Jurnal Sains Nuklear Malaysia, 2012, 24 (2): 14-18

ISSN: 2232-0946

Correspondence author: muhamat@nuclearmalaysia.gov.my


RADIONUCLIDE CONCENTRATION OF SPENT RESINS
FROM PUSPATI TRIGA REACTOR COOLANT PURIFICATION SYSTEM


Muhamat Omar, Zalina Laili, J ulia Abdul Karim, Zarina Masood, Nik Marzukee Nik I brahim
and Mohd Abd Wahab Yusof


Malaysian Nuclear Agency,
Bangi, 43000 Kajang, Selangor, Malaysia.


ABSTRACT

A study to assess the concentration of radionuclides in spent resins of the PUSPATI TRIGA Mark II
reactor coolant purification system has been carried out. Fresh spent resins collected and analysed in
May 2010, after the changing of leaked heat exchanger in Sept. 2009 was found to contain
24
Na,
122
Sb,
51
Cr,
124
Sb,
58
Co,
65
Zn,
54
Mn and
60
Co. Old spent resins removed in 2001 and 2002 but analysed in
2010 indicated the presence of
60
Co and
152
Eu as radionuclides with half-lives of < 1 year might have
already been decayed out. These results can be used to establish radionuclide inventory of the spent
resins as part of radiation protection programme.

Keywords: activation products, fission products, radionuclide, spent resin, TRIGA Reactor


INTRODUCTION


PUSPATI TRIGA Reactor (Reaktor TRIGA PUSPATI RTP) of the Malaysian Nuclear Agency
(Nuclear Malaysia) has a purification system to remove radionuclides from the coolant. The schematic
diagram of the reactor cooling and purification system is shown in Fig. 1.The hot primary coolant
from the reactor tank is pumped and mixed with demineralised coolant from the demineraliser prior to
being passed through the heat exchanger (HEX). A portion of the cold coolant from HEX is returned
to the reactor tank, while the other portion is passed through the fibre cartridge filter prior to the
demineraliser containing resins to remove insoluble materials and activated and non-activated products
from the coolant.

Amberlite resin (a strongly acidic gelular polystyrene cation exchange resin containing sulphonic
functional group) is used in the demineraliser. As the coolant gets into contact with fuel elements and
other metals parts in the reactor tank, corrosion products may be generated and then activated by
neutron to produce radioactive elements. Some radionuclides from the fuel might also get into the
coolant especially when the fuel claddings fail. The resin is capable of removing metal ions including
radioactive materials in the form of activation and fission products present in the coolant. As there is a
very limited report available on the radioactivity level of spent resins from this RTP, this qualitative
and quantitative study has been carried out. Recently, a brief study was carried out to characterise the
radionuclide and water content, pH, conductivity and radionuclide leachability of a wet spent resin
Jurnal Sains Nuklear Malaysia, 2012, 24 (2): 14-18
ISSN: 2232-0946

15

sample from the RTP as a preliminary basis to develop treatment process for the spent resin (Laili et al.,
2010).
For the purpose of this study, the reactor operational period is divided into two phases, i.e. prior to (old
phase) and after (new phase) the changing of heat exchanger (mid-September, 2009). In the old phase,
the reactor was in operation for more than 27 years with several changing of resins, usually after a year
of usage. In the new phase, first changing of resins was carried out in May 2010 after 8 months of
usage. All fuel rods used since the commissioning of RTP (1982) are still in the reactor tank. Currently,
112 fuel rods are in use (in the core) and another 11 are kept on the storage racks in the reactor tank. A
study carried out by Masood (2010) showed that two fuel follower control rods (FFCR) had blemishes.
These FFCR (made up of boron carbide and fuel in the upper and lower sections, respectively) are kept
on the storage rack. If there is any leakage of fuel elements or fuel section of FCCR, some fission
products in the fuel might dissolve and enter the coolant and finally trapped by the resins.

This study is related to the previous report on the radioactivity level of reactor coolant (Omar et al.,
2011a). The study reported that the coolant sampled in 2010 (after the changing of leaked HEX)
contained
24
Na,
41
Ar,
42
K,
51
Cr,
54
Mn,
56
Mn,
99m
Tc,
122
Sb,
124
Sb and
187
W. On the other hand, in the
same study, late analysis of water from old tubular heat exchanger (made of cast iron) which was
removed due to leakages indicated the presence of
65
Zn,
54
Mn,
60
Co,
154
Eu and
152
Eu. It is believed that
the leakages had caused the mixing between primary coolant water and the secondary water in heat
exchanger to some extent. Most of the radionuclides present in the coolant might be able to be adsorbed
by the resins. The resin is changed regularly, usually once a year. It is estimated that 50kg of spent resin
is generated when the changing is taking place. The spent resin is stored at the storage facility under the
Waste Technology Development (WasTec) Group of the Nuclear Malaysia.

In pressurized water reactor (PWR) and boiling water reactor (BWR), the volume of spent resins
produced were in the range of 2 to 7 and 20 m
3
/unit/yr, respectively (IAEA, 2002). In nuclear power
plant such as KANUPP, the highly radioactive fission and corrosion products were removed by the use
of ion exchange resin columns (Tahir & Ali, 1999). In nuclear power industry, spent resin is also
produced from cleanup process of spent fuel pool (IAEA, 1985; IAEA 2002). Principal radionuclides
released to the pool water are
131
I,
134
Cs,
137
Cs and
144
Ce (IAEA, 1982b), and these radionuclides are
expected to be present in the spent resin.

This paper describes the radioactivity level of spent resins generated from coolant purification system
of a TRIGA Mark II research reactor in Malaysia. The results can be used to serve multiple purposes,
i.e. to assess the effectiveness of resins used in removing radionuclides from the reactor coolant, to
evaluate if there is any possible leakage of fuel (through detection and accumulation of fission products
in the spent resins), to obtain radionuclide inventory of the spent resins as part of radiation protection
programme and to assist in strategy development in the management (treatment, storage, disposal) of
the spent resins.



METHODS AND MATERIALS


A fresh unused resin and two old spent resins (2001 and 2002 samples) from storage area were
sampled, packed and analysed for radionuclides concentrations. One 2010 fresh spent resins sample
was collected in May 2010, packed and analysed almost immediately in wet condition to detect short-
lived radionuclides. A water sample drained from the fresh spent resin was also collected, packed in
Jurnal Sains Nuklear Malaysia, 2012, 24 (2): 14-18
ISSN: 2232-0946

16

1150-ml Marinelli container and analysed. The activity concentrations of radionuclides for old samples
were normalized (corrected) to May 2010 for direct comparison and estimation of current spent resin
inventory for management purposes. The analysis was carried out using a gamma spectrometry system.
Brief description of the method has been reported by Omar et al. (2004, 2011a, 2011b and [in press]). A
Canberra HPGe gamma spectrometry (n-type detector, Multiport II, AFT Research Amplifier Model
2025, HV Power Supply Model 31060, with a resolution of 1.9 keV at 1332.5 keV of
60
Co) and Genie-
2000 analysis software were mainly used in the analysis of samples. The system counting efficiency
was calibrated using certified multi-nuclide standard source containing
241
Am,
109
Cd,
57
Co,
123m
Te,
51
Cr,
113
Sn,
85
Sr,
137
Cs,
88
Y dan
60
Co in 350-ml container and 1150-ml Marinelli container purchased
from Isotope Production Laboratory (IPL, USA). The resin samples were packed in 350-ml
polyethylene container and analysed at a distance from the detector to reduce the dead time. The
analysis of the presence of radionuclides was carefully done based on guidance given by Omar et al.
(2011a and [in press]).



RESULTS AND DISCUSSION


Radionuclides in the reactor primary coolant water get concentrated in the resins. With time,
radionuclide initially not detected (low in concentration) in the coolant could be detected in resin. Fresh
(blank) resin was analysed and was found to be free from artificial radionuclides. A measurement of the
drained water from fresh spent resins showed that the water was free from radioactive material. Table 1
shows the concentrations of radionuclides in spent resins collected from different years of generation.
Most of these radionuclides were also found in spent resins from PWR with very much higher
concentrations (MacKenzie et al., 1983). The resins collected in the year 2001 and 2002 were very
similar as both contained activation products (
60
Co,
152
Eu).


Table 1: Radionuclide concentration (Bq g
-1
) in spent resin from RTP

Nuclide Half-life
$
2001 2002 2010
24
Na 0.6 d * * 7.10.3
122
Sb 2.7 d * * 4.60.2
51
Cr 27.7 d * * 16.81.1
124
Sb 60.2 d * * 3.40.2
58
Co 70.82 d * * 12.70.4
65
Zn 243.9 d * * 3.1 0.3
54
Mn 312.5 d * * 25.1 0.7
60
Co 5.27 y 5.00.1 34.40.5 33.8 0.6
152
Eu 13.33 y 0.160.01 0.870.03 -
$ d = day; y= year

Although Masood (2010) had reported to observe blemishes on the fuel section of two fuel follower
control rods (in particular REGULATING and SHIM) in September 2008, it was suggested from this
study that there was no leakages of either fuel elements or FFCR that could lead to release of
137
Cs to
the coolant. However, it is rather unfortunate that there were no measurements made systematically to
Jurnal Sains Nuklear Malaysia, 2012, 24 (2): 14-18
ISSN: 2232-0946

17

detect radionuclides and their activity concentrations in the reactor coolant to observe the presence of
137
Cs prior to changing of HEX in September 2009. In the systematic approach carried out recently,
with the most sensitive method using 1 litre sample (5-fold concentration from 5 litre) in marinelli
container, no
137
Cs was detected in the coolant (Omar et al., 2011a). This is in agreement with the
finding that
137
Cs was also not detected in most recent spent resin removed 8 months after the changing
of HEX, supporting the earlier suggestion that the fuel elements and FFCR were not leaked.

A fresh spent resin generated in May 2010, i.e. 8 months after the installation of new plate-type HEX
(made of Al), contains no fission products. Gaseous and volatile fission products are able to escape into
the cooling system if fuel cladding fails (IAEA, 1982a). A number of activation products (
24
Na,
51
Cr,
54
Mn,
58
Co,
60
Co,
65
Zn,
122
Sb and
124
Sb) were detected in the spent resins. Except
24
Na,
51
Cr and
122
Sb,
other radionuclides were either at trace or non-detectable levels in the primary coolant of RTP (Omar,
et al. 2011a). Since the sample was immediately analysed, some short-lived radionuclides were
detected. This is different from old resins (2001 and 2002 samples) whereby only
60
Co and
152
Eu were
detected and radionuclides with half-lives of < 1 year were not detected, i.e. expected to be decayed out
with time. This is obvious as these samples were only analysed after 8-9 years of storage.

In all cases, the concentration of
60
Co was the highest, being 30% of the total activity in the 2010 resin
sample. In the 2002 sample, whereby short-lived nuclides had already decayed out, the concentration of
60
Co in the resin was 98% of the total activity.

With regard to
152
Eu, it was found in leaked HEX water which was removed in September 2009 (Omar
et al., 2011a). Thus, it is not surprising to observe this radionuclide in spent resins removed in 2001 and
2002 (Table 2). However,
154
Eu [gamma-ray energy 123.07 (overlapped with 121.78 of the
152
Eu and
requires interference correction), 722.3, 873.2, 1004.76 and 1274.51 keV] which was found in the HEX
water was not detected in old resins. It is noted that the concentration of
154
Eu in the HEX water was
only about 8 Bq l
-1
.

Overall, the resin was successfully and efficiently used to purify the reactor primary coolant through
removal of radionuclides.



CONCLUSION


A fresh spent resin sample from PUSPATI TRIGA Reactor coolant purification system was found to
contain 8 radionuclides with half-lives between 0.6 days (
24
Na) and 5.27 years (
60
Co). Two old spent
resins contained
60
Co and traces of
152
Eu. This qualitative and quantitative analysis of radionuclides is
vital for radionuclide inventory of the accumulated spent resins from the reactor operation.



ACKNOWLEDGEMENT


The authors wish to thank all the colleagues for providing technical assistance in carrying out this
study.

Jurnal Sains Nuklear Malaysia, 2012, 24 (2): 14-18
ISSN: 2232-0946

18

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