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ORNL-TM-2677.txt
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ORNL-TM-2677.txt
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LOCKHERED MARTIN ENERGY RESEARCH LIBRARIES
4
)
b
v
i
'
1
|
[T
3 yy5L 0513220 0
.............................................. o LEGAL MOTICE -~ ettt S
This !epor! wirs prepared os an am:ount of Govemment spuasored work. Meither fhe Um?ed Sta’tas
nor thes Commission, nos any p{.r.scn ‘asting on behalf of the Commission:
- A, Makes any wnrraniy or represghtution, expressed ar implied, with respect to the adouracy,
cm-r.p?afeneas or wsefulness of the information cbfi?cingd in this repart, or. thet the dse of
any’ information, opporotus,: maethsd, or prozuss. disclosed in this report may rol infiings
privately owned rights; of . ' :
B. Assumes ony labilifjes with rexpect to the Use .of, or fot dumagss resulting. ffom the use of
“any information, npp-:xra‘luf, rr\“fl‘tm,, 27 process drs&aset} iothis meporf,
‘As used in the above, ‘oerson’acting on: behall of the” Commission’ insludes cny employee. or
contructor of the Commission, or emplcsya» ol sueh t:nnm:.m‘.af, to the axtant’ fhat sueh employee
ot confraster ol The fgmmssmn, o err.ployoe i such confracter praporas,. d:ssammurm; ot
pravides acsess 1, ony :r.iumo‘uon pursuent to hus amp}uymem Bi confroct: wnh !he hammrsblan
or hsz emp!aymem with auc‘h cantiacter,
&
ORNL-TM- 2677
Contract No. W-THO5-eng-26
CHEMICAL TECHNOLOGY DIVISION
MANAGEMENT OF NOBLE-GAS FISSION-PRODUCT WASTES FROM
REPROCESS ING SPENT FUELS
J O.'Blomeke
J. J. Perona®
¥
Consultant, University of Tennessee
OAK RIDGE NATTIONAL LABORATORY
Oak Ridge, Tennessee
operated by
UNION CARBIDE CCRPORATION
for the
UJ.5. ATOMIC ENERGY COMMISSION
LOGKHEED MARTIN ENERGY RESTARCH LIBRARIES
[NVR RO
3 445k 0513220 0
|
i
MANAGEMENT OF NOBLE~GADS FISS5ION-PRODUCT WASTES FROM
REFROCESSING SPENT FUELS
d o OG:BLomeke
o Jfi‘Perona%
ABETRACT
In an expanding nuclear power economy, it may become desir-
able to remove noble~gasg Tisslon preoducts from spent-fuel proc-
2ssing plant off-gases. Technology is presently available for
removal of krypton and xenon, and alter they have been sep-
arated, it 1s proposed that the krypton be compressed in stand-
ard gas cylinders (either mixed with xencon, or after having
been separated from it), and shipped to a salt-mine repository
for permanent storage. ’
A plant reprocessing 2800 tons/year of fuel would produce
only 28 50-liter gas cylinders per vear of krypton, each con-
taining about a million curies of Kr and generating about
5800 Btu of heat per hour. If the krypton and xenon were nob
separated from each obher, 160 Ly1%fiderh/year would be proeduced,
each containing 180,000 curies “Kr and generating heatl at
a rate of 1000 Bhtu/hr.
The pressurized gas cylinders could be stored Lemporarily
at the plant in water-filled canals, and then shipped to =&
salt mine in specially-designed casks containing from one to
five cylinders each. AT the mine, the cylinders could be
stored above the floor in rooms later sealed to isolate them
from the remainder of the mine. Under these conditions, the
carbon-steel cylinders should last many decades, and the mine
space required would be only about l-to-2 percent of that
regquired for btorage of soliditied high- level waste '
The cost of noble-gas management by this method, p&clu ive
of the cost of separaling the gases from the plant's process
off-gas, is estimated to range from $190,000 to $220,000 per
year. This corresponds te 0.0003 to 0.00035 mills/kwhr of
electricity originally produced from the fuel. From the stand-
point of the projected scale of operations, thelr estimated
costis, and considerations of safety, the proposed method appears
reasonable and manageable over the next several decades.
.}é.
Consultant, University of Ten essee,
1. INTRODUCTLON
In the processing of spent fuels, the noble-gas Tission products are
separated from the fuel during the claddiag-removal and core-dissolution
steps. At post-irradiation decay times of 150 days and longer, 10.8-y
85Kr contributes greater than 99.9% of the total activity present in
these gases, and in the case of plants processing only a Tew tons per
day of 150-day-decayed fuel, they can gencrally be released through a
stack to the atmosphere without exceeding current discharge limits. Recent
studies have shown, however, that to avoid exceeding the current guidelines
f'or radiation exposure of the public al a site boundary that is 2-to-3 km
distant, removal of noble gases may be required if the plant capacity ex-
ceeds about Y tons/day of 150-day-decayed f1_1el.,:L If the fuel is processed
after only 30 days decay, as might be the case in a fast-breeder econony,
removal may be required for plant capacities of only about 0.5 tons/day.
Reprocessing costs scale s¢ as Lo favor larger plants, and since the cost
of rare-gas remcval 1s expected to be less than that otherwise required
to extend the site boundaries, thelr removal can probably be Justified
cconomically as well as from the standpolnt of improved public relations.
There are a number ol processes Icr separating the noble gases from
- . . 2
procesg off-gas wihich are either presently available or under development.
Of these, the most attractive appear to be a process based on absorption
3
in a fTluorocarbon solvent and the cryogenic distillation process cur-
rently in use at the Idaho Chemical Processing v’E)la:rlt‘,LL The absorption
process has been tested extensively on a pilot-plant scale, while the
crycogenic distlillation process has been successfully applied in actual
plant operations. Bach has the potential Ior recovering greater than
99% of the gases with only a percent, or less, of nitrogen and oxygen
impurities in the final product.
Once the noble gases have been collected, however, there is less
certainty how best to contain them for the scores of years that are re-
quired for decay of most of the 85KT to stable 85Rbn One possibllity
5,6,7
might be to inject the gases into porous underground formstions.
An acceptable formation for this purpose would have to be overlain with
LAl
a capping formation of very low permeabllity, be free of cracks or {rac-
tures, and be located in a zone of lowest seismic risk. These congsidera-
tions appear to be too restrictive in determining fuel reprocessing plant
siting requirements for this method to serve as a generally applicable
solution to the problem.
Other possibilities which have been suggested, and in zome cases
investigated to limited extents, include dispersion of the gases in glasses
or resins, and entrapment in molecular sieves, clathrates, or small pres-
surized steel bulbs which are in turn encased in epoxy resin. In our
view, some of these methods may posglibly have long-range applications, but
their technical and economic practicalilty can not be established until
they have received considerably more experimentsl development.
On the other hand, we belleve that a valld and generally applicable
method for management.of these gases, requiring little or no additional
experimental development, Is to encapsulate them in high-pressure cylinders
and then ship the cylinders to a salt-mine repository where they would be
stored permsnently with bthe solidified high-level wastes also generated
at the reprocessing plants. This proposed schedule of management operations,
including handling and temporary storage of the gases at the reprocessing
plants, Shipment of the pressurized cylinders in specially-designed casks
of high integrity, and emplacement?of the cylinders in rooms mined in a
salt formatlon, is examined below.
The authors gratefully acknowledge the help of W. €. T. Stoddart in
the conceptual design of a shipping cask for pressurized cylinders of noble
gases, and of W. G. Stockdale in estimating the capital cost of the gas
vackaging facility.
2. HANDLING OF COMPRESSED GASES IN CYLINDERS
The characteristics ol the nbfile~gas fission products present in a ton
of spent:fuel from a "byplcal' light-water reactor (IMWR), decayed 150 days,
and a liguid-metal-cooled Tast-breeder reactor {(IMFBR), decayed 30 days and
150 days, are given in Table 1. There are no significant differences in
the characteristics of mixtures from fuels having equivalent exposures
Table 1. Characteristics of Noble Gases from One Metric Ton of Spent Fuel
30 Days Decay 150 IDmys Decay
Xe Kr Total Xe Kr Total
Light-water reactor?®
Cram-atoms 50, L L. b 44,8
Curies 2.3 11,200 11,200
0.51k-Mev gamma disintegrations/sec 1.7 x 1012 1.7 x 1012
Heat genersbion rate, watts ¢.003 18.0 18.0
Nurber of cylinders reguired 0.05146 0.0105 0.0621
Fast breeder reactor®
Gram~-atoms 31.9 3.7 35.6 31.9 3.7 35.6
Curies 50,700 10,200 90, 900 7.4 10,000 10,000
Gamme disintegrations/sec ‘ .
0.51h Mev 1.5 x 1042 1.5 x 10ie 1.5 x 1012 1.5 x 10+°
0.08L Mev 3.0 x 1077 3.0 x 1019
Heat generation rate, watis 86.4 6.4 102.8 0.007 16.1 16.1
Number of cylinders requiredb 0.0k15 0.0100 0.0515 0.0U15 ©.01i00 0.0515
STWR fuel exposed to 33,000 Mwd/ton at 30 Mw/tor.
Ges contained in 50-liter cylinders, pressurized to 2200 psig at TOOF.
IMFBR mixed core and blankets with an average exposure of 33,000 Mwd/ton at 58 Mw/ton.
and decay times. Although fasi~breeder fuels may be processed with cooling
times of only 30 days, as compared with 150 days for IWR fuels, the only
radioisotope of conseguence remaining after 150 days in either case is
BSKr, All subsequent considerations refer to mixtures of this age obtaihed
from the fuels defined in Tsble 1.
The noble gases: can be held in standard 50-liter cylinders, 9 in. in
diam by 52 1in. higho. Those confofming te ICC Specification 3AA9 have a
wall thickness slighfily less than:l/h in., welgh 135 1lb, and are normally
filled to 2200 psig in nitrogen service. Xenon and krypton are fairly
compressible at ambient temperatures, with compressibility factors (7 =
PV/nRT)‘reaching minima of 0.21 for xenon at 880 psia, and of C.72 for
krypton at 2800 psia. Gas volumes per ton of fuel processed are shown in
Fig. 1 as functions of storage pressure. At 2200 psiz for LWR fuels, these
values agre 0.1 ftS/ton if both xenon and krypten are stored, or 0.018
ft3/ton if the xenon is separated from the krypton and released. Volimes
for IMFER fuel are aboubt 10% lower.
A 2600-ton/year (10 tons/day) plant processing INR fuel would produée
160 cylinders per year if both xenon and kryptdn are encapsulated, or 28
cylinders per year if only krypton is stored. The krypton activity is
11,200 curies/ton, or about 106 curies per cylinder 1f the krypton is
stored alone. On the other hand, the activity of a cylinder containing
both xenon and krypton is 180,000 curies.,
3. ACCIDENTAL RELEASE
The consequences of an accldental release were studied using the
Geuszlan plume formula of Giffordlo to determine the noble gas concen-~
traticon as =a functiofl of distance from the source, and time. Damage would
occur by personnel exposure alone, since the gases would not remain as
contamination to cause property damage. The xenon activity is negligible
and the most important exposure would be the external whole-body beta dose
from the krypten. Following the formulation of Binford, Barish, and Kam;ll
the concentration Is given by
ORNL DWG 69-12143
10 1 T T T
IDEAL GAS ]
- N
B LWR
- XENON + KRYPTON {
5 LMFBR
m\.
Qo4 - i
[ | o
L. —_ -
O
s ] LWR B
3 KRYPTON { LMFBR
O L — ]
>
0.04 | | L 11 | | [
100 1000 10,000
STORAGE PRESSURE (psi)
FMig. 1. Volume of Noble Gases as a Function of Pressure in a Ton of
Spent Fuel from Light-Water and Fast Breeder Reactors
T
X = ng R | (1)
where X = concentration, curies/m3
q
S
g
The dose rate, D, is directly proportional to the concentration.
f
source strength, curies/min
i
stack factor, min/ms,
12
no
D= = X(&E) , (2)
7 2 )
3% pa(Pa;Ptj
t
where D dose rate,'rem/min
ZE = effective énergy per B disintegration, mev (0.23 for BBKT)
p, = density of air (0.0012 g/cnd)
Ps/Pt = stopping pbwer of air relative to tissue (0.885 for B particles).
The total dose is
o w o0
f D 4T = 3.89(ZE) f X dT = 3.89(zE)s [ Q dT. (3)
o YO gdo
According to Binford et al.,
o
- o O «Kx/u '\
g/; AT = 5T ¥ (&)
Traction of activity released per min
=
=
0
H
1)
Q
b
‘ .o =1
A = decay constant, min
qpiz total amount of release, curies
1 = wind velocity, meters/min
x = distance in direction of wind, meters.
Assuming o > > A and (Ax/u) —0, Equation (4) reduces to q;. The stack
factor is
. ., . .
- s : :
e /&(UY) ~Z2/EJ§ ~(2h+z)2/2§i ‘
= S | & +e T (5)
g :Fuoycz :
where y = horizontal distance perpendicular to wind dirvection, meters
£
= vertical distance relative to release point, meters
o ,0 = dispersion .paramebers, meters
gtack heighf, meters.
o
o
The concentration at ground level (z = ~h) in the direction of the wind
(y = 0) reduces to
s e lf o (6)
The expressicn for the total dose (qu 3) can be written in the form
g
[‘m’ D dt = 0.285 qfi : (7)
Q
w
Values of 6 as functions of distance, x, and weather conditions are plot-
13
ted for a stack height, h, of 100 meters by Hilsmeier and Gifford.”
>
The
maximum value of 8 is 6.41 x 10 7m © and occurs at a distance of 400 meters
with extremely unstable weather conditions (condition A). For a l-million-
curie release and a wind velocity of 100 meters/min, the maximum dose at
ground level is about 200 mrem. At a site boundary 1 kam distant, the
highest value of 9 occurs with slightly unstable conditions (condition C)
and ylelds a total dose of 120 mrem. For a release at a height of 10
meters, the maximum dose with any weather conditions and a wind velocity
of 100 m/sec is less than 15 rem. Present regulations (10 CFR 20 arnd 10
CFR 100) specify that chronic exposures of average popitlation groups shall
not exceed an annual whole-body dose of 170 mrem, and suggest that acute
whole-body exposures resulting from accidents should not result in = dose
grealter than 25 rem.
“. ON-SITE INTERIM STORAGE
Although there is little incentive to keep the gases on-site for any
time longer than necessary to fill a shipping cask, a storage facility for
a 2600_ton/year plant would not be large or expensive, even 1f the gases
were stored for 10-to-20 years. 'The cylinders could he stored safely in
elther air or water, provided they were securely anchored in compartments
or enclosures that afforded protection against impact by an accidentally
ruptured cylinder. However, the requirements for biolegical shielding and
neat dissipation would tend to favor the use of water-filled canals for
interim storage whether kryvpLbon was stored sevparatel or mixed with xenon.
I 2
If the cylinders are filled with krypton alone, and stored on 2-1%
centers, a little more than 100 ftg of floor area is reguired for one
year's production of 28 cylinders. The heat-generation rate of a cylinder
is 5820 Btu/hr, and if it is cooled in air by natural convection and
v1-fl
radiation, the ylinder would reach a temperature of about 3157F These
cylinders would re quflre about 2.6 inches of lead shielding for the dose
rate to be reduced to 10 mrem/hr at 1 meter.
If krypton and xenon are nob separated, the 160 cylinders produced
a year would require about 640 ftg.of storage floor area. In this case,
the heat-generation rdte per cyll der 1s 990 Btu/hr; and the'shielding
requirement is 0.8 in. of lead.
. oHIPPING
M
The shipping cask iz basically a tank filled with water (Fig. 2). It
is a modification of one which has been shown to meet the im@act} puncture,
and fire resistance specifications of the AEC Manual, Chapber 0529, and
which has been licensed for shipping capsules of curium oxi&é.14 The cask
5 £4 in diameter, 1s made of Il-in.-thick, type 304 stainless steeal, and
is equlipped with externai fins to enhanee heat il& lpation. The water
provides shielding, serves as a heat transfer medium, and provides the
heat capacilty needed to withstand a lMTSOF fire:for 30 minubes. A 200
pelg rupture disc is provided as afsafety measure in addition te 16 fusible
plugs, which are designed to allow steam to escape in case of a fire. In
addition, a vapor space 1ls provided sufficiently large to nold the contents
ol a leaky cylinder without causing the rupture disc to vent. In a cask of
the dimensions shown, the cylinder tempersture would be aboub QODF above
the ambient, and the rate of heat dissipation would bte sufficient for one
cylinder of krypton,.or about 5 cylinders of krypton-xzenon mixture. A
loaded cask would weigh about 7 tons and we EDtJmate it would cost about
$40,000. Standard railreoad cars, AO to 7O £t in length, could carry
several casks.
IIJ
U?‘Q'
ORNL DWG 69-4976
PUNCTURE SHIELD LIO GASKET
; TIE-DOWN EYE
O
\'o
FUSIBLE-ALLOY VENTS
~f—————— COOLING FINS
PRESSURIZED GAS CYLINDERS
N
]
\
N
N
N
X
) N
N
\ N
N _ RUPTURE D158
6 \ N
N N STAINLESS STEEL SHELL
X NP
\ \
\ N S50TTOM FiNS
\ \
N g CASK FEET
N // 1
N
i N . . . . \}\ AN
e 5 ft
. 2. Conceptual Design of Snipping Cask for Cylinders of Compressed Fission-Product Gases.
OT
11
6. PERMANENT STORAGE
The cylinders could be stored permanently in & sallt mine operated for
disposal of solidilied high~level fuel-reprocessing wastes. Current plans
tor high-level wastes are to place them in holes in the Tloor of rcooms
mined in salt and, after filling, the roows would be packiilled with crushed
15
galt and sealed.
Disposal in the floor in this manner was conceived
primarily because ofithe shielding requirements for personnel protection.
Cylinders of compreséed gases, requiring only light shielding, could be
placed fin racks above the mine floor and the rooms sealed without back-
fillingfwith salt. The carbon-steel containers, in contact only with dry
air on the outside and noble gaseé on the inside, and isolated from
short~term temperatufe fluctuations, should last many‘decadés and perhaps
centuries.
If the cylinders were stored in the immediate vicinity of the high~level
wastes, they would eVentually reach a temperature of 200°C and a pressiure
of 3500 psig. Therefore, 1¥ mighfi ve desirable to increase the cylinder
wall thickness vy I/S inch. The allowable heat~generation rate per unit
areg of mine floor would be aboul 15=-to-20 Btu/hrwftgg therefore, the space
reguirements fTor a 2600-ton/year plant are about 1/4 acre per year for the
gases as opposed to about 16 acres per year for 6-year-old scolidified
high-level wastes.
7. PRELIMINARY COST ESTIMATE
The economic feasibility ol the scheme under consideration is indi-
cated by a cost estimate based on the requirenents for a 2600=-ton/year
reprocessing plant. The sequence of operations is divided into three
stages: (1) filling, testing, and temporary storsge of cylinders; (2)
shipment of the cylinders to a szalt mine; and (2) permanent storage in the
mine.
A cell equipped for filling and testing cylinders would be contiguous
to the fuel reprocessing plant to Tacilitate the transfer of the noble gases
after they have been separated from the process off-gas; therefore, the
12
same canal used to store spent fuel and/or cans of solidified high-level
wastes can also be used to store the gas cylinders (Fig. 3). The cylinders
are moved from one station to the next by a dolly equipped with a
motor-driven chain drive, and they are unloaded and placed in a corner
of the storage canal with a hand-operated chain hoist suspended Irom a
menorall. A compressor transfers the noble gases from a gas holder (not
shown in Fig. 3) and cowpresses them in the cylinders. After a cylinder
is filled, a wvacuum pump 18 used to evacuate the lines and return the
residuval gases to the holder. During the filling operation, the equipment
is operated from cutside the cell, and a lead-glass window is provided for
viewing. The cell contalns a shadow-shield, however, to enable many oper-
atlons such as gas-line connectlions to the cylinders, remcval of the filled
cylinders from the dolly, and maintenance of the compressor and vacuum
pump to be performed by personnel in the cell. The ventilation air in the
cell is monitored continuously for 5Kr, and provisions are made to seal
the cell automatically and contain the air if radicactivity 1s detected.
In such a case, the air in the cell could be recycled to the noble-gas
separation plant for deceontamination. This facility is capable of packag-
ing either the 160 cylinders/year of krypton-xenon mixtures, or the 28
cylinders/year that would be required if krypton, alone, were to be
encapsulated.
The total capital cost of the facility is estimated to be $230,000
(Table 2). If the equipment is amortized over 10 years, and the structure
over 20 years, at 5% interest, the equivalent annual capital cost is
$24,000 (Table 3). The cost of the cylinders should not exceed $100 each,
based on the cost of ordinary nitrogen cylinders of about $50. Therefore,
the annual cylinder cost is $16,000 for krypton-xenon mixtures, or $2800
for krypton., alone. Annual operating costs, based on an estimated requilre-
ment of 1 man year for mixtures and 1/2 man year for krypton are $20,000
and $10,000, respectively.
Shipping costs consist of the cask capital costs, freignht, and labor
costs. For round-trip shipments of 1000, 2000, and 3000 miles, tTransit
times (ioeg) the tlmes required between successive shipments in the same
cask) are estimated at 7, 9, and 11 days. Therefore, even for the longest
ORNL DWG 69-12154
LEAD GLASS WINDOW
WATER-FILLED .
STORAGE POOL_. __.
. GAS
T CYLINDERS
Z~ IN STORAGE
—m s
STATION C STATION B STATION A
O
TESTING &
UNLOADING
Vil
WELDING FILLING
SHADOW SHIELD
COMPRES-
SCR
VACUUM
PUMP
£AD DOOR
YN ae
: e - h
Fig. 3. Plan View of Krypton Packaging Facility.
€T
Table 2.
1h
Batimated Costse of a Krypton Packaging Facility
Equipment
Modified H,, 2000 psig, h-stage compressor
Remote welder
Chain hrolist, monorail, hand-operated
Dolly,
Vacuum pump
Subtotal "A"
Containment structure
Concrete
Door (lead and steel) and window
Ventilation system
Painting
Electrical,
Floor drain and normal water piping
lighting
Subtotzal "BR"
Piping, process
Electrical, process
Suktotal "C"
Radiation detection instruments (subtotal
Construction overhead 35% of "A, B, C, D"
Subltotal
HEH
rails, motor-driven chain drive
nDn)
Architect engineer alliocation, 12.5% of "E"
Contingency, 25% of above
Preliminary budget estimate
$ 12,000
50,000
500
1,000
1,000
$ 64,500
$ 26,000
15,000
4,000
2,000
1,000
1,600
$ 19,000
$ 3,000
2,500
$ 5,500
$ 2,000
Lp,000
$163,000
$ 20,000
..116,000
$230,000
Table 3. Estimated Annual Costs of Noble Gas Waste Management
for a 2600~ton/year Reprocessing Plant
(Exclusive of Gas Separations Cost)
Krypton and Xenon Krypton
(160 cylinders/year) (28 cylinders/year)
Gas encapsulation
Capital cost $ 24,000 $ 2k, 000
Cylinder cost 16,000 2, 800
Operating cost 20,000 10,000