Assessment of Radiological Safety for Irradiated Thorium Fuel Handling Operations

P. Srinivasan*, P. C. Gupta, D. N. Sharma and H. S. Kushwaha# Radiation Safety Systems Division # Health Safety and Environment Group Bhabha Atomic Research Center, Trombay, Mumbai, India
Thorium oxide rods irradiated in a nuclear reactor contain actinides like 232U, 233U and 228 fission products and hence pose special radiological safety problems while handling. Th, the daughter of 232U has an alpha-decay half life of 1.91160.0016 y and has a chain of daughter products of which 220 Rn (thoron), 208Tl and 212Bi are of major radiological concern. Special ventilation measures are required for 220Rn, a noble gas with a half life of 55.6 0.1 sec, which contributes to inhalation exposure hazards along with its particulate progeny. Hard gamma emitters, 208Tl and 212Bi contribute to external exposure hazards in thorium fuel-cycle operations. Radiological source term estimation, the gamma dose rate evaluation methodology and the results of calculations are presented in this paper. Special emphasis is placed on the effect of neutron cross section data employed on estimated values of radionuclide source term in thorium bundles irradiated in PHWRs. Theoretically estimated values of radioactivity source terms and gamma dose rates in PHWR irradiated thorium rods were compared with experimentally measured values. Dose rate values generated using modified neutron cross-section data for ORIGEN code shows better agreement with the experimental values in contrast to the original cross-section data set that was part of ORIGEN2. Modified neutron cross section data for simulating thorium irradiation in Indian PHWR yields a value of 550 ppm for 232U in irradiated thorium oxide whereas the ORIGEN based cross section data yields a value of 90 ppm of 232U against the experimental value of 500 ppm. Radiological safety evaluation of irradiated thorium oxide fuel reprocessing is discussed. Radiological aspects of handling freshly fabricated 233 U fuel containing ppm levels of 232U are also discussed in this paper. Contact gamma dose rate on fresh AHWR (Advanced Heavy Water Reactor) fuel cluster containing about 1.5 kg of 233U is estimated to be 750 mSv/h, 3 years after fabrication due to build up hard gamma emitting daughters from 232U. Validation of simulated gamma dose rate values generated by radiation transport methods was done with experimental measurement results of external gamma ray exposure rates on irradiated thorium bundles and natural thorium pellets. Experimental validation of radioactivity source terms and the dose rate calculations indicate that the theoretical simulation methods adopted for assessment of radiological safety provide adequate margin of safety for protection of both occupational workers and the public, during handling/processing of irradiated thorium oxide rods and freshly fabricated 233U fuel bundles.

Abstract:

KEYWORDS: Safety; Radiological; Thorium fuel; ORIGEN; neutron cross section; U-232, source terms; Thoron progeny; radiation transport; fuel cycle; inhalation dose; 1. Introduction Thorium oxide rods irradiated at PHWRs (Pressurized Heavy Water Reactor) contain actinides like 232U, 233U and fission products. 228Th, the daughter of 232U has a half-life of 1.91160.0016 y and has a chain of daughter products of which 220Rn (thoron), 208Tl and 212Bi are of major radiological concern. 220Rn is a noble gas with a half life of 55.6 0.1s, which contributes to inhalation exposure hazards along with its particulate progeny. 208Tl and 212Bi are hard gamma emitters contributing to external exposure hazards in the thorium fuel cycle operations. ORIGEN code is used to estimate the radioactive source terms in an irradiated thorium oxide bundle, and the dose rate evaluation is carried out using the Monte Carlo code, MCNP. Studies were carried out to assess the effect of neutron cross section sets, employed for certain major nuclear reactions
------------------------------------------------------------------------------------------------------------------* Presenting au thor, E- ma il: pr ak a17@ yahoo. com, ps r i@ba rc .gov. in

in ORIGEN code, towards estimation of radionuclide source term in thorium bundles irradiated in PHWRs. Radiological shielding requirements due to the presence of hard gamma emitting radionuclides and primary ventilation requirements for removal of thoron (220Rn) gas in freshly fabricated AHWR (Advanced Heavy Water Reactor) fuel bundle containing 500 ppm of 232U are also presented in this report. 2. Radionuclide Source Term Estimation

2.1 Neutron flux and irradiation Data Thoria Bundles irradiated for about 500 days in PHWRs experience high burn-up [1]. Simulation of neutron irradiation in PHWR was carried out using the ORIGEN code [2] for four different values of average neutron flux at the Thorium oxide bundle location. Viz. 8.6x1013 n/cm2/s, 1.3x1014 n/cm2/s, 1.5x1014 n/cm2/s, 1.7x1014 n/cm2/s respectively. The irradiation time considered was 500 days and the cooling period considered for the bundles was 3 years. 2.2 Computations The fission product and the actinide activity calculations were carried out using ORIGEN code. The fission product and actinide activity for given irradiation and cooling periods are worked out considering the rate of formation through all possible routes, rate of decay due to neutron capture and the rate of natural radioactive decay of the products formed. The reaction cross-section sets for all routes of formation and decay are included in the ORIGEN code. For the convenience of the reader we summarize the basics of the ORIGEN code. A radioactive isotope of an element, upon decay, can produce a daughter element that is itself radioactive. This element again, on decay can give rise to radioactive element, and so a decay chain is formed which terminates when a stable nucleus is reached. Bateman devised a series of equations to determine the amounts of each isotope present in a sample after a given time interval. These equations for natural radioactive decay processes, obtained by a generalized form of the well-known equation, N=N0e- t, are:

N n = n Ci e
i =1
where,

Nn is the number of atoms of isotope n at time t, i is the radioactive decay constant for isotope i,
nCi

are the term coefficients given by:

Cm

n 1 0 i N1 = i =1

n i =1 (i m )

m )
2

n where denotes the product function i.e. product of the terms occurring next. i=1 This form of equation doesnt have inherent support for branching decay, though that may be calculated by repeated application to each individual branch, and plugging the actual decay constant for the particular mode of decay of the element at which branching takes place. Although this method has been implemented in some algorithms to evaluate isotope-concentration-buildup due to natural radioactive decay processes, in the absence of external particle flux, starting with a pure sample of a substance at the top of the decay chain, it is not very useful for most purposes involving simulation of neutron irradiation. If initial concentrations of isotopes present lower down the chain, and branching decay have to be taken into account, the algorithm becomes too complex to be considered feasible in view of its limited applicability. A more useful form of the Bateman Equation, which inherently takes branching into account, and also back formation, fission and other decay modes appearing due to a particle flux, is given below.

dN dt

= N i dji +
ji

( E , t )

tr ji

( E ) dE +

ji

d ij

( E , t )

tr ij

( E ) dE N

This is the equation for the concentration Ni of isotope i in a sample, subject to neutron flux where, dij is the rate constant with respect to time for transmutation from isotope j to i, (E, t) is the magnitude of the neutron flux of energy E (units=cm-2 s-1), and ijtr is the neutron cross-section (1 barn = 10-24cm2) for transmutation from isotope j to i The summation is taken over all nuclides present in the material. This is solved by using the exponential matrix method in order to simulate the fuel burn up during neutron irradiation in a nuclear reactor. 2.3 Results and Discussion on source terms The fission product and the actinide activity source terms corresponding to different irradiation levels of the thorium oxide bundles were estimated using the ORIGEN code. This constitutes the source terms for radiological safety evaluation and fuel material inventory accounting purposes. The results of computations using the original cross section set that comes along with the ORIGEN code are presented in Table 1. Studies [3, 4] have shown that the neutron cross sections that come along with ORIGEN are not applicable for thorium fuel cycle due to the physical reason [4] that the effective one-group values are applicable, as infinite dilution one group cross sections, to traces of thorium in natural uranium rods and not to the irradiation of pure thorium oxide pins in 19-rod cluster in our PHWRs. Hence, simulation of neutron irradiation of pure thorium oxide in PHWRs needed updated nuclear cross-section data for 232Th(n, 2n), 231Pa(n, ) and other nuclear reactions in the database of ORIGEN code. The nuclear reactions for which the ORIGEN cross-section data was updated are given in Table 2 for reference.

Table 1 Radioactive inventory of PHWR irradiated Thoria bundles using the cross section set (Old data) that comes along with ORIGEN code for 508 FPDs and cooled for 3 years Irradiation flux (n/cm2-s) 1.7E14 1.5E14 1.3E14 8.6E13 Actinides (Ci/rod) Fission products (Ci/rod)
233

U (gram/rod)

4.74 4.17 3.60 2.33

5830 4882 3967 2059

185 177 168 136

Amount in ppm of 232U in 233U (see Section 2.4 in the text) 117 100 85 54

Table 2. The nuclear reactions that have been updated. The new nuclear data are taken from the BARC work [4] and incorporated by us in the database of the ORIGEN code (Tape 9; No. 402 for actinides; library candunau.lib) to carry out the present study Sr.no 1 2 3 4 5 6 7 8 9 10 11 12
233 233 231 231

Nuclear Reaction
232

Th(n, 2n) 231Th Th(n, ) 233Th

232

232

Th(n, f)

Pa(n, ) 232Pa
231

Pa(n, f)

Pa(n, 2n) 230Pa

233

U(n, f)

U(n, 2n) 232U U(n, ) 234U

233 233

Pa(n, ) 234Pa
233

Pa(n, f)

Pa(n, 2n) 232Pa

The BARC updated cross-section sets [3] were incorporated in the ORIGEN code and the activity source terms were obtained using the revised cross-section data for the certain nuclear reactions occurring in the thoria bundles in the PHWR core. Results of source term estimations using the ORIGEN code based upon the BARC updated cross-section data sets are presented in Table 3. The inventory of 233U per bundle is expected to be about 103 gm per bundle. Fission Product and actinide activity per bundle can be read from Table 3 according to the reactor burn up of the bundle under consideration. 232U will be present at 500 ppm by weight of 233U. For three year cooling period, the thorium oxide bundle will contain about 0.9 Curies of 228Th activity (equilibrium-value of attained after 11 y) Hence, 220Rn activity may also be assumed

conservatively as 0.9 Ci (equilibrium value). But, for longer cooling periods over 10 years, the 228 Th (and hence 220Rn) inventory would be 1.12 Curies. Table 3 Radioactive inventory of PHWR irradiated Thoria bundles using BARC updated cross section set in ORIGEN for 508 FPDs and cooled for 3 years Neutron Irradiation flux (n/cm2-s) 1.7E14 1.5E14 1.3E14 8.6E13 Alpha (Ci/rod) Fission products (Ci/rod) U (gram/rod)
233

8.07 6.64 5.32 3.02

1370 1115 877 422

102.8 95.4 88.2 67.8

Amount in ppm of 232 U in 233U (see Section 2.4 in the text) 526 458 396 270

2.4 Discrepancy in 232U estimation and remarks The 232U content in the bundles went up to 520 ppm by weight of 233U on using the revised cross section data against the 90-ppm value corresponding to the original nuclear cross section data library that was part of ORIGEN. The new values are closer to the experimentally measured value of about 500 ppm. The cross-sections that come along with the ORIGEN code are applicable, as infinite dilution one group cross sections, to traces of thorium in natural uranium rods and not to the irradiation of pure thorium oxide pins in 19-rod cluster in our PHWRs. This physics understanding serves in imparting confidence on the estimated value of 233U, 232U and thoron (220Rn)inventory in irradiated thorium oxide bundles as the 232U ppm levels play a major role in deciding the 228Th and hence the 220Rn (thoron) inventories during various stages of reprocessing. 3. Dose Rate evaluation

3.1 Thorium oxide bundle As source of radiation, a single spent fuel bundle was considered. The geometrical arrangement was similar to those for CANDU fuel bundles used at PHWRs. Zircalloy rods, filled with Thorium oxide pellets compose the thoria bundle. The geometrical arrangement of the bundle consists in two concentric rings (of 6, 12 rods, respectively) and 1 central rod (Figure 1) Fig. 1 Schematic view of the thorium oxide bundle used in PHWRs 1) Zircalloy bearing pads, 2) zircalloy sheath, 3) zircalloy end plate 4) Thorium oxide pellet, 5) zircalloy spacers, 6) zircalloy end cap

Fig. 2 Geometrical models considered for the dose computations

Model 1
Homogeneous model

Model 2
Semi-Heterogeneous model

For simulating the fuel bundle, two geometrical models were used based on the principle of conservation of material mass of different components. Refer to the Fig. 2 above. Homogeneous Model: The fuel bundle was represented as a single cylinder containing a homogenous mixture of fuel and clad materials. This results in a reduced effective density of the homogenized medium. Semi-Heterogeneous Model: The thorium oxide bundle along with the zircalloy was represented as three concentric cylinders (1st for the thorium oxide rods, 2nd for the air gap and the 3rd for the zircalloy clad. This model does not lead to a reduced effective density as the previous model but uses the actual densities of the thorium oxide, air and zircalloy clad media, thus resulting in a closer similarity to the actual bundles. The effective dimensions of the bundle and the clad media are computed according to the principle of conservation of mass of material in the bundle. The homogenized densities of the constituents of the thoria bundle is given in the Table 4

Table 4 Effective densities of the various constituents of the thoria bundle Material Thorium Oxide Zrcalloy Air Effective-Density Density ( g/cc) Model-1 Model- 2 4.262 9.5 0.595 6.5 0.000164 0.001293 4.8 real physical densities

3.2. Dose rates on thorium oxide bundles, Theory vs. Experiment To estimate the dose rates, the above geometry models were realised into the Monte Carlo software MCNP, run in the analogue mode without adopting any biasing for the particle parameters. 10 million particle histories were traced to improve upon the precision of the estimates. The computations were done for the thoria bundles of high burn up, 500 days in the

PHWR because the experimentally measured values are available for a bundle with comparable irradiation level in the reactor [1] Experimental measurements of gamma dose rates were carried out inside the fuel storage pool. Hence, the values quoted are the dose rates in the water medium. The results of the Monte Carlo computations of the dose rates on the fuel bundle are presented in the Table 5. Also shown are the experimentally measured values for comparison. Table 5 Gamma dose rates (mSv/h) on the thorium oxide bundles irradiated in PHWR at flux = 1x1014 ncm-2s-1 for 508 FPDs and cooled for 3 years Geometrical model Gamma dose rates (mSv/h) on the thoria bundle inside water Radial Axial Contact 1 cm 1 Contact 1 cm 1 10520 8000 250 8750 7400 240 9860 7000 210 8230 7000 200 4000 ----3500 -----

Model -1 Model-2 Experimental

It can be seen that there is a slight reduction in the dose rates as one switch over from Model-1 to Model-2. This reduction is expected as per the model description presented in the previous sections. Model-1 calculation yields a net lower effective medium density and hence higher dose rates as compared to the model-2. However, a sharp deviation is observed from the experimentally measured value as can be seen in the last row of the table. These differences could be explained, mainly, in terms of uncertainties in values fission product inventory caused by uncertainties in the rates of formation, fission and (n,2n) reactions of 233U in the core. The uncertainties associated with the evaluation of the gamma photon spectrum of fission products and the actinides add to the observed differences in the dose rate values. The second cause for the deviation could be due to the response of the instrument used to measure the dose rates in water especially when the gamma flux is quite large. The conventional teletector used for measurements has a flat energy response range 0.1 MeV up to 1.8 MeV, where as in the irradiated fuel bundle, considerable contribution (20 % - 30%) to the dose rates comes from gamma photons outside the response range i.e. below 0.1 MeV and above 2 MeV. For instance, the 2.2 MeV gamma ray photons emitted by the 144Pr, the daughter of 144Ce contributes appreciably to the dose rates on the irradiated bundle. 144Ce is a fission product with appreciable yield from thermal fission of 233U. The computed value of actinide contribution to the gamma dose rates on the bundles as a result of 2 different cross section sets are presented in Table 6 and Table 7. The difference in the actinide contribution to gamma dose rates could be attributed to the change in the quantities of 232U and 228 Th decay chain in the bundles as one switches over from ORIGEN based cross section library to BARC based library. Table 6 Actinide contribution to gamma dose rates (mSv/h) on the PHWR thorium oxide rods using the original set of cross sections that comes along with ORIGEN Geometrical model Gamma dose rates (mSv/h) on the thoria bundle inside water Radial Axial Contact 1 cm 1 Contact 1 cm 1 22 16 0.67 20.2 15.6 0.57 20 15.2 0.55 18.7 13.6 0.46

Model -1 Model-2

Table 7 Actinide contributions to gamma dose rates (mSv/h) on the irradiated PHWR thorium oxide rods using the BARC updated cross section data in ORIGEN Geometrical model Gamma dose rates (mSv/h) on the Thoria bundle inside water Radial Axial Contact 1 cm 1 Contact 1 cm 1 112 84 3.6 105 78 3.3 104 78 2.8 96.5 70 2.4

Model-1 Model-2

It can be seen from Table 6 and Table 7 that using BARC updated cross section set in ORIGEN leads indeed to a much higher dose rates due to actinides than the ones generated using the original cross section data that comes along with the ORIGEN-2. This can be attributed clearly to the higher content of 232U using the revised cross section data (about 500 ppm) as compared to the earlier value of about 90 ppm of 232U in the 233U present in the irradiated thorium oxide rod. The 232 U content goes up by about 5 times when one uses the BARC based data set. Hence the 228Th, 220 Rn, 208Tl and 212Bi are as well likely to be about 5 times higher than the values predicted using the original set of cross section data that comes along with ORIGEN. Figure 3 shows the gamma photon emission spectrum from irradiated thorium oxide rod based upon both the older sets and updated sets of cross section data used in ORIGEN. The revised data sets yield higher values of gamma-photon emission rates. Figure 4 shows the variation in radioactive source terms and the ppm levels of 232U in the bundle as a function of irradiation flux in the reactor. Graph shows the source term values for both the old and revised sets of neutron irradiation cross section data employed in ORIGEN calculations.

Fig. 3 Gamma photon emission spectrum from PHWR irradiated thorium oxide bundle due to new and old set of cross section data used in the ORIGEN code
Photon emission spectrum on thorium oxide bundle irradiated for 508 FPDs in PHWR
Actinid new data 1.00E+14 Fission Products Actind -old data

Photons /sec

1.00E+12 1.00E+10 1.00E+08 1.00E+06 1.00E+04 1.00E+02 0.00 0.50 1.00 1.50 2.00 2.50 3.00 3.50 4.00

Energy ( MeV)

Fig .4 Variations in radioactive source terms, 233U and the ppm levels of 232U in the bundle
as a function of bundle irradiation level in the reactor. Results shown for both earlier (ORIGEN) cross section and BARC updated cross section sets
Variation of radionuclide inventory per thoria bundle with neutron irradiation for 508 FPDs and 3 year cooling
10000 FP(Ci) BARC FP(Ci) ORIGEN 1000 U-232(ppm) BARC U-232(ppm) ORIGEN U-233(g) BARC U-233(g) ORIGEN Actinide(Ci) BARC Actinide(Ci) ORIGEN 1 8.00E+13 10 100

1.00E+14

1.20E+14

1.40E+14

1.60E+14

1.80E+14

Neutron Flux (n/cm2-s)

4.1

Dose rate on freshly fabricated 233U-Th fuel rods

Table 7 above shows the dose rates on the fuel rod due to the contribution of actinide- chains like 232 U, 228Th, 224Ra, 220Rn, 216Po, 212Pb, 212Bi and 208Tl present in the irradiated thorium oxide bundle containing 500 ppm of 232U in 233U. Table 8 shows the dose rates on the cluster of AHWR fuel bundle containing 1.482 kg of 233U along with 500 ppm of 232U. Buildup of gamma dose rates with time in fresh bundle is shown in Fig 5. The contact gamma dose rates on the fresh bundle increases to 750 mSv/h (75 Rad/h), 3 years after fabrication. Table 8 Gamma dose rate build up with time for a fresh 54-pin AHWR* composite cluster containing 500 ppm of 232U in 1.482 kg of 233U (* Advanced Heavy Water Reactor) Time after fabrication (years) 0.001 0.01 0.1 0.5 1 3 5 Gamma dose rates (mSv/h) on the fresh bundle in air Radial Axial Contact 1 1m Contact 1 1m 2.32 0.73 0.20 4.00 0.75 0.07 5.04 1.53 0.45 8.20 0.84 0.08 23.5 3.32 0.84 28.0 0.96 0.09 120 18.3 4.60 150 4.00 0.41 212 33.2 8.42 250 7.52 0.82 480 71.3 18.2 750 16.5 1.88 578 87.6 22.4 890 20.2 2.33

Fig. 5 Gamma dose rate build up with time for a fresh 54 pin AHWR composite cluster containing 500 ppm of 232U in 1.482 kg of 233U
Gamma dose rate build up with time after fabrication for fresh 54 pin AHWR composite cluster containing 500 ppm of U-232 in 1.482 kg of U-233
1000

Maximum contact dose rate ( mSv/h)

100

10

1 0.001

0.01

0.1 Time after fabrication (years)

10

Buildup of 232U daughter activity with time in the freshly fabricated 233Ufuel rod is shown in the Fig 6.a and Fig 6.b. It can be seen that the daughter product activities in freshly separated 233 Uincrease by over 9 orders of magnitude in just 10 days time. Also it is observed that the daughter products attain 40%, 80% and 99.99% of the maximum (equilibrium) activity in 1 y, 3 y and 26 years respectively.

Fig 6.a Build up of 232U daughter product activities in 1 kg of a freshly separated 233 U (plus 500 ppm of 232U) in the first 24 hours after separation
Build up of daughter product activity in 1 kg of freshly separated U-233 (plus 500 ppm of U-232)
1.00E+02 1.00E+00 1.00E-02 1.00E-04 1.00E-06 1.00E-08 1.00E-10 1.00E-12

Radioactivity (Curies)

5 10 15 20 Time ( hours) after separation in reprocessing plant

PB212 TH228 BI212 U232 PO212 PO216

24

TL208 RA224

RN220

10

Fig 6.b Build up of 232U daughter product activities in 1 kg of a freshly separated 233 U (plus 500 ppm of 232U) with time.
Build up of daughter product activities in 1 kg of freshly separated U-233 (plus 500 ppm of U-232)
100

Radioactivity (Curies)

10 1 0.1 0.01 0.001 0.0001 1 10 100 1000 10000

Time ( days)
TL208 RA224 PB212 TH228 BI212 U232 PO212 PO216 RN220

Gamma photon energy build up with time in a freshly fabricated fuel rod containing 1 kg of 233 U with 500 ppm of 232U is shown in Fig. 7. The effect of gamma emission spectrum hardening up to a period of one year may be observed clearly attributable to build up of 212Bi and 208 Tl

Fig. 7 Photon energy build-up in a fresh fuel bundle containing 1 kg of 233U with 500 ppm of 232U
Photon energy build up in a fresh fuel bundle containing 1 kg of U-233 with 500 ppm of U-232 1.00E+12
1.00E+11 1.00E+10 1.00E+09 Photon em ission rates ( photons/sec) 1.00E+08 1.00E+07 1.00E+06 1.00E+05 1.00E+04 1.00E+03 1.00E+02 1.00E+01 1.00E+00 1.00E-01 0.015 0.025 0.0375 0.0575 0.085 0.125 0.225 0.375 0.575 0.85 1.25 1.75 2.25 2.75 3.5 Energy (MeV)

15 min

2 hrs

12 hrs

1d

10 d

50 d

100 d

1 yr

11

4.2

Benchmarking the simulation results

The results of source term radioactivity inventory and dose rate estimation by ORIGEN and MCNP based simulation methods were verified by conducting controlled experimental measurements. Experimental measurements of gamma dose rates on a natural, un-irradiated thorium oxide pellet of dimensions 2.5 cm dia x 2.5 cm ht, 30 years old, was carried out using teletector AD5, that has flat response up to 3 MeV gamma photon energy. The gamma photon spectrum in the pellet due to build up of daughter products such as 228Th, 212Bi and 208Tl etc., from natural thorium, is estimated by the ORIGEN code. This information along with the pellet geometry and material density is realized by MCNP Monte Carlo program to estimate the gamma dose rates at various locations. A comparison of the estimated values of dose rates from the natural thorium pellet, with measured values for various distances is presented in Table 9. Table. 9 Gamma dose rates (mSv/h) on natural (un-irradiated) thorium oxide pellet of dimensions 2.5 cm ht x 2.5 cm dia, 30 years old. Geometrical model Gamma dose rates (mSv/h) on the thorium oxide pellet Radial Axial Contact 1 cm 1 Contact 1 cm 1 0.73 0.20 9x10-4 0.08 0.05 6.7x10-4 0.65 0.17 8x10-4 0.07 0.04 5.0x10-4

ORIGEN/MCNP simulation Experimental

Considerable agreement of experimental values with simulation results in this simple benchmark case study, served in imparting confidence in using simulation methods for arriving at source term inventory and gamma dose-rates during different potential operational conditions involving fresh and irradiated thorium-oxide fuel bundles containing 233U contaminated with 232U impurity. 4.3 Assessment of environmental fuel-reprocessing operations impact due to irradiated thorium oxide

4.3.1 Buildup of Thoron (220Rn) gas in the fuel bundle Thoron (220Rn ) gas continuously builds up from the parent 232 U. The complete decay chain of 232U is shown in table 10. Table 10 Decay Product Chain of 232U & daughters

224

Ra present in the decay chain of

Parent Nuclide 232 U 92 228 Th 90 224 Ra 88 220 Rn 86 216 Po 84 212 Pb 82 212 Bi 83

208 212

Half life 1.4 x 1010 y 1.91 y 3.64 days 55 sec 0.16 sec 10.64 h 60.5 m 3.1min 0.31 sec

Type of Emission (36%) (64%)

Tl 81 Po 84

Daughter Product 228 Th 90 224 Ra 88 220 Rn 86 216 Po 84 212 Pb 82 212 Bi 83 208 Tl 81 212 Po 84 208 Pb 82 208 Pb 82

12

As can be seen from the discussions in the previous sections, hard gamma emitting thoron daughters give rise to external exposure hazards in irradiated fuel handling operations. Thoron gas builds up in the decay chain of 232U.from its immediate precursor 224Ra at the rate given by the following equation

QRn220 = QRa224 {1-exp (-Rn220*t)}

Where Rn220 = 0.0126 sec-1 and QRa224 is the activity of 224Ra in equilibrium with 228Th in the decay chain of 232U at any given time. The above equation along with the data presented in Table 3 can be used to evaluate the desired rate of removal (primary ventilation) of thoron gas during reprocessing operations on irradiated thorium fuel bundle. The environmental impact in public domain was assessed in terms of thoron progeny inhalation doses to adult member of public due to reprocessing of PHWR irradiated thorium oxide fuel bundles. Various steps of the methodology adopted for public dose computation is listed below Estimation of liquid to bubble thoron transfer factor Estimation of thoron release rate into the Free Board Volume (FBV) of process equipments containing 228Th. c) Modeling thoron release rate from the FBV of the equipment d) Simulation of the transport of thoron to exhaust ducts and then to the exhaust stack e) Atmospheric dispersion of released nuclides by Gaussian Plume model and estimation of the concentration of thoron & daughters in air in the public domain f) Application of working level methodology to compute thoron inhalation dose to a reference member of the public. Table 11 presents a summary of radiological impact of thorium fuel reprocessing on the public Table11 Estimated upper bound values of 220Rn release rates through the stack and resulting annual public doses due to reprocessing PHWR irradiated Thorium oxideFuel bundles (calculations based upon BARC updated nuclear data) Equipment/operation Stage of reprocessing Dissolution Feed Conditioning Solvent extraction Waste Tanks During Sparging @ 1000 lpm 35 hr/ annum No sparging(7000 hr/y) Total 4.4 12.5 0.018 21414* Curies/annum 0.18 0.053 2.63* 0.018 0.0053 0.263* Thoron release rate mCi/s 0.137 0.274 7.835 Annual inhalation dose to public Sv 0.15 0.15 2.10 mRem 0.015 0.015 0..210 a) b)

Radiological safety of freshly fabricated 233U Fuel bundles

Radiological safety requirements for handling fresh 233U fuel were studied. Radiation shielding requirements for handling a fresh composite cluster of AHWR fuel bundle containing 500 ppm of 232 U, for a typical time gap of 3 years after fuel fabrication is shown in Table 12. It may be noted

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that, the shield requirements increase with time after fabrication, due to the rapid build up of 208Tl & 212Bi, the hard gamma emitting daughter products of 228Th in the bundle. Based on the maximum estimated values of gamma dose rates, lead shielding thickness of the charging cask was evaluated to be 200 mm for five irradiated thorium oxide bundles per charge. This yields a dose rate of 1 Sv/h (0.1 mrem/h) at 1 m from the cask Table 12 Radiological shielding requirements for handling fresh AHWR 54-pin fuel bundle containing 500 ppm of 232U & daughters, three years after fuel fabrication Shield Thickness(cm) to obtain 0.1 mSv/h at 1m from the bundle based on material* Updated cross-section Old Cross-sections Iron 14 8.2 Concrete 49 29 Lead 8.5 5 Aluminium 42 25 * In case of water, the dose rate of 0.1 mSv/h would be obtained only after a thickness of 120 cm as per the updated cross sections (80 cm as per the old data) Acknowledgements The authors express their sincere gratitude to Dr. R. Srivenkatesan, Head, RPDD, Dr. S. Ganesan, Head, Nuclear Data Section, Reactor Physics Design Division, Shri. K. Somanathan, & Shri. D. V. V. Rao, Radiation Hazards Control Unit, south-site, Dr. P. C. Gupta, Head, Radaition Hazards Control Section, Radiation Safety Systems Division, Shri. K. A. Pendharkar, Head, Health Physics Division, Shri. Sanjay Kumar & Shri. Shyamal Das, Nuclear Recycle Group, for their constant support in terms of encouragement and technical guidance in completion of this work. REFERENCES 1. Fuel engineering Division, BARC, Internal Report on Thorium Assemblies Irradiated at KAPS, 2001 2. Croff, A. G ORIGEN2: A versatile computer code for calculating the nuclide composition and characteristics of nuclear materials", Nuclear Technology, 62, 335-352 (1983). 3. Ganesan. S., Nuclear Data Needed to Develop Advanced Nuclear Systems, pp. 9-17, Proceedings, Invited talks, Sixteenth Annual Conference of Indian Nuclear Society (INSAC- 2005), Ganesan S. et al., (Editors), Nov. 15-18, 2005, Mumbai. 4. Sadhana Mukherji, B. Krishna Mohan, S. Ganesan, P. D. Krishnani and Jagannathan, V. Thorium Irradiation in Indian PHWRs- Applications and Limitations of ORIGEN code. presented in the 1st National Conference on Nuclear Reactor Safety, November 25-27, 2002. 5. Srinivasan, P., Ganesan, S. Sharma D. N and Kushwaha H. S. Estimation of dose rates on the PHWR irradiated thorium oxide bundles based on BARC updated nuclear data for ORIGEN code presented in the NWND2006, the Nuclear Data Symposium conducted at Mangalore, Nov-2006 6. Pushparaja, Srinivasan, P., Sharma, D. N. and Venkatraj, V. Radiological safety considerations of Th/233U fuel cycle operations presented in the 11th International Radiation Protection Conference conducted by the International Radiation Protection Association (IRPA) in May 2004 in Spain. 7. Srinivasan, P., Mayya, Y. S., Pushparaja and Sanjay Kumar Assessment of inhalation dose due to thoron daughters to the public from the operation of the Power Reactor Thorium Reprocessing Facility, Trombay Internal Report, Aug 2005

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