Progress in NuclearEnergy,Vol. 32, No. 314,pp. 525-530.

1998
Pergamon 0 1997Publishedby Elsevier Science Ltd
Printed in Great Britain
0149-1970/98 $19.00 + 0.00
PII: SO149-1970(97)00063-2

A CONSIDERATION TO REDUCE THE POTENTIAL HAZARD

OF I-129 IN RADIOACTIVE WASTES

H.NAKAMURA Y.INAGAKI MSENOO S.TASHIRO

Radioactive Waste Management Center

No.15.Mori Bldg. 2-8-10, Tranomon, Minato-ku Tokyo, Japan, 105

ABSTRACT

Transmutation of I2 ’ I to ’3’ I by (n, 7 ) reaction and isotope

dilution with stable iodine were discussed. The transmutation in LWR is
calculated by supposing that targets irradiated for 25 years are
substituted with new targets. The result showed that initial amount
of ’’’ I will be reduced to 11.5%. In order to lower dose equivalent of
general public than O.lmSv/y, 400 times isotope dilution of 1” I is
required. The feasibility of the isotope dilution was discussed at
dissolution process of spent fuel, conditioning process of the waste and
disposal conditions.
0 1997 Published by Elsevier Science Ltd

INTRODUCTION

The potential hazard of ’’’ I on mankind from disposal of reprocessing plant wastes has
been estimated relatively high. This is due to its high mobility in certain geological
environment. It can migrate easily away from underground repositories and, hence, eventually
reach the biosphere. The environmental condition including geosphere can hardly be estimated
for the long term comparable to the half life of ’” I. Therefore, reduction of ’* ’ I potential
hazard would be desirable.
One possible method may be reduction of 1’’ I as a source by transmuting it to 13’ I by
(n, 7 1 reaction. As Iodine is eventually separated and recovered in the dissolver off-gas
treatment system in reprocessing plant, it is possible to prepare the target material for the
transmutation of “’ I by changing the chemical form without any more separations.
R.J.M.Koning and coworkers irradiated PbI 2 , CeI 3 , NaI and others with thermal neutrons
with a flux of 1.5X10 ’4 cm _ ’ s _ ’ . The results show that they are stable enough against the
irradiation condition[l]. M.Hugon and coworkers calculated the transmutation rate of ’” I
in core region of a fast reactor and showed that 22kg of lZ9 I could be transmuted with a
transmutation half-life of around 44 years[2].
Isotope dilution with stable iodine is also a possible method to reduce maximum potential
dose equivalent. The iodine content in a thyroid is limited. Therefore the maximum potential
dose equivalent is determined by the specific activity of iodine. Once the required isotope
dilution is practiced, the potential dose equivalent after the dilution will be determined by the

525
526 H. Nakamuraet al.

specific activity for any ingestion scenario. The sea water contains relatively large amo_Jnt of
iodine. If proper siting for underground disposal is carried out, the efficient isotope dilution
will be possible.
Feasibility of the above two methods was discussed on supposing simple conditions.

1. PRODUCTION OF IODINE IN SPENT FUEL

Production rate of iodine in LWR and the specific activity was estimated by using
ORIGEN and shown in Table 1.

Table 1 Production of iodine and it specific radioactivity in spent fuel

Burn up 45 GWD/t
Production rate of iodine 3.07x10 2 g/t
15X10 ’ Bq/t
Specific activity of 1’’ I 503x10 ’ Bqlg
Uranium needed for 1 GW LWR 20 t/Y
Production rate of iodine for years 6 kg/y

As most all1 from the fuel dissolution process is collected on the absorber of the off-gas
system, the absorbed I should be the only one target for the transmutation.

2. TRANSMUTATION RATE OF ’’’ I

The transmutation half life of I ’’ I by 1” I(n, 7 ) ’ 3 ’ I reaction with thermal neutron is

shown as follows.
N = N o exp(- CJ4 t )
= N o exp(- 0.0864t)
Where N o : number of ’* ’ I nuclide in target material
N : number of ’’’ I nuclide in target after the irradiiation for t
cr : cross section for thermal neutron (27 b: 2.7x10 _ ’3 cm ’ )
@ : neutron flux( 1x10 ’4 cm _ * s _ ’ in core region of 1 GW LWR)
t : irradiation time( 1 y: 365x24~60~60 = 3.2x10 7 s )

The reduction ratio of ’’’ I in the target after one year irradiation is as follows.
N 1ye a r /N o = exp(-0.0864X1) = 0.9.
The transmutation rate par evry one year is about 10 %.
For one practical system, it is supposed that a target is irradiated for 25 years. and
substituted with new one. The reduction ratio of ’” I after irradiation of 25 years is
calculated as follows.
N/N o = exp(-0.0864X25) = 0.115
The irradiation capacity is necessary for 150 kg iodine which is produced for 25 years The
 Potential hazard of I-129 in radioactivewastes 527

ratio of the total amount of ’’’ I in a reactor(N II ) to annual production(N o ) is calculated as

follows.
N, Ma = exp(-0.0864t)dt
= (1 - 0.115)/0.0846 = 10.5
If this system will be operated continuously for ever, initial amount of ’’’ I will be reduced to
11.5 %. When it is ceased,however, the amount of ’” I corresponding to the production in the
LWR for about 10.5 years will remain in the reactor finally. When irradiation facilities are
installed out of core region, larger capacity and longer irradiation period will be required.

3 . ISOTOPE DILUTION IN FUEL REPROCESSING

1) Calculation of dose equivalent on supposing all iodine in environment being substituted by

iodine with the same specific activity as iodine in spent fuel.
Effective dose(whole body) coefficient of ’* ’ I ingestion is 1.1x10 _ 7 Sv Bq -’ based on
ICRP Pub.68[3]. Intake of iodine by general public is 0.2 mg/d based on ICRP Pub.23[4].
Supposing that all iodine in environment are substituted by the iodine of the same specific
activity as that in spent fuel, ingestion of ’’@I in a year is calculated to be 3.6x10 ’ Bq and
40 mSv/y by using the above values and the specific activity shown in Table 1.
In order to lower the dose equivalent of general public less than O.lmSv/y, 400 times
isotope dilution of ’* !aI is required. Once the dilution is carried out, dose equivalent with any
ingestion scenario will not be over 10% of 1 mSv/y(whole body) recommended by ICRP as dose
limit for general public.

2) Isotope dilution process

Supposing 400 times isotope dilution is performed during fuel reprocessing, an addition of
about 2.4 t of iodine is required for processing 20 t of spent fuel. One of possible methods is the
addition to the dissolver and another is the addition to matrix of solid waste of the iodine
absorber.
The addition to the dissolver may result in efficient isotope dilution and higher recovery of
’” I by carrier effect. In this case the amount of iodine contained in off-gas may be too large
for solid absorber and then absorbing process by alkaline solution should be used instead. The
unfavorable effect of iodine addition on downstream separation steps must be examined. Since
this method requires change of the plant design and re-examination of the process, the
application will not be expected without new plant construction. The conventional process has
been completed by long term research and development. No change of the main process should
be kept and the isotope dilution process should be added to the waste management steps.
Isotope dilution on waste conditioning process may depend on waste forms. Following
conditioning process are considered.
0 Iodine is dissolved from the absorber which could be reused and the dissolved iodine
solution will be solidified with cement.
@ The absorber is solidified with cement directly.
In the case @ the process may be simple and reliable for the isotope dilution because
most of iodine may be I _ in the solution. In the case @ an iodine compound with low
solubility should be mixed in the cement because if the added iodine leach away before
528 H. Nakamura et al.

leaching of 1* ’ I in absorber, isotope dilution will not be expected.

The Ag doped absorbent are used generally. The reduction effect of leachability by dboping
Ag + compound is not reliable for geological disposal because AgI is unstable in reducing
underground condition where AgI will decomposed to Ag metal and soluble iodine compounds,
Therefore isotope dilution by adding iodine compounds to cement may be efective if iodine
wastes are disposed of into reducing underground condition.

4 . ISOTOPE DILUTION ON THE MIGRATION

IN NATURAL ENVIRONMENT

1) On leaching to ground water

Isotope dilution effect was discussed by supposing following conditions.
The ground water is same as sea water in which concentration of iodine ‘a’ is 6.4x10 -’ I:
cme3.
R.D.Scheele and coworkers determined leachability of iodine for various waste forms[5].
The results shows that normalized leaching rate from cementation from of AgI is 1X10 -’ g
cm -’ y -’ and the one of Ba(I0 3 ) 2 -cements is 2X10 -3 g cm -’ y -’ Supposing
concentration of iodine in waste forms is lo%, leaching rate of iodine ‘b’is 1X10 -’ g cm ’
Y ~’ for AgI-cement and is 2X10 m4 g cm -’ y 1 for Ba(I0 3 ) 2 -cement.
When the change of rate of ground water in leaching cell is ‘n’y _ ’ , surface area of waste
form is s cm ’ and volume of leaching cell is ‘A cm 3 , the value of ‘nA/s’ express
approximately ground water flux. Maekawa and coworkers analyzed the hydrology of Tcthoku
district in Japan[G] and found that hydraulic gradient at 500 m depth is distributed mostly in
0.004 - 0.04. In this discussion lower value 0.004 was used since low ground water flux area
may be selected for siting process. By supposing that hydraulic conductivity is 25X10 5 cm
set ~’ and porosity of rock matrix is 5 %, ground water flux v is estimated to be 63cm y ’
Isotope dilution ratio I d is calculated as follows.
AgI-cement: I d = anA/bs = av/b = 6.4X10 -’ X63/1X10 mu= 4.0X10 3
Ba(I0 3 ) 2 -cement: I d = 6.4X10 -’ X63/2X10 -4 = 20
Based on above calculation the dose equivalent for any ingestion scenario after leaching
will be less than 0.01 mSv/y for AgI-cement and 2 m&/y for Ba(I0 3 ) 2 cement.
If the ground water is not saline water, isotope dilution will not, be expected. As Agl and
Ba(I0 3 ) 2 will change to soluble material in case of reducing condition, it is difficult to expect
isotope dilution on leaching process.

2) Isotope dilution with natural iodine contained in coast sea water

The dilution factor of discharged radioactive liquid waste with coastal sea water at Pacific
side in northern Japan is assessed to be 5.8x10 ~I0 (Bq/cm 3 )/(Bqls) shown in the applicat.ion
form for authorization of Rokkasho Fuel Reprocessing Plant[7]. Isotope dilution rate by natural
iodine in coastal sea water is calculated to be 3.4x10 6 g/y by using above dilution factor and
iodine concentration in sea water.
To calculate the discharge rate ,it was supposing that I ” I containing wastes from
reprocessing of the spent fuel of 30,000 tU of 50 LWR(lGW) for 30 y operation is disposed of in
an underground silo 25 m diameter and 50 m depth.
 Potentialhazardof I-129 in radioactive wastes 529

Other assumptions are follows;

a) Hydraulic conductivity in the cement grouted silo is same as rock matrix and iodine is
dissolved homogeneously in pore water.
b) Ground water flows up in the silo of‘50 m depth by Darcy flow rate of 3.15 cm/y which is
calculated by using above parameters.
c) The ground water flow into the sea without dispersion.
From these assumptions discharge rate of iodine is calculated.
(3.07X10 ’ )X(3.0X10 4 ) + (5000 13.15) = 5.8X10 ’ g/y
Then the isotope dilution is
3.4x10 B + 5.8X10 3 = 5.9X10 ’
Once the ground water is discharged into the sea, dose equivalent will not be over 0.07 mSv/y
for any ingestion scenario.

5. DISCUSSION

1) For transmutation of ’” I, it is possible to balance between production rate and

transmutation rate if about 10 times of ’’’ I corresponding to the production in LWR Earone
year is irradiated constantly by thermal neutron flux of 10 ’’ cm _ ’ s _ 1 . However, following
two items should be examined.
a) The self-shielding effect of target material on neutron distribution in reactor and its
deteriorating effect on transmutation rate
b) The concentration of I ’g I required for finally disposable waste form.
The irradiation condition will depend on the requirement for the final concentration. When the
irradiation time is too long, the feasibility may be decreased from not only technical problems
but also social ones.
2) For isotope dilution in dissolution process and waste conditioning process, it may be possible
to add necessary amount of iodine on both processes.
If iodine is added to dissolution vessel, off-gas process should be changed and effects on the
efficiency of down stream separation steps should be examined. The addition of iodine
compound to solidification materials may be more feasible. However, it is necessary to study
the stability of the material in the reducing underground condition where the leachability of
iodine may increase.
3) Deep ground water is saline water somewhere at coast. These place is suitable to dispose of
not only 1” I waste but other radioactive waste, because drinking water scenario may be not
considered due to salinity and migration rate of nuclides may be very low, where flow rate of
ground water may be very slow or stagnant. Isotope dilution will be expected by saline ground
water in disposal sites when the waste is disposed in deep underground at coast.

[l] R. J. M. Konings, et.al.,: Global 1995, Verailles in France Proc. p1631(1995)

[2] M. Hugon., et.al.,:Third Information Exchange Meeting on Actinide and Fission Product
Partitioning and Transmutation Cadrache in France p21 (1995)
[3] ICRP Pub.68 (1994)
(41 ICRP Pub.23 (1975)
[5] R. D. Scheele, et.al.,: * Leach Resistance of Iodine Compounds in Portland
530 H. Nakamura et al.

Cement” Geochemical Behavior of Radioactive Waste, Am. Chem. Sot. 0097~6166/84/0246

p373-387(1984)
[6] K.Maekawa, et.al.,:PNC TN7410 94-029(1994)
[7] JNFL : Application form for reprocessing project authorization in Rokkasho 7-S-131(1989)