.89
.56
4.98
5.31
4.16
4.95
Average 5.03
Post addition
5.36 5.82 3.71 4.43 3.56 3.19 4.61
N
N
N
N
4.34
4.98
4.92
4.75
12
12
14
14
269
290
269
269
Average
5
4
5
3.6 5
.26
NR
.84
.25
.12
5.89
NR
5.37
5.18
5.48
2.97
2.44
2.62
2.56
2.65
3.34
2.63
N
3.02
3.00
2.93
2.53
2.47
2.69
2.66
3.66
4.35
N
2.26
3.42
6
6
5
5
5
.48
.24
.35
.31
.85
N
N
N
4.71
4.71
Bench scale studies
Range
3.6
4.6
4.9
5.3
5.3
5.7
3.7
4.1
3.5
4.1
3.7
4.2
4.7
5.1
5.9
6.1
6.1
7.5
Soil settling study
after 4 hours
n = 3 4.5
5.8
6.1 4.7
4.5
4.6
5.9
6.6
6.1
N indicates either the dissolved or particulate phase was undetectable.
NR indicates no analysis performed on either the dissolved or particulate
phase.
73
-------
400
I300
1
•o
RADIUM PARTICULATE SIZE FRACTIONS
TANK -12
•ZOO
I
0>
TOTAL 400
RADIUM PARTICULATE SIZE FRACTIONS
TANK -14
¥300-
f
'ZOO-
100-
B
-B- TOTAL
-»~ <2S um
Z43
303
339
3«9
245
309
333
389
30
JULIAN DAY
RADIUM PARTICULATE SIZE FRACTIONS
TANK -13
JULIAN DAY
RADIUM PARTICULATE SIZE FRACTIONS
ts-
•13-
3-
TOTAL SO'
-------
with low radioactivity and very small sample sizes. Results from
mesocosm 14 suggest that the majority of the Ra was found in the
<25 urn fraction; the general trend in the other mesocosms, both
control and experimental, tend to support this conclusion. Data
on other nuclides are insufficient to draw any conclusions
regarding size associations.
Sediment resuspension
A potential source of particles in the water column is resuspended
surface sediment particles. Previously it was indicated that a
major effect of the soil addition was to reduce the rate of
resuspension. In spite of this, nuclide activity in particles
caught in sediment traps within 4 days of completing soil
additions compares favorably with activities found in surface
sediments (Fig. 34). The lower activities observed in mesocosm 14
sediment trap samples are probably due to dilution of the soil
with low nuclide bearing sediments and indicates the sediment in
this system may have been less compact allowing more immediate
mixing of indigenous sediments with the soils. If so this is most
likely an artifact of the the previous experiment with clams.
Regardless of cause, evidence indicates that particles carrying
radionuclide activity can be resuspended and made available to
filter feeding organisms. These results also suggest that post
depositional transport of the nuclides may occur in association
with these resuspendable particles.
The activity of radium in resuspended particles decreased as a
function of time following deposition (Fig. 35), indicating that
one of two processes was operating: 1) resuspendable soil was
diluted with underlying marine sediment as a result of
bioturbation and physical settling or 2) radium was lost from the
resuspendable soil particles to the water column. For radium,
both processes are probably important as previously discussed.
Limited analysis of the U and Th nuclides also shows this
depletion in the resuspended matter four weeks after the soil
addition. The strongly particle-reactive nature of Th suggests
dilution by sediments low in nuclides is a significant factor, not
just mobilization to the water column. These results suggest
that, given time, the soil will become mixed with ambient
sediments, thus decreasing transport from the site.
In addition, nuclide activity in suspended particulate matter
(Fig. 36) was 2 to 3 times higher than found in the sediment trap
particles throughout the experiment in mesocosm 14 and by the mid
point in mesocosm 12. The relatively constant temporal Ra
concentration in the particulate matter suggests that uptake onto
particles generated in the water column, not those resuspended
from the sediment, was probably the dominant source of particulate
bound nuclides. Thus, particulate bound nuclides were most likely
made available to filter feeding organisms through post disposal
mobilization processes with subsequent incorporation into
particles generated in the water column, rather than directly from
unaltered, resuspended soil particles.
75
-------
SEDIMENT VS SEDIMENT TRAP
MESOCOSM 12
450
400
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ISOTOPE
SEDIMENT VS SEDIMENT TRAP
MESOCOSM 14
SEDIMENT!
SED.TRAP
SEDIMENT
SED.TRAP
ISOTOPE
Fig. 34 Comparison of radioisotope activity in resuspended and
surface sediments (upper 0.5 cm) four days after soil addition to
the mesocosms.
76
-------
300
245
RADIUM VS TIME
SEDIMENT TRAP DATA
275 305
JULIAN DAY
335
365
Fig. 35 Radium activity in resuspended particles versus time,
Control mesocosms T-13 and 15, soil amended mesocosms T-12 and 14,
77
-------
COMPARISON OF ISOTOPES IN PARTICULATES
RADIUM, Mesocosm 12
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COMPARISON OF ISOTOPES IN PARTICULATES
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JULIAN DAY
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Total
Sad. Tr
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319
341
Fig. 36 Comparison of radium activity in particles, sediment and
resuspended sediments as a function of time in soil amended
mesocosms.
78
-------
Bioaccumulation of nuclides
Mytilus edulis
Growth parameters
Blue mussels, Mytilus edulis. exposed to mesocosm effluent water
actively filtered the water supplied throughout the two exposure
experiments. Organisms of relatively uniform length (42 to 47 mm)
were used in Experiment 1 while organisms for Experiment 2 were
slightly shorter, at 39 to 43 mm. Growth was observed in all
treatments but the final length attained varied among animals
within a treatment (Fig. 37a), time of exposure and also among
treatments (Fig. 37b).
The greatest average change in length was observed in the external
controls and soil amended mesocosm 14 (Fig. 38). The length of
M. edulis in mesocosm 14 increased systematically from day 1 of
the experiment. A similar systematic increase in average length,
but of smaller magnitude, was found for organisms exposed to
effluents from mesocosms 13 and 15. Over the experimental period
organisms from mesocosm 12 did not show growth. As expected,
individual organisms exhibited a wide range in growth within a
treatment for a given period of exposure (Fig. 38a). The ranking
in growth increment between the mesocosms was similar to the
ranking of average chlorophyll abundance in the mesocosms for a
given exposure period (Table 20). Particularly, mesocosm 14 had
significantly higher chlorophyll concentrations and the largest
average increase in animal length. Mesocosm 12 appears as the
exception during both experiments having a consistently lower rank
in growth relative to chlorophyll ranking.
Individual dry tissue weight varied within a treatment (Fig. 39a)
for a given exposure interval but on average showed little change
from organisms sampled after one day of exposure. No evidence of
spawning was observed in these animals. Only mesocosm 14, with
relatively high chlorophyll, and the external control organisms
showed a significant gain in tissue weight (Fig. 39b). With the
exception of mesocosm 14 the organisms appeared to have had a food
supply which was adequate to increase shell length but not body
weight.
Uptake of radionuclides - Experiment #1
Incorporation of radium into the tissues of M. edulis was rapid
upon initial exposure (Fig. 40 a&b). After one day of exposure
tissue concentrations had increased 4 to 5 fold over the
background radioactivity in the day 0 external control animals.
Animals from the control mesocosms were not analyzed for Ra after
1 day. However, after 14 and 56 days, Ra activities in the
control animals averaged 1.6 to 2.5 times greater than in external
control organisms, respectively. Thus, organisms exposed to
control tank effluents also experienced an increase in Ra activity
relative to the external controls immediately after transfer. On
79
-------
55
E
E
to
§
45-
35
FINAL LENGTH
Mytilus edulls
x
V
V
X
/*
D
*
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CJ T-12. £
x T-14. E
v T-13. C
3 T-15. C
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DAYS
AVERAGE FINAL LENGTH
Mytilus edulis
E
C9
45-
40
B
—i—
14
—i—
21
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—i—
35
—i—
42
—i—
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-x— T-14. E
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-*- EXT. C
0 7 14 21 28 35 42 49 56 63
DAYS
Fig. 37 A. Final shell length of individual mussels held in
effluents from the mesocosms as a function of time after exposure
initiated. A. Individual organisms. B. Mean final shell length
of 5 animals per treatment per time interval. Error bars for
mean shell length not shown to reduce confusion on graph.
Standard deviation of the lengths were similar and ranged between
1 and 2 mm.
80
-------
GROWTH VS TIME OF EXPOSURE
Mytilus edulis
£
-£
O
£n
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5-
4-
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DAYS
AVERAGE GROWTH VS TIME
Mytilus edulis
38
83
Fig. 38 A. Increase in shell length of organisms vs time A
individual mussels. B. Average growth increment vs time. Error
bars for mean growth increment not shown to reduce confusion on
graph.
81
-------
Table 20 a). Average chlorophyll a concentrations (ug/1) in the water column
of the mesocosms during the Mytilus edulis exposure experiments 1 and 2.
b). Rank in abundance of chlorophyll a or average change in shell length
after 28 and 56 days of exposure.
a.
Mesocosm
12
14
13
15
28
1.
6.
2.
1.
Experiment
days
90
27
27
94
1
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Experiment 2
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23
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79
28
2.
3.
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1.
days
64
54
73
52
b.
Mesocosm
Experiment 1
28 days 56 days
Chi a Growth Chi a Growth
Experiment 2
28 days
Chi a Growth
12
14
13
15
3
1
2
4
4
1
2
3
2
1
3
4
3
1
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4
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4
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2
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82
-------
TISSUE DRY WEIGHT
Mytilus edulis
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DAYS
AVERAGE TISSUE DRY WEIGHT
.8-
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rt .
Mytilus edulis
-> T « n I-
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0 7 14 21 28 33 42 49 36 63
DAYS
Fig 39 Tissue dry weight of mussels as a function of time A.
Individuals. B. Average.
83
-------
ACTIVITY VS TIME OF EXPOSURE
RADIUM IN MUSSELS
4-
3-
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AVERAGE ACTIVITY VS TIME OF EXPOSURE
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DAYS
Fig. 40 Ra activity in Mvtilus edulls tissue, pCi/g dry weight
as a function of time in all mesocosms and in control organisms
held external to the exposure systems. A. Individuals. B.
Average Ra activity.
84
-------
this basis, the net initial increase in Ra activity in the mussels
from the experimental systems was only a factor of 2 to 3 times
greater than the control mesocosms.
Radium activities continued to increase throughout the 56 days the
organisms were exposed to elevated radium concentrations (Fig.
consistent manner between mesocosms. The
spite of a continuous decline in total
40b) although not in a
increase in Ra came in
radium activity in the water
supplied to these
data are equivocal with respect to the rate of
whether an equilibrium activity was achieved.
mesocosm 12 and 14 appear to have reached some
activity after about 14 days of
increases again after 56 days.
organisms. The
increase and
Mussels from
limiting Ra
exposure, but mesocosm 12
Attempts to obtain constants for
the rate of increase through regression analysis using a variety
of rate laws (exponential, linear, logarithmic) were only
partially successful. The best fit regressions suggest that a
linear increase with time best describes the rate following the
initial increase on day 1. Much of the difficulty probably lies
with the large range in activities found for each sample period
and possibly the ecological response (food supply) of each
mesocosm.
Cullen (1983) has shown that some of the difficulty in
interpreting incorporation of metals into the tissue of the
by variation in dry tissue
bivalve Merceneria merceneria
weight between animals
is caused
variability can be reduced by
total radionuclide activity
opposed to the weight normalized
the mussel data from this
uptake in mesocosm 12 did not
This
calculating and comparing the
associated with each animal as
radioactivity. Examination of
perspective suggests that radium uptake in
increase significantly beyond that observed after the initial 24
hours of exposure until after day 28 (Fig. 41a&b). However,
mussels from mesocosm 14 (with a better food supply) did increase
in total radioactivity through day 28 after which tissue activity
became constant. From the chlorophyll a and growth data it
appears that mesocosm 14 mussels were growing better and building
new tissue, and thus may have had greater opportunity to increase
radium concentrations with addition of new tissues. The evidence
is relatively unequivocal that these organisms, when exposed to
elevated radium activity in the water column, do increase their
tissue residue level and that the amount of growth as affected by
the food supply influences the total uptake of nuclides. It is
less clear what rate law best describes the uptake and whether
some equilibrium activity per unit dry weight will be reached.
Clearly the food availability question will influence these
issues.
Uptake of radionuclides - Experiment #2
Organisms from experiment 2 were exposed to effluents for a
maximum of 28 days. Animals were collected on a logarithmic time
series. Growth parameters and nuclide uptake in the mussels
exposed for 28 days were compared with mussels exposed for a
85
-------
TOTAL ACTIVITY PER ANIMAL VS TIME
RADIUM IN MUSSELS
1.5-
O 1 "
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DAYS
AVERAGE TOTAL ACTIVITY PER ANIMAL
RADIUM IN MUSSELS
1
o
a
O£.
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DAYS
42
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T-12. E
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EXT. C
36
63
Fig. 41 Total Ra in tissues of Mytilus edulls tissue, pCi/animal, as a
function of time in all mesocosms and in control organisms held external
to the exposure systems. A. Individuals. B. Average total Ra per
animal
86
-------
similar period from experiment #1 to test the dependence of uptake
on exposure concentrations. The average dissolved and total
radium in the water column was a factor of 2 lower in experiment 2
than in experiment 1 (Table 21) but activities of particulate
bound Ra on a volume basis were similar in both experimental
mesocosms during both experimental periods.
Mytilus edulis used in experiment 2 exhibited similar variability
in shell length but were slightly shorter than those in experiment
1 (Fig. 42 a&b). Similar increases in length occurred within each
treatment with the exception of mesocosm 15, in which growth was
about 30 percent of that observed in experiment 1 (Fig. 43 a&b).
Growth of external control animals from experiment 2 was similar
to that observed in animals from mesocosm 13, but less than in
mesocosm 14 and greater than in mesocosms 12 and 15. This pattern
is the same as found during experiment 1 and indicates the
relative food supply had not changed within each treatment between
experiments. Dry tissue weight of individual and average animals
are also less in experiment 1 as expected for the smaller animals
(Fig. 44a&b).
The radium activity in the mussel tissue for both experiments was
similar (Fig. 45a&b) in spite of smaller animals and a factor of
two difference in the total radium activity in the source water
during experiment 2. However, total activity per animal (Fig. 46)
was greater in animals from experiment 1 due to the larger tissue
weight in these animals. Thus any food chain transfer scenario
must incorporate estimates for the total radioactivity associated
with an organism and not rely just on concentrations in the
tissues.
The similar Ra activity in the mussel tissue of the two
experiments, in the face of a two-fold decrease in the total Ra
activity in the source water, suggests Ra accumulation in the
mussels is either insensitive to changes in supply of this
magnitude or that the source of the Ra to the animals is not
associated with measures of total radioactivity. Comparison of
the average total particulate radium (pCi/1) between experiments
(Table 21) suggests less variability between and within treatments
in this phase than in the dissolved phase. This implies that
uptake of radium is through the particulate phase, as Tracey
(personal comm.) has found for Cu.
Radium in Mytilus edulis Fecal Matter
The mass of fecal material passing through the mussels was
determined for known time intervals. Comparing the temporal rate
of fecal production, mg an-1 d~l. to the total suspended load in
the water column shows general agreement in that both decreased
through the experimental period (Fig. 47). The initial decrease
in fecal production on Julian Day 292 (1 day of exposure) is
probably related to clearance of particles ingested while mussels
were held in the feed water to the mesocosms and reflects a
greater source of particles than were available in the mesocosms.
87
-------
Table 21. Average concentration of radium-226 in dissolved and participate
phases during mussel exposure experiments 1 and 2. Units are pCi/1.
Experiment 1 Experiment 2
28 day
Tank
12
14
13
15
Dis
59
68
.18
.19
Part
.14
.61
.23
.04
Total
59
69
.41
.23
56 day 28 day
Dis Part Total Dis Part Total
47 .18 47 25 .25 25
51 .5 52 27 .40 27
-------
ANIMAL LENGTH, FINAL
28 DAY EXPOSURE COMPARISON, EXPERIMENTS 1 AND 2
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28 DAY EXPOSURE COMPARISON, EXPERIMENTS 1 AND 2
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Fig. 42 Comparison of the shell length of mussels in control and
experimental mesocosms and external control organisms (C-I and
C-F, Initial and final) after exposure for 28 days to two levels
of Ra activity (Exp. 1 at higher levels than Exp 2). A. Indivdual
organisms. B. Average length, standard deviation for 5 animals
per treatment shown.
89
-------
GROWTH INCREMENT
28 DAY EXPOSURE COMPARISON, EXPERIMENTS 1 AND 2
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AVERAGE GROWTH INCREMENT
28 DAY EXPOSURE COMPARISON, EXPERIMENTS 1 AND 2
12
C-F
Fig. 43 Comparison of the increase in shell length of mussels
from control, experimental mesocosms and external controls (C-I
and C-F, Initial and final) after exposure for 28 days to two
levels of Ra activity (Exp. 1 at higher levels than Exp 2). A.
Indivdual organisms B. Average increase, standard deviation for 5
animals per treatment shown.
90
-------
TISSUE DRY WEIGHT
28 DAY EXPOSURE COMPARISON, EXPERIMENTS 1 AND
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EXP.2
in
TANK
AVERAGE TISSUE DRY WEIGHT
28 DAY EXPOSURE COMPARISON, EXPERIMENTS 1 AND 2
13 15 C-l C-F
TANK
Fig. 44 Comparison of the tissue dry weight of mussels from
control, experimental mesocosms and external controls (C-I and
C-F, Initial and final) after exposure for 28 days to two levels
of Ra activity (Exp. 1 at higher levels than Exp 2). A. Indivdual
organisms B. Average increase, standard deviation for 5 animals
per treatment.
91
-------
3.5
RADIUM ACTIVITY
28 DAY EXPOSURE COMPARISON, EXPERIMENTS 1 AND 2
3-
2.5-
O)
fc 2H
I
o:
1.5-
i -
.6-
0
10
4^
EXP.2
-------
TOTAL RADIUM PER ANIMAL
28 DAY EXPOSURE COMPARISON, EXPERIMENTS 1 AND 2
o
a
I
lull
EXP. 1
EXP.2
m
in
TANK
AVERAGE RADIUM PER ANIMAL
28 DAY EXPOSURE COMPARISON, EXPERIMENTS 1 AND 2
EXP. 1
1
12 U 13 16 C-l C-F
TANK
Fig. 46 Comparison of total Ra activity, pCi/ animal, in mussels
from control, experimental mesocosms and external controls (C-I
and C-F, initial and final) after exposure for 28 days to two
levels of Ra activity (Exp. l at higher levels than Exp 2). A.
Indivdual organisms B. Average increase, standard deviation for
each treatment shown.
93
-------
WATER COLUMN SUSPENDED LOAD, TOTAL
4-
3-
2-
1 -
T-12
- T-U
- T-13
- T-15
OH 1 1 1 1 1 1 1 1
285 292 299 506 SIS 320 327 SS4 341 346
1.5-
PARTICLE FLUX THROUGH MUSSELS
B
T-12
T-U
T-13
T-15
1 1 1 1 1 1 1 1
285 292 299 306 313 320 327 334 341 348
JULIAN DAY
Fig. 47 Comparison of changes in total suspended load (graph A)
and flux of fecal material from mussels (grapgh B) as a function
of time.
94
-------
The mesocosm with the lowest suspended load exhibited the lowest
particle flux through the animals. The other mesocosms exhibited
similar ranking order between suspended loads and fecal pellet
production.
Several samples of fecal matter were counted for Ra activity. The
radioactivity is generally high in the soil amended systems and low in
the controls. (Fig. 48a,b). The data suggests the animals from the
control mesocosms had relatively constant Ra activity in the fecal
material, ranging between 1 and 2 pCi/g. The experimental systems
showed a maximum in Ra activity 2 to 4 weeks after exposure was
initiated, which diminished by the end of the experiment. The cause of
the decrease in radioactivity at termination is not known as particulate
samples from this period were not analyzed for Ra activities. Evidence
presented in figure 33 suggests the concentration of Ra in the
particulates was relatively constant prior to this period and presumably
remained so through the end of the experiment. Comparison of the
average Ra activity in the particulates and fecal material during the
exposure period suggests that little Ra was extracted by the organisms
(Fig. 49), which is consistent with the limited accumulation found in M.
edulis tissues.
From the radioactivity in the fecal material and the rate of fecal
production, the flux of Ra through the organisms was calculated. The
calculated Ra flux peaked after one week of exposure, then decreased,
particularly in organisms from mesocosm 14. By day 56 the calculated
flux reached values equal to or less than found after one day of
exposure (Fig. 50). Tissue residues from organisms exposed for 56 days
(Fig. 40) tended to decrease relative to animals exposed for 28 days
suggesting that the mussels from mesocosm 14 responded to this lower
flux by decreasing the tissue residue of Ra. Mussels from mesocosm 12
increased their Ra tissue residues more slowly than those from mesocosm
14, which is consistent with the lower, more constant supply of
particulate Ra during the experiment as measured by the Ra flux in the
fecal material. The sharp increase in Ra tissue residues in M. edulis
from mesocosm 12 after 56 days of exposure is not reflected in the flux
of Ra in the fecal material at the end of the experiment.
Effects on mussel growth parameters
Bioaccumulation of metal may result in toxicological responses in the
growth of the organism. Tracey (in preparation) has demonstrated that
exposure of Mytilus edulis to elevated Cu concentrations and to sewage
sludge results in reduction of both growth and food conversion
efficiency, if these parameters are normalized against chlorophyll a as
a measure of food availability. The experiment, when originally
designed, did not include plans to examine these parameters. However,
since data required to evaluate these responses were collected during
the experiment (as part of the ecosystem effects testing and as a matter
of routine for the mussel bioaccumulation study) the growth
95
-------
RADIUM IN FECAL MATERIAL OF MUSSELS
SOIL AMENDED MESOCOSMS
300
330-
300-
270-
0>240-
O
O.210-
180-
ISO-
120-
90
285 292
299
T-12
T-14
309 313
320
327
334 341
346
RADIUM IN FECAL MATERIAL OF MUSSELS
CONTROL MESOCOSMS
3-
i -
B
285 292 299 300 313 320 327
JULIAN DAY
334
—i—
341
T-13
T-15
348
Fig. 48 A. Radium activity in Mvtllus edulls fecal matter from
soil amended mesocosms as a function of time. B. Radium activity
in Mvtilus edulis fecal matter from controls mesocosms as a
function of time.
-------
RADIUM, PARTICULATES vs FECAL MATERIAL
AVERAGE OVER EXPOSURE PERIOD
250
200-
150-
O
Q.
100-
50-
T-12
T-14
T-13
T-15
<25 um
T-TSM
FP
Fig. 49 Average Ra activity in participates (total and < 25
micron size class) and fecal matter from mussels exposed to water
from control and the soil amended mesocosms.
97
-------
RADIUM FLUX THROUGH MUSSELS
7-
6-
5-
C
04-1
o
a.
3-
2-
1 -
3- T-12
<— T-14
?- T-13
^- T-15
0
285 292 299 306 313 320 327 334 341 348
JULIAN DAY
Fig. 50 Calculated flux of Ra passing through Mvtilus edulls as a
function of time.
98
-------
and food chain indices were calculated for the mussels used in
experiment 1. The indices were obtained by dividing the average
growth increment or dry tissue weight from each collection period
by the average chlorophyll a concentration over the total exposure
period. The results, plotted as a function of time, suggest that
food conversion efficiency was similar for the two control systems
and one of the experimental systems. Lower efficiencies were
found for mesocosm 14, the experimental system with highest
chlorophyll a (Fig.51). This mesocosm also showed increasing food
conversion efficiency as average chlorophyll a levels decreased in
the latter phase of the experiment, indicating greater utilization
of available food.
Growth efficiency estimates increased during the first 28 days of
exposure in all treatments but decreased in control mesocosm 15
after 56 days. This probably reflects some unknown difficulty
with the exposure of these animals in the effluent system, since
they presumably received an identical amount of food through day
28. Regardless of cause, this response negates detection of
potential effects over the 56 day exposure period caused by uptake
of radionuclides or other element(s) which were not measured.
However, if the growth efficiency parameter is compared for each
treatment through day 28, the indices for both experimental
systems were found to be about one-half that of the control
mesocosms. This suggests the two tanks receiving soils
experienced reduced growth efficiency relative to the controls.
Whether this is due to a direct toxicity resulting from exposure
to elevated radionuclide activity or other toxic elements or
compounds found in the soil can not be directly proven from this
data. However, the evidence is sufficient to raise concerns for a
more thorough examination and quantification of this potential
effect and its cause.
Other nuclides
A limited set of other nuclides were analyzed in the mussel
samples. Those samples analyzed indicate Po-210, and Uranium
nuclides were accumulated (Fig 52), but results for Pb-210 and Th
nuclides are inconclusive. The apparent lack of accumulation of
these nuclides most likely results from their particle-reactive
nature, which may not have allowed them to be exported from the
sediments, into the water column and out of the system.
Zooplankton
Relative to the control systems, bioaccumulation of all
radionuclides was observed in zooplankton for at least four weeks
following the soil addition (Figs. 53 - 57). The cause of the
very high Ra activity in the mesocosm 14 sample on Julian day 307
is not known. More data are required to determine if a temporal
trend of decreasing activities occurred as the total nuclide
activity in the water column declined. Such a trend is not
apparent for Ra through the first 8 weeks of the experiement.
99
-------
GROWTH EFFICIENCY, MYTILUS EDULIS
Delta length / Average Chi a
T-12. E
UJ
60
.2
FOOD CONVERSION EFFICIENCY
Dry tissue wt / Average Chi a
.15-
o
C
.H
B
10
20
—i—
30
DAY
40
—i—
50
-B- T-12. E
-*-- T-14. E
—v-- T-13. C
-*- T-)S. C
60
Fig. 51 Comparison of Mvtilus edulis growth efficiency (A) and
food conversion efficiency (B) in control and soil amended
mesocosms as a function of time.
100
-------
AVERAGE ACTIVITY IN MYTILUS EDULIS
14 DAY EXPOSURE
AVERAGE ACTIVITY IN MYTILUS EDULIS
14 DAY EXPOSURE
B
1
M
U-234
U-Z39
U-238
T-lt
T-14
T-1I
T-1B
T-lf
T-14 T-1»
MESOCOSM
AVERAGE ACnVITY IN MYTILUS EDULIS
14 DAY EXPOSURE
TH-227
TH-Z30
TH-Z3Z
Fig. 52 A. Average Po-210 and Pb-210 activity in mussels exposed
14 days to effluents from mesocosms. B. Average U isotope
activities in mussels exposed for 14 days to effluents from
mesocosms. C. Average Th isotope activities in mussels exposed
for 14 days to effluents from mmesocosms.
T-14 T-1*
MESOCOSM
T-1B
-------
400
350-
300-
0)
o
a.
200 -
(N
(N
I
a:
150-
100-
50-
245
RADIUM VS TIME
ZOOPLANKTON
-&- T-12
—x-- T-14
-*- T-13
1-15
275
305
JULIAN DAY
335
365
Fig. 53 Ra activity in zooplankton as a function of time.
102
-------
50
40-
t7)
CM
20-
10-
245
U-234 VS TIME
ZOOPLANKTON
275
305
335
-B- T-12
—x--- T-14
—9- T-13
- *- T-1 5
305
Q_
lO
1 -
B
246
U-235 VS TIME
ZOOPLANKTON
275
305
JULIAN DAY
335
—B- T-12
—*— T-14
—v— T-13
—*- - T-1 5
305
Fig. 54 Uranium 234 and 235 in zooplankton as a function of time.
103
-------
70
50-
30 H
CD
OL
20-
10-
246
LEAD-210 VS TIME
ZOOPLANKTON
275
305
335
T-12
T-14
T-13
T-15
365
350
300-
250-
^.200-
I
O
O.
150-
100-
50-
B
245
PO-210 VS TIME
ZOOPUNKTON
305
JULIAN DAY
335
Fig. 55 Pb-210 and Po-210 in zooplankton
-e- T-12
—x— T-14
—v- T-13
—*— T-15
385
as a function of time.
104
-------
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U-238 VS TIME
ZOOPLANKTON
-B- T-12
—*- T-14
-v- T-13
—*-- T-15
275
335
305
JULIAN DAY
TH-230 VS TIME
ZOOPLANKTON
365
-e- T-12
-x- T-U
-?- T-13
-*-- T-15
275 305
JULIAN DAY
335
395
Fig. 56 Uranium 238 and Th-230 in zooplankton as a function of time.
105
-------
o
a
cs
1 •
245
O
a
o-i
ro
04
B
245
TH-227 VS TIME
ZOOPLANKTON
-B- T-12
-^- T-U
—v--- T-13
--*-- T-15
275
305
JULIAN DAY
335
365
TH-232 VS TIME
ZOOPUNKTON
-B- T-12
-*— T-U
—v— T-13
-*-- T-15
275 305
JULIAN DAY
335
395
Fig. 57 Thorium 227 and 232 in zooplankton as a function of time.
106
-------
Benthic organisms
Several species of benthic animals were recovered at the
termination of the experiment (see methods above) for
determination of nuclide activity. Of these, five species common
to at least one control mesocosm and one experimental system were
sent to EERF for nuclide determinations. The bivalve Pi tar
morrhuana was in sufficient numbers to allow analysis of
individual organisms.
Bioaccummulation in Pi tar morrhuana
Both Ra-226 and Po-210 activities increased in P. morrhuana
exposed to the radioactive soils (Fig. 58 a&b). Larger organisms
appear to take up less radium activity per unit dry tissue weight
than smaller organisms. Converting the radioactivity per unit dry
weight to total activity per animal (Fig. 59 a&b) reveals strong
linear correspondence for both Ra and Po-210 to the shell length
of the P. morrhuana, as observed for Cu and Ni in Merceneria
merceneria by Cullen (1984). Table 22 summarizes statistical
results for these relationships. In mesocosm 14, Ra activity
normalized to dry tissue weight shows significantly higher
correlation to shell length than found for mesocosm 12, but not
when shell length is regressed against total Ra in the tissues of
the animal. The correlation between length and total Ra for
organisms from the control system is also high but the slope is
significantly different than in the experimental systems. Thus,
the exposure field of the two soil amended systems appears to have
been similar, resulting in similar uptake of Ra in spite of
differences in water column food resources.
107
-------
RADIUM ACTIVITY IN PITAR
3-
2-
1 -
S
S
S
n T-12
H T-13
• T-14
0 T-15
5-
1 -
B
PO-210 ACTIVITY IN PITAR
—t-
S
123436
LENGTH, cm
Fig. 58 A. Ra-226 activity, pCi/g dry weight, in Pi tat morrhuana
recovered from the sediments at the termination of the experiment as
function of shell length. Controls T-13 and 15, soil amended mesocosms
T-12 and 14.
B. Po-210 activity, pCi/g dry weight, in Pi tar morrhuana recovered from
the sediments at the termination of the experiment as function of shell
length. Po activities are not decay corrected to day of collection.
Key as for A.
108
-------
TOTAL RADIUM ACTIVITY PER ANIMAL
PITAR
n 1-12
S T-13
• T-14
0 T-15
B
0
0 S
TOTAL PO-210 ACTIVITY PER ANIMAL
PITAR
D
E
'c
12
D
12
D
14
P
u
D
U
D
15
O
12
13
15
D
13
CJ
LENGTH, cm
Fig. 59 A. Total Ra-226 activity, pCi/animal, in Pi tar morrhuana
recovered from the sediments at the termination of the experiment as
function of shell length. Controls T-13 and 15, soil amended mesocosms
T-12 and 14.
B. Total Po-210 activity, pCi/animal, in Pitar morrhuana recovered from
the sediments at the termination of the experiment as function of shell
length. Po activities are not decay corrected to day of collection.
Key as for A.
109
-------
Table 22. Summary statistics for Ra in Pi tar morrhuana. A. Length
versus pCi Ra/ g dry tissue. B. Length versus pCi Ra/ animal
Mesocosm Intercept 95% Slope 95% n r2
CI CI
A.
12
14
12 + 14
13 + 15
2.97
4.34
3.37
0.30
0.70
0.35
0.37
0.091
-0.377
-0.884
-0.516
-0.24
0.62
0.37
0.33
0.08
10
10
20
9
0.20
0.79
0.38
0.07
12 -0.88 0.25 0.49 0.23 10 0.75
14 -0.21 0.13 0.27 0.16 10 0.67
12 + 14 -0.61 0.13 0.42 0.13 20 0.73
13 + 15 -0.13 0.04 0.075 0.038 9 0.76
no
-------
Bioaccumulation in other benthic organisms
Among the benthic organisms collected, Leptocheirus pinquis,
Pherusa affinis, and Molqula manhattensis displayed the highest
tissue concentration (25 to 48 pCi/g dry wt) of radium (Fig. 60a).
Nephtys insisa had body burdens only slightly above the P-
morrhuana. Relative to the control systems, P. affinis, M.
manhattensis and L. pinquis concentrated Ra by a factor of 100 to
150 , N. insisa about 20 times and P. morrhuana less than a factor
of 5 (Fig. 60b). In all cases the ratio of experimental to
control was less than that observed between the sediments in the
various treatments.
Po appears to have accumulated less in L. pinquis and equally in
P. morrhuana and N. insisa relative to control mesocosm animals.
Po-210 results are probably skewed because samples were not
decay-corrected to the day of collection. Clearly, however, some
bioaccumulation of this element occurred in these organisms.
Comparison of bioaccumulation in all organisms
Two distinct levels of bioaccumulation appear to be present in
this experiment (Fig. 61). Those organisms living in closest
proximity to the soil tended to acquire the highest body burdens
while those that live further away, i.e., live deeper in the
sediment (£. morrhuana) or in the water column (zooplankton and
mussels), had the lowest accumulation relative to control animals.
The high body burdens of the L. pinquis are also consistent with
organisms with high turnover rates of body tissue.
Ill
-------
RADIUM ACTIVITY IN BENTHIC ORGANISMS
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Fig. 60 A. Comparison of Ra activty in benthic animals recovered
at the termination of the experiment. LEP= Leptocheirus pinguis;
NEP= Nephtvs incisa; PIT= Pitar morrhuana; PHE= Pherusa affinis;
MOG = Molgula manhattensis B. Ratio, experimental to controls, of
Ra and Po-210 in benthic animals recovered at the terminatin of
the experiment.
112
-------
BIOACCUMULATION, CONTROL VS EXPERIMENTAL
150
RADIUM
125-
100-
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r\V\i
NEP PIT PHE UOO
ORGANISM
zoo
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U56
Fig. 61 Comparison of the ratio of Ra (experimental/control) in
all organisms recovered from the mesocosms during and at the
termination of the experiment.
113
-------
CONCLUSIONS
Ecosystem
1. No long-term (3 months) planktonic species effects were
observed as a result of adding soils contaminated with elevated
levels of natural radionuclides. In the short term, the dissolved
Si response suggests the soil may have limited diatom production
relative to the controls.
2. Soil additions did reduce the rate of sediment resuspension
thereby reducing availability of >25 urn particles to the water
column. Sediment resuspension rates appeared to increase as the
soil was mixed into underlying marine sediments and diluted with
depositing water column detritus.
3. Even though some benthic species may have been reduced due to
soil addition, the reduction did not measurably affect functioning
of the ecosystem.
4. No long-term effects on system production and respiration were
observed even though system respiration exceeded production
shortly after soils were added. The system apparently compensated
for reduced sediment respiration by shifting respiration to the
water column.
Radionuclide geochemistry
1. Between 10 and 17 percent of the soil associated Ra and
U-series nuclides were released to the water column on contact
with sea water.
2. Ra continued to be released from the sediments over the next 3
months such that an additional 5 percent of the soil-associated Ra
was added to the water column.
3. Over the course of the experiment 15 percent of the soil
associated Ra was released to the water column.
4. A small (0.2%) but measurable fraction of the soil-associated
nuclides was found in terrestial plant detritus that floated to
the surface of the mesocosm. This material may provide a pathway
for the nuclides into surface feeding organisms, particularly
birds.
5. Over 97 percent of the Ra in the water column of the
soil-amended mesocosms was found in the dissolved phase.
6. Most particle-bound Ra was found in the <25 urn particle size
class, as were total suspended solids. Higher Ra concentrations
were observed in the <25 urn size particle class than in the total
suspended solids.
114
-------
7. Distribution coefficients (Kj) of Ra in the water column of
soil-amended systems were up to 2 orders of magnitude less than in
control systems. The lower Kd's probably resulted because
particulate concentrations were too low to sorb the excess
dissolved Ra. As a result, equilibrium conditions did not exist
between dissolved and particle phases.
8. Distribution coefficients determined using laboratory bench
scale and mesocosm protocols were not consistent due to different
particle to seawater ratios and time of equilibration. The
results suggest care must be exercised in extrapolating
experimental determinations of distribution coefficients.
Uptake of radionuclides by organisms
1. Uptake of Ra by Mytilus edulis exposed to the ecosystem
effluents was initially rapid followed by a slow, variable
increase. Increases after one day of exposure were 2 to 3 fold
over control systems.
2. Tissue residues in M. edul is continued to increase in spite of
decreasing total Ra activity in the mesocosm effluent.
3. A two fold decrease in average total Ra activity did not
significantly lower tissue residues in the mussel, Mytilus edulis,
exposed for 28 days. However, Ra activity in particulates was not
different during these experiments, indicating that the
particulate field, not dissolved or total radioactivity, was the
important exposure pathway.
4. A functional relationship between Ra uptake and time for the M.
edulis could not be developed, partially due to differences in
food supply to the mussel. After the initial increase, tissue
residues may have increased linearly. Available food and growth
also may influence the observed uptake rate of contaminants.
5. Limited data indicate increase in tissue residues in M. edulis
of Po-210 and U-series nuclides over time but are inconclusive
with respect to Pb-210 and Th-series nuclides.
6. Zooplankton bioaccumulated all radionuclides measured.
7. Benthic organisms living in closest proximity to the soil and
with the highest body turnover rates accumulated the highest Ra
tissue residues. Slower growing, larger animals accumulated less
radioactivity in their tissues.
8. Bioaccumulation in the bivalve, Pi tar morrhuana, could be
described as a linear relationship between organism length and
total radioactivity in the tissue of the animal. There was no
significant difference in Ra uptake between the two experimental
systems.
115
-------
9. The increase in radionuclide activity found in zooplankton from
the experimental systems relative to control systems was similar
to relative increase for P. morrhuana and M. edulis but a factor
of 100 to 150 times less than in the arthropod Leptocheirus
pinqius and polychaete Nephtys insisa.
10. Potential toxicological effects (growth efficiency) to the
mussel Mytilus edulis were observed from exposure to effluent from
the mesocosms. These potential effects could not be related to
specific elements or radionuclides but are sufficient to warrant
further testing.
General
1. Addition of soil to controlled marine ecosystems coupled with
specific measures of biological and geochemical behavior has
provided a unique opportunity to examine uptake of radionuclides
under defined natural ecosystem conditions. The control provided
by the mesocosms enabled knowledge of changing exposure fields to
be coupled to biological uptake and growth. Only time and money
have limited the ability to look at the geochemical and biological
responses in greater and probably more revealing detail.
2. Concurrent exposure of organisms to mesocosm effluents and
examination of organisms in situ to the mesocosms have provided
unique means of examining uptake of contaminants under known
ecological conditions and relating uptake in organisms from
several ecosystem compartments.
116
-------
Appendix A. Middlesex soil size and radioactivity distributions.
Size distribution plots show the soil sample added to the
ecosystem to be primarily centered around the 250 urn size class
with significant contributions from the > 1000 and < 63 urn
fractions (Figure A). Cumulative mass fraction versus particle
diameter shows that this sample of Middlesex soil is dominated by
sand size particles smaller than 1 mm (Fig. B) with a median grain
size of approximately 350 urn (Bonner et al., 1985).
Total Gamma-Beta and total alpha emanating from a known mass of
each size class (CPM/g) determined significant radioactivity was
associated with each size class but the radioactivity was not
uniformly distributed between size classes on a unit mass basis
(Bonner et al., 1985). Auto-radiography of the soils demonstrated
that the radioactivity was associated with discrete particles
(Fig. C). The median in gross radioactivity was found at the 125
urn size class. Analysis of individual radionuclides in each size
class reveals that the <180 urn particles have higher nuclide
activity per unit dry weight than the > 180 urn particles except
for the 700 to 1000 urn size classes (Fig. D). Pb-210 shows an
exceptionally high concentration relative to the other nuclides in
the 1000 urn size class (Fig. E).
Calculation of the mass weighted nuclide distribution shows the
individual nuclides are distributed similarly within the soils
(Fig. F). However, comparison of the mass weighted nuclide
distributions in individual size classes with the grain size
distribution reveals the radioactivity distribution does not
correspond to the grain size distribution (Figs. G and H). Thus,
a greater percentage of the radioactivity is carried in the
smaller grain size particles.
The review comments of James Neiheisel are particularly important
to the auto-radiography. The evidence of discrete mineral phases
in this particular soil creates a potentially unique means of
monitoring its fate should these wastes be disposed of in the
oceans. His assessment, that the soil will have a distinctly
different minerology from sediments at any ocean disposal site due
to the nature of the contaminant, is highly likely. His
recommendation that the soil be tested for the presence of
diagnostic mineral phases should be accepted. If identified, they
may form the basis for one of the best mechanisms for examining
the transport of the soil during any uncontained disposal
operation and post depositional transport at the dump site.
117
-------
15
oo
UJ
u
o:
LJ
a,
10
>2000 1000 710 500 355 250 180 125 106 90 75 63 <63
microns
H CRAIN SIZE
Fig. A Distribution of soil grain size.
-------
CUMULATIVE DISTRIBUTION
m
u
2
a.
lOOr
90-
80-
70-
60-
50-
40-
30-
20-
10-
>2000 1000 710 500
355 250 180 125 106
microns
90 75 63 <63
GRAIN SIZE
Fig. B Cumulative distribution of soil grain size
-------
90 to 106 micron Particles
Soil Particles
Exposed X-ray film
Fig. C. Auto-radiography of soil particles showing discrete
distribution of activity in soil particles
120
-------
ISOTOPE CONCENTRATIONS
o
N.
t— i
U
Q_
800
700-
600-
500-
400-
300-
200-
100-
>2000 1000 710 500
RA-226
PO-210
355 250 180 125 106
microns
U-238
90 75 63 <63
Fig. D. Distribution of Ra, Po, and U-238 as a function of soil grain size
in soii sample Bl
-------
ISOTOPE CONCENTRATIONS
PO
ro
a
tn
C3
CJ
a,
1400
1260
1120
980
840
700
560
420
280
140
>2000 1000 710 500
U-238
355 250 180 125 106
microns
PB-210
90 75 63 <63
Fig. E. Distribution of U-238 abd Pb-210 as a function of soil grain
size in sample Bl
-------
MASS WEIGHTED COMPOSITION
PO
CJ
LJ
U
a
UJ
a.
>2000 1000 710 500 355 250 180 125 106 90 75 63 <63
microns
RA-226
PO-210
U-238
Fig. F. Mass weighted composition of Ra, U-238, and Po in soil sample Bl
-------
Ul
u
Qi
LU
CL
>2000 1000 710 500 355 250 180 125 106 90 75 63 <63
microns
GRAIN SIZE
RA-226
Fig. G. Comparison of mass weighted distribution of Ra to grain size
distribution in soil sample Bl
-------
UJ
U
a:
UJ
a.
>2000 1000 710 500 355 250 180 125 106 90 75 63 <63
microns
GRAIN SIZE
U-238
Fig. H. Comparison of mass weighted distribution of U-238 to grain size
distribution in soil sample Bl
-------
Appendix B. Suranary of sediment porosity and nuclide activity.
126
-------
Table A. Distribution of water content and porosity as a function of depth
in the sediment column. Mean of 2 pooled samples (5 cores per sample depth).
Mesocosm
Depth
0.25
0.5
0.75
1.5
2.5
3.5
4.5
5.5
6.5
7.5
8.5
9.5
Mesocosm
0.5
1.5
2.5
3.5
4.5
5.5
6.5
7.5
8.5
9.5
Mesocosm
0.5
1.5
2.5
3.5
4.5
5.5
6.5
7.5
8.5
9.5
Mesocosm
0.5
1.5
2.5
3.5
4.5
5.5
6.5
7.5
8.5
9.5
12
Pre
54.8
49.4
48.4
45.1
43.8
43.1
44.9
42.0
43.6
41.6
14
58.0
50.4
46.3
47.5
45.1
44.7
43.6
43.3
41.5
42.5
13
55.7
51.2
51.7
42.2
46.1
47.7
45.5
45.0
45.0
44.5
15
57.1
51.7
50.5
48.2
45.9
44.2
43.0
43.3
42.5
42.2
Percent
Post
35.5
38.9
46.1
47.7
45.8
45.7
38.1
47.2
48.1
46.3
45.5
Water
Mid
37.6
45.4
48.8
49.1
48.8
47.9
46.6
47.1
46.5
46.1
39.6
44.3
48.2
47.4
47.4
46.3
44.9
43.9
45.1
44.9
Final
38.1
45.6
47.3
43.1
44.8
45.5
44.9
45.2
44.4
42.6
43.8
39.4
47.6
47.9
46.7
46.4
45.8
45.6
45.4
45.8
58.3
52.6
50.0
42.2
46.6
47.0
45.9
47.6
46.9
46.7
60.1
51.9
50.9
50.0
48.3
45.8
45.6
45.4
45.8
45.9
Pre
75.4
71.3
70.4
67.7
66.5
65.8
67.5
64.8
66.3
64.5
77.9
72.1
68.7
69.7
67.7
67.3
66.3
66.0
64.4
65.3
76.2
72.8
73.1
69.7
68.5
69.9
68.0
67.6
67.6
67.2
77.2
73.2
72.2
70.3
68.3
66.8
65.8
66.1
65.3
65.0
Porosity
Post Mid
58.3
60.6
61.8
68.5 67.9
69.9 70.8
68.2 71.1
68.2 70.8
70.0
69
69.4
68.9
68.5
61.1 62.5
69.4 66.9
70.4 70.3
68.7 69.6
68.0 69.1
68.7
67.5
66.6
67.8
67.5
Final
61.1
68.1
69.6
65.9
67.4
68.0
67.5
67.8
67.1
65.4
66.5
62.4
69.8
70.1
69.1
68.8
68.3
68.1
68.0
68.3
78.0
73.9
71.8
65.0
68.9
69.3
68.4
69.8
69.3
69.1
79.3
73.3
72.5
72.2
70.4
68.2
68.1
68.0
68.2
68.4
127
-------
Table B. Concentration of nuclides in sediments before and after soil
additions. Units are pCi/g dry weight. Other nuclides show similar patterns.
Ra-226
Depth
0.25
0.5
0.75
1.5
2.5
3.5
4.5
6.5
8.5
0.25
0.5
0.75
1.5
0.25
0.5
0.75
1.5
0.25
0.5
0.75
1.5
2.5
4.5
8.5
0.25
0.5
0.75
1.5
2.5
8.5
Pre
0.82
0.77
0.81
0.98
0.94
0.81
0.73
1.9
1.8
2.3
1.7
0.75
0.74
0.79
0.67
0.62
1.03
12
Post Final
332
578
200
21.3 42
17.3 8.1
1.7 4.4
1.0 1.5
0.9
323
307
48
383
307
66
335
153
175
31
10
2
322
202
30
Pre
0.66
0.76
0.67
0.73
0.67
0.63
1.7
1.8
1.7
1.8
0.94
0.82
0.92
0.79
14
Post Mid Final
Ra-226
283 227 117
41 3 166
51 16 20
1.8 12 0.4
1.2 8
3
Po-210
346
50
Pb-210
315
63
U-234
276
41
Th-230
292
46
13
Pre Post
0.84 0.72
0.82
1.04 0.72
0.78
0.72
0.69
1.8
1.7
2.3
2.0
0.78
0.80
0.80
1.7
15
Pre Post
1.00 0.74
0.79 0.50
0.70
1.7
1.2
0.69
0.83
0.48
128
-------
Appendix C. Benthic flux of radionuclides determined from chamber
studies.
129
-------
Table A.
RA BENTHIC FLUX COMPARISON BY TREATMENT
ORP PROJECT, OCTOBER 26, 1985
MESOCOSM
12
14
13
15
FINAL
INITIAL
TIME, hr
RA FLUX, Ci/m2/h
5.88e-ll
4.01e-ll
4.5
5.4e-10
9.23e-ll
7.41e-ll
4.67
5.07e-10
7.2e-14
1.8e-13
5
-3e-12
2.7e-13
2e-13
5.08
2e-12
PB-210 flux NM
PO-210 NM
U-234, 235, 238 ND
TH-227, 228, 230 ND
NM
NM
ND
ND
NM
ND
ND
NM
NM
ND
ND
130
-------
Appendix D. Summary of radionuclide activity in benthic
organisms.
This appendix lists all data pertinent to the benthic organisms
collected at the termination of the experiment. Length refers to
the axial length of the organism in cm. Dry wt is the dry tissue
weight of the organism in g/animal. Wet/dry is the ratio between
wet tissue and dry tissue weight. Activities are reported in
terms of pCi/g dry tissue and the 2 sigma counting errors
included. Nuclides marked with ND were not detectable; those with
NR did not have analysis requested.
131
-------
SUMMARY OF BENTHIC OR6ANISH DATA.
File; BENTHIC. RADS. 84
Report: BENTHIC ANIMALS
EERF 1 HERL 1 TANK ANIMAL
52860
52863
52864
52862
52861
52865
52871
52873
52872
52874
52855
52854
52857
52856
52858
52859
52866
52869
52868
52867
52870
52833
52832
52832
52831
52830
52829
52828
52827
52826
52824
52825
52847
52846
52845
52844
52843
52842
52841
52840
52839
52838
52837
52837
52826
52835
52834
52853
52852
52851
52850
52850
52849
52848
B-64
B-15
B-16
B-92
B-91
B-30
8-65
B-17
B-89
B-34
B-59
i-58
B-21
B-88
B-32
B-33
B-67
B-23
B110
B-110
B-55
B-87
B-86
B-86
B-85
B-84
B-81
B-80
B-74
B-73
B-69
B-70
B-14
B-ll
B-9
B-6
B-109
B-108
B-107
8-105
B-104
B-101
B-99
B-99
B-98
B-97
B-96
B-54
8=53
B-51
B-50
B-50
B-46
B-39
12
13
13
14
14
15
12
13
14
15
12
12
13
14
15
15
12
13
14
14
15
12
12
12
12
12
12
12
12
12
12
12
13
13
13
13
14
14
14
14
14
14
14
14
14
14
14
15
15
15
15
15
15
15
LEPTOCHEIRUS
LEPTOCHEIRUS
LEPTOCHEIRUS
LEPTOCHEIRUS
LEPTOCHEIRUS
LEPTOCHEIRUS
K06ULA
H06ULA
MQ6ULA
H08ULA
NEPHTHYS
NEPHTHYS
NEPHTHYS
NEPHTHYS
NEPHTHYS
NEPHTHYS
PHERUSA
PHERUSA
PHERUSA
PHERUSA
PHERUSA
PITAR
PITAR
PITAR
PITAR
PITAR
PITAR
PITAR
PITAR
PITAR
P3TAR
PITAR
PITAR
PITAR
PITAR
PITAR
PITAR
PITAR
PITAR
PITAR
PITAR
PITAR
PITAR
PITAR
PITAR
PITAR
PITAR
PITAR
PITAR
PITAR
PITAR
PITAR
PITAR
PITAR
ORP PROJECT, MARCH 11, 1986.
LENGTH 8 ANIMALS DRY UT NET/DR RA226
1.75
2.18
2.18
3.35
3.46
3.81
3.85
4.47
4.47
4.91
5.04
1.53
2.41
4.43
5.02
1.58
2.24
2.42
2.61
2.68
3.02
3.29
3.29
3.45
4.20
4.31
2.12
2.55
3.27
3.73
3.73
4.42
5.31
2
45
45
17
20
45
2
17
5
10
20
20
22
15
26
20
6
15
5
5
9
7
2
2
1
1
5
1
1
1
5
3
3
1
3
3
1
1
1
1
1
0.035
0.012
0.012
0.021
0.31
0.013
0.155
0.109
0.10
0.08
0.10
0.09
0.11
0.10
0.10
0.11
0.10
0.053
0.154
0.144
0.156
0.061
0.12
0.12
0.42
0.50
0.50
0.76
1.07
0.96
1.14
1.37
0.04
0.16
1.17
1.43
0.054
0.16
0.19
0.26
0.34
0.52
0.67
0.67
0.56
0.93
1.35
0.97
0.22
0.37
0.62
0.58
1.00
1.34
6.14
8.07
7.35
4.94
4.79
6.76
12.7
11.5
11.3
16.0
5.40
5.77
6.09
5.59
5.16
5.42
7.21
7.39
7.75
8.33
7.08
5.14
7.29
7.29
6.43
5.88
6.48
5.87
5.68
6.17
7.79
6.47
5.00
5.38
7.23
8.40
5.33
5.66
5.65
6.62
4.71
5.13
4.90
4.9
6.3
7.05
6.04
4.72
5.64
5.41
5.52
5.52
7.57
6.84
2.58
0.25
0.41
43.5
38.3
0.37
21.7
0.17
27.2
0.36
3.95
4.68
0.42
2.23
0.036
0.064
48.2
0.30
25.6
15.9
0.21
3.92
NR
0.67
0.86
.88
.38
.64
.49
.08
.75
0.98
0.19
0.50
0.26
0.18
3.58
2.00
1.79
2.37
1.76
1.38
NR
1.02
1.64
0.62
0.86
0.18
0.23
0.14
NR
0.18
0.15
0.20
RA+-
4.0
10.0
19.0
0.81
1.0
18.0
0.92
0.2
1.0
13.0
1.0
2.0
31.0
3.0
19.0
25.0
3.0
12.0
0.69
2.0
7.0
2.0
22.0
6.0
6.0
4.0
5.0
2.0
6.0
4.0
3.00
32.0
44.0
16.0
15.0
7.0
3.0
6.0
4.0
8.0
4.0
7.0
3.0
9.0
3.0
24.0
28.0
25
32.0
10.0
16.0
Page 1
MARCH 11, 1986
P0210 PO+-
ND
5.30
0.26
NR
3.30
0.48
NR
NR
NR
NR
NR
5.30
0.31
4.10
0.23
NR
NR
NR
NR
NR
NR
0.19
0.19
NR
NR
NR
4.9
NR
NR
3.73
NR
NR
0.86
NR
0.24
NR
NR
NR
NR
4.45
NR
3.34
3.34
NR
2.26
NR
NR
3.86
NR
0.561
0.56
NR
NR
90.0
10.7
57.2
16.6
40.0
10.7
29.5
16.6
34.0
117
116
13.7
14.1
68
46.0
23.6
18.4
18.4
18.4
17.2
43.4
43.4
132
-------
Appendix E. Summary of Mytilus edulis growth and nuclide data.
This appendix contains data pertinent to the mussels in exposure
experiments 1 and 2. The MERL and EERF sample designations are
listed along with the length of exposure in days, the initial and
final axial length of the animal in mm, dry tissue weight in g,
the wet/dry ratio, radionuclide activities in the animals in pCi/g
dry weight and 2 sigma counting errors. Mussel.1 and Mussel.2
refer to the two experimental periods. NR indicates nuclide data
was not requested of EERF. ND indicates sample was counted for
the nuclide but not detected.
133
-------
Summary of mussel data recieved as of MARCH 11, 1986.
File: MUSSEL.RAD.81
Report: MUSSELS.ORP, 1984:1 MARCH 11, 1984
TYPE TANK MERL EERF fl [>AY X-IN1 X-FIN DRY WT UET/DR RA226 RA<- PB210 PB+- P0210 PO-t-
MUSSEL.l 12
MUSSEL.l 12
MUSSEL.l 12
MUSSEL.l 12
MUSSEL.l 12
MUSSEL.l 12
MUSSEL.l 12
MUSSEL.l 12
MUSSEL.l 12
MUSSEL.l 12
MUSSEL.l 12
MUSSEL.l 12
MUSSEL.l 12
MUSSEL.l 12
MUSSEL.l 12
MUSSEL.l 12
MUSSEL.l 12
MUSSEL.l 12
MUSSEL.l 12
MUSSEL.l 12
MUSSEL.l 12
MUSSEL.l 12
MUSSEL.l 12
MUSSEL.l 12
MUSSEL.l 12
MUSSEL.l 12
MUSSEL.l 12
MUSSEL.l 12
MUSSEL.l 12
MUSSEL.l 12
MUSSEL.l 13
MUSSEL.l 13
MUSSEL.l 13
MUSSEL.l 13
MUSSEL.l 13
MUSSEL.l 14
MUSSEL.l 14
MUSSEL.l 14
MUSSEL.l 14
MUSSEL, 1 14
MUSSEL.l 14
MUSSEL.l 14
MUSSEL.l 14
MUSSEL.l 14
MUSSEL.l 14
MUSSEL. 1 14
MUSSEL.l 14
MUSSEL.l 14
MUSSEL.l 14
MUSSEL.l 14
MUSSEL.l 14
MUSSEL.! 14
MUSSEL.l 14
MUSSEL.l 14
MUSSEL.l 14
M-22
M-23
M-24
M-25
M-26
M-34
M-oc>
M-36
M-37
M-38
M-70
M-71
M-72
M-73
M-74
M-91
M-92
M-93
M-94
M-P5
M-lll
M-112
M-113
M-114
M-115
M-221
M-222
M-223
M-224
M-225
M-81
M-82
M-83
M--84
M-85
M-27
M-29
M-31
M-44
M-46
M-48
M-76
M-78
M-80
M-100
M-96
M-97
M-98
M-99
M-116
M-118
M-120
H-226
M-228
M-230
52749
52750
52751
52752
52753
52754
52755
52756
52757
52758
52759
52760
52761
52762
52763
52764
46945
52765
46946
52766
52767
52768
52769
52770
52771
52772
52773
52774
52775
52776
52795
52796
46947
46948
52797
52777
52778
52779
52780
52781
52782
52783
52784
52785
46950
46949
52786
52787
52788
52785
52790
52791
52792
52793
52794
1
1
1
1
1
3
-.
3
^i
3
7
7
7
7
i
14
14
14
14
14
28
28
28
28
28
56
56
56
56
56
14
14
14
14
14
1
1
1
^'
q
3
•?
(
7
7
14
14
14
14
14
28
28
28
56
56
56
42.8
45.2
46.1
43.4
45.3
46.4
43.8
45.1
43.3
46.0
45.7
47.1
42.5
42.9
44.5
42.3
45.8
47.0
46.5
43.5
45,5
44.9
43.9
43.5
44.6
46.0
42,2
42.2
42.4
43.2
41.2
44,2
42.9
47.9
44.5
43.8
43.2
46.4
41.?
46.8
47.5
44,5
42.6
42.2
42.7
44.2
42.6
42.4
41.4
42,0
45,9
43.4
44.1
42.9
45.9
42.8
45.2
46.1
43.4
45.3
46.5
43.9
45.1
43.4
46,1
45.9
47.3
43.0
43.1
44.3
43.3
46.3
47,5
46,8
43,7
45,9
45.2
44.0
43.9
44 . 6
47.3
42,9
42.9
44,5
43.7
41.5
44.5
42,9
48.3
44,4
43.8
43,2
46.4
41.9
46.7
47.7
44.8
4^.6
43.1
43.1
44.9
43.3
43.2
42.7
43.2
47.9
44.3
45.3
45,9
50.8
0.25
0.30
0.49
0.31
0.52
0.33
0.27
0.31
0.28
0.44
0.40
0.35
0.36
0,37
0.34
0.18
0.29
0.24
0.44
0.38
0.35
0.34
0.34
0.30
0.17
0.37
0.31
0.29
0.37
0.29
0.24
0.28
0.25
0.31
0.23
0.28
0.34
0.41
0.27
0.24
0.55
0.39
0.31
0.47
0.34
0.44
0.31
0.30
0.34
0.36
0.51
0.39
0.52
0,4^
0.53
7.88
7.23
6.47
6.23
5.?8
7.15
6.7
7.58
7.93
5.75
6.43
6.09
6.25
6.14
7.00
11.0
7.76
9.46
7.14
6.71
8.11
7.62
7.76
8.07
9.41
8.27
8.58
8.14
7.68
7.62
7.75
6.46
8.6
7.1
8.09
6.82
7.18
5.90
7.44
8,92
5.82
6.08
7.52
5.66
7.03
6.32
7.13
7.57
6,09
7.36
7.27
7.64
6.65
7.11
7.25
1,08
1.68
0.77
1.2
0.95
1.4
0.59
1.0
1.61
1.0
1.84
1.22
0.90
0.96
2.03
2.15
1.56
1.8
1.74
0.90
1.88
1.41
1.11
2.23
1.9?
2.1
2.96
3.1
3.65
3.4
0,70
0.42
0,81
0.47
0.2?
1.04
1.15
0.63
1 . 8t
1.69
1.10
1.54
1.12
1.16
1.27
1.92
1.5
2.5
2.1
2.17
2.12
2.39
2.2
1.7
2,1
7.0
5.0
6.0
6
5.0
10.0
10.0
13.0
5.0
11
4.0
5.0
6.0
6.0
4.0
5.0
12
10.0
9
6.0
4.0
5.0
6.0
4.0
6.0
7.0
3.0
7.0
3.0
7.0
23.0
29.0
22
29
48.0
7.0
6.0
7.0
5.0
5.0
4.0
4.0
6.0
4.0
12
-?
10.0
9.0
9.0
4.0
3.0
3.0
6.0
7.0
9.0
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
5.2
NR
7.00
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
12.9
1.4
NR
NR
NR
NR
NR
NR
NR
NR
NR
NP
7.6
5.4
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
180 20.6
5.9
62 11. 9
NR
NR
NR
NR
NR
NR
5.95
NR
5.49
NR
5.59
1.69
59 7.2
319 5.9
NR
NR
NR
NR
NR
NR
NR
NR
NR
78 16.5
131 15.5
3.53
4.43
4.24
NR
NR
NR
4.54
5.15
6.36
11
35.0
11
22.5
19.5
23.5
33.5
14
15
11
11
30,5
27.0
23.0
16.7
18.3
13.6
134
-------
Summary oi mussel data recieued a= of MARCH 11, 19H6.
Flip; MUSSEL.RAD,84 Page 2
Report: MUSSELS.ORP, 1^84:1 MARCH 11/1986
TYPE TANK MERL EERF H DAY X-1W X-FIN t'RY (JT WE1/DR RA226 PA<- PB210 PB+- P0210 PCn-
MU8SEL.1 15
MUSSEL. 1 15
MUSSEl.l 15
MU'33EI .1 15
MU8SEL.1 15
MUSSEL. 1 15
MUSSEL.l 15
MUSSEL. 1 BT.
MUSSEL.I E;a.
MUSSEL. 1 E"J.
MUESEL.l EAT.
MUSSEL. 1 EXT.
MUSE L.I Da.
MUSS EL. 1 EXT.
MUSSEL.l EXT.
MUSS EL. 1 Exl.
MUSSEL.I E;A~?
*>i.'- H .-
52748
52803
52805
52804
52806
52807
52809
5280 6
52810
52811
52812
52813
52816
52814
52815
52817
52818
52821
52819
52820
52822
52823
14
14
C £
i_l\_'
5.f
56
56
56
0
0
0
0
0
56
56
56
56
c;^
w'L*
28
28
28
28
28
28
28
28
28
28
28
28
28
28
28
28
41.6
42.8
41.9
44.0
44.3
45.1
47.0
47.6
46.8
43 _ 9
48.1
47.6
46.6
42.8
41.6
41.9
44.9
41.1
41.6
40,0
41.6
37.6
39.9
40.9
40.6
41.6
39,5
38.8
39.7
39.6
40.1
41.8
37.9
41. 8
44.8
42,1
44.2
44.6
45,3
47.2
47.6
46.8
43. 9
43.1
47.6
SO 7
i-'ii i i
45,0
45,4
47.1
47.1
41.3
41.8
40.3
42.2
39.0
41.1
41,0
40.7
41.8
39.9
39.1
40.4
40.8
40.7
42.5
38.8
0.2?
0.37
0.24
0.26
0.23
0.24
0.25
0.60
0.40
0.27
0.46
0.60
0.67
0.54
0.54
0.50
0.71
0.38
0.25
0.21
0.29
0.24
0.26
0.16
0.19
0.22
0.18
0,19
0.22
0.16
0.20
0.24
0.12
t.,74
6.84
7 '-;-;
8.81
*.91
8.25
9.56
5.88
6.78
7.19
6 . 37
5.78
6.3?
5.94
6.44
6 . 66
5.76
7.92
e.oe
7.95
8.17
7.71
7.65
9 . 69
8.95
8.59
8.78
9.37
9.09
9.19
7.80
7.25
9.17
0.36
0.36
0 , 30
0.38
0.49
0.40
0 . 34
0.19
0 , 1 3
0.44
0.15
0.20
0.10
0.1^
0.18
0.18
0.095
1.52
2.46
3.43
9 '";9
1.89
1 , 95
0.70
0.53
0.29
0.47
0.37
0 . 55
0.36
0.52
0.28
0 . 62
39 ND
30.0 fll)
25.0 NP
25 NR
39. [i NR
26 IMP
25 NP
27.0 NR
24 NR
33.0 NR
18 NR
29.0 NR
26.0 NP
30.0 NR
24,0
27.0
35
4.0 NR
7.0
6.0
6.0
7.0
7.0
27.0 NR
22.0
34.0
23.0
35.0
33.0 NR
23.0
24 , 0
31.0
33.0
4400 6.4
380 4.3
0 . 55
1 . 92
NP
3.0
1.16
NR
NR
1.23
4.49
7.28
3.63
16
17
58.5
34.0
27 . [i
28
27. i7
23.5
23.2
29.2
135
-------
Sumary o^ mussel data recieved as o-f HAECH 11, 1984.
File: MUSSEL. RAD. 84
Report: HUSSELS.ORP, 1934:2
EERF f U234 234-1- U235 235^ U233 238<- TH227 227*- TH228 228*- 1H23Q 230+- TK232
52749
52750
52751
52752
52753
52754
52755
5275(5
52757
52758
52759
52740
52761
527,52
52743
52744
46945
52745
46944
52746
5276?
52749
5274?
52770
5277]
52772
52773
52774
52775
52776
52795
52794
46947
46948
5279?
52777
52773
52779
52780
5278!
52782
52783
52784
52735
46950
4494?
52784
52787
52783
52739
52790
52791
52792
527'?3
52794
NR
NR
NR
NR
NR
NR
NR
NR
NR
RN
NR
NR
NR
1.3 29
i.l 26
NR
NR
NR
NR
NR
NR
NR
NR
0.11 136
0,27 40
NR
NR
NR
NR
NR
NR
NR
NR
NR
1.2 2?
1.9 20
RN
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
0.0? 115
0.10 76
NR
NR
NR
NR
NR
NR
NR
NR
0.04 128
0.02 200
NR
NR
NR
NR
NR
NR
NR
NR
NR
0,02 182
0.0? 82
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
RN
NR
NR
NR
NR
NR
NR
NR
0.92 33
0.94 24
NR
NR
NR
NR
NR
NR
RN
NR
0,0? 159
O.OC 3000
NR
NR
NR
NR
NR
NR
NR
NR
NR
0,78 32
1.5 23
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
0.54 4?
NR
0.26 70
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
0,2? 95
0.04 200
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
0,11 123
0.2 79
NR
NR
NR
NR
RH
NR
NR
m
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NO
NR
NO
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
ND
NO
NR
RN
NR
NR
HR
NR
NR
NR
HR
NR
HO
ND
NR
NR
HR
NR
NR
NR
NR
NR
HR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR NR
NR
NR
NR
NR
NR
77 1.0 34
NR
48 0,40 42
NR
NR
NR
NR
NR
NR
NR
NR
NR
Nft
NR
NR
NR
78 0,64 45
54 0.29 49
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
43 0,4? 38
256 0.4 31
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
0.17
NR
0.14
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
0,11
0.0?
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
0.055
0
NR
NR
NR
NR
NR
NR
NR
NR
NR
Page 1
MARCH 11, 1984
232*-
8?
61
145
158
123
0
136
-------
Summary Oi mussel data recieved as of MAECH 11, 1986.
File: MUSSEL.RAD,84 Page 2
Report: NUSStLS.ORP, 1984:2 WRCH 11, 1984
EERF S U234 23
-------
Appendix F. Summary of water column radionuclide data.
This appendix lists all available data on various parameters
measured in the water column during the soil experiments. The
MERL and EERF codes are listed for cross reference. Julian refers
to the Julian Date samples were collected. NR indicates nuclide
analysis was not requested; ND indicates the nuclide was counted
but not detected. Units for the measurements are as follows:
RADIONUCLIDES
Dissolved samples pCi/1
Particulate, sediment, fecal pellets, sediment trap, zooplankton
and soil samples are in pCi/g dry weight
Counting errors are listed next to the radioactivity under heading
Ra+-, PO+-, etc. These are 2 sigma counting errors.
PHYSICAL PARAMETERS
The column headed TSM/FLUX has units depending on the type of
sample. These are:
NAP indicates there are no applicable numbers.
Particulate mg/1
Sediment trap g/m2/h
Zooplankton mg/m3
Floatables g/tank
138
-------
DATA RECIEVED FROM EERF AS OF MAR, 11, 1986. ECOSYSTEM EXPERIMENT
File: ORP.RAD3.FALL84
Report: DATA PRINTOUT!
TYPE TK HERL ft EERF ft JULIAN TSM/FLX RA-226 RA +- PB-210 P8 +-
DIS.
DIS.
DIS.
DIS.
DIS.
DIS.
DIS.
DIS.
DIS.
DIS.
DIS.
DIS.
DIS.
DIS.
DIS.
DIS.
DIS.
DIS.
DIS.
DIS.
DIS.
DIS.
DIS.
DIS.
DIS.
DIS.
DIS.
DIS.
DIS.
DIS.
DIS.
DIS.
DIS.
DIS.
DIS.
DIS,
DIS.
DIS.
DIS.
DIS.
DIS.
DIS.
DIS.
DIS.
DIS.
DIS.
DIS.
DIS.
DIS.
DIS.
DIS.
DIS.
BAY
ElAY
MY
E«Y
BAY
BAY
BAY
BAY
BAY
12
12
12
12
12
12
12
12
12
12
12
12
12
12
13
13
13
13
13
13
13
13
14
14
14
14
14
14
14
14
14
14
14
14
14
15
15
15
15
15
15
15
15
.022
.023
.023
.025
.024
.028
.030
.030
.032
.BF1
.BF2
.020
.021,1
.021.2
.021.3
.022
.023
.025
.025
.024
.028
.030
.032
.BF1
.BF2
.020
.021
.023
.025
.024
.030
.BF1
.BF2
.026
.020
,021.1
.021.2
.021.3
.022
.023
.025
.026
.030
.032
BF1.1
BF1.2
,BF2
.020
.021
.023
.025
.026
46374
46388
46388
4685-4
44899
52666
52670
52670X
52674
46904
46905
46340
44353
46354
46355
46370
46376
46890
46890X
46895
52663
52667
52671
44902
46903
44343
46358
46379
46891
46896
52669
44906
46907
52664
46347
46341
46362
46363
46372
46382
46892
46897
52668
52472
44900
44900X
44901
46350
46367
46385
46893
44898
272
276
276
290
297
312
325
325
338
303
303
261
269
249
269
272
276
290
290
297
312
325
338
300
300
261
269
276
290
297
325
303
303
312
261
269
269
269
272
276
290
297
325
338
300
300
300
261
269
276
290
297
NAP
NAP
NAP
NAP
NAP
NAP
NAP
NAP
WP
NAP
NAP
NAP
WP
NAP
NAP
NAP
NAP
NAP
NAP
NAP
NAP
NAP
NAP
NAP
WP
NAP
WP
NAP
WP
NAP
NAP
NAP
NAP
NAP
WP
NAP
WP
NAP
WP
NAP
WP
NAP
WP
NAP
NAP
NAP
NAP
NAP
NAP
NAP
WP
NAP
0.14
0.16
0.16
0.24
0.14
0.20
0.15
0.16
0.14
40.1
58.8
0.12
106
134
115
121
100
65.4
63.4
49.3
33,0
23.8
0.18
0.072
0.097
0.12
0.12
0.23
0.16
0.16
74.1
92.3
54.4
0.13
146
90.8
21.0
107
120
91.7
54.5
24.5
29.4
0.20
0.27
0.15
0.13
1.44
0.17
0.22
23
16
16.0
24
21
43.0
18.0
19.0
19.0
2
1.0
12
1.0
1.0
1.0
1.0
1.0
1.0
0.6
2.0
3,0
3.0
14
34
35
35
22
13
16
17
1.0
1.0
1.0
11
1.0
1.0
3.0
1.0
1.0
1.0
1.0
2.0
2.0
15
12
17
21
4.0
16
14
NO
NR
MR
NR
NR
NR
NR
NR
0.2?
1.3
0.43
2.3
0.90
3,5
NR
NR
3.7
NR
NR
NR
NR
1.8
0.44
ND
NR
NR
0.33
NR
NR
0.14
6.7
NR
0.34
11.0
5.0
9.3
NR
NR
ND
NR
NR
NR
0.15
2.5
0.44
NR
NR
0.92
NR
3000
1747
355
640
210
722
142
134
75
240
159
287
3300
78
830
45
89
77
348
724
42
747
147
ONLY.
PO-210 PO +-
0.16
NR
NR
NR
NR
NO
1.0
ND
0,52
0.88
0.70
NR
NR
0.43
NR
0.16
0.13
ND
NR
NR
0.70
NR
NR
0.37
ND
0.13
0.49
1.3
1.5
NR
NR
1.1
NR
0.17
ND
0.13
NR
NR
0.12
NR
60
51
35
88
50
44
45
50
42
45
52
18
43
403
45
53
29
33
38
39
440
75
48
- U-234
1.0
NR
NR
NR
0.97
NR
101
101
1.25
150
142
147
NR
NR
114
126
107
1.1
1.2
1.1
NR
NR
1.1
1.2
117
133
1.3
177
182
179
NR
NR
152
135
1.0
1.1
1.14
0.87
NR
NR
0.98
1.04
234+- U-235
22
17
10
10
20.5
13
14
10
9.5
9.5
9.3
15
15
22
14
21
9.0
10
20
12
10
9.3
9.4
10
14
14
16
26
17
2.5
0.015
NR
NR
NR
0.036
NR
3.8
3.7
0.045
4,43
6.0
5.4
NR
NR
3.5
5.06
4.3
0.02
0
0.08
N
NR
0.036
0.06
3.3
4.5
0.063
6.2
7.9
4.6
NR
NR
3.0
6.6
0.025
0.045
0.029
0.084
NR
NR
0.046
D.059
Page 1
MARCH 11, 3986
235+- U-238 238+-
147
72
19
17
93
32
30
28
39
14
17
9?
0
74
71
84
18
27
81
21
17.5
26
32
16
98
72
79
74
44
86
1.1
NR
NR
NR
0.83
NR
101
103
0.92
158
159
151
NR
NR
131
127
108
0.49
0.97
0.91
NR
NR
1.0
3,2
315
130
1.21
174
182
170
NR
NR
153
140
0.85
1.1
0.93
1,2
NR
NR
0.85
0.73
21
18
10
10
23.7
13
34
10
9.5
9.5
9.3
18
16
24
16
21
9.0
9.7
20
12
10
9.3
9.4
10
17
14
17
23
17
24
139
-------
DATA RECIPJED FROM EERF AS OF MAR. 11, 1984. ECOSYSTEM EXPERIMENT ONLY.
File: ORP.RADS.FALL84 Pa9e ?
Report: DATA PRINTOUTI MARCH 11, 1984
TYPE TK MERL I EERF fl JULIAN TSH/FLX RA-224 RA 4- PB-210 PB 4- PO-210 PO 4- U-234 2344- 11-235 235*- U-238 238*-
DIS.
DIS.
FP.
FP.
FP.
FP.
FP.
FP.
FP.
FP.
FP.
FP.
FP.
FP.
FP.
FP.
FP.
FP.
PART.
PART.
PART.
PART.
PART.
PART.
PART.
PART.
PART.
PART.
PART.
PART.
PART.
PART.
PART.
PART,
PART .
PART.
PART.
PART.
PART.
PART.
PART.
PART.
PART.
PART.
PART.
PART.
PART.
PART.
PART.
PART,
PART.
PART.
15
15
12
12
12
12
12
13
13
13
34
34
14
14
34
15
15
15
BAY
BAY
BAY
BAY
BAY
BAY
EfiY
BLA
BLA
BLA
12
12
12
12
12
12
32
12
12
13
33
13
13
13
13
14
14
14
34
14
14
14
14
14
.028
.032
,003
.004
.004
.009
.010
.003
.004
.009
.003
.004
,004
.009
.010
.003
.004
.010
.022
.023
.025
.024
.028
.030
,032
.1
.2
.3
.020
.021
,022
.023
.025
.024
.028
.030
,032
.020
.021
.023
.025
.024
.030
.020
.021.2
.021.1
.022
.023
.025
,024
,028
.030
52445
52673
44915
52724
52727
52730
52733
44916
52726
52732
4493?
52725
52728
52731
52734
44918
52729
52735
44375
44389
44927
44936
52478
52482
52686
46390
44391
44392
44343
46354
44371
44377
44939
44928
52475
52679
52683
46344
44359
46380
44921
44930
52481
44348
44365
44364
44373
46383
44923
46932
52474
52680
312
338
296
303
317
345
345
296
303
345
296
303
317
345
345
296
337
345
272
276
290
297
312
325
338
261
269
272
274
290
297
332
325
338
263
249
276
290
297
325
261
249
269
272
274
290
297
332
325
NAP
NAP
0.337
0.344
0.317
0.330
0.275
0.969
1.032
0.406
0.537
0.904
0.611
0.472
0.369
0.572
0.331
0.199
4.7
11.6
3.33
6.25
5.38
3.34
4.54
3.94
4.03
3.93
3.12
3.84
1,51
1.22
1.18
1.44
6.44
6.25
7.78
4.31
3.95
2.58
3.40
3.28
2.12
4.48
2.84
3.34
3.09
2.02
i.82
0.17
0.19
148
269
213
98.1
107
0.94
1.59
0.99
192
328
344
141
120
2.1
1.15
3.0
9.5
4.9
14.6
8.7
10.0
5.4
40.2
.18
0.13
0.22
23.7
301
144
120
142
75.4
205
117
243
20.3
11.2
32.1
25.2
4.3
4.6
29.8
249
241
89.4
158
184
174
333
194
15.0
14.0
2.0
0.74
0.65
0.9
0.92
23
8,0
11.0
1.0
0.53
0.62
1.0
1.0
18
12.0
18
24
17.0
19.0
20
24.0
25.0
31.0
2-1
40
20
29,0
5
4.0
4.0
7.0
6.0
6.0
11.0
5.0
31
33
21
21.0
29
27.0
23
9.0
10
9.0
7.0
6.0
5.0
5.0
4.0
NR
NR
288
NR
NR
NR
NR
3.0
NR
NR
204
NR
NR
NR
NR
21.0
NR
NR
NR
NR
NRN
23.9
NR
NR
NR
ND
0.75
1.4
ND
421
NR
NR
NR
NR
NR
NR
NR
79
203
NR
NR
NR
NR
83
883
741
NR
NR
NR
NR
NR
NR
NR
NR
21.0 187
NR
NR
NR
NR
250 3.7
NR
NR
24 135
NR
NR
NR
NR
74 5.7
NR
NR
NR
NR
NR
323 41.6
NR
208 7.6
184 0.8
92 0.05
490 35.2
91 402
NR
NR
NR
NR
249 13.2
85 ND
NR
NR
NR
NR
298 ND
64 199
81 114
NR
NR
NR
NR
NR
8.2 50.5
NR
NR
NR
NR
25.4 1.1
NR
NR
9.2 42.2
NR
NR
NR
m
23 1.3
NR
NR
NR
NR
NR
21.7 4.0
NR
NR
10 0.009
22 0.01?
91 0.05
41 37.2
35 139
NR
NR
31.5
NR
NR
NR
75 4.0
40 3.8
NR
4.6
NR
NR
48 2.01
28 45.8
35 74.2
NR
NR
24,7
NR
NR
12.9
33.4
11.0
42
50
294
233
87
44
21
30.0
84
124
104
128
38
40
35
NR
1.8
NR
NR
NR
NR
0.25
NR
NR
1.4
NR
NR
NR
NR
ND
NR
NR
NR
NR
NR
0.77
NR
NR
ND
0.013
0.004
0
10,2
NR
NR
1.5
NR
NR
NR
0
3.44
Nil
4.4
NR
NR
0
8.2
0
NR
NR
3.2
NR
NR
19.2
44
3?
22!
113
200
184
24?
0
72
129
0
149
89
0
104
0
94
NR
53.3
NR
NR
NR
NR
0.92
NR
NR
39.0
NR
NR
NR
NR
1.5
NR
NR
NR
NR
NR
1.0
NR
NR
0.032
0.003
0.017
32.1
136
NR
NR
37.2
NR
NR
NR
3.8
ND
NR
3.7
NR
NR
2.9
90
51
NR
NR
32.7
NR
NR
12.7
36
11
38
118
96
572
208
54
21
27.4
94
447
123
104
33
48
30.3
140
-------
DATA RECIEVED FROM EERF AS
File: ORP.RADS.FALL84
Report: DATA PRINTOUT!
TYPE TK MERL tt EERF «
PART. 14
PART. 15
PART. 15
PART. 15
PART. 15
PART. 15
PART. 15
PART. 15
PART.SF, 12
PART.SF. 12
PART.SF. 12
PART.SF. 12
PART.SF. 12
PART.SF. 12
PART.SF. 12
PART.SF. 12
PART.SF. 13
PART.SF, 13
PART.SF. 13
PART.SF. 13
PART.SF. 13
PART.SF. 13
PART.SF. 13
PART.SF. 13
PART.SF. 14
PART.SF. 14
PART.SF. 14
PART.SF. 14
PART.SF. 14
PART.SF. 14
PART.SF. 14
PART.SF. 14
PART.SF. 15
PART.SF. 15
PART.SF. 35
PART.SF. 15
PART.SF. 15
PART.SF. 15
PART.SF. 15
SED.TRAP 12
SED.TRAP 12
SED.TRAP 12
SED.TRAP 12
SEO.TRAP 12
SED.TRAP 12
SED.TRAP 12
SED.TRAP 12
SED.TRAP 12
SED.TRAP 13
SED.TRAP 13
SED.TRAP 13
SED.TRAP 13
.032
.020
.021
,023
.025
.026
.028
.032
.020
.021
.023
.025
,026
,028
.030
.032
.020.1
.020.2
.021
.023
.025
.02(5
.030
.032
.020
.021
.023
.025
.02i
.028
.030
.032
.020
.021
.023
.025
.024
.028
.032
.001
.002
.003
.004
.005
.007
.008
.011
.013
.001
.002
.003
.004
52694
4*5351
4(5368
46386
46925
46934
52677
52685
46342
46357
46378
46920
46929
5268?
52690
52693
46345
46346
46360
46381
46922
46931
52692
52695
46349
46366
46384
46924
46933
52686
52691
52694
46352
4636?
46387
46926
46935
52689
52696
46405
46406
46413
46414
46421
46937
46941
52719
52721
46407
46408
46415
46416
OF HAR. 11, 1986, ECOSYSTEM EXPERIMENT ONLY.
JULIAN TSH/FLX RA-226 RA +- PB-210 PB +- PO-21Q PO +- U-234
338
261
269
276
290
297
312
338
261
26?
276
290
29?
312
325
338
261
261
269
276
290
29?
325
338
261
26?
276
290
297
312
325
338
261
26?
276
290
297
312
338
261
261
26?
269
277
291
298
319
341
261
261
269
269
2.87
6.13
5.06
4.59
3.02
3,5?
1.56
1.86
2.66
3.49
2.23
1.54
1.50
1.07
1.23
1.07
5.11
6.33
5.03
5.14
3.71
3.20
2.38
1.38
3.75
2.34
2.56
2.49
2.22
1.14
1.81
2.24
4.87
4.33
3.02
2.56
2.85
1.12
1.22
0.86
0.94
0.44
0.44
0.34
0.19
0.22
0.07
0.11
2.11
2.42
1.67
1.84
152
20,8
40.2
16.7
32.6
9.0
3.4
9.2
34.9
304
156
242
140
238
172
364
25.8
17.5
23.3
18.9
19.0
21.0
6.9
14.1
25.6
252
123
131
206
134
182
194
8.2
66.5
32.7
35.8
10.5
19.4
45.5
4.4
2.3
273
261
130
113
93.6
24.0
110
2.8
1.3
2.5
1.6
7.0
i?
3.0
35.0
24
19.0
57.0
34.0
37
5
6.0
8.0
7.0
15.0
25.0
10.0
31
33
22
41
25
17.0
36.0
45.0
25
7.0
9.0
10
5.0
17.0
11.0
6.0
42
22
21.0
32
35.0
21.0
29.0
24
25
3.0
3.0
3.0
5.0
6.0
12.0
20
17
16.0
15.0
18.0
NR
95
111
NR
NR
NR
NR
NR
308
762
NR
444
NR
NR
NR
NR
ND
172
ND
NR
NR
NR
NR
NR
ND
ND
NR
ND
NR
NR
NR
NR
155
505
NR
NR
NR
NR
NR
36
NR
300
388
NR
NR
NR
NR
NR
5.5
NR
NR
NR
211
381
12?
44
139
346
155
243
202
476
206
102
113
154
NR
31
29
306
85
48.5
NR
NR
NR
NR
NR
60.4
254
NR
240
NR
97
51, (5
46.6
NR
NR
NR
NR
ND
179
NR
111
NR
3.0
48.5
NR
NR
NR
NR
3.5
NR
343
268
NR
NR
NR
NR
NR
2.3
NR
NR
NR
22
39
42
18
.30
31
35
35
47
42
31
141
56
58
10
11
40
3.3
12.8
NR
11.9
NR
NR
NR
16.1
106
NR
28.4
NR
NR
NR
NR
10.9
20.8
5.3
NR
8.9
NR
NR
NR
4.5
82
NR
37.3
NR
2.7
37.3
NR
14.1
NR
NR
3.2
NR
167
182
NR
NR
NR
NR
0.39
NR
NR
NR
234+- U-235
132
59
73
68
24
55
70
53
81
63
130
32
47
124
62
78
47
13
13
93
!.?
1.3
NR
4.1
NR
NR
NR
10.6
1.9
NR
2.1
NR
NR
NR
NR
ND
1.3
0
NR
3.4
NR
NR
NR
2.8
5.5
NR
3.5
NR
0.42
ND
NR
9.3
NR
NR
0.74
NR
5.1
6.9
NR
NR
NR
NR
0.0
NR
NR
NR
Page 3
HARCH 11, 1986
235+- U-238 238+-
338
384
123
83
16
30?
20?
213
0
170
112
196
221
819
283
95
130
59
46
0
3.0
2.7
NR
4.5
NR
NR
NR
5.8
106
NR
38.3
NR
NR
NR
NR
4,7
2.5
0.22
NR
7.6
NR
NR
NR
1.9
58
NR
30.5
NR
2.4
21.0
NR
16.6
NR
NR
2.0
NR
142
204
NR
NR
NR
NR
0.50
NR
NR
NR
89
172
117
113
24
45
91
141
1173
74
133
38
55
131
97
72
59
13.5
12
72
141
-------
DATA RECIEVED FROM EERF AS OF MAR, 11, 1984, ECOSYSTEM EXPERIMENT ONLY.
File: ORP.RADS.FALL84
Report: DATA PRINTOUT!
TYPE TK MERL I EERF « JULIAN T9VFLX RA-224 RA *- PB-210 PB «- PO-210
SED.TRAP 13
SED.TRAP 13
SED.TRAP 13
SED.TRAP 13
SED.TRAP 14
SED.TRAP 14
SED.TRAP 14
SED.TRAP 14
SED.TRAP 14
SED.TRAP 14
SED.TRAP 34
SED.TRAP 14
SED.TRAP H
SED.TRAP 14
SED.TRAP 15
SED.TRAP 15
SED.TRAP 15
SED.TRAP 15
SED.TRAP 15
SED.TRAP 15
SED.TRAP 15
SED.TRAP 15
SOIL
SOIL 12
SOIL 14
ZOO. 12
200. 12
ZOO. 12
200. 12
ZOO, 12
200. 12
ZOO. 13
200. 13
ZOO. 13
200. 13
200. 13
200. 13
ZOO. 14
200. 14
ZOO. 14
200. 14
ZOO. 14
ZOO. 14
ZOO. 15
ZOO. 15
ZOO. 15
ZOO. 15
ZOO. 15
ZOO. 15
.005
.007
.008
.013
.001
.002
.003
.004
.005
.007
.008
.009
.011
.013
.001
.002
.003
.004
.005
.007
.008
.009
.BIB
FLOATAB
FLOATAB
.010
.011
.012
,014
.015
.018
.010
.01 1
.012
.034
.015
.018
.010
.013
=012
.014
.015
.018
,010
.011
.012
.014
.015
.018
44422
44938
44942
52723
44409
44410
44417
44418
44423
44939
44943
52717
52720
52722
44411
44412
44419
44420
44424
44940
44944
52718
44912
44913
44914
44393
44397
44401
52734
44908
52740
44394
44398
44402
52738
44909
52742
44395
4439?
44403
52737
44910
52741
4439,<
4440Q
46404
52739
44911
52743
277
291
298
341
241
261
249
269
277
291
298
305
319
341
241
261
249
269
277
291
298
305
?
269
249
261
248
276
289
296
317
261
248
276
289
296
317
261
248
276
289
296
317
261
248
276
289
296
3!7
1.38
0.94
1.11
0.47
2.22
2.27
0.32
0.24
0.14
0.31)
0.34
0.44
0.25
0.15
1.79
2.11
1.51
1.94
0.89
0.7?
0.91
0.78
NAP
24.7
20.9
153
78.8
34.3
13.8
5.9
4.4
102
94.8
55.3
54.2
29.2
15.6
39.1
26.4
13.7
11.4
6.0
5,9
107
71.8
72.4
23.4
11,4
9.0
2.5
9,7
321
2.74
2.5
1.3
331
140
47.1
28.5
27.2
72.7
84.0
48.3
1.9
1.4
1.4
1.8
2.7
3.0
3.4
9.3
735
1331
1228
3.63
47.8
39.3
22.9
77.9
49.5
2.6
4.9
4.1
2,48
9,6
8.0
10.1
18.2
16.8
42.0
52.8
390
2.8
8,0
2.5
4.93
45.2
20.6
15.0
21.0
2
20
15.0
17.0
4.0
5.0
8.0
4.0
5.00
4.0
3.0
7.0
26
17.0
25.0
14. fl
20
20.0
24
10.0
2.0
0.89
1.0
17
5.0
8.0
20.0
5.0
24.0
31
20
36
26.0
25
33.0
21
17
33
14
23
4.0
28
15
33
22.0
17
20.0
NR
NR
NR
NR
5.3
NR
249
220
NR
NR
NR
NR
NR
NR
13
NR
NR
NR
NR
NR
NR
NR
3980
2293
2753
11
42.4
67
NR
NR
NR
ND
ND
8.7
NR
NR
NR
ND
ND
47
NR
NR
NR
ND
30
6.7
NR
NR
NR
248
44
57
152
18.1
50
122
148
90
110
1000
447
485
2900
415
443
875
334
532
NR
NR
NR
NR
7.0
NR
329
114
NR
NR
NR
NR
NR
NR
7.0
NR
NR
NR
NR
NR
NR
NR
3233
4312
10520
20
44.1
144
NR
8,8
ND
7.9
NR
NR
0.87
312
255
NR
3.1
9.1
5.5
NR
NR
NR
PO +-
23
14
16
27
8,9
9.4
11.1
17
14
14
27
544
41
46
11
15
46
33
40
• LI- 234
NR
NR
NR
1.3
NR
93
96.3
NR
NR
15.2
NR
NR
NR
0.80
NR
NR
NR
NR
NR
2.3
NR
478
1253
1134
0.35
44.9
26
26.9
1.4
0.93
2.1
NR
1.3
4.8
17
9.7
28.0
1.3
0.85
0.3
10.2
NR
234*-
51
16.5
18
15.0
72
60
11
9.0
10
112
15
25
40
84
43
63
159
54
33
45
51
55
81
148
66
U-235
NR
NR
NR
0.08
NR
4.8
3.3
NR
NR
0.72
NR
NR
NR
0.54
NR
NR
NR
NR
NR
0.51
NR
17.2
35.3
36.4
0.49
1.4
3.2
ND
0.16
ND
0
NR
ND
0.30
2.1
0.7
3.2
0.064
0.33
0,07
2,4
NR
Page 4
MARCH 11, 1984
235<- U-238 238*-
180
71
83
57
78
124
37
18
25
310
61
47
493
400
1400
0
976
346
92
218
149
249
130
307
133
NR
NR
NR
0.77
NR
94.4
84.3
NR
NR
15.4
NR
NR
NR
1.3
NR
NR
NR
NR
NR
0.40
NR
444
1234
1134
0.24
45
27
17.4
0.95
0.32
1.0
NR
0.83
1.8
21.8
15
26.8
3.3
1.7
0.7
1.3
NR
43
14
19
15.0
51
114
11
9.0
10
168
15
24
48
114
134
91
18?
94
29
48
55
56
42
95
3?0
142
-------
DATA RECIBJED FROM EERF AS OF MAR. 11, 1984. ECDS'fSTEH EXPERIMENT ONLY.
File: ORP.RADS.FALL84 page 1
Report; DATA PRINTOUT2 MARCH 11, 1?8
-------
DATA RECIEJED FROM EERF AS OF MAR. 11, 1986. ECOSYSTB1 EXPERIMENT ONLY.
File: ORP.RADS.FALL84 ^9* 2
Report: DATA PR1NTOUT2 MARCH 11, 1984
TYPE TK HERL ft EERF H JULIAN TH-227 227*-.TH-228 228+- TH-230 230*- TK-232
FP,
FP,
FP.
FP.
FP.
FP.
FP.
FP.
FP.
FP.
FP.
FP.
FP.
FP.
FP.
PART.
PART.
PART.
PART.
PART.
PART.
PART.
PART.
PART.
PART,
PART.
PART.
PART.
PART.
PART.
PART.
PART.
PART.
PART.
PART.
PART.
PART.
PART,
PART.
PART.
PAR! .
PART.
PART.
PART.
PART.
PART.
PART.
PART.
PART.
PART,
PART.
PART.
PART.
PART.
PART.
12 .004
12 .006
12 .009
12 .010
13 .003
13 .004
13 .009
14 .003
14 .004
14 .006
14 .009
14 .010
15 .003
15 .006
15 .010
BAY .022
BAY .023
BAY .025
BAY .024
BAY .028
BAY .030
BAY .032
BLA .1
BLA ,2
BLA ,3
12 .020
12 .021
12 .022
12 .023
12 .025
12 .024
12 .028
32 ,030
12 .032
13 .020
13 .02!
13 .023
13 .025
13 .02*
13 .030
14 .020
14 .021.2
14 .021.!
14 .022
14 .023
14 .025
14 .024
14 .028
14 .030
14 .032
15 ,020
15 .021
15 .023
15 .025
15 .024
52724
52727
52730
52733
44916
52726
52732
46917
52725
52728
52731
52734
44918
52729
52735
46375
44389
46927
44936
52678
52462
52684
44390
46391
44392
44341
44356
46371
44377
44919
4492S
52675
5247?
52683
44344
46359
44380
44923
44930
52681
44348
44345
44364
44373
44383
44923
44932
52674
524SO
52684
44351
44368
44386
44925
44934
303
317
345
345
296
303
345
296
303
317
345
345
296
31?
345
272
276
290
297
312
325
338
261
249
272
276
290
297
312
325
338
261
269
276
290
297
325
263
269
249
272
276
290
29?
312
325
338
261
26?
276
290
297
NR
NR
NR
NR
0.15
NR
NR
15.5
NR
NR
NR
NR
0.72
NR
NR
NR
NR
NR
0
NR
NR
NR
0.06
0
0.03
ND
5.5
NR
NR
4.5
NR
NR
NR
NR
ND
3.5
NR
1.7
NR
NR
ND
31
43
NR
NR
1.4
NR
MR
NR
NR
1.2
2,2
NR
4.8
NR
115
18
76
0
100
0
200
346
141
187
245
115
200
136
82
300
346
347
200
141
NR
NR
NR
NR
0.23
NR
NR
8.4
NR
NR
NR
NR
1.4
NR
NR
NR
NR
NR
ND
NR
NR
NR
ND
ND
ND
1.2
1,5
NR
NR
ND
NR
NR
NR
NR
1.3
ND
NR
ND
NR
NR
ND
5.4
ND
NR
NR
ND
NR
NR
NR
NR
0,59
0.81
NR
ND
NR
287
24
89
1095
116
317
92
1300
1058
444
1300
72
55?
27
555
101
238
21 (SO
1620
123
1.54
NR
NR
90.6
1.9
NR
NR
NR
NR
5.6
MR
NR
NR
0.075
0.09
0.09
3.0
478
NR
NR
122
NR
NR
NR
NR
4.8
0.56
NR
6,7
NR
NR
1.5
245
212
NR
MR
54,8
NR
NR
NR
NR
8.
-------
DATA RECIEVED FROM EERF A3 OF MAR, 11, 1984. ECOSYSTEM EXPERIMENT ONLY.
File: ORP.RADS.FALL84
Report: DATA PRJNTQUT2
TK MERL (I EERF « JULIAN TH-22? 227+- TH-228 228-t- TH-230 230+- TH-232 232+-
Page 3
MARCH 11, 1984
PART.
PART,
PART.SF.
PART.SF.
PART.SF.
PART.SF.
PART.SF.
PART.SF.
PART.SF.
PART.SF.
PART.SF.
PART.SF.
PART.SF,
PART.SF.
PART.SF.
PART.SF.
PART.SF.
PART.SF.
PART.SF.
PART.SF.
PART.SF.
PART.SF.
PART.SF.
PART.SF.
PART.SF.
PART.SF.
PART.SF.
PART.SF.
PART.SF.
PART.SF.
PART.SF.
PART.SF.
PART.SF.
SED.TRAP.
SED.TRAP.
SED.TRAP.
SEO.TRAP.
SED.TRAP.
SED.TRAP.
SED.TRAP.
SED.TRAP.
SED.TRAP.
SED.TRAP.
SED.TRAP.
SED.TRAP.
SED.TRAP.
SED.TRAP.
SED.TRAP.
SED.TRAP.
SED.TRAP.
SED.TRAP.
SED.TRAP.
SED.TRAP.
SED.TRAP.
SED.TRAP.
15
15
12
12
12
12
12
12
12
12
13
13
13
13
53
13
13
13
14
14
14
14
34
14
14
14
15
15
15
15
15
15
15
12
12
12
12
12
12
12
32
12
13
13
13
13
13
13
13
13
14
14
14
14
14
.028
.032
.020
.021
.023
.025
.024
.028
.030
.032
.020.1
.020.2
.021
.023
.025
.026
.030
.032
.020
.021
.023
.025
.024
.028
.030
.032
.020
.021
.023
.025
.024
.028
.032
.001
.002
.003
.004
.005
.007
.008
.011
.013
.001
.002
.003
.004
.005
.007
.008
.013
.001
.002
.003
.004
.005
52477
52685
44342
44357
44376
44920
445'29
52687
52490
52693
44345
46344
44360
44381
44922
44931
52492
52695
44349
46364
44384
44924
44933
52688
52691
52694
44352
44369
4438?
44926
44935
52689
52496
44405
44406
46413
44414
46421
44937
44941
52719
52721
44407
46408
44415
46414
44422
44938
44942
52723
44409
44410
46417
444 IB
46423
312
338
241
269
276
290
2?7
312
325
338
241
261
249
276
290
297
325
333
241
269
276
290
297
312
325
338
261
269
276
290
297
312
336
261
261
269
249
277
291
298
319
341
261
261
249
269
277
291
298
341
261
261
269
249
277
NR
NR
0
34
NR
4.7
NR
NR
NR
NR
0
2,7
5.5
NR
0
NR
NR
NR
0
28
NR
0
NR
NR
NR
NR
0
19.0
NR
4.6
NR
NR
NR
ND
NR
27.2
23.8
NR
NR
NR
NR
0.41
NR
NR
NR
NR
NR
NR
ND
NR
10.8
11.4
NR
0
60
200
0
200
114
0
0
86
0
0
100
200
282
32
34
114
200
58
75
NR
NR
ND
ND
NR
ND
NR
NR
NR
NR
ND
ND
ND
NR
ND
NR
NR
NR
ND
ND
NR
22.9
NR
NR
NR
NR
ND
ND
NR
ND
NR
NR
RN
1.7
NR
24.9
24.6
NR
NR
NR
NR
1.2
NR
NR
NR
NR
NR
NR
ND
NR
ND
7.9
NR
2300
150
3700
142
107
449
51
144
84
187
154
243
45
150
29
33
67
3000
6400
119
NR
NR
14.9
519
NR
125
NR
NR
NR
NR
6.3
3.9
5.2
NR
4.4
NR
NR
NR
9.4
234
NR
73
NR
NR
NR
NR
1.3
18.2
NR
12.8
NR
NR
NR
0.55
NR
410
401
NR
NR
NR
NR
1.4
NR
NR
NR
NR
NR
NR
1.2
NR
178
165
NR
4?
11
32
105
94
125
94.4
61
18
33
141
79
87
221
4.3
6.8
44
43
10
11
NR
NR
4.4
12.1
NR
0
NR
NR
NR
NR
1.1
1,3
ND
NR
1.5
NR
NR
NR
ND
3.8
NR
5.2
NR
NR
NR
NR
2.5
2.3
NR
4.8
NR
NR
NR
0.55
NR
22.9
22,1
NR
NR
NR
NR
0.73
NR
NR
NR
NR
NR
NR
0.67
NR
4.8
14.4
NR
100
47
0
447
200
200
200
245
141
174
122
200
114
149
24
27
87
75
66
39
145
-------
DATA REC1EVED FROM EERF AS OF MAR. 11, 1986. ECOSYSTEM EXPERIMENT ONLY.
File: ORP.RAOS.FALL84
Report: DATA PRIMTOUT2
TYPE TK MERL » EERF « JULIAN TH-227 227+- TH-228 223+- TH-230 230+- TH-232 232+-
Pige 4
MARCH 11, 1966
SED.TRAP.
SED.TRAP.
SED.TRAP.
SED.TRAP.
SED.TRAP.
SED.TRAP.
SED.TRAP.
SED.TRAP.
SED.TRAP.
SED.TRAP.
SED.TRAP.
SED.TRAP.
SED.TRAP.
SOIL
SOIL
SOIL
ZOO.
ZOO.
ZOO.
200.
ZOO.
200.
ZOO.
200.
ZOO.
200.
ZOO.
200.
ZOO.
200.
ZOO.
200.
ZOO,
zoo,
zoo.
zoo.
zoo.
200.
zoo.
200,
14
14
14
14
14
15
15
15
15
15
15
15
15
12
14
12
12
12
12
12
12
13
13
13
13
13
13
14
14
14
14
14
14
15
15
15
15
15
15
.007
.008
.009
.011
.013
.001
.002
.003
.004
.005
.007
.008
.009
.BIB
FI.OATA
FLOtiTA
.010
.011
.012
.014
.015
.013
.010
.011
.012
.014
.015
,018
.010
.011
.012
.014
,015
.018
.010
.011
.012
.014
.015
.018
46939
44943
52717
52720
52722
44411
46412
44419
44420
44424
44940
44944
52718
44912
44913
44914
44393
44397
46401
52736
46908
52740
44394
44396
44402
52738
46909
52742
44395
44399
46403
52737
44910
5274!
46394
44400
46404
52739
44911
52743
291
2S'8
305
319
341
26!
261
249
269
277
291
298
305
•>
269
249
261
248
276
289
296
317
261
248
276
289
296
317
261
268
276
289
296
317
261
268
276
289
296
31?
NR
0.79
NR
NR
NR
0.70
NR
NR
NR
NR
NR
0.94
NR
21.3
54.2
51.7
0.46
1.1
5.2
NR
3.7
NR
0.23
0.45
ND
NR
ND
NR
0.56
3.4
3.5
NR
0
NR
0
0.59
0.7
NR
ND
NR
86
100
115
41
16
25
115
14!
76
141
200
200
245
200
346
115
141
0
0
141
200
200
NR
0.97
NR
NR
NR
0.50
NR
NR
NR
NR
NR
ND
NR
34.0
93.1
77.1
ND
ND
ND
NR
ND
NR
ND
ND
ND
NR
ND
NR
ND
ND
ND
NR
ND
NR
ND
ND
ND
NR
ND
NR
139
267
71
31
10.3
17
157
267
213
89
234
254
78
2533
927
232
73
1990
75
12?
121
389
MR
31.9
NR
NR
NR
1.3
NR
NR
NR
NR
NR
2.6
NR
588
619
492
0.5
33,8
24
NR
31.1
NR
0.44
0.11
2.1
NR
3.44
NR
2.4
IB
12
NR
24.3
NR
1.5
1.3
1.8
NR
32.2
NR
8.8
74
49
6.3
4.8
4.4
104
13
25
35
173
200
49
94
74
35
55
54
55
67
75
66
m
2.1
NR
NR
NR
0.42
NR
NR
NR
NR
NR
1.2
NR
40,2
59.8
44.2
ND
2.2
1.4
NR
1.8
NR
ND
0
ND
NR
ND
NR
0
2.2
0.85
NR
1.6
NR
0.3
0.28
ND
NR
0
NR
33.0
132
7!
22.1
12.1
19
600
50
100
200
115
0
141
149
0
100
200
344
114
200
200
0
146
-------
Appendix G. Summary of sediment radionuclide results
Sediment parameters are listed in this appendix. MERL and EERF
sample numbers are listed along with mesocosm, collection period
and depth interval. Pre indicates prior to soil addition, Post
indicates within one week of collection, Mid after 6 weeks and Fin
indicates the final sample collection after 13 weeks of the
experiment. NR indicates nuclide data was not requested; ND
indicates analysis was requested but was not detected. Percent
water, porosity, and radioactivity (in pCi/g dry weight) are
reported.
147
-------
Sediment data at of MARCH 11, 1986, ORP Project,
File: SED.RAD.84
Report: Sediment.1
JULIAN EERFS TYPE TK REP MERL tf DEPTH POROS X
ItfTER Y. RA226 RA+- PB210
Page 1
11, 1986
PB+- P0210 POt-
255
255
255
255
255
255
255
255
255
255
255
255
255
255
255
255
255
255
255
255
255
255
270
270
270
270
270
270
270
270
270
270
270
270
270
305
305
305
305
305
345
345
345
345
345
345
345
345
345
345
345
345
345
345
345
46953
46954
46955
46956
46957
4 6958
46959
46960
46961
46962
46963
46964
46965
46966
46967
46968
46969
46970
46971
46972
46973
46974
46975
46976
46977
46978
46979
46980X
46980
46981
46932
46983
46984
46985
46986
52697
52698
52699
52700
52700X
52701
52702
52703
52704
52705
52706
52707
52708
52709
52710
5271 Ox
5271 1
52712
52713
52714
SED.
SED.
SED.
SED.
SED.
SED.
SED.
SED.
SED.
SED.
SED.
SED.
SED,
SED.
SED.
SED.
SED.
SED.
SED.
SED.
SED.
SED.
SED.
SED.
SED.
SED.
SED.
SED
SED
SED.
SED.
SED.
SED
SED
SED
SED.
SED.
SED.
SED.
SED.
SED.
SED.
SED.
SED.
SED.
SED.
SED.
SED.
SED.
SED.
SED
SED.
SED.
SED.
SED.
12
12
12
12
12
12
12
13
13
13
13
13
13
15
15
15
14
14
14
14
14
14
12
12
12
12
12
12
12
14
14
14
14
14
14
14
14
14
14
14
14
14
14
14
14
14
13
13
15
15
35
12
12
12
12
.1.
.1.
.1.
.1.
.1.
.1.
.1.
.1.
.1.
.1.
.1.
.1.
.1.
.1.
.1.
.1.
.1.
.1.
.1.
.1.
.1.
.1.
.2.
f\
f,
• £•
,2.
,2,
,2.
.2.
.1.
,2.
7
.2.
*"}
.2,
PRE.l
PRE.2
PRE.3
PRE.4
PRE.5
PRE.7
PRE.9
PRE.l
PRE.2
PRE.3
PRE.4
PRE.5
PRE.9
PRE.l
PRE.3
PRE.5
PRE.l
PRE.2
PRE.3
PRE.4
PRE.5
PRE.7
POST. 05
POST . 1
POST. 2
POST. 3
POST. 4
POST, 5
POST, 5
POST.l
POST.l
POST. 2
POST. 3
POST. 4
POST. 5
.MI D.I
.MID. 2
.MID. 3
.MID. 4
.MID. 4
.FIN.l
.FIN. 2
.FIN. 3
.FIN. 4
.FIN. 5
.FIN.?
.FIN.l
.FIN. 3
.FIN.l
.FIN. 3
.FIN. 3
.FIN.l
.FIN. 2
.FIN. 3
.FIN, 4
0.5
1.5
2.5
3.5
4.5
6.5
8.5
C
• -J
1.5
2.5
3.5
4.5
8.5
0.5
2.5
4.5
0.5
1.5
2.5
3.5
4.5
6.5
.25
.75
1.5
2.5
3.5
4.5
4.5
C
.5
1.5
2.5
3.5
4.5
0.5
1.5
2.5
3.5
3.5
0.5
1.5
2.5
3.5
4.5
6.5
0.5
2.5
0.5
2.5
2.5
0.5
1,5
2.5
3.5
72.8
69.3
68,8
66.6
65.9
67.2
65.7
77.4
72.6
74.5
69.5
67.3
66.8
77.4
73.0
69.7
78.1
72.1
6?.l
68.5
67.9
66.3
59.6
63.7
68.1
69.1
68.2
68.2
68.2
60.3
61.8
69. 6
70.2
69.6
69.7
62.5
66.9
70.3
69.6
69.6
66.5
62 . 4
69.8
70.1
69.1
68.3
78.0
71.8
79.3
72.5
72.5
61.1
68.1
69.6
65.9
51.3
46.9
46.4
43.9
43.2
39.9
42.9
57.4
50.9
53.4
47.2
44.7
44.1
57.4
51.5
47.4
58.3
50.3
46.7
46.0
45.4
43.6
36.7
37.1
45.5
47.7
45.8
45.7
45.7
37.4
38.9
47.6
48.1
46.3
45.5
39.6
44.3
48.2
47.4
47.4
43.8
39.4
47.6
47.9
46.7
45.8
58.3
50.0
60.1
50.9
50.9
36.1
45.6
47.3
43.1
0.82
0.77
0.81
0.98
0.94
0.81
0.73
0.84
0.82
1.04
0.78
0.72
0,69
1.00
0,79
0.70
0.66
0.76
0.67
0.73
0.67
0.63
332
200
21.3
17.3
1.7
0.97
0.98
354
212
40.9
51.0
1.8
1.2
227
140
15.9
12.1
10.9
195
166
19.8
0.41
7,8
3.2
0.72
0.72
Q.74
0.50
0.71
626
43.4
8.1
4.4
4.0
5.0
5.0
5.0
5.0
6.0
5.0
5.0
5.0
6.0
6.0
6.0
5.0
6.0
6.0
4.0
6.0
6.0
6.0
5.0
6.0
1.0
1.0
3.0
2.0
3.0
5.0
5.0
0.93
1.0
2.0
0.6
3.0
4.0
2.0
18,0
2.0
2.0
2.0
2,0
2.0
2.0
15.0
2.0
2.0
4.0
4.0
3.0
4.0
4.0
1.0
2.0
2.0
2.0
2.3
1.7
NR
NR
NR
NR
2.6
2.3
2.0
NR
NR
NR
NR
1.17
NR
NR
1.7
1.8
NR
NR
NR
NR
383
307
66.4
419
212
62.7
NR
NRN
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
37 1.9
99 1.76
NR
NR
NR
NR
43 1.6
27 1.8
32 1.7
NR
RN
NR
NR
44 1.7
NR
NR
30 1.6
67 1.5
NR
NR
NR
NR
17.9 323
14.6 160
27.6 47.6
16.9 429
20.5 263
27.1 49.8
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
10.6
15
14.3
11
11
11
11
14
8.0
9.1
10.0
7.7
8.1
10.6
148
-------
Sediment data at of MARCH 11, 1986, GRP Project.
File: SED.RAD.84 Page 2
Report: Sediment.1 MARCH 11, 1966
JULIAN EER.F* TYPE TK REP MERL ft DEPTH POROS X WATER X. RA226 RA+- PB210 PB+- P0210 PO+-
345 52715 SEO. 12 .FIN,5 4.5 67.4 44.B 1.5 4.0 NR NR
345 52716 SED. 12 .FIN.? 6.5 67.5 44.9 0.92 3.0 NR NR
149
-------
Sediment data recieved as of MARCH 11, 1986, ORP Project.
File: SED.RAD.B4 Page 1
Report: Sediment.2 MARCH 11, 1986
EERFH U234 234+- U235 235+- U238 238+- TH227 227+- TH228 228+- 7H230 230+- TH232 232+-
4*953
46954
449-55
46956
44957
46958
46959
46960
44961
46962
46963
46944
46965
46966
46967
46968
46969
46970
46971
46972
46973
46974
46975
46976
46977
46978
46979
46980K
46980
46981
46982
46983
46984
46985
46986
52697
52698
52699
52700
52700X
52701
52702
52703
52704
52705
52706
52707
52708
52709
52710
52710*
5271 1
52712
52713
52714
.75
0.74
NR
NR
NR
NR
.79
0.78
0.80
NR
NR
NR
NR
0.69
NR
NR
0.94
.82
NR
NR
NR
NR
335
175
30.9
3f,— \
Cu
215
41.0
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
0.83
0.8!
153
NR
9.5
NR
15.2 .032 56
18 .037 71
NR
NR
NR
NR
1? .055 54
19.5 0.02 88
15 0.03 54
NR
NR
NR
NR
15 0.02 79
NR
NR
15 0.06 49
18 0.03 87
NR
NR
NR
NR
9.7 10.5 19.0
9.3 4.8 23.7
11.9 1.4835.7
9.6 13.5 17.5
9.3 7.6 19.7
10.9 1.2 38.2
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
14.8 0.02 90
15 0.05 43
11.1 4.9 43
NR
10.3 0.68 23.9
NP
.078 15
.73 19
NR
NR
NR
NR
.76 17
0.66 21
0.75 15
NR
NR
NR
NR
0.82 15
NR
NR
.7? 16
.83 18
NR
NR
NR
NR
308 9.7
176 9.3
30.6 11.9
338 9.6
218 9.3
38.5 11.0
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
0.80 15.8
0.83 14
148 11.2
NR
9,5 10.3
NR
.0298 76
.036 100
MR
NR
NR
NR
0.029 149
0.042 89
0.042 75
NR
NR
NR
NR
0.004 200
NR
NR
.005 346
0.04 90
NR
NR
NR
NR
18.3 16.4
12.3 20.5
.41 120
2-0.4 15.6
13,4 20.1
.44 132
NR
NR
NR
NR
NR
NR
NR
NP
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
.66
.58
NR
NR
NR
NR
0.93
0.85
0.65
NR
NR
NR
NR
0.41
NR
NR
.88
.59
NR
NR
NR
NR
34.1
17.0
2.55
21.9
28.4
6.7
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
13 .67
21 .62
NR
NR
NR
NR
18 1.03
17 0.80
1 *"t * ">
] J' I i /
NR
NR
NR
NR
18 0.48
NR
NR
13 .92
21 .79
NR
NR
NR
NR
9.7 322
15.0 202
41.1 30.2
12.5 342
11.1 241
21.5 46.4
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
12 .85
16 .77
NR
NR
NR
NR
14.4 1.00
14 0.84
7.6 0.97
NR
NR
NR
NR
13 0.42
NR
NR
IS. 5 1.1
15 .84
NR
NR
NR
NR
4.2 32.3
4.7 21.9
8.9 3.5
4.1 27.8
4.6 29.7
7.9 6.3
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
NR
11
14
14.6
14
10
14
11
14
8.9
11.0
22
9.58
9.6
17.6
150
-------
Sediment data retrieved at o{ t-ttRCH 11, 1?6
-------
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