SUMMARY REPORT OF THE 2003 FNCA WORKSHOP
ON THE UTILIZATION OF RESEARCH REACTORS
January 12–16, 2004
This document presents a summary on the implementation of the 2003 FNCA Workshop on the Utilization of Research Reactors held in Dalat, Vietnam from January 12 to 16, 2004. The workshop discussed two fields of activities, Neutron Activation Analysis (NAA) and Research Reactors (RR). It was attended by scientists and technical specialists from China, Indonesia, Japan, Korea, Malaysia, the Philippines, Thailand, and Vietnam. A summary of the discussions, progress reports and future programs of each group are presented below.
1. NEUTRON ACTIVATION ANALYSIS
The 2003 FNCA workshop on the utilization of research reactors for the NAA group was held at Dalat, Vietnam on 12-16, January 2004, with participants from China, Indonesia, Japan, Korea, Malaysia, Philippines, Thailand and Vietnam. The workshop consisted of two meetings; one was allocated for ko method on 12th and another was for main discussion on the remaining days. The ko-related meeting was held at the Nuclear Research Institute and the main meeting was at the Sofitel hotel, Dalat. This report consists of three parts; a summary of the ko-session, a summary of country reports and a summary of “round-table” discussions.
1.1. SUMMARY OF THE Ko-SESSION
The first day of the workshop (12th January) was allocated for the ko-method. At the beginning of the session, all participants were welcomed by peoples of the Nuclear Research Institute. Following the short ceremony, ko-experiment was performed for several samples brought from Japan, which are three geological reference samples having well certified values. After the lunch break, we heard the current status of ko-method in each participating countries, as summarized in the following. Among them, there were two long presentations by Japanese and Korean participants, which are summarized separately below. Finally, calculated results by using ko-Dalat were live-shown mainly for short-lived nuclides and were compared with literature values. Generally, most of elements (Al, Ca, K, Mn, Na, Ti and V) were consistent with literature values, although one or two eelements (Mg/Dy) were found to be different from literature values.
|| China: Ko method has been used for 20 years as a routine analytical tool.
|| Malaysia: The ko-NAA method using the ko-Dalat procedure has just been set up for practical use. After completion of setting up, ko-method will be applied to PM samples.
|| Indonesia: Although the ko-software has been already introduced, some calibrations need to be done for practical use.
||Philippines: Although no research reactors are operated, the performance of ko-method is interesting and beneficial. INAA was done by Japanese participants.
||Thailand: There is an agreement for installing ko-software among the groups at OAP utilizing NAA. An IAEA software is considered for its being introduced in future.
|| “The effect of uncertainty of reactor parameters obtained using ko-NAA on results of analysis” by Mr. Fumio Sasajima of JAERI, Japan. The effect of uncertainties of a factor and f factor measured from actual measurements on the result was estimated. Assuming that the a factor for the PN-3 irradiation site of JRR-3M has an uncertainly of 200%, concentrations of 19 elements in PM samples were found to be affected by about 1% at best.
||“Data inter-comparison of air filter analysis by ko-NAA software” by Dr. Hyun Je Cho of KAERI, Korea. Comparison of analytical results for PM samples was made among three ko-softwares, namely, Korea, CIAE and Dalat versions. Data were also obtained by using comparison method. As a result, a fairly good agreement was observed between those by comparison method and KAERI ko-software. In contrast, a systematic difference was observed between KAERI values and data obtained by using CIAE and Dalat softwares.
1.2. SUMMARY OF INVITED AND COUNTRY REPORTS
There were three invited talks (called general lectures for this workshop) at the plenary session on 13th January, just after the welcoming, opening remarks. Among three talks, two talks were related with NAA and are summarized here.
|| “INAA- A struggle for keeping the position in sub-ppm multi-element analysis” by Prof. Pham Duy Hien of Vietnam Atomic Energy Commission. INAA and other multi-element analytical methods such as PIXE, ion chromatography and ICP-MS are compared from several performance criteria. Several recommendations are presented for keeping INAA as an advantageous analytical method applicable for large numbers of samples.
||“New trends in neutron activation analysis in Japan” by Prof. Mitsuru Ebihara of Tokyo Metropolitan University. Although the number of research reactors usable for NAA is decreasing in Japan, several projects to overcome such a difficult situation are undertaken; multi-Ge detector counting system, multi-Ge PGA (MPGA) and neutron beam generated by an accelerator. The current situation around these projects was reported.
Country reports were delivered by participants from individual countries. These are mainly focused on airborne particulate matters (PMs) as was requested. Some reports presented by Vietnamese guests are out of this scope.
|| “Air pollution study in 2003 by using neutron activation analysis” by Prof. Ni Bangfa of China Institute of Atomic Energy. PM samples collected in Beijing are analyzed by k0-NAA method. More than 40 elements are determined. Data were evaluated by using enrichment factors, statistical factor analysis and time series.
||“Environmental pollution studies: Quantitative determination of elements in the air particulate matter by NAA” by Mr. Sutisna of BATAN, Indonesia. Data for the PM samples collected at two sites in 2002 were presented. In addition, some data for SRM including NIST 1632c were reported for QC/QA assessment.
||) “Evaluation of 2002 PM monitoring data” by Tsunehiko Otoshi of Tohoku University of Community Service and Science, Japan. 2002 data for PMs reported by five countries were evaluated from several viewpoints such as seasonal variation and regional variation.
||“Activation analysis of atmospheric particulate collected in Japan in 2003 including analysis of SRM for atmospheric particulates” by Dr. Yasuji Oura of Tokyo Metropolitan University, Japan. Data of PM samples collected at two sites in Japan (Hachioji and Sakata) were presented. In addition, data for SRM samples were also presented for discussing the difference in reproducibility of NAA data between comparison method and ko-method.
||“Study on air monitoring at urban site in Korea”, by Dr. Hyun-Je Cho of KAERI, Korea.
Data for PM sample collected in 2002 were presented and evaluated from many aspects such as locality, seasonality, PM size and so on. Elemental correlations and enrichment factors are also considered to characterize the elemental composition in PM samples.
||“Implementation of ko-standardization method for neutron activation analysis at MINT”, by Dr. Abdul K. B. H. Wood of MINT, Malaysia. Airborne particulate materials collected in 2003 were continuously analyzed and some of their data were presented. Some samples are being reanalyzed for assuring the quality of data. As for the analytical method. the ko-standardization method was introduced in collaboration with the NRI, Dalat, Vietnam. Reasonable agreements of data between ko-derived values and reference values were confirmed for several elements in a reference material, CRM Soil-7.
||“Application of INAA and XRF for characterization of Metro Manila air particulate samples”, by Ms. Flora L. Santos of PNRI, Philippines. Particulate mass data were presented for Poveda (2001-2003) and UST (2001-2002). Simple graphical analysis was used to show difference in coarse and fine contributions to PM10 for the 2 sites. The Cl/Na ratios were also compared for the 2 sites. Analysis of the samples by INAA in addition to XRF demonstrated the benefits of multi-technique approach (XRF and INAA) for analyzing PM samples.
||“INAA of airborne particulate matter collected in Bangkok and Pathumthani, Thailand”, by Dr. Wanna Chueinta of OAP, Thailand. Data of PM samples collected at two sites during Jan. 2003 to Dec. 2003 were presented. In addition of measurement of PM mass and black carbon contents for coarse and fine fractions, 23 elements were determined by INAA with comparative method. Data obtained were extensively analyzed from several viewpoints such as compositional difference by size, enrichment factors, time variations, and so on. By using factor analysis, possible sources for coarse and fine PMs were enstimated. Experimental data on SRMs also were presented.
||“Facility and application of nuclear and supplementary analytical techniques at Dalat Nuclear Research Institute”, by Prof. N. M. Sinh of DNRI, Vietnam. Firstly, an outline of analytical techniques developed in DNRI were introduced, which was followed by somewhat detailed explanation concerning NAA. It was emphasized that NAA was of great benefit to socio-economy in Vietnam.
||“The development of ko-standardization method of NAA on Dalat research reactor”, by Dr. H. M. Dung of DNRI, Vietnam. Following the preceding talk, some developments in NAA were presented, among which the ko-standardization method was focused in the following aspects; creating the computerized nuclear data library, accurately calibrating the irradiation facilities and Ge detectors, putting into operation the software namely ko-Dalat (for gamma-spectrum analysis and ko-assisted concentration calculation) and validating the procesure by analyzing a number of SRMs.
||“Applied research on air pollution and its source apportionment in Ho Chi Minh City using nuclear and nuclear-related analytical techniques and chemometrics”, by Mr. Truong Y., DNRI, Vietnam. Data for PM samples collected in 2001 and 2002 at two sites in Ho Chi Minh City were presented. These data were mostly obtained by INAA while Pb and Ni were determined by polarography. By using factor analysis, possible sources for coarse and fine PMs were estimated.
||“Determination of toxic elements in foodstuffs in Vietnam”, by Ms. L. N. Trinh of DNRI, Vietnam. Large numbers of foodstuffs collected in HCM City and other two industrial cities were analyzed for several toxic elements such as As, Se, Hg, Cr by INAA in addition to RNAA, AAS and ASV. Concentrations seemed to be related with the collecting locality. The concentration level of toxic elements in industrial area were observed to be still lower than maximum permissible concentrations of corresponding elements.
1.3. summary of “round-table” discussions
At the “round-table” discussions, the following subjects were taken up;
(1) The 2002 report
(2) Progress in 2003
(3) Plan for 2004
(5) New project(s) for the next term
Minutes are summarized individually for each of them.
(1) The 2002 report
(2) Progress in 2003
At the last year’s workshop at BATAN, Indonesia, we agreed to prepare the manuscript of chemical compositions of PM samples collected in 2002 and discussed a possible timetable and a practical procedure. According to the agreement, data and accompanying information were sent to Japan by September 1, 2003 (2nd and postponed deadline) from five countries (Japan, Korea, Malaysia, Philippines and Thailand). Based on these data, the manuscript was prepared by Japanese representatives with many efforts and was distributed to other countries by email prior to the workshop. At the workshop at Dalat, it was discussed how to handle the draft at the next stage. After extensive discussion, it was agreed that (i) the manuscript would be submitted to an appropriate journal at the present form, that is, no additional data from other countries would not be incorporated so that any further delay could be avoided, (ii) any correction should be made as soon as possible and no later than January 30, 2004, (iii) data from Indonesia would be incorporated if its incorporation makes any additional delay, (iv) any correspondence should be addressed to the project leader (M. Ebihara) with cc to other Japanese participants, and (v) a final draft would be submitted in February, 2004.
It was admitted that the progress in 2003 was satisfactory in three aspects; (i) our main project of this term (2002-2004) (sampling and analyzing PM samples in each participating countries) has been put into practice without any problem, (ii) the ko-standardization method has been introduced in Malaysia and (iii) two scientific reports in addition to the 2002 report described above will be prepared in due course. As for two additional manuscripts, their possible titles and related discussions are summarized in the following;
|| “Reproducibility of INAA data for 1 mg of two SRM samples (NIST 1632c and NIES no. 8)”(person in charge: Wanna Chueinta)
Size-dependent reproducibility will be discussed by using INAA data for about 1 mg of NIST 1632c and NIES No. 8. If any country likes to join this manuscript, at least ten sets of data obtained by INAA for each SRM have to be sent to Dr. Wanna Chueinta as soon as possible and no later than March 31. Either ko-method or comparison method may be used. Japan is to prepare ten samples (about 1 mg each) for two SRMs and send them to Vietnam as soon as possible (within the week starting 18th).
||“Comparison of XRF and INAA data for airborne particulate matter” (person in charge: Flora L. Santos)
As PM samples collected in Philippines in 2002 were analyzed by XRF as well as INAA, some elements were determined by both methods. This gives us a good opportunity to compare their data. Such a comparison must be informative for peoples using XRF and INAA as analytical tools for many substances such as geological samples, environmental samples and so on. The draft manuscript will be prepared by Ms. Flora Santos by the end of February.
(3) Plan for 2004
As a year of 2004 is the final year for the current term, we are to be continuously working on the presently standing (main) project, that is, collecting and analyzing airborne particulate matter by NAA. At the next workshop, it is required for all participants that data of PM samples collected during the term of 2002-2004 are summarized. Current status for the PM project is summarized below (as of January 16, 2004).
*Number of sampling site. #Sampling frequency. $Quantification method. &Partly done.
||part. done &
Obviously, the PM project seems to have been well conducted so far. Samples collected in 2002 have been completely analyzed. By the next workshop, each country is supposed to complete analyzing all the samples collected in 2003 and some of 2004.
Besides the main project, a sub-project related with QC/QA was discussed in consideration of keeping the quality of our NAA data as high and reliable as possible. After some discussion, the following plan was consented;
||Name of sub-project: QC/QA of INAA data among FNCA countries
||A person in charge: Dr. Abdul Khalik Bin Wood (Malaysia)
||Experimental procedure: A geological standard reference material (in powder) is used. Korea is responsible for preparing and distributing such a sample to participating countries. An aliquant of about 100mg is used for one specimen. In Philippine, XRF is to be conducted so that INAA data can be compared with XRF data. For XRF, 2 g sample is used. At least, six measurements are to be done. A detailed instruction will be prepared by Khalik and be distributed to our group. Data should be sent to Khalik one month prior the next workshop.
There were two points at issue related with ko-method; introducing ko-method in our group countries and inconsistency in data obtained by three different ko-softwares. The former point is our standing issue in our group. Following the discussion held at the last year’s workshop, it was aimed for Malaysia to introduce the ko-method in INAA in 2003 with the help of ko-INAA procedure developed by DNRI and successful results were presented at this workshop. In the meanwhile, it was heard that IAEA was preparing new software for ko-method and would supply the software to any country free of charge. So far, Thailand has not used a ko-method. Considering Thailand as a possible site for the 2004 workshop and an availability of the IAEA ko-software in 2004, it was discussed that Thailand could be the first country to introduce the IAEA ko-software. Depending upon the timing of the issue of the software and the 2004 workshop, it must be sought for us to find the most effective way for introducing the ko-method in Thailand. If the situation permits, a training course will be considered to be held at the occasion of the 2004 workshop with the help of IAEA. A project leader (M. Ebihara) will contact with Dr. M. Rossbach of IAEA for seeking for such a possibility.
The second issue regarding ko-method was raised by Dr. Cho, who compared ko-derived values for several SRMs and showed an apparent discrepancy in analytical values among three sets of data, namely, data obtained by using ko-CIAE, ko-Dalat and ko-KAERI; Ko-Dalat values and ko-CIAE values seem to be systematically higher that ko-KAERI values, with Dalat values being higher than CIAE values. After rather extensive discussion for a cause of such an inconsistency, it was suggested that such a systematic difference could have been due to the difference in handling of gamma-ray data for efficiency calibration and peak search/peak integration. It was agreed that a similar comparison would be conducted among four or five ko-softwares under the well-organized experimental guideline in future, probably in the next term (in 2005 and later).
(5) New project(s) for the next term
Although one more year is allocated to the current project, we have started to discuss new project(s). Before starting the discussion on this matter, we confirmed that this FNCA/NAA workshop was profitable for all participating countries and, therefore, was hoped to be continued after the current term was terminated in 2004. Then, we have discussed new project(s) for the next term starting in 2005. Following a proposal by Vietnam at the 2002 coordinators’ meeting, marine samples were discussed for our next target from several viewpoints. With recognition of their importance for monitoring the marine environment, it was agreed that marine samples could be a main target for the next term. After free and lively discussion, it was unanimously agreed that marine biota could be an appropriate substance. The detailed guideline for the analysis of biological substances will be discussed at the next year’s workshop. Until then, each country is required to consider any aspect which could be incorporated in the guideline. For helping us in having an experience of analyzing marine biological samples, Japan will find an appropriate SRM of marine biota and send its aliquants to all group countries if available.
The 2003 FNCA workshop on the utilization of research reactors for the NAA group was held at Dalat, Vietnam on 12-16, January 2004, with participants from China, Indonesia, Japan, Korea, Malaysia, Philippines, Thailand and Vietnam. The workshop consisted of two meetings; one was allocated for ko method on 12th and another was for main discussion on the remaining days. The ko-related meeting was held at the Nuclear Research Institute and the main meeting was at the Sofitel hotel, Dalat. This reports consists of three parts; a summary of the ko-session, a summary of country reports and a summary of “round-table” discussions.
2. RESEARCH REACTORS
The main objectives are to introduce the current status of research reactor in the participating countries and to determine proposals from the participating countries which are worthy for the new project on “Research Reactor Technology for Effective Utilization”.
2.2 Country Reports
“Status of Research Reactors in China” by Mr. Yuan Luzheng
Current status of research reactors in China was presented. Upgrading and renovations for the aging research reactors made them running safely. The progress of CARR project was described. Status of BNCT program in China was mentioned. Some proposals on research reactor technology for effective utilization were involved.
“Improvement Plan on Utilization of the RSG-GAS Reactor” by Mr. Iman Kuntoro
As a multipurpose reactor, RSG-GAS provides facilities for utilization on material testing, radioisotope production, R&D using neutron irradiation as well as training. The reactor was brought into operation since 1987. Because of fact that national nuclear power program was delayed, so, R&D on material testing associated to nuclear power plant were not carried out. The reactor is operated mainly for serving radioisotopes production, neutron activation analysis, neutron beam experiments and general irradiation for research and development activity. Reactor description, achievements and improvement plan in conduct of operation and its utilization were discussed.
“The Current Status of Research Reactors in JAERI” by Mr. Hisashi Sagawa
There are several research reactors including critical facilities in JAERI. Of these research reactors, JRR-3, JRR-4 and JMTR are utilized widely by a large number of researchers. The recent topics on utilization of JRR-3, JRR-4 and JMTR were presented, and the troubles which occurred in JRR-3 and JMTR recently were also presented.
“Research Reactor Activities in Korea” by Mr. Byung Jin JUN
Two research reactors are in operation, another two are waiting for decontamination & decommissioning, and a feasibility study for a medical isotope production reactor is ongoing. Safe and effective management and the active utilization of the research reactors are important concerns of the Korean Government who funds the major part of the research reactor programs. The Government is promoting research for the non-power application of nuclear technology, for which research reactors have an important role as well as for nuclear power programs. Among the four research reactors, HANARO is the only facility providing a high neutron flux to various national demands. Its utilization and management records show remarkable improvement since its power operation in 1996, and ambitious national plans have been made for a further dissemination of its utilization.
“The Present Status and Future Perpectives of PUSPATI TRIGA REACTOR” by Mr. Adnan Bokhari
The PUSPATI TRIGA Reactor, operated by the Malaysian Institute for Nuclear Technology Research (MINT) in Bangi has recently completed 21 years of successful operation. Since its commissioning in June 1982 to end of 2003, the 1MW pool-type reactor has accumulated more than 20,585 hours of operation, corresponding to cumulative thermal energy release of about 13,714 MW-hours. The reactors is equipped with five major types of experimental facilities, consisting of the central thimble, a rotary specimen rack, two pneumatic transfer systems, four beam ports and a thermalizing column. Presently, most of the operating hours are spent on irradiation of samples for the neutron activation analysis purpose. To enhance Malaysian research and development in reactor related technology, MINT has made a dedicated commitment to strengthen the utilizing and maintaining the reactor to its optimal usage.
“Progress Activity of Thai Research Reactor in 2002” by Mr. Sakda Charoen
Thai Research Reactor-1/Modification1 (TRR-1/M1) is a multipurpose research reactor with normal power of 2 MW. The reactor is a swimming pool type, cooled and moderate with light water, using the LEU-fuel. TRR-1/M1 has been operated and utilized for various applications such as neutron activation analysis, radioisotope production, gem irradiation, neutron radiography and research works. To expand and promote the utilization of research reactor, the new 10 MW Research Reactor will be established in the Ongkarak Nuclear Research Center (ONRC) project and the project will be finished in the near future.
“Current Status of Operation and Utilization of the Dalat Research Reactor” by Dr. Nguyen Nhi DIEN
Outline of NRI and IVV-9, reactor management and the status of reactor utilization are presented.
“Application of Relap5/Mod3.2 Code for the Dalat Nuclear Research Reactor” by Mr. Le Vinh VINH
The safety principle and criteria of Dalat Research Reactor were introduced, and the results of thermal-hydraulics safety analysis using Relap5/Mod3.2 Code were also presented.
“Neutronics Analysis of Dalat Research Reactor” by Mr. Nguyen Kien CUONG
The calculation codes used for neutronics analysis in NRI were introduced, and the results of neutronics analysis using these codes were presented.
2.3 Proposal for new Project from each country
(1) The proposal from Japan
Prior to the proposal from participating countries, Japan delegate showed the aim of new Project. As fundamental technology on Research Reactor, the followings are considered.
- Development of irradiation field suitable to experimental purpose
- Technique to evaluate neutron field with accuracy
- Technique to supply stable neutrons
- Techniques to acquire irradiation data
(2) The proposal from China
Chinese delegate proposed the followings to enhance the experience exchange in extending field of utilization of research reactors.
- Service study on nuclear power plant development
- Techniques to improve the RI production
- Neutron transmutation doping of silicon
- Study on sea water de-salt technology
- Design or thoughts of new type reactor concept
- Experience in safety operation
- Renovation and upgrading measures
- Other utilization, such as cable exposure, gem irradiating, track-etched membrane, anti-bogus mark, etc.
(3) The proposal from Indonesia
Indonesian delegate proposed the followings.
- Development of irradiation facility
- Safety assessment of irradiation facilities and target
- Aging assessment technique
(4) The proposal from Korea
Korean delegate proposed the followings.
- Reactor physics
- Instrumentation and control
- Thermal-hydraulics analysis
(5) The proposal from Malaysia
Malaysian delegate proposed the following.
- Fuel management towards safe reactor operation
(6) The proposal from Thailand
Thai delegate proposed the following.
- Dynamic Neutron Radiography
(7) The proposal from Vietnam
2.4 Discussion and Summary
Vietnamese delegate proposed the followings.
- Study on the upgrading and modernization of the reactor control and instrumentation systems
- Reactor core management including core analyses and measuring techniques
Above proposals were discussed and summarized into three categories after removing the parts of proposals that are not suitable to the new project.
||Assessment of irradiation field (including reactor physics, thermal hydraulics analysis and core management)
||Aging management (including renovation and upgrading measures)
||Experience in safety operation
As the result of discussion, participating countries agreed that above “b&c” would be included in the Country Report as an information exchange. Considering above “a”, the followings were agreed by participating countries.
The title of the new project is “Research Reactor Technology (RRT) for Effective Utilization”.
The topic of the project is “Innovation of Research Reactors as Neutron Sources”.
The followings were determined as activities of “Innovation of Research Reactors as Neutron Sources” to improve basic technologies of research reactors.
- Reactor Physics (Neutronics)
- Thermal Hydraulics analysis
- I&C modification
2.5 Next year plan
In the 2004 Workshop, each country shall report on item “a” and items “b&c” separately, and concrete plan including activity item, schedule, details of activities in each year and so on will be discussed and determined based on the country reports.
3. Round Table Discussion
3.1 Workshop Summary
Under the chair of Dr. Nguyen Nhi Dien, PL of Vietnam, and Mr. T. Kosugi, acting PL of Japan, summary of the workshop of Neutron Activation Analysis and Research Reactors were reported by Professor M. EBIHARA and Mr. H. SAGAWA respectively. All participants of the workshop agreed the summary reports.
3.2 Additional remark at the Round Table Discussion
It was agreed to propose to 5th FNCA Coordinators Meeting that Thailand be the hosting country for the 2004 workshop by agreement of all participants for FNCA 2003 Workshop on Utilization of Research Reactors held in Vietnam.
SUMMARY REPORT OF THE 2003 FNCA WORKSHOP
ON THE UTILIZATION OF RESEARCH REACTORS
Sub-workshop on Tc-99m Generator Production
Expert Meeting of Neutron Scattering Experiment
January 12 –16, 2004
This document presents a summary on the implementation of the 2003 FNCA Workshop on the Utilization of Research Reactors held in Jakarta/Serpong from January 12 to 16, 2004. The workshop discussed two different fields of activities as technetium generator technology (TCG) in the sub-workshop and neutron scattering (NS) experiment in the expert meeting. It was attended by scientists and technical specialists from China, Indonesia, Japan, Korea, Malaysia, the Philippines, Thailand, and Viet Nam. A summary of the discussions, progress reports and future programs of each group are presented below.
1. Sub-Workshop Report of Tc-99m Generator Group
In the 2003 Workshop on Utilization of Research Reactors held in Serpong Indonesia, one delegate from each of China, Korea, Malaysia, the Philippines, Thailand and Viet Nam, four delegates from Japan were hosted by Indonesia to participate and promote the technology of Tc-99m generator using poly zirconium compound (PZC) as an adsorbent for neutron activated (n, γ) Mo-99.
1.1 Evaluation of the experiments conducted by each country
Following the agreement of the workshop held in Indonesia in January 2003, PZC materials have been distributed to participating countries in April, August and October 2003 from Kaken Co. The amount of PZC material sent by Kaken was 15 grams for each laboratory each time. Special distribution was done according to the request from CIAE, China. For these experiments, use of secondary column of alumina and oxidizing agent NaOCl in saline were compulsory to follow the standard protocol issued by FNCA for the elution process.
In the present sub-workshop, the results of the experiments in terms of Mo-99 adsorption, Tc-99m elution and Mo-99 breakthrough were reported and discussed to evaluate the performance of PZC based Tc-99m generator. They are summarized in the Table 1.
The comments from each country for the results are as follows.
Two experiments with different batch of PZC with different technical process showed different quality of 99Mo-PZC generator. The adsorption process (the temperature, intensity and frequency of shaking and the PZC volume in solution etc.) can seriously affect the adsorption efficiency of 99Mo in the solution.
The adsorption efficiency of 99mMo at 90°C for 3 hours is not as high as that before, and the reason of the increase of elution yield along with the elution date in the second experiment should be ulteriorly discussed. The 99mMo-PZC generator system can be put into commercial application after further improvement of the performance of PZC.
Because the PZC is breakable, there is much fine PZC powder after the Mo adsorption process. After removing the fine PZC powder and washing the PZC powder, the rate of remained 99Mo (adsorbed onto PZC powder) is about 70.0%. It is necessary to take measures to reduce the loss of 99Mo adsorbed onto the fine PZC powder and to quicken the 99mTc elution process. Further experiment will be requested.
Coated PZC showed adsorption capacity and 99mTc yield as high as those of PZC with better property of the 99Mo-PZC slurry.
The contents of total Mo, Zr, and Al in 99mTc solution are <0.2 ppm for Mo and <5.0 ppm for Al and Zr. The values are in agreement with the specification of clinically used 99Mo/99mTc generators.
It is concluded that PZC is applicable to a practical 99mTc generator based on natural Mo (n, gamma) 99Mo. The generator assembly is almost same as the ordinary fission type generator. Further trial of using 99Mo as high as 37 GBq (1 Ci) level is to be justified in this stage in order to realize a practical generator.
The performance of PZC distributed in 2003, although molybdate adsorption capacity decreased by 10-20%, seems to be improved in less breakthrough of 99Mo, higher material stability, better elution efficiency, etc. compared to other PZC batches. Especially, the PZC coated with TEOS seems to be suitable as an absorbent for the commercial application of 99Mo/99mTc generator.
Because of renovation of hot facilities in MINT, all PZC samples distributed by Kaken are kept until new facility becomes available. The PZC technology can be adopted if only the production procedure is established because changing the current alumina based column technology to PZC column requires major changing of production equipments and facilities. Issue of evaluations and registration by local drug authority is also necessary. In order to meet the local demand, irradiation service for Mo and shipment to Malaysia is required.
The experiments on PZC showed that the coated PZC gave better elution yield than the previous uncoated batches. The adherence to the standard protocol for preparing the PZC column as 99Mo-99mTc generator is emphasized to obtain the high elution yield and low Mo breakthrough. If the PZC will be exported as column material, a study on the shelf life of the material may be needed.
The coated PZC seemed to be a suitable material for generator preparation owing to its high molybdenum adsorption, high 99mTc elution yield and very low percentage loss of fine powder.
It is strongly believed that in the near future this technology will be established and utilized under the framework of FNCA which will benefit the countries operating small research reactors to overcome the difficulties in production of 99Mo/99mTc generator.
Table 1. Results of experiments conducted by each participating country
The procedures and relevant 99mTc generator designs for the preparation of PZC based 99mTc generators were successfully set up. The columns of from 1.0 gram to 4.0 gram weight of PZC and from 200 mCi to 1000 mCi 99Mo can be used to produce portable, chromatographic type 99mTc generators which have a good performance for application in clinical investigations.
Among the established procedures the column pre-loading procedure was highly evaluated, because it proved to be prominent figures for easy and safe operation, for low cost of technology facilities and equipment and for the capability to match the traditional technology of the fission 99Mo based 99mTc generator production.
*Special participation for inter-laboratory experiment **Not according to the protocol.
|Viet Nam ***
1.2 Demonstration of PZC based 99mTc generator using the loading machine
Demonstration of the remote controlled system for 99Mo-99 loading/PZC column packing was carried
out during the present workshop as planned in the 2002 Workshop in Jakarta/Serpong. It was installed in the hot cell of BATAN in December 2003 under the cooperation with Kaken and BATAN
The system itself worked as intended but the adsorption ratio was very low. The results of the experiments are summarized in Table 2. Two columns were subjected to be loaded for the experiment. The results for the first column showed very low Mo adsorption ratio which might be due to insufficient reaction with the PZC material or failure in transfer of the PZC slurry. For the second column, the adsorption ratio was higher than the first but still not enough. Further elution of 99mTc was not possible. In this case gel phase PZC with many fine particles of the PZC might have blocked the pass of solution.
The elution rate for 99mTc, however, was fairly good as more than 80% and breakthrough of 99Mo in eluate of 99mTc was low enough to meet the criteria of medical application.
Table 2. Results of demonstration experiment of the loading system
* Oxidizing agent (NaOCl) is used in the elution step.
||99m Tc elution*
** Secondary column (alumina) is applied.
1.3 Work plan for 2004
1.3.1Cause finding and improve of loading system
BATAN investigates (1) the cause of improper processing of reaction of PZC with 99Mo solution and (2) transfer process problems, that can be useful for improvement. Reports of findings and results of improvement are to be sent to the project leader of Japan to distribute to all participants.
1.3.2 Establish a high quality PZC synthesis procedure
Kaken Co. establishes strict quality control system for synthesizing PZC
1.3.3 Labeling test
Confirmation of quality of 99mTc solution obtained from PZC generator through labeling test with various radiopharmaceutical kits.
1.3.4 Distribution of PZC material
Kaken Co. distributes PZC materials to participating laboratories 3 times within fiscal year 2004 for the labeling test and other experiments related to PZC type 99mTc generator development.
1.3.5 Expert exchange for loading system development
Experts visit and stay to collaborate in further improvement of loading system installed in BATAN to share experiences of how to operate the machine. Travel and accommodation cost is, in principle, to be born by the institution of the expert.
1.3.6 Clinical trial in hospitals
BATAN conducts the clinical trials of PZC based 99mTc labeled kits under cooperation with several hospitals in Jakarta and Bandung.
1.3.7 Pre-loading system test
BATAN and other interested laboratories test the pre-loading system developed by Viet Nam using high radioactive 99Mo.
1.3.8 Publish comprehensive report
Table 3. Work plan for 2004
Publish the comprehensive report on PZC type 99mTc generator technology containing historical details, comparison of different types of generators, synthesis of PZC material, assembly of generator, column loading systems and reference articles etc.
1.4 Work plan for 2004
The work plans for 2004 is summarized in Table 3.
|1) Cause finding and improve of loading system
2) Establish quality PZC synthesis
3) Labeling test for RF kits
4) Distribution of PZC material
5) Expert exchange for loading system development
6) Clinical trial in hospitals
7) Pre-loading system test with high radioactivity Mo-99
8) Publish comprehensive report
3 times per year, Japan
Stay/Visit to BATAN/Kaken
Indonesia and others
1.5 Comments and suggestions
||BATAN can provide the neutron irradiated natural Mo of high radioactivity with free of charge except the cost of transportation and container.
||NRI, Dalat will demonstrate a column pre-loading procedure for the preparation of PZC based 99mTc chromatographic generator in the forthcoming next workshop.
||It is hoped that FNCA sends a letter for each government to appeal the importance of setup of the automatic loading system in order to spread high quality PZC based 99mTc generators.
||As a special session after the opening ceremony, HE Mr. Hatta Radjasa, the State Minister of Research and Technology of Indonesia gave a speech and a testimonial letter to the President of Kaken Co. for his contribution to the 99mTc generator project.
||As the invited talks, the current status of production of fission 99Mo and 99mTc generator in
Indonesia was presented by BATAN Teknologi and a comparative study on the labeling of 99mTc kits using fission type generator and PZC type generator was presented by BATAN. And also the application of PZC to 188W/188Re generator was presented by JAERI.
||The FNCA coordinator of Japan made a key note speech on “Radiation and Isotope Application for Improving Everyday Life” and. the “Proposal of Future Program for Dissemination of (n, gamma) PZC-99mTc Generator” was presented by the President of Kaken Co.
2. Expert Meeting of Neutron Scattering Experiment
2.1 Project Title
Development of Evaluation Technology of Natural and Synthetic Polymer Materials (mainly NR-TPE) using Small Angle Neutron Scattering (SANS)
China, Indonesia, Japan, Malaysia, Philippines, Thailand, Vietnam
The neutron scattering project was initially proposed and adopted at the 5th Workshop of the Utilization of Research Reactors held in 1995. The calibration of SANS instrument in the stage 1 of the project and the establishment of data analysis technique using the standard polymer samples in the stage 2 were followed by the current stage 3, conduct of research and development of the natural polymers using SANS, which was accepted by the coordinators meeting held in March, 2002.
The property of polymers such as natural rubber thermoplastic elastomer (NR-TPE) and natural carrageenan (NC) produced dominantly in the member countries depends on their macroscopic and microscopic structures. Using the unique method of SANS, polymer scientists and neutron scientists cooperatively explore the relationship between the property and the nano-scaled structures of the natural polymers. The information of the relationship should become a powerful guide for the industrial application of the natural polymers. Therefore, the activities of the neutron scattering project will contribute to the socio-economic development in the member countries.
2.3 Current activities
2.3.1. Natural rubber thermoplastic elastomer
Thailand reported the strengthening linkage between the OAP, MTEC and Mahidol University to carry out the SANS experiments of the natural rubber/polyethylene blends (NR/PE). The mechanical properties of the blends were measured. Twenty-one samples were provided to professor Hasegawa in Kyoto University for the SANS-J experiments at JRR-3M. The experimental results revealed the contrast between NR/PE and carbon black, that leads to see the interface structure of these blends.
Mr. Jipawat Chamchang visited Dr. S. Koizumi of JAERI to study the structural properties of poly-trimethylene terephthalate (PTT) and poly-ethylene naphthalene (PEN) blends by SANS-J.
Vietnam reported that the research on radiation vulcanization of natural rubber latex and preparation of copolymers by grafting monomers onto natural rubber latex and/or onto other synthetic polymers have been started since 1990. In the FNCA project natural rubber thermo-plastic elastomer (NR-TPE) and copolymers have been prepared mainly by radiation cross-linking and grafting methods. The resulting products were characterized by SANS, SAXS, TEM, and thermo-mechanical and physio-mechanical measurements. The physio-mechanical properties of NR-PTE have been improved, and the thermal stability and salinity of the PVA-graft-AAM have been improved dramatically as a result of copolymer formation.
From Indonesia, Mr. Utama reported the trial production of low protein irradiated natural rubber latex in factory scale by gamma and electron beam irradiation technique. Dr. Suratno reported the effect of ultra violet light, temperature, moisture on automotive rubber bushing. Mr. Syamsu reported the development and prospects of modified natural rubber product. These reports drew strong attention of participants to the linking between the cross-linked polymer particles and the possible application of the SANS technique to observe the linkage. Dr. Ikram reported that the SANS profiles of five NR/PE samples from Thailand were obtained by using BATAN SANS instrument. The sample-to-detector distance employed was 1.5 and 10 m with the neutron wavelength of 0.4 nm. The results were comparable to the SANS data obtained with SANS-J at JAERI, Tokai, Japan. The control computer of the SANS went wrong in the middle of the measurements. He also reported that the SANS at RSG-GAS will be operated in February or March, 2004 after the repair works on the computer system and will welcome natural polymers to be investigated in the project.
Malaysia reported the effects of molecular weight of LNR, as a compatibilizer on NR/LLDPE(Linear Low Density Polyethylene) blend. Rheological studies and mechanical properties of the blend showed that the molecular weight of LNR influences the compatibility of the blend. Improvements in the mechanical properties were in agreement with the increase in gel contents of the blend. From the DSC(Differential Scanning Calorimeter) study, it has been observed that increasing LNR content decreases the melting point, Tm, and the heat of fusion, DHf, which are indicators of the crystalline part of the blend. The decrease reflects a reduction in the degree of crystallinity which is due to the interference in the form of LNR dissolution into the LLDPE phase. SEM examination further confirmed the improved compatibility of NR/LLDPE blend by LNR addition.
Professor Hasegawa reported his SANS and SAXS experiments on the provided samples from Thailand, Vietnam and Indonesia. They studied the phase-separated structures of natural rubber thermoplastic elastomers (NR-TPE) which are recyclable materials without vulcanization and consume less energy for processing than vulcanized rubbers. Therefore, NR-TPE’s are friendly to the environment and their production is expected to increase in the future. However, their structure-property relationships are not clarified yet. The main problem is that the techniques for quantitative evaluation of their structures are not established. In this study, they could show that SANS was an extremely useful technique to evaluate the thickness of the interfaces between coexisting two phases, which was strongly related to the mechanical properties of NR-TPE.
Philippines reported that the research proposal on carrageenan was accepted to be conducted in collaboration with the Prof. M. Shibayama of ISSP-Tokyo University on the basis of the economic importance and support of the Philippine government. Two studies were proposed by the Philippines, that are structural investigation of -ray irradiated -carrageenan (KC) and structural investigation of -carrageenan/PVP blend cross linked by -irradiation.
Professor Shibayama reported that the structure and dynamics of -ray irradiated -carrageenan (KC) aqueous solutions were investigated by dynamic light scattering (DLS) and SANS as a function of irradiation dose and temperature. The DLS data showed that the intensity correlation function (ICF) shifted towards shorter relaxation times with increasing radiation dose as a result of radiolysis. The characteristic decay time distribution function (CDF), G(), indicates the presence of fast and slow mode peaks respectively at around 0.1 to 10 ms and 100 to 1000 ms. A peak broadening of the fast mode peak in G() appeared with decreasing temperature, indicating that coil-to-helical conformation transition took place. The conformation transition temperature (CTT) decreased with increasing radiation dose. No transition was observed for KC irradiated at 300 kGy. A new faster relaxation mode appeared at around 0.1 to 1 ms at temperatures below the CTT. This peak is found in KC irradiated at doses exclusively between 75 to 175 kGy. The peak height of this mode is largest at 100 kGy which corresponds to the optimum biological activity of KC reported previously. The SANS intensity from KC in deuterated water increased dramatically by gelation, indicating that conformational rearrangement, e.g., helix formation accompanying aggregation, underwent by gelation. However, no noticeable irradiation-dose dependence was observed.
2.4 Upgrade of neutron facility
China reported that the China Advanced Research Reactor (CARR) now is being built at CIAE to meet the increasing demand of neutron scattering research in China. CARR is a tank-in-pool inverse neutron trap type research reactor with nuclear power of 60 MW, and the unperturbed thermal neutron flux is 8x1014 n/cm2s. Seven out of nine tangential beam tubes are designed for neutron scattering researches. A liquid hydrogen cold source at 20 K will be installed, and 4 cold neutron guides will be used for transportation of the cold neutron beams to the guide hall. The objective of neutron scattering program on CARR is establishment of a complete set of spectrometers as the tool for neutron scattering research in the fields of life sciences, material sciences, physics, chemistry and chemical engineering, minerals, environment sciences, industrial and engineering applications et al. Therefore FNCA cooperation will also be welcome to CARR.
Dr. Morii of JAERI reported that an upgrade plan of JRR-3M was made and will be published in February 2004 by the task force under the neutron beam utilization committee held for the last two years. Upgrade of the cold source and the installation of supermirror neutron guide are strongly recommended. He also reported the capability of the Japanese spallation neutron source, JSNS, at the Japan intense Proton Accelerator research Complex (J-PARC) which will be completed in 2007. Effective intensity of the JSNS will be nearly 100 times higher than that of JRR-3M in some research area, while time averaged cold neutron intensity will be only 3-5 times high. FNCA members may be carried out as one of the instrument users and/or owners at the J-PARC in future.
Dr. Mohamed of MINT reported the recent progress of the MySANS, ‘mini’ SANS facility, and its present applications in materials science and technology research and education. The formation of Reactor Interest Group (RIG) has lead to several experimental projects with collaborative work between MINT and the local universities/research institutes.
2.5 Future program
We strongly propose the continuous research on natural polymer such as natural rubber (NR)-TPE and carrageenan in 2004 and the following years, since we have just got the first experimental results of the structure of the polymers which show that SANS is useful to understand the macroscopic properties of the polymers. We propose to have FNCA workshop 2004 to summarize the current researches and to seek future researches. The mailing list will be continuously updated to strengthen the linkage between neutron facility and the polymer researchers as end-users for the socio-economic development in the member countries.
To carry out the experiments efficiently in future, deuterated monomers need to be provided, and the exchange of the researchers between the member countries is necessary.
2.5.1. Natural rubber thermoplastic elastomer
Through the FNCA project natural rubber thermoplastic elastomer (NR-TPE) samples were provided by Thailand and Vietnam. It was proved that small-angle neutron scattering (SANS) was an excellent technique to evaluate the interfacial thicknesses of the phase-separated structures that tremendously affect the mechanical properties of not only NR-TPE but also polymer blends in general. Indonesia proved that their SANS (BATAN) was useful to measure the interfacial thicknesses of NR-TPE by showing that the obtained data on Thai samples were comparable to those measured by SANS-J (JAERI). These are good news for the participating countries and the contribution of Indonesia to the NR-TPE project through the SANS experiments of NR-TPE in BATAN is expected to increase.
(1) Proposal by Malaysia
As the third largest NR producer, diversification of NR utilization is prime activity to produce new NR-based products. NR-TPE polymer blend is a good candidate for this initiative; Polymer blend is one of the fastest growing areas of polymer technology. Blend compatibility is an important issue to be addressed in relation to industrial uses of polymer blend materials. Good physical and mechanical properties are influenced by good compatibility of the blend component materials.
LNR has been recognized as one of the compatibilizer that gives better NR-TPE polymer blend systems. Its molecular conditions and properties are influencial to this compatibility. The study of these parameters at molecular level is therefore essential. SANS has proven to be a good method to study the structure in relation to the understanding of the compatibility process. This will finally assist the good fabrication procedure of the final products of polymer blend.
We propose two projects as follows:
1. Compatibilization study of NR-TPE blend: the role of LNR.
2. Development of new compatibilizer for NR-TPE blend based on NR
In the fiscal year 2004, Malaysia will provide new samples of NR-TPE with compatibilizer for the interfacial thickness measurements by SANS. The success of this experiment will benefit the NR-TPE industries of the participating countries by providing an irreplaceable evaluation method of compatibilizer efficiency.
(2) Proposal by Indonesia
Indonesia will prepare deuterized latex and observe its particle size using BATAN-SANS machine. Study on deproteinized natural rubber will be carried out as well if necessary to suit the q range that observable by BATAN-SANS machine. Interfacial thickness is another parameter that could be also derived from SANS data measurements. In order to push the SANS-Polymer Program further, one young scientist will be sent to Japan under the financial scheme from outside source, such as Scientific Exchange Program of MEXT. It is required that the young scientist has adequate basic knowledge both in SANS and polymer fields.
(3) Proposal by Thailand
Thailand would like to propose two topics as follows.
1) NR/PE Sample:
Thailand would like to prepare the NR/PE sample with reinforcing agent such as silica for studying the structure and morphology, especially on interfacial thickness by using SANS. This NP/PE with reinforcing agent (silica) is used in the automobile part. If we understand the structure, we can produce a good NR/PE for the purpose.
2) Human Resource Development
Because most of the SANS facility existed only in few places such as JAERI, BATAN and etc., we need to send young scientist to the facilities to get practice in using and analyzing the sample that we prepared.
FNCA could conduct the 1-2 week workshop on experiment and analysis of NR/PE sample that provides the opportunity to the young scientists and engineers of the member countries as well as polymer scientists to be involved in this workshop.
(4) Proposal by Vietnam
1. Preparation of NR-TPE by radiation grafting method.
–NR-graft-PMMA blending with fillers such as clay/or wood powder
–NR-graft- polystyrene (PS) blending with fillers as clay/or wood powder.
The samples will be prepared with different grafting degrees.
2. Preparation of copolymers by radiation-grafting methods based on polyvinyl alcohol (PVA).
-PVA-graft-PAAM with different molecular weights of PVA and grafting degrees.
-PVA-graft-PAAM blending with natural polysaccharides (CM-chitin/chitosan)
3. Evaluation of the ability of application of researched product in industry.
(1) Proposal by Philippine
In the study it is necessary to identify the best sample that could give the desired information and to prepare the needed samples such as
||Continuation of the SANS experiment of -irradiated -carrageenan that had been started in 2003. This will enable us to complete the preliminary experiments.
|| SANS study of the KC-PVP hydrogel
The objective is to gain information on the network produced after gamma irradiation, with the end goal of explaining the very large absorptive capacity of the hydrogel for water
|| gel samples of the desired formulation,
|| gamma-irradiated gel sample at the optimum dose,
|| irradiated hydrogel that had been allowed to absorbed the maximum water,
|| sample wherein all the free carrageenan, pvp and unbound water have been removed
Quantitative SANS studies on 0 - 300 kGy irradiated KCs in D2O at 60 and 25 °C is planned by professor Shibayama and Ms. Abad to explore the structural origin of the unique biological functions in April, 2004.
2.5.3 Neutron scattering facility and relationship between FNCA countries
(1) Proposal by China
China will continuously participate and support FNCA program, especially on natural polymer application study by SANS. Meanwhile, China will propose and join a SANS on the job training program for young scientists in this field through various channels, and the major purposes is to master SANS technique on natural polymer studies. In the following few years, CIAE might not contribute to either SANS beam time or suitable sample for natural polymer study, since China is concentrating on building the 60 MW CARR. After CARR becomes critical, instruments at CARR will welcome FNCA members. At this moment, China hopes to contribute in earlier stage and also to get support from FNCA, since CARR is expected to be built as an regional and international facility in Asian area. Chinese neutron scattering scientists will keep on working with polymer and SANS scientists in the FNCA member countries on natural polymer investigations by SANS, especially on experiment processing, data reduction and analysis.
(2) Proposal by Japan
Japan will collaborate with the FNCA member countries for the study of the natural polymers planned in 2004. The planned SANS experiments will be carried out at SANS-J and SANS-U, although allowed neutron beam time will be limited under the highly competitive circumstances in Japan. Japan will ask Korea and Australia whether SANS at HANARO of KAERI and HIFAR of ANSTO are available for the FNCA project in accordance with their installation of a cold source at HANARO and the construction of RRR at ANSTO for the polymer science and other sciences in their countries.
JAERI will continuously pursue the study on the structure of synthetic polymers with Japanese companies using SANS-J for the socio-economic development in Japan.