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Journal Articles

Estimated isotopic compositions of Yb in enriched $$^{176}$$Yb for producing $$^{177}$$Lu with high radionuclide purity by $$^{176}$$Yb($$d,x$$)$$^{177}$$Lu

Nagai, Yasuki*; Kawabata, Masako*; Hashimoto, Shintaro; Tsukada, Kazuaki; Hashimoto, Kazuyuki*; Motoishi, Shoji*; Saeki, Hideya*; Motomura, Arata*; Minato, Futoshi; Ito, Masatoshi*

Journal of the Physical Society of Japan, 91(4), p.044201_1 - 044201_10, 2022/04

https://doi.org/10.7566/JPSJ.91.044201
 Times Cited Count：4 Percentile：47.58(Physics, Multidisciplinary)

Recently, $$^{177}$$Lu is considered as one of the most important medical RIs for treating neuroendocrine tumors. A plan to produce $$^{177}$$Lu with high purity by using enriched $$^{176}$$Yb samples with irradiation of deuteron beams in accelerators has been discussed. However, since the other Yb isotopes contained in the Yb sample interacts with deuterons, Lu isotopes other than $$^{177}$$Lu are produced as impurities. Since the purity of $$^{177}$$Lu is important for medical use, a method to evaluate the impurity of Lu has been required. In this study, we proposed a new method to estimate production yields of each Lu isotopes in Yb samples with arbitrary isotopic compositions by using excitation functions of Yb($$d,x$$)Lu reactions and the particle transport calculation code PHITS. The method plays an important role in discussing the isotopic composition of enriched samples to produce high-purity $$^{177}$$Lu using accelerators.

Journal Articles

Large scale production of $$^{64}$$Cu and $$^{67}$$Cu via the $$^{64}$$Zn(n, p)$$^{64}$$Cu and $$^{68}$$Zn(n, np/d)$$^{67}$$Cu reactions using accelerator neutrons

Kawabata, Masako*; Motoishi, Shoji*; Ota, Akio*; Motomura, Arata*; Saeki, Hideya*; Tsukada, Kazuaki; Hashimoto, Shintaro; Iwamoto, Nobuyuki; Nagai, Yasuki*; Hashimoto, Kazuyuki*

Journal of Radioanalytical and Nuclear Chemistry, 330(3), p.913 - 922, 2021/12

https://doi.org/10.1007/s10967-021-07987-3
 Times Cited Count：8 Percentile：67.14(Chemistry, Analytical)

Both $$^{64}$$Cu and $$^{67}$$Cu are promising radionuclides in nuclear medicine. Production yields of these radionuclides were quantified by irradiating 55.4 g of natural zinc with accelerator neutrons. Clinically suitable $$^{64}$$Cu and $$^{67}$$Cu yields were estimated by experimental based numerical simulations using 100 g of enriched $$^{64}$$Zn and $$^{68}$$Zn, respectively, and elevated neutron fluxes from 40 MeV, 2 mA deuterons. A combined thermal- and resin-separation method was developed to isolate $$^{64}$$Cu and $$^{67}$$Cu from zinc, resulting in 73% separation efficiency and 97% zinc recovery. Such methods can provide large scale production of $$^{64}$$Cu and $$^{67}$$Cu for clinical applications.

Journal Articles

Anomalous radioisotope production for $$^{68}$$ZnO using polyethylene by accelerator neutrons

Tsukada, Kazuaki; Nagai, Yasuki*; Hashimoto, Shintaro; Minato, Futoshi; Kawabata, Masako*; Hatsukawa, Yuichi*; Hashimoto, Kazuyuki*; Watanabe, Satoshi*; Saeki, Hideya*; Motoishi, Shoji*

Journal of the Physical Society of Japan, 89(3), p.034201_1 - 034201_7, 2020/03

https://doi.org/10.7566/JPSJ.89.034201
 Times Cited Count：2 Percentile：17.95(Physics, Multidisciplinary)

We found anomalously large yields of $$^{67}$$Ga, $$^{66}$$Ga, $$^{rm 69m}$$Zn and $$^{64}$$Cu by neutron irradiation on a $$^{68}$$ZnO sample in a polyethylene shield. Neutron beams are generated from the $$^{9}$$Be($$d,n$$) reaction for 50 MeV deuterons. The yields obtained were more than 20 times larger than those in the unshielded sample. On the other hand, the yields of $$^{67}$$Ga, $$^{66}$$Ga, $$^{rm 69m}$$Zn and $$^{64}$$Cu from a metallic $$^{68}$$Zn sample and the yields of $$^{67}$$Cu, $$^{65}$$Ni and $$^{65}$$Zn from the $$^{68}$$ZnO and $$^{68}$$Zn samples were almost insensitive to the shield conditions. This finding would provide us a unique capability of accelerator neutrons to simultaneously produce a large amount of several radioisotopes, including proton induced reaction products, by using a single sample. The experimental data were compared with the yields estimated by using the Particle and Heavy Ion Transport code System and the result was discussed.

Journal Articles

$$^{99}$$Mo yield using large sample mass of MoO$$_{3}$$ for sustainable production of $$^{99}$$Mo

Tsukada, Kazuaki; Nagai, Yasuki*; Hashimoto, Kazuyuki*; Kawabata, Masako*; Minato, Futoshi; Saeki, Hideya*; Motoishi, Shoji*; Ito, Masatoshi*

Journal of the Physical Society of Japan, 87(4), p.043201_1 - 043201_5, 2018/04

https://doi.org/10.7566/JPSJ.87.043201
 Times Cited Count：10 Percentile：56.34(Physics, Multidisciplinary)

Journal Articles

Measurement and estimation of the $$^{99}$$Mo production yield by $$^{100}$$Mo($$n,2n$$)$$^{99}$$Mo

Minato, Futoshi; Tsukada, Kazuaki; Sato, Nozomi*; Watanabe, Satoshi*; Saeki, Hideya*; Kawabata, Masako*; Hashimoto, Shintaro; Nagai, Yasuki*

Journal of the Physical Society of Japan, 86(11), p.114803_1 - 114803_6, 2017/11

https://doi.org/10.7566/JPSJ.86.114803
 Times Cited Count：11 Percentile：58.95(Physics, Multidisciplinary)

We have measured the yield of $$^{99}$$Mo, the mother nuclide of $$^{99m}$$Tc used in nuclear diagnostic procedure. $$^{99}$$Mo was produced by $$^{100}$$Mo($$n$$,$$2n$$)$$^{99}$$Mo using neutrons with thermal energy up to about 40 MeV, provided by C($$d$$,$$n$$). The $$^{99}$$Mo yield agrees with an estimated yield with the use of the latest data of C($$d$$,$$n$$) and the evaluated cross section given in the JENDL. Based on this, a new calculation was carried out to produce $$^{99}$$Mo to seek for a good economical condition. Various conditions such as the $$^{100}$$MoO$$_{3}$$ sample mass, the distance between the carbon target and the sample, the radius of the deuteron beam, and the neutron irradiation time were considered. The calculated $$^{99}$$Mo yield indicates that about 30% of the $$^{99}$$Mo demand in Japan can be fulfilled with a single accelerator. The elusion of $$^{99m}$$Tc from the $$^{99}$$Mo twice per day would meet about 50% of the $$^{99}$$Mo demand.

Journal Articles

Application of $$^{67}$$Cu produced by $$^{68}$$Zn($$n,n'p+d$$)$$^{67}$$Cu to biodistribution study in tumor-bearing mice

Sugo, Yumi*; Hashimoto, Kazuyuki*; Kawabata, Masako*; Saeki, Hideya*; Sato, Shunichi*; Tsukada, Kazuaki; Nagai, Yasuki*

Journal of the Physical Society of Japan, 86(2), p.023201_1 - 023201_3, 2017/02

https://doi.org/10.7566/JPSJ.86.023201
 Times Cited Count：15 Percentile：66.59(Physics, Multidisciplinary)

$$^{67}$$Cu produced by the $$^{68}$$Zn($$n,n'p+d$$)$$^{67}$$Cu reaction was used for the first time to determine the biodistribution of $$^{67}$$CuCl$$_{2}$$ in colorectal tumor-bearing mice. High uptake of $$^{67}$$Cu was observed in the tumor as well as in the liver and kidney which are the major organs for copper metabolism. The result showing $$^{67}$$Cu accumulation in the tumor suggests that $$^{67}$$CuCl$$_{2}$$ can be a potential radionuclide agent for cancer radiotherapy. It would also encourage further studies on the therapeutic effect in small animals using an increased dose of $$^{67}$$Cu produced by the $$^{68}$$Zn($$n,n'p+d$$)$$^{67}$$Cu reaction using intense neutrons available at present.

Journal Articles

SPECT imaging of mice with $$^{99m}$$Tc-radiopharmaceuticals obtained from $$^{99}$$Mo produced by $$^{100}$$Mo(n,2n)$$^{99}$$Mo and fission of $$^{235}$$U

Hashimoto, Kazuyuki; Nagai, Yasuki; Kawabata, Masako; Sato, Nozomi*; Hatsukawa, Yuichi; Saeki, Hideya; Motoishi, Shoji*; Ota, Masayuki; Konno, Chikara; Ochiai, Kentaro; et al.

Journal of the Physical Society of Japan, 84(4), p.043202_1 - 043202_4, 2015/04

https://doi.org/10.7566/JPSJ.84.043202
 Times Cited Count：8 Percentile：50.90(Physics, Multidisciplinary)

Journal Articles

New phenomenon observed in thermal release of $$^{99m}$$Tc from molten $$^{100}$$MoO$$_{3}$$

Kawabata, Masako; Nagai, Yasuki; Hashimoto, Kazuyuki; Saeki, Hideya; Motoishi, Shoji*; Sato, Nozomi*; Ota, Akio*; Shiina, Takayuki*; Kawauchi, Yukimasa*

Journal of the Physical Society of Japan, 84(2), p.023201_1 - 023201_4, 2015/02

https://doi.org/10.7566/JPSJ.84.023201
 Times Cited Count：6 Percentile：43.32(Physics, Multidisciplinary)

$$^{99m}$$Tc for medical use can be separated by thermochromatography from a molten $$^{99}$$MoO$$_{3}$$ sample. Effect of moist oxygen gas on the $$^{99m}$$Tc release from molten $$^{99}$$MoO$$_{3}$$ samples was investigated using a $$^{99}$$Mo/$$^{99m}$$Tc generator. $$^{99}$$Mo was produced with $$^{100}$$Mo(n,2n)$$^{99}$$Mo. A new phenomenon has been observed: release rate, separation- and recovery-efficiencies of $$^{99m}$$Tc were higher in the moist oxygen gas than those in the dry oxygen gas. The present result is a significant progress towards the stable production of a high quality $$^{99m}$$Tc from a molten MoO$$_{3}$$ sample with high separation efficiency. The result would also give us a new insight into the interaction between the moist oxygen gas and the molten MoO$$_{3}$$.

Journal Articles

First measurement of the radionuclide purity of the therapeutic isotope $$^{67}$$Cu produced by $$^{68}$$Z($$n$$,$$x$$) reaction using $$^{rm nat}$$C($$d$$,$$n$$) neutrons

Sato, Nozomi; Tsukada, Kazuaki; Watanabe, Satoshi; Ishioka, Noriko; Kawabata, Masako; Saeki, Hideya; Nagai, Yasuki; Kin, Tadahiro*; Minato, Futoshi; Iwamoto, Nobuyuki; et al.

Journal of the Physical Society of Japan, 83(7), p.073201_1 - 073201_4, 2014/07

https://doi.org/10.7566/JPSJ.83.073201
 Times Cited Count：13 Percentile：62.40(Physics, Multidisciplinary)

We have for the first time demonstrated that the therapeutic nuclide of $$^{67}$$Cu produced by $$^{68}$$Zn($$n$$,$$x$$)$$^{67}$$Cu has highest radionuclide purity compared to previous ones. We measured a $$gamma$$-ray spectrum of the reaction product produced by bombarding an enriched $$^{68}$$Zn sample with neutrons with a HPGe detector. The neutrons were obtained by $$^{rm nat}$$C($$d$$,$$n$$) using 41 MeV deuterons provided from Takasaki Ion Accelerators for Advanced Radiation Application of Japan Atomic Energy Agency. Relative production yields of impurity radionuclides such as $$^{65}$$Zn to $$^{67}$$Cu are extremely low, which allow us to chemically separate $$^{67}$$Cu from an irradiated $$^{68}$$Zn sample with a few steps and to reuse high cost an enriched $$^{68}$$Zn sample. The present result strongly suggest that the $$^{68}$$Zn($$n$$,$$x$$)$$^{67}$$Cu reaction is the most promising route to produce high quality $$^{67}$$Cu and could solve a longstanding problem of establishing an appropriate production method of $$^{67}$$Cu.

Journal Articles

High thermo-separation efficiency of $$^{99m}$$Tc from molten $$^{100}$$MoO$$_{3}$$ samples by repeated milking tests

Nagai, Yasuki; Kawabata, Masako; Sato, Nozomi; Hashimoto, Kazuyuki; Saeki, Hideya; Motoishi, Shoji*

Journal of the Physical Society of Japan, 83(8), p.083201_1 - 083201_4, 2014/07

https://doi.org/10.7566/JPSJ.83.083201
 Times Cited Count：11 Percentile：58.43(Physics, Multidisciplinary)

Journal Articles

Generation of radioisotopes with accelerator neutrons by deuterons

Nagai, Yasuki; Hashimoto, Kazuyuki; Hatsukawa, Yuichi; Saeki, Hideya; Motoishi, Shoji; Sonoda, Nozomi; Kawabata, Masako; Harada, Hideo; Kin, Tadahiro*; Tsukada, Kazuaki; et al.

Journal of the Physical Society of Japan, 82(6), p.064201_1 - 064201_7, 2013/06

https://doi.org/10.7566/JPSJ.82.064201
 Times Cited Count：46 Percentile：85.28(Physics, Multidisciplinary)

JAEA Reports

Measurement of tritium activity in the aluminum pipe of JRR-2 heavy water primary cooling system using imaging plate

Motoishi, Shoji; Kobayashi, Katsutoshi; Saeki, Hideya*

JAERI-Tech 2000-070, 34 Pages, 2000/12

JAERI-Tech-2000-070.pdf:5.19MB

no abstracts in English

Oral presentation

Medical use radioisotope production with accelerator neutrons by deuterons

Tsukada, Kazuaki; Watanabe, Satoshi*; Ishioka, Noriko*; Hatsukawa, Yuichi*; Hashimoto, Kazuyuki*; Sugo, Yumi*; Sato, Nozomi*; Kin, Tadahiro*; Kawabata, Masako*; Saeki, Hideya*; et al.

no journal, , 

A new system has been proposed for the generation of radioisotopes with accelerator neutrons by deuterons, especially the production of Mo-99, Y-90, Cu-67, and Cu-64. Enriched Mo-100, Zr-90, Zn-68 and Zn-64 oxide samples were irradiated with neutrons, which were obtained by the $$^{nat}$$C(d,n) and Be(d,n) using 12 - 50 MeV deuterons provided from the TIARA cyclotron and the JAEA tandem accelerator. Mo-99, Y-90, Cu-67, and Cu-64 were successfully produced via the (n, x) reactions, and we clearly observed the $$gamma$$-rays. The present results demonstrate that the radioisotopes, Mo-99, Y-90, Cu-67, and Cu-64, can be produced by using fast neutrons, and strongly suggest that the reaction system is one of the most promising routes to produce high quality medical radioisotope.

Oral presentation

Medical radioisotope production with accelerator neutrons by 50 MeV deuterons

Tsukada, Kazuaki; Hashimoto, Kazuyuki*; Hatsukawa, Yuichi*; Kawabata, Masako*; Saeki, Hideya*; Minato, Futoshi; Iwamoto, Nobuyuki; Nagai, Yasuki*; Sugo, Yumi*; Watanabe, Satoshi*; et al.

no journal, , 

no abstracts in English

Oral presentation

Development of an apparatus to concentrate $$^{188}$$Re solutions by a multi column system for cancer therapeutic experiments

Hashimoto, Kazuyuki; Motoishi, Shoji*; Saeki, Hideya*; Sorita, Takami; Matsuoka, Hiromitsu

no journal, , 

Rhenium-188 is a useful generator-produced radioisotope for therapeutic applications because of their energetic beta particles and $$gamma$$ rays suitable for imaging. Because the $$^{188}$$W parent is obtained in a relatively low specific activity from the irradiation of enriched $$^{186}$$W in a reactor, relatively large volumes of normal saline are required to elute the $$^{188}$$Re from alumina based $$^{188}$$W/$$^{188}$$Re generators. In this study, a simple apparatus for effective concentrations of 188Re solutions from alumina-based $$^{188}$$W/$$^{188}$$Re generators was developed by a tandem cation-anion column system. Concentration ratios greater than 50:1 can be achieved with this apparatus.

Oral presentation

High quality $$^{99m}$$Tc obtained from $$^{99}$$Mo produced by $$^{100}$$Mo(n,2n) using accelerator neutrons

Nagai, Yasuki; Kawabata, Masako; Sato, Nozomi*; Hashimoto, Kazuyuki; Saeki, Hideya; Motoishi, Shoji*; Hatsukawa, Yuichi; Ota, Akio; Shiina, Takayuki; Kawauchi, Yukimasa

no journal, , 

$$^{99m}$$Tc, the daughter nuclide of $$^{99}$$Mo, is widely used for medical diagnosis. In Japan, about 0.9 million diagnostic procedures are carried out using $$^{99m}$$Tc. $$^{99}$$Mo has been mostly produced using $$^{235}$$U in research reactors. Because of recent shortages of $$^{99}$$Mo, a variety of alternative production methods of $$^{99}$$Mo or $$^{99m}$$Tc were proposed. We proposed to produce $$^{99}$$Mo by $$^{100}$$Mo(n,2n) using neutrons from an accelerator. The route is characterized to produce a large quantity of high-quality $$^{99}$$Mo with a minimum level of radioactive wastes, since the cross section of the $$^{100}$$Mo(n,2n)$$^{99}$$Mo reaction at 11 $$<$$ En $$<$$ 18 MeV is large, and the cross sections of the (n,He), (n,n'p), and (n,p) reactions on $$^{100}$$Mo are quite small. Intense neutrons are available because of recent progresses of accelerator and target technologies. In the talk, we show our recent experimental results to obtain $$^{99m}$$Tc with high-quality using $$^{99}$$Mo produced by $$^{100}$$Mo(n,2n).

Oral presentation

Production and purification of medical radioisotope Y-90 with accelerator neutrons by deuterons

Tsukada, Kazuaki; Sato, Tetsuya; Hashimoto, Kazuyuki; Saeki, Hideya; Hatsukawa, Yuichi; Nagai, Yasuki; Watanabe, Satoshi; Ishioka, Noriko; Takeda, Shinsaku*

no journal, , 

A new system has been proposed for the generation of radioisotopes with accelerator neutrons by deuterons, especially the production of $$^{90}$$Y (T$$_{1/2}$$ = 64 h), which has been used for the nuclear medicine. Enriched $$^{90}$$Zr nitrate samples were irradiated with neutrons, which were obtained by the $$^{nat}$$C(d,n) using 40 MeV deuterons provided from the TIARA cyclotron. $$^{90}$$Y was successfully produced via the (n, p) reaction, and separated from the Zr nitrate target by three columns method with a hydrochloric acid. After the purification, a labelling of DTPA with $$^{90}$$Y had been performed. In this result, the yield was about 90% under $$>$$2.5 $$mu$$M of DTPA, although the yields were decreased at the DTPA concentration below 2.5 $$mu$$M.

Oral presentation

Medical radioisotope production with accelerator neutrons by deuterons

Tsukada, Kazuaki; Sato, Nozomi*; Watanabe, Satoshi; Ishioka, Noriko; Hatsukawa, Yuichi; Hashimoto, Kazuyuki; Kin, Tadahiro*; Takeda, Shinsaku*; Kawabata, Masako; Saeki, Hideya; et al.

no journal, , 

A new system has been proposed for the generation of radioisotopes with accelerator neutrons by deuterons, especially the production of Mo-99, Y-90, Cu-67, and Cu-64. Enriched Mo-100, Zr-90, Zn-68 and Zn-64 oxide samples were irradiated with neutrons, which were obtained by the $$^{nat}$$C(d,n) and Be(d,n) using 40 MeV deuterons provided from the TIARA cyclotron. Mo-99, Y-90, Cu-67, and Cu-64 were successfully produced via the (n, x) reactions, and we clearly observed the $$gamma$$-rays. Particularly, yields of impurity radionuclides were much smaller than that of Mo-99 and Cu-67, and therefore radioactive waste produced during chemical processing would be reduced compared with other proposed reaction systems. The present results demonstrate that the radioisotopes, Mo-99, Y-90, Cu-67, and Cu-64, can be produced by using fast neutrons, and strongly suggest that the reaction system is one of the most promising routes to produce high quality medical radioisotope.

Oral presentation

Measurement and estimation of the $$^{99}$$Mo production yield by the acceleration neutron

Tsukada, Kazuaki; Nagai, Yasuki*; Hashimoto, Kazuyuki*; Kawabata, Masako*; Minato, Futoshi; Saeki, Hideya*; Motoishi, Shoji*; Watanabe, Satoshi*; Ito, Masatoshi*

no journal, , 

no abstracts in English

Oral presentation

Evaluation of Lu-177 production in the research reactor JRR-3

Fujino, Shunsuke; Hashimoto, Kazuyuki; Saeki, Hideya*; Kawauchi, Yukimasa*; Kawabata, Masako*; Chiba, Yusuke

no journal, , 

Lutetium-177 (Lu-177)is a medical radioisotope used in approved radiopharmaceutical "Lutathera" to treat neuroendocrine tumours. And it is one of the promising radionuclides for new therapeutic radiopharmaceuticals. However, Lu-177 is dependent on imports from overseas, and there are concerns that transportation problems etc. may affect domestic distribution and development of new pharmaceuticals. In order to confirm whether JAEA can produce a portion of the Lu-177 for research, we conducted a production test of Lu-177 using JRR-3.

32 (Records 1-20 displayed on this page)