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ORNL-4762.txt
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-+ W sy
CENTRAL RESEARCH LIBR
0
TR R AR
3 445k 0023182 &k %'5
ORNL-4762
UC-70 — Waste Disposal and Processing
CONSIDERATIONS IN THE LONG-TERM
MANAGEMENT OF HIGH-LEVEL
RADIOACTIVE WASTES
Ferruccio Gera
D. G. Jacobs
OAK RIDGE NATIONAL LABORATORY
operated by
UNION CARBIDE CORPORATION
for the
U.S. ATOMIC ENERGY COMMISSION
ORNL-4762
.Contract No. W-74L05-eng-26
HEALTH PHYSICS DIVISION
CONSIDERATIONS IN THE LONG-TERM MANAGEMENT
OF HIGH-LEVEL RADIOACTIVE WASTES
Ferruccio Gera and D. G. Jacobs
FEBRUARY 1972
OAK RIDGE NATIONAL LABORATORY
Oak Ridge, Tennessee 37830
operated by
UNION CARBIDE CORPORATION
e T
3 445k 0023182 &
CONTENTS
ADStract vttt it i i i i i s st s i e e
IntrodUCTion v eieeinnieneeesesnoaseasessancsocsonsonss .
Projected Waste Problem ....v.ivsveeennvensnaseoconossas cen
2.1 Potential Hazard Index .......... c et e i e e e e
2.2 Potential Hazard from Plutonium Isotopes ..............
2.5 Comparison of Inhalation and Ingestion Hazards ......
2.4 Steps in High-Level Waste Management ........eoe... coes
2.5 Evaluation of Risks Associated with Waste Management ..
2.6 Advantages‘of Disposal in Salt Formations .....ceeovue.
2.7 Retrievability of Stored Wastes .........cvveunnn voee
2.8 References .uv.eeeeeecesnennns e es et con
Characteristics of Solidified High-Level Wastes ........ oo
5.1 Leachability covieeieerioeeeaesoeseserssosonsosoanansns
5.2 Heat Generation Rate ....eiie ittt neennanonns
9.9 RETEreNCES titeeceeeesesesossecossosossossascsosesosssassosssss
Interim Storage of Solid Waste ...iv it nnorenronerennanns .
4.1 Routine Operation of Interim Storage Facility ...... .o
.2 Siting Considerations ..iveieeeseseeesanssennonnnas cene
4.3 Possible Mechanisms of Activity Release During Interim
SLOragE tovreeenersennoeonsassnesones ceecanae ce e
h.L Movement of Radionuclides Through the Ground ..........
.S CONCLUSIONS vttt e tonereneeeeaenoenseesoesenoeaasnnans
o6 REFEIEIICES 4evreersonoonssseessoansssssaanoosssesnnnases
Geologic Processes Relevant to the Ultimate Disposal .......
5.1 Stream ErosSion c.oeeeeeieireeieesesoseeetssosesssencosasss
5.2 Orogenic and Epeirogenic Uplift .........civieiieenn,
5.3 (Glacial EroSion «eeeeeeeeasoecesosessassssosssesonsoasse
5.3.1 Cause of Glaciation ...ceveioiesecescssoconnnnss
5.3%.2 Uplift of Previously Glaciated Areas ...........
5.4 SUDSIAENCE ver ittt ittt C et et
e VOlCANiSM teseeesooessoeasasoosssosssssossssossssosssssases
5¢6 Faultifg veeeeeneeoeosessaanasss et eees et ceeeea
5.7 HyQroOlogy ceeeeeseeeenetsoesesocaosssaoossossaoscnssasss
iii
38
45
51
56
60
69
71
7h
75
76
79
79
80
CONTENTS (contad)
5.8 ConcluSions v.veveeeeeeeeeneens C et ettt e e
5.9 RelerencCes tuieeeesesesseseenesssssonossosssssssssosssoassas
5.10 Bibliography +oeeeeeesisneestessessossasessassnsonssnss
Possible Release Mechanisms After Disposal in the Geologic
FOormation .s.eeeeeeieeeenenseenonsenns C et e e et e
6.1 Catastrophic Bvents ........eviiiiiiiuiiiiiiiiiiiiinn..
6.1.1 Meteoritic IMPACE vuuerereresnerenneennsonnennnns
6.1.2 Volcanic ACTiVIEY wewerrrrreeereeeeeeenonnennnnns
6.2 S1oW Ge0logic ProCESSES it vrereererersennonnnnnnnnenas
6.2.1 FaUlbing ceveeeeeenenennnnnneeeneoeeeeneaennnnnns
6.2.2 Erosion seeeeeeeeerianenann e ee e,
6.2.3 Leaching and Transport by Groundwater ...........
6.3 Plastic Deformation of the Disposal Formation ..........
6.3.1 Salt Diapirism ..evevveeennnnn.. e ceees
6.3.2 Shale DiapirishM .vuveeeerrennennnn et e e et s st
6.4 ConcluSions eeeeeereeenereeenan et eeee e et
DD RO O O ICEE ettt sosunessonsesseessassoseesssessnneneas
Summary and ConcCluSionsS t.eeiieertoseenaseessosassensnnnssoses
Appendix A--Estimates of Radionuclide Movement Through the
GIrOUL G v e v ensosseeessossasosesosssassssscsssosassssosesonsses
Appendix A--References ...ceeeievnoesencens f et e e
iv
LIST OF TABLES
Estimated Wastes from Light Water Reactors in the USA..
Estimated Wastes from Liquid Metal Fast Breeder Reac-
tors 1n the USA ..ttt eersnnnnns ceeeesaennas oo
Amounts of Some Transuranium Isotopes in Light Water
Reactor Fuel ...iiiiiiiiiieiniesaseesnssnsscsnsassnas
Amounts of Some Transuranium Isotopes in Liguid Metal
FFast Breeder Reactor Fuel ......ciiiiiii ittt innenns
Potential Hazard Index of Several Significant Radionu-
clides Accumulated in High-Level Solid Waste by the
Year 2020 v eeuieereeoeseseeosossnsssssssossesssonsoennas
Fifty-Year Dose Commitments Resulting from the Inhala-
tion of 1 uCi of @IIPUO, verrrrnrervnnnnn.. e,
Characteristics of Solidified High-Level Waste ........
Range of Chemical Compositions of High-Level Liquid
Waste coeeennnns .
Chemical Composition of Major Materials from Nuclear
B IS d0n v ittt st i ineeeneotessoeseseeeoesacoocsacenenees
Heat Generation Rate in the Waste from the Reprocessing
of 1 Ton of LWR Spent Fuel .....iiiii e irnnnnns
Heat Generation Rate in the Waste from the Reprocessing
of 1 Ton of LMFBR Spent Fuel ....uiiiiiiiiinienrnnenssss
Heat Generation Rates in Solid Waste ..oe.ve e reneeenns
Thermal Conditions of Cylinders Full of Waste with the
Highest Heat Generation Rate ...t iieninennonnnns
Total Heat Generation Rate and Thermal Flux in Freshly
Filled CylindersS veeeeeeseeeeenosoeesoesssssssssenscoens
Inventory of Volatile Radionuclides in Freshly Filled
CyLlindersS ot eieneeeeessssoeseseoassssssssessesssssans
Past and Present Rates of Denudation ....veievevinenn..n.
Rates of Regional Erosion in the United States ........
Rates of Erosion Based on Data from Archeological Sites
NEeQy ROME 4 ewesesescesessesssssossssesasoseessossnesoens
Sediment and Surface Water Yields ....eeeeeeeeoeeoceonss
Relative Rates of Denudation in Uplands and Lowlands in
Different Climates ...viieerieeoenrennososossscsasssonnsns
Partial List of Highlands Uplifted in Pleistocene Time.
Page
11
22
25
26
27
28
29
52
52
L3
62
63
ol
65
66
70
Number
5.7
5.8
5.9
5.10
6.1
Al
A.2
A.3
Ak
A.5
LIST OF TABIES (contad)
Some Present Rates of Uplift .......... e escessensanenas
Greatest Known Fjord Depths ...veveiiernneeeennn ceseeaae
Present Rates of Glacial Erosion ......... ceen o ceeees .o
Geothermal Gradients at Selected Localities in the
United States .cevevvvnnnn... teeecssecceas o ssessseesanss
Possible Types of Deep-Seated Vertical Tectonic Move-
ments .seeee.. ceeesenas tessocecsrssnas cecssecssnacnnannne
Listing of Program FPDSOILS ....... oo Cevcecesceanoas
Listing of Program FPTSOILS .....cv000.e ce s e s e ceens
summary of Kd Values Used in Calculating Radionuclide
Movement ....ecveeeencsns crovssces ¢eosens beesseseranns o
Output of Program FPDSOILS ........... teveseasaans oo
Output of Program FPTSOILS «e.vieeesn.. Che e e e e s e
Vi
Tl
95
153
137
143
Lhl
Number
5.1
LIST OF FIGURES
Variation of Heat Generation Rate in Solid Waste with
Time After Discharge from Reactor ............ et
Predicted Movement of 9OSr from the Leaching of Pot
Calcine Material ...e.tieineeennnoseneeescnonsoonnens
Predicted Movement of 137Cs from the Leaching of
opray Melt Material ..... e e e e s s s eec s e s e e se st eansan
Predicted Movement of 259Pu from the Leaching of Glass
Having a Leach Rate Controlled by Diffusion of 10-2
I /B C 4 ettt et ettt ettt
Predicted Movement of 241Am from the Leaching of Glass
Having a Leach Rate Controlled by Diffusion of 107
2 S0 4 e e et et e e et ettt e ceeas
Cumulative Fraction of 9OSr Originally Present in Vari-
ous Forms of Waste That Would Reach a Seep 60 Meters
from the Source Under Conditions of Continuous Leaching
Cumulative Fraction of 157Cs Originally Present in
Various Forms of Waste That Would Reach a Seep 60
Meters From the Source Under Conditions of Continuous
LEACHING v et eet e tnneeetotesessonensasesotosossansasas
2
Cumulative Fraction of lAm Originally Present in
Various Forms of Waste That Would Reach a Seep 60
Meters From the Source Under Conditions of Continuous
ST ] 4 =
Cumulative Fraction of 259Pu Originally Present in
Various Forms of Waste That Would Reach a Seep 60
Meters From the Source Under Conditions of Continuous
Leaching e ettt it i i i e i e e i i e
Relation of Denudation Rates to Relief-Length Ratio
and Drainage Basin Relief ... ..ttt ieieeeeennnnns
Graph Showing the Dependence of the Average Velocity
of the Vertical Tectonic Movement on the Duration of
the Time Interval of AVEraging .e.eeeeeeeenesovnonsons
Average Relationships Between Shale Density and Depth.
North-South Structural Cross Section, Iowa Salt Dome..
Diagrammatic Cross Section of a German Salt Diapir and
Associated Rim Syncline .....c...iiiianesn. et ieoas cee
Mutual Relationships of Depth, Porosity, and Fluid
Pressure-Overburden Ratio in ar Average Shale or Mud-
S V)4 T
vii
Page
%0
L6
47
L8
L9
52
53
Sk
55
68
96
106
110
112
117
LIST OF FIGURES (contd)
Number Page
6.6(a) Diagrammatic Representation of the Development of a
Mud-Lump Family ..... ceseeeesas teesssseoan cesesaenne 120
6.6(b) Diagrammatic Representation of the Development of a
Mud-Lump Family .eceeeeeoecesesonnnsanns cheeeseanae 121
viii
CONSIDERATIONS IN THE LONG-TERM MANAGEMENT
OF HIGH-LEVEL RADIOACTIVE WASTES
Ferruccio Gera* and D. G. Jacobs
ABSTRACT
High-level radiocactive wastes generated by the
reprocessing of spent fuel elements in the projected
nuclear power industry require the development of an
organic waste management scheme. The presence in
these wastes of long-lived transuranics requires as-
surance of waste containment for a time period of the
order of several hundreds of thousands of years.
For such long time periods only deep geologic forma-
tions offer the stability required for preserving
the necessary degree of containment.
Projections are made of the amounts of radioac-
tive wastes accumulated to the year 2020. Important
radionuclides in the waste are compared on the basis
of their potential hazard to mankind over their en-
tire physical lifetime. On the basis of these con-
siderations, it seems that the most prudent scheme
of management of these wastes involves solidification
with final disposal into a suitable deep geologic for-
mation in such a manner that further handling will be
minimized.
The characteristics of products from various sug-
gested solidification processes are compared. The con-
ditions of interim storage of high-level solid waste
are reviewed, and possible mechanisms of activity re-
lease from the storage facility are considered.
In order to insure safe containment of the waste
for hundreds of thousands of years, the possible rate
of several geologic processes capable of affecting
the disposal formation must be estimated.
Possible mechanisms of activity release from the
deep geologic formation are described.
*Visiting scientist on leave from Italian National Committee for
Nuclear Energy.
1. INTRODUCTION
The nuclear industry is expected to expand rapidly during the next
few decades, and the processing of reactor fuels will result in accumula-
tion of much larger volumes of highly radioactive waste than have been
generated to date. It seems reasonable to assume that the overall scheme
of management will include a number of steps:
1. Interim storage as liquid.
2 Conversion to solid.
3 Interim storage as solid.
4. Transportation to an ultimate disposal site.
5 Ultimate disposal in a geologic formation.
In order to provide the basis for the development of a rational
policy for the management of these wastes, it is necessary to make pro-
jections concerning the quantities and characteristics of the wastes
that will be produced and to make an evaluation of the radiological
safety aspects of each of the steps enumerated above. Radiological
safety evaluations for the first four steps do not differ appreciably
from those encountered in most nuclear operations. However, because
of the increasing amounts of long-lived transuranics expected to be
present in future wastes and because of their potential radiological
hazards, the radiological safety evaluation for ultimate disposal in
geologic formations must consider extremely long time spans. Required
containment times are on the order of hundreds of thousands of years,
which is much longer than recorded human experience. Based on geologic
evidence, global climatic conditions may undergo extensive changes dur-
ing such time periods. Local geologic conditions might also be altered
significantly. '
No attempt 1s made in this report to establish criteria for the
long~term management of high-level radiocactive waste. Rather, the in-
tert is to elaborate on some of the many factors that must be considered
in the development of sultable criteria and to illustrate how several
of the environmental factors may be considered in determining their po-
tential impact upon a facility or upon the consequences of an activity -
release. If the consequences of a particular accident result in activity
- releases that cannot be tolerated, then the mechanisms responsible for
such a release must be evaluated to determine the likelihood of their
occurrence and the type of engineered safeguards that must be employed
to minimize the impact or reduce the activity release to an acceptable
level.
2. PROJECTED WASTE PROBLEM -
With the development of the nuclear industry assumed in Phase 3,
Case 42, of the Systems Analysis Task Force,g'l the amounts of waste
shown in Tables 2.1 and 2.2 will be accumulated in the United States
through the year 2020. These projections are based on a nuclear power
economy having both light water reactors and liquid metal fast breeder
reactors. Other advanced reactor types, such as molten salt reactors,
may require different waste management schemes.
259
The amount of transuranium isotopes, especially Pu, that will
be present in the wastes seems to dictate containment times far exceed-
ing the 1000-year period that would be necessary for the decay of 9OSr
157
and Cs, which have often been considered the radionuclides of major
hazard potential in long-term waste management. Tables 2.3 and 2.4 list
estimates of the amounts of transuranium isotopes that are expected in
the spent fuel of typical light water reactors (LWR's) and liquid metal
fast breeder reactors (LMFBR's) of the future. In Table 2.5 are shown
the total quantities of activity produced through the year 2020 for the
radionuclides that apparently control the long-term management of radio-
active wastes. The table shows that the amounts of transuranics cannot
be neglected. With the assumptions used in compiling Tables 2.1 and 2.2,
the solid waste from reprocessing of LWR fuel would contain 18 uCi/cm5
of 259Pu and 55 uCi/cm5 of 2LLOPu, assuming that 0.5% of the plutonium
present in the spent fuel is not recovered and finds its way into the
waste stream. These concentrations of plutonium correspond to 450 and
1375 maximum permissible body burdens (MPBB) per cubic centimeter of
solid waste. With the same recovery of plutonium from LMFBR fuel, the
solid waste would contain 190 uCi/cm3 of 259Pu (4700 MPBB/cm5) and 235
uCi/en® of 2Py (5900 MPBB/cm).
Table 2.1. Estimated Wastes from Light Water Reactors in the USA
(Modified from ORNL-LL51, 19702‘2)
Calendar Year
1980 1990 2000 2020
Installed capacity, 10° Mi(e)® 153 223 209 5l 1
Fuel processed, 10° tons/yearb’C 2.95 6.01 4.77 4.1
Volume of waste generated, as liquidd
Annually, 1o5 m : 3.67 7.49 5.98 17.5
Accumulated, 100 m 16.5 81.0 148. 4 330.8
Volume of waste generated, as solia®
Annually, o . 275 560 4hs5 1310
~ Accumulated, m 1245 6060 11,100 2L, 800
Accumulated radioisotopesf
Total weight, tons 451 2180 4000 8960
Total activity, megacuries | 18,900 54,500 62,550 142,700
Total heat-generation rate, 106 cal/sec 19.5 54 58 136
9OSr, megacuries 962 4340 7085 13,900
70s, megacuries 1280 5800 9530 18,900
258p,, megacuries® 1.20 6.3 11.6 2k.5
239py, megacuries® 0.022 0.107 0.196 0.438
240, megacuries® 0.0409 0.239 0.53 1.37
1o, megacuries® 6.63 07.7 40.3 7h. 1
EhlAm, megacuries® 2.31 11.3 20.8 46.6
3am, megacuries® 0.232 1.13 2.07 b. 62
2ung, megacuriesg 43,2 90 72 211
kb, megacuries® 29.9 130 200 379
. 2.1
®Data from Phase 3, Case 42, Systems Analysis Task Force (April 11, 1968)
bBased on an average exposure of 33,000 MWd/ton and a delay of 2 years be-
tween power generation and fuel processing: aqueous processing.
CThroughout this report metric tons are used (1000 kg or 2205 1lb).
dAssumes 1250 liters of liquid waste per ton of fuel.
5
®Assumes 1 m” of solid waste per 10.7 tons of fuel.
fpssumes fuel continuously irradiated at 30 MW/ton to 33,000 MWd/torn and
fuel processing 90 days after discharge from reactor.
€Assumes 0.5% of plutonium and 100% of americium and curium in waste.
Table 2.2.
2.2)
Estimated Wastes from Liquid Metal Fast Breeder Reactors in the USA
(Modified from ORNL-4451, 1970
Calendar Year
1985 1990 2000 2020
Installed capacity, 10° MW (e)® 28 145 546 1669
Fuel processed, 10° tons/yearb 0. 36 2.15 9.23 27.6
Volume of waste generated, as ].iquidC
Annually, 10° 0.447 2.69 11.L4 3.k
Accumulated, lO5 m3 0.939 9.1 79 570
Volume of waste generated, as solidd
Annually, m3 33 201 855 2570
Accumulated, m5 70 680 5920 42,590
Accumulated radioisotopese
Total weight, tons 25 260 2200 15,640
Total activity, megacuries 4388 30,000 146,450 523,300
Total heat-generation rate, 106 cal/sec 4.2 28 13k L66
9OSr, megacuries 31.8 300 2465 15,500 '
157Cs, megacuries 78.3 740 6070 38,600
238Pu, megacuriesf 0.18 1.98 9.1 141.5 .
2395y, megacuries® 0.013 0.128 1.1l 8.01 )
2”0Pu, megacuriesf 0.0161 0.156 1.38 10.0
2ulPu, megacuriesf 2.12 19.5 150.7 835
21‘LlAm, megacuriesf 1.18 11.4 100 716
21LBAm, megacuriesf 0.037 0.3%6 3,12 224
2u2Cm, megacuriesf 4.5 95 L15 1279
2uqu, megacuriesf 0.73 7 55 321
%Data from Phase 3, Case 42, Systems Analysis Task Force (April 11, 1968).2'l
bBased on an average exposure of 33,000 MWd/ton, and a delay of 2 years be-
agueous processing.
tween power generation and fuel processing:
“Assumes 1250 liters of liquid waste per ton of fuel.
5
dAssumes 1lm
of solid waste per 10.7 tons of fuel.
®Assumes core continuously irradiated at 148 MW/ton to 80,000 MWd/ton,
axial blanket to 2500 MWd/ton at 4.6 MW/ton, radial blanket to 3100 MWd/ton
at 8.4 MW/ton, and fuel processing 30 days after discharge from reactor.
fAssumes 0.5% of plutonium and 100% of americium and curium in waste.
Table 2.3.
in Light Water Reactor Fuel
(Burnup = 33,000 MWd/ton; Specific Power = 30 MW/ton;
90 days after discharge from reactor)
Amounts of Some Transuranium Isotopes
Specific
Content Activity Activity Half-1life
Isotope (kg/ton) (ci/g) (ci/ton) (years)
258Pu 0.16 17.2 2,780 88
239, 5.38 0.0613 330 24,413
Quopu 2.11 0.227 478 6,580
gulpu 1.10 105 115,800 14
Eugpu 0.36 0.00382 1.36 3.869 x 10°
g 0.050 3.1 172 432
2MAm 0.087 0.200 17.4 7,340
2“20m 0.006 3,320 19,300 0.45
b o 0.031 81.1 2,500 18
2.1 Potential Hazard Index
We have attempted to compare the potential hazards for mankind re-
sulting from the presence in high-level waste of several nuclides hav-
ing long half-lives.
the PHI (Potential Hazard Index), defined as:
2.3,
2.4
In order to make this comparison, we
T.
1
" 0.693
total activity of nuclide i (uCi),
Maximum Permissible Annual Intake of nuclide i (uCi), and
introduce
Qi
PHL; = Py Wor.
i
where
Qi =
MPI. =
i
T, =
physical half-life of nuclide i (years).
Pi 1s a factor dependent on the biological availability of radionuclide
i once it is dispersed into the environment and on the reliability of
Table 2.4. Amounts of Some Transuranium Isotopes in Liquid Metal Fast Breeder
Reactor Fuel
(Burnup
= 33,000 MWd /ton; Specific Power™
= 58 MW /ton; 30 days after discharge from reactor)
opecific
Content Activity Activity Half-1life
Isotope (kg/ton) (ci/g) (ci/ton) (years)
258Pu 0.65 17.2 11,220 88
239py 57. 42 0.0613 3,530 2h,h13
guoyu 18.77 0.227 L ,260 6,580
2kl 5.71 105 600,000 1
242 5
Pu 3.%3% 0.00382 13 3.869 x 10
A lpm 0.46 5.1, 1,570 430
2”5Am 0.25 0.200 50 7,340
o2
h Cm 0.02 3320 65,500 0.45
ko 0.015 81.1 1,240 18
a . .
Fuel is mixture of core + blanket; burnup
values for the mixture.
and specific power are average
Table 2.5. Potential Hazard Index of Several Significant Radionuclides
Accumulated in High-Level Solid Waste by the Year 2020
MPI's in Wastea | Potential Hazard Index
Quantity
Nuclide (ci) Ingestion Inhalation Ingestion Inhalation
At Year 2020
Pgp 2.9 x 1010 9.0 x 10-° 1.0 x 1016 3.6 x 107" u.0 x 10Y7
157Cs 5.7 X lOlO h.7 x 101“ 3,6 x lOlL‘L 2.0 x 1016 1.5 x 1016
28p® 17 x10° k2 x 102 s ox 10 5.3 x 0% 4.3 x 1018
239Pu 8.4 x 106 2.3 x lO]'l 2.1 x lO15 8.1 x 1015 7.h x 1019
MOpt 15 %100 3.6 x 10t 3.2 x 10%7 34 x 1087 3.1 x 1019
QulAmd 7.9 x 108 2.6 x lO15 5.3 x 1016 1.6 x 1016 3.3 x 1019
M 2.7x 100 7.7 x 108 1.9x 108 8.2 x 10" 2.0 x 109
After 300 Years Decay
Pgr 1.6 x 10/ 5.0 x 10%° 5.5 % 10 2.0 x 1olu 2.2 X lolu
157Cs 5.7 x 107 h.7 x lOll 3.6 x lOll 2.0 x lO13 1.5 x lO]'5
258Pu 1.6 x 107 4.0 x 10™F 3.2 x 101° 5.1 % 1017 .1 x 10%
259Pu 8.4 x 106 2.% x lOll 2.1 x lO15 8.1 x lO15 7.4 x 1019
M0p, 1.3 x 107 3.6 x 10 32x 1080 34 x 1087 3.1 x 1019
2LLlAm 5.0 x 108 1.7 x lO15 5.5 x 1016 1.1 x 1016 2.1 x 1019
Mam 2.7 x 107 7.7 x 1077 1.9 x 1077 8.2 x 102 2.0 x 107
®MPI is the Maximum Permissible Annual Intake.
242 258Pu.
bAssumes all Cm decayed to
“Assumes all guqu decayed to 240Pu'
qusumes all gulPu decayed to 2ulAm.
10
waste containment, and represents the probability of the nuclide leaving
the disposal site and reaching man. Presently, we are not able to give
the probability of exposure, and therefore in Table 2.5, P is taken equal
Q.
to 1 for all radionuclides. MP% is the number of Maximum Permissible
i
Annual Intakes of nuclide i present in the waste, and the hazard is con-
sidered to be proportional to this value. The MPI was chosen instead of
the Maximum Permissible Organ Burden Equivalent (a Maximum Permissible
Organ Burden Equivalent is the quantity of a radionuclide that must be
introduced into the body to result in the retention of a Maximum Permis-
sible Organ Burden in the critical organ), because equivalent dose com-
mitments are considered the most satisfactory expression of equivalent
risks.
The mean life (Ti/O.695) is a measure of the time span during which
the radionuclide will exist and is important in determining the potential
global hazard. Normally, when one 1s concerned with radiological hazards
to individuals, the exposure period of concern is limited to 70 years.
However, when exposure of mankind is considered, the potential hazard
can be considered to last for the physical mean life of the radionuclidex*.
Two PHI values are obtained, one for ingestion and one for inhalation;
these two values can differ by as much as four orders of magnitude.
2.2 Potential Hazard from Plutonium Isotopes
In the case of inhalation, the Potential Hazard Indexes for several
transuranium isotopes are greater than those for cesium and strontium.
In relation to the hazard from inhalation of plutonium, several authors
have argued that the MPC and the MPI presently used are too high. Ap-
parently, in the case of inhalation of insoluble plutonium, the highest
dose 1s absorbed by the tracheo-bronchial lymph nodes. There is also
*For the sake of simplicity, the contribution to the potential haz-
ard from the daughter nuclides has been neglected. However, when the
decay chain of a nuclide includes hazardous daughters, the PHI should be
modified to consider the additional potential hazard.
11
- evidence that substantially less plutonium reaches the skeleton than is
assumed in ICRP Publication 2.2'5 According to Voillequé, Shleien, and
others, the dose to the tracheo-bronchial lymph nodes is orders of magni-
tude higher than the dose to other organs.2'6_2'8 In Table 2.6 are
listed 50-year dose commitments to various organs for the intake of 1
uCi of 259PuO
5y @S calculated by Voillequé. With the assumptions and
constants used, an intake equal to the present Maximum Permissible Annual
Intake (occupational = 0.0043 uCi) would result in a 50-year dose commit-
ment to bone of 1.1 to 2.0 rem, depending on the value assumed for the
Table 2.6 Fifty-Year Dose Commitments Resulting
From the Inhalation of 1 uCi of 239PuO
’ 2.6 2
(Data from Voillequé, 19687 ")
50-Year Dose Commitment (in rem) for Activity Median
Aerodynamic Diameter (AMAD) of:
Organ 0.05 um 0.10 um 0.50 um
Lymph nodes 260,000 221,000 132,000
Lungs 1,160 980 588
Liver 497 Lok 277
Bone L71 Lo2 262
Kidney 97.5 ' 83.2 5Lh.3
activity medium aerodynamic diameter (AMAD). The same intake would re-
sult 1n a dose commitment of 570 to 1120 rem to the lymph nodes and from
2.5 to 5 rem to the lungs. If these considerations are valid, the MPC
for inhalation of plutonium should be recalculated with the lymph nodes
as the critical organ. With a MPD to lymph nodes of 15 rem/year (which
is the MPL for unspecified body organs), the MPC would be lowered to
10"lLL uCi/cmi, with an equivalent MPI of 7 x 107~ uCi (calculated for an
AMAD of 0.1 u). With the reduced value for the MPI, the Potential Hazard
Indexes in Table 2.5 for inhalation of plutonium isotopes would be in-
creased about two orders of magnitude. The whole question of dose to
12
respiratory lymph nodes and of recalculation of MPC for inhalation of
plutonium is rather controversial and has been reviewed recently by the
ICRP.2'9 The main points of the problem are briefly summarized as fol-
lows. The mechanism of clearance from the lungs results in accumulation
of particles of insoluble plutonium in the respiratory lymph nodes. The
clearance from the lymph nodes i1is nonexistent or extremely slow; there-
fore, the lymph nodes can be considered as a "sink.'" The total mass of
the lymph nodes in question is about 10 g, and this gives rise to the
very high local doses reported. If the exposure were averaged over the
total mass of the complete lymphatic system (about 700 g), the average
dose to the lymph system would be almost two orders of magnitude lower.
This procedure might be justified in consideration of the lymph circula-
tion, but the noncirculating tissues of the lymph nodes will receive
much higher exposure. Perhaps further long-term experimentation will
indicate that respiratory lymph nodes are not so sensitive to radiation
as to require limitation to an annual MPD of 15 rems. The Task Group
on Spatial Distribution éf Radiation Dose of Committee I, International .
Commission on Radiological Protection, has recently commented on this
problem and expressed the opinion that a change in the dose limit for
plutonium on the basis of risk to the lymphoid tissue is not warranted
2.9
at the present time.
2.5 Comparison of Inhalation and Ingestion Hazards
Going back to the Potential Hazard Index, we realize that two values
for each radionuclide have little meaning and that they should be combined
to give a total Hazard Index. Theoretically, each should be weighted by
a factor representing the probability that the dose will be delivered
to man through ingestion or inhalation. Unfortunately, the statistically
valid data on the long-term behavior and distribution of the significant
radionuclides in the environment that would be necessary for a meaningful
comparison of ingestion and inhalation hazards are not available. .
The only information on global behavior of radionuclides is derived
from fallout data. However, the usefulness of fallout data to evaluate
the possible behavior of radionuclides originally present in solid waste
15
is somewhat limited. The main problem is that fallout radioactivity is
initially released to the atmosphere in finely divided particles; there-
fore, the importance of inhalation is greatly stressed. From the data
available in the literature, however, it can be concluded that even in
this situation only a small fraction of the total intake is from inhal-
2.10-2.12 90
ation. The amount of Sr taken into man through the food
chain is 25 to 50 times higher than the amount inhaled. Fifty to one
137 239,
hundred times more
4 240
Cs 1is ingested than inhaled. The intake of
an Pu by ingestion is only two to four times higher than the intake
by inhalation. In the case of fallout, it is possible to assume that
inhalation is a direct pathway with an intake proportional to the quan-
tity of radionuclide present in the atmosphere. With this assumption,
the different ratios of ingestion to inhalation can be used to indicate
relative transfer coefficients of the various radionuclides along the
food chains. Transfer coefficients for strontium and plutonium will be
0.5 and 0.0k, respectively, of that for cesium. These relative transfer
coefficients are dependent on deposition and suggest foliar interception
as a primary mechanism of entry into the food chains. If the major frac-
tion of the activity reached the ground, one would expect the transfer
coefficients to be much different. Cesium, for example, 1s normally
quite efficiently restricted in its transfer to crops because of its
selective absorption onto soil minerals, but it is quite mobile in bio-
logical systems.2 15
At this time the problem of introducing factors to weight the con-
tributions to total hazard related to ingestion and inhalation seems
exceedingly complex. However, even considering the low mobility of plu-
tonium and americium through food chains, it seems that their content
in high-level waste is such that exclusion from the biosphere will be
required for times greatly in excess of the time period necessary for
decay of cesium and strontium. A decay period of a quarter of a million
259Pu by only three orders of magnitude.
years will reduce the amount of
If such long decay times are necessary, there is no man-made structure
that can be guaranteed to provide safe containment. Because the relative
seriousriess of the potential hazard from plutonium due to inhalation 1is
so much greater than that due to ingestion, we believe that the most
14
prudent scheme of management would be to dispose of the wastes in a suit-
able geologic formation in such a way that further handling will be mini-
mized. It also seems certain that the waste to be disposed of will be
in solid form and that every attention will be given to using as little
space as possible in the geologic formation chosen for ultimate disposal.
2.4 Steps in High-Level Waste Management
The considerations discussed in the previous section imply that the
management of high-level radiocactive waste will include the following
steps, starting at the exit of the fuel processing plant.g'2
1. Interim Storage as Liquid. Liquid storage before solidification
will be necessary to allow the decay of very short-lived radionuclides.
This storage will be on the site of the reprocessing plant in underground
tanks. The alternative solution of storing irradiated fuel for a suit-
able period before reprocessing would result in increased fuel cost, but
it should be evaluated in relation to the possible reduction in risk.
2. Conversion of Waste to Solids. At the present time 1t seems