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Journal Articles

Overvoltage reduction in membrane Bunsen reaction for hydrogen production by using a radiation-grafted cation exchange membrane and porous Au anode

Sawada, Shinichi*; Kimura, Takehiro*; Nishijima, Haruyuki*; Kodaira, Takahide*; Tanaka, Nobuyuki; Kubo, Shinji; Imabayashi, Shinichiro*; Nomura, Mikihiro*; Yamaki, Tetsuya*

International Journal of Hydrogen Energy, 45(27), p.13814 - 13820, 2020/05

 Times Cited Count:0 Percentile:100(Chemistry, Physical)

An electrochemical membrane Bunsen reaction using a cation exchange membrane (CEM) is a key to achieving an iodine-sulfur (IS) thermochemical water splitting process for mass-production of hydrogen. In this study, we prepared both the radiation-grafted CEM with a high ion exchange capacity (IEC) and the highly-porous Au-electroplated anode, and then used them for the membrane Bunsen reaction to reduce the cell overvoltage. The high-IEC grafted CEM exhibited low resistivity for proton transport, while the porous Au anode had a large effective surface area for anodic SO$$_{2}$$ oxidation reaction. As a result, the cell overvoltage for the membrane Bunsen reaction was significantly reduced to 0.21 V at 200 mA/cm$$^{2}$$, which was only one-third of that of the previous test using the commercial CEM and non-porous anode. From the analysis of the current-voltage characteristics, employment of the grafted CEM was found to be more effective for the overvoltage reduction compared to the porous Au anode.

Journal Articles

Reliability improvements of corrosion-resistant equipment for thermochemical water splitting hydrogen production iodine-sulfur process

Kamiji, Yu; Noguchi, Hiroki; Takegami, Hiroaki; Tanaka, Nobuyuki; Iwatsuki, Jin; Kasahara, Seiji; Kubo, Shinji

Nuclear Engineering and Design, 361, p.110573_1 - 110573_6, 2020/05

 Times Cited Count:0 Percentile:100(Nuclear Science & Technology)

JAEA has been conducting R&D on the thermochemical iodine-sulfur (IS) process for nuclear-powered hydrogen production. The IS process is one of the promising candidates of heat application of the high-temperature gas-cooled reactors. The glass-lined steel is one of the candidate materials which has both corrosion resistance and structural strength. This paper reveals technical matters to improve reliability of the glass-lined steel equipment. It found that the improved glass-lined steel showed soundness in the process environment from the results of stress analyses for the glass layer by FEM, tests for heat cycle, bending load and corrosion.

Journal Articles

Development of strength evaluation method of ceramic reactor for iodine-sulfur process and hydrogen production test in Japan Atomic Energy Agency

Takegami, Hiroaki; Noguchi, Hiroki; Tanaka, Nobuyuki; Iwatsuki, Jin; Kamiji, Yu; Kasahara, Seiji; Imai, Yoshiyuki; Terada, Atsuhiko; Kubo, Shinji

Nuclear Engineering and Design, 360, p.110498_1 - 110498_6, 2020/04

 Times Cited Count:1 Percentile:24.17(Nuclear Science & Technology)

Japan Atomic Energy Agency (JAEA) has been conducting R&D on the thermochemical iodine-sulfur (IS) process for nuclear-powered hydrogen production. The IS process is one of the promising candidates of heat application of the high-temperature gas-cooled reactors. JAEA fabricated main chemical reactors made of industrial structural materials and confirmed their integrity in practical corrosive environments in the IS process. Based on the results of these confirmation tests, JAEA have constructed a 100 NL/h-H$$_{2}$$-scale test facility made of industrial structural materials. In this report, we succeeded in extending the hydrogen production time from 8 hours to 31 hours by developing a stable hydrogen iodide solution transfer technology in a continuous hydrogen production test. In addition, using the fracture test data of the ceramic specimen, an equation for estimating the strength of the ceramic component was developed.

Journal Articles

Comparison of experimental and simulation results on catalytic HI decomposition in a silica-based ceramic membrane reactor

Myagmarjav, O.; Tanaka, Nobuyuki; Nomura, Mikihiro*; Kubo, Shinji

International Journal of Hydrogen Energy, 44(59), p.30832 - 30839, 2019/11

 Times Cited Count:2 Percentile:70.22(Chemistry, Physical)

Journal Articles

Contribution of membrane technology to hydrogen society; Development of membrane IS process

Inagaki, Yoshiyuki; Sakaba, Nariaki; Tanaka, Nobuyuki; Nomura, Mikihiro*; Sawada, Shinichi*; Yamaki, Tetsuya*

Nippon Kaisui Gakkai-Shi, 73(4), p.194 - 202, 2019/08

The thermochemical IS process is a promising hydrogen production method which can produce hydrogen in a large amount and stably with high efficiency by thermal splitting of water. Research and development on chemical reaction technology with membranes was conducted for the purpose of improving the efficiency of IS process and application of solar heat. The basic technology of ceramic membranes applied to decomposition reactions of hydrogen iodine and sulfuric acid was developed, and it is expected that the conversion rate on decomposition in each reaction can be remarkably improved. The basic technology of a cation exchange membrane applied to Bunsen reaction was developed with radiation-induced grafting technique, it is expected that the amount of iodine can be reduced to about one-fifth compared to the conventional method. These achievements are important technologies for practical use of the IS process.

Journal Articles

Research and development on membrane IS process for hydrogen production using solar heat

Myagmarjav, O.; Iwatsuki, Jin; Tanaka, Nobuyuki; Noguchi, Hiroki; Kamiji, Yu; Ioka, Ikuo; Kubo, Shinji; Nomura, Mikihiro*; Yamaki, Tetsuya*; Sawada, Shinichi*; et al.

International Journal of Hydrogen Energy, 44(35), p.19141 - 19152, 2019/07

 Times Cited Count:6 Percentile:32.44(Chemistry, Physical)

Journal Articles

R&D status of hydrogen production test using IS process test facility made of industrial structural material in JAEA

Noguchi, Hiroki; Takegami, Hiroaki; Kamiji, Yu; Tanaka, Nobuyuki; Iwatsuki, Jin; Kasahara, Seiji; Kubo, Shinji

International Journal of Hydrogen Energy, 44(25), p.12583 - 12592, 2019/05

 Times Cited Count:1 Percentile:84.47(Chemistry, Physical)

JAEA has been conducting R&D on thermochemical water-splitting hydrogen production IS process to develop one of heat applications of high-temperature gas-cooled reactor. A test facility was constructed using corrosion-resistant industrial materials to verify integrity of the IS process components and to demonstrate continuous and stable hydrogen production. The performance of components installed in each section was confirmed. Subsequently, a trial operation of integration of the processing sections was successfully carried out for 8 hours with hydrogen production rate of approximately 10 NL/h. After that, hydrogen production operation was extended to 31 hours (approximately hydrogen production rate of 20 NL/h) by introducing a corrosion-resistance pump system with a developed shaft seal technology.

Journal Articles

Module design of silica membrane reactor for hydrogen production via thermochemical IS process

Myagmarjav, O.; Tanaka, Nobuyuki; Nomura, Mikihiro*; Kubo, Shinji

International Journal of Hydrogen Energy, 44(21), p.10207 - 10217, 2019/04

 Times Cited Count:5 Percentile:38.99(Chemistry, Physical)

Journal Articles

Current R&D status of thermochemical water splitting hydrogen production iodine-sulfur process in Japan Atomic Energy Agency, 1; Hydrogen production test and component development

Takegami, Hiroaki; Noguchi, Hiroki; Tanaka, Nobuyuki; Iwatsuki, Jin; Kamiji, Yu; Kasahara, Seiji; Imai, Yoshiyuki; Terada, Atsuhiko; Kubo, Shinji

Proceedings of 9th International Topical Meeting on High Temperature Reactor Technology (HTR 2018) (USB Flash Drive), 7 Pages, 2018/10

Japan Atomic Energy Agency (JAEA) has been conducting R&D on the thermochemical iodine-sulfur (IS) process for nuclear-powered hydrogen production. The IS process is one of the promising candidates of heat application of the high-temperature gas-cooled reactors. JAEA fabricated main chemical reactors made of industrial structural materials and confirmed their integrity in practical corrosive environments in the IS process. Based on the results of these confirmation tests, JAEA have constructed a 100 NL/h-H$$_{2}$$-scale test facility made of industrial structural materials. This report will present an outline and results of hydrogen production tests and reliability improvements of operation stability and components, such as development of a strength estimation method for heat-resistant and corrosion-resistant ceramics components made of silicon carbide.

Journal Articles

Current R&D status of thermochemical water splitting hydrogen production iodine-sulfur process in Japan Atomic Energy Agency, 2; Reliability improvements of corrosion-resistant equipment

Kamiji, Yu; Noguchi, Hiroki; Takegami, Hiroaki; Tanaka, Nobuyuki; Iwatsuki, Jin; Kasahara, Seiji; Kubo, Shinji

Proceedings of 9th International Topical Meeting on High Temperature Reactor Technology (HTR 2018) (USB Flash Drive), 7 Pages, 2018/10

Japan Atomic Energy Agency (JAEA) has been conducting R&D on the thermochemical iodine-sulfur (IS) process for nuclear-powered hydrogen production. The IS process is one of the promising candidates of heat application of the HTGR. JAEA achieved continuous hydrogen production for one week with a hydrogen production rate of 30 NL/h by using a test apparatus made of glass and fluororesin material. Subsequently, JAEA fabricated main chemical reactors made of industrial materials and confirmed their integrity in corrosive environments in the IS process. Based on the results, JAEA has constructed a 100 NL/h-H$$_{2}$$-scale test facility made of industrial materials; one of the important materials is the glass-lined steel for corrosion resistant components such as vessels, pipes and protective sheaths of sensors. This report will present technical matters to improve reliability of the glass-lined protective sheaths of thermocouple. In addition, results of quality confirmation will be presented, which are stress analyses for the glass layer by FEM, tests for heat cycle, bending load and corrosion.

Journal Articles

Development of ion-exchange membranes for the membrane Bunsen reaction in thermochemical hydrogen production by iodine-sulfur process

Nomura, Mikihiro*; Kodaira, Takahide*; Ikeda, Ayumi*; Naka, Yasuhito*; Nishijima, Haruyuki*; Imabayashi, Shinichiro*; Sawada, Shinichi*; Yamaki, Tetsuya*; Tanaka, Nobuyuki; Kubo, Shinji

Journal of Chemical Engineering of Japan, 51(9), p.726 - 731, 2018/09

 Times Cited Count:2 Percentile:78.15(Engineering, Chemical)

Thermochemical hydrogen production by the iodine-sulfur process decomposes water into hydrogen and oxygen by combining the chemical reactions of iodine and sulfur. Two types of acids are produced through the Bunsen reaction. To improve the performance of this reaction, ion-exchange membranes for the membrane Bunsen reaction should be developed. In the present study, a cation-exchange membrane was prepared by using a radiation-graft polymerization method. It was found that a divinylbenzene crosslinking procedure was very effective in reducing water permeation through the membrane, and the membrane Bunsen reaction was successfully carried out by using the developed crosslinked membrane. Therefore, the developed crosslinked membrane is a potential candidate for cation-exchange membranes for the membrane Bunsen reaction.

Journal Articles

Faradaically selective membrane for liquid metal displacement batteries

Yin, H.*; Chung, B.*; Chen, F.*; Ouchi, Takanari*; Zhao, J.*; Tanaka, Nobuyuki; Sadoway, D. R.*

Nature Energy (Internet), 3(2), p.127 - 131, 2018/02

 Times Cited Count:12 Percentile:25.19(Energy & Fuels)

We disclose a new porous electronically conductive membrane, which achieves chemical selectivity by preferred faradaic reaction. This shift in membrane mechanism grants access to a variety of heretofore forbidden choices for positive and negative electrode metals and allows the battery to charge-discharge at high rate without degradation. Fitted with a porous membrane of TiN, a displacement cell comprising a Pb positive electrode, a Li Pb negative electrode, and LiCl-KCl eutectic electrolyte was cycled at 410$$^{circ}$$C and exhibited a coulombic efficiency of 92%. The capacity fade rate was measured to be 0.00172% per cycle, which is tantamount to retention of greater than 94% of initial capacity after 10 years. Most significant from the standpoint of scalability, we show that the faradaic membrane can be fashioned out of metal so as to be mechanically durable and therefore easily mass-produced at large scale with a thin cross-section for minimal ohmic drop in cell voltage.

Journal Articles

R&D status in thermochemical water-splitting hydrogen production iodine-sulfur process at JAEA

Noguchi, Hiroki; Takegami, Hiroaki; Kasahara, Seiji; Tanaka, Nobuyuki; Kamiji, Yu; Iwatsuki, Jin; Aita, Hideki; Kubo, Shinji

Energy Procedia, 131, p.113 - 118, 2017/12

 Times Cited Count:9 Percentile:0.22

The IS process is the most deeply investigated thermochemical water-splitting hydrogen production cycle. It is in a process engineering stage in JAEA to use industrial materials for components. Important engineering tasks are verification of integrity of the total process and stability of hydrogen production in harsh environment. A test facility using corrosion-resistant materials was constructed. The hydrogen production ability was 100 L/h. Operation tests of each section were conducted to confirm basic functions of reactors and separators, etc. Then, a trial operation for integration of the sections was successfully conducted to produce hydrogen of about 10 L/h for 8 hours.

Journal Articles

Hydrogen production tests by hydrogen iodide decomposition membrane reactor equipped with silica-based ceramics membrane

Myagmarjav, O.; Tanaka, Nobuyuki; Nomura, Mikihiro*; Kubo, Shinji

International Journal of Hydrogen Energy, 42(49), p.29091 - 29100, 2017/12

 Times Cited Count:10 Percentile:50.46(Chemistry, Physical)

The catalytic decomposition of hydrogen iodide in a membrane reactor using silica membranes derived from hexyltrimethoxysilane (HTMOS) was investigated for the production of hydrogen in the thermochemical water splitting iodine-sulfur process. The silica membranes were prepared by counter-diffusion chemical vapor deposition using porous alumina support tubes in both the absence and presence of a $$gamma$$-alumina layer. The silica membranes formed on $$gamma$$-alumina-coated $$alpha$$-alumina tubes displayed a higher H$$_{2}$$ permeance than that formed directly on an $$alpha$$-alumina tube. A silica membrane based on a 1.5 $$mu$$m-thick $$gamma$$-alumina layer fabricated under deposition conditions of 450$$^{circ}$$C, 1200 s, and a N$$_{2}$$ carrier gas velocity of 0.044 m s$$^{-1}$$ exhibited a high H$$_{2}$$ permeance of 9.4 $$times$$ 10$$^{-7}$$ mol Pa$$^{-1}$$ m$$^{-2}$$ s$$^{-1}$$ while maintaining an H$$_{2}$$/N$$_{2}$$ selectivity of over 80.0. The performance of a membrane reactor based on an HTMOS-derived silica membrane was evaluated at 400$$^{circ}$$C by measuring the HI conversion and H$$_{2}$$ flow rates. The conversion was approximately 0.48 when the HI flow rate was 9.7 mL min$$^{-1}$$.

Journal Articles

Role of multichance fission in the description of fission-fragment mass distributions at high energies

Hirose, Kentaro; Nishio, Katsuhisa; Tanaka, Shoya*; L$'e$guillon, R.*; Makii, Hiroyuki; Nishinaka, Ichiro*; Orlandi, R.; Tsukada, Kazuaki; Smallcombe, J.*; Vermeulen, M. J.; et al.

Physical Review Letters, 119(22), p.222501_1 - 222501_6, 2017/12

 Times Cited Count:26 Percentile:8.29(Physics, Multidisciplinary)

Fission-fragment mass distributions were measured for $$^{237-240}$$U, $$^{239-242}$$Np and $$^{241-244}$$Pu populated in the excitation-energy range from 10 to 60 MeV by multi-nucleon transfer channels in the reaction $$^{18}$$O + $$^{238}$$U at the JAEA tandem facility. Among them, the data for $$^{240}$$U and $$^{240,241,242}$$Np were observed for the first time. It was found that the mass distributions for all the studied nuclides maintain a double-humped shape up to the highest measured energy in contrast to expectations of predominantly symmetric fission due to the washing out of nuclear shell effects. From a comparison with the dynamical calculation based on the fluctuation-dissipation model, this behavior of the mass distributions was unambiguously attributed to the effect of multi-chance fission.

Journal Articles

Current R&D status of thermochemical water splitting iodine-sulfur process in Japan Atomic Energy Agency

Kasahara, Seiji; Iwatsuki, Jin; Takegami, Hiroaki; Tanaka, Nobuyuki; Noguchi, Hiroki; Kamiji, Yu; Onuki, Kaoru; Kubo, Shinji

International Journal of Hydrogen Energy, 42(19), p.13477 - 13485, 2017/05

 Times Cited Count:25 Percentile:19.73(Chemistry, Physical)

Current R&D on the thermochemical water splitting iodine-sulfur (IS) process in Japan Atomic Energy Agency is summarized. Reactors were fabricated with industrial materials and verified by test operations: a Bunsen reactor, a H$$_{2}$$SO$$_{2}$$ decomposer, and a HI decomposer. Reactors of industrial materials showed corrosion stability. Demonstration of the test facility verified integrity of process components and stability of hydrogen production. An 8 hours continuous operation of the total IS process was performed in February 2016 with H$$_{2}$$ production rate of 10 L/h.

Journal Articles

Preparation of an H$$_{2}$$-permselective silica membrane for the separation of H$$_{2}$$ from the hydrogen iodide decomposition reaction in the iodine-sulfur process

Myagmarjav, O.; Ikeda, Ayumi*; Tanaka, Nobuyuki; Kubo, Shinji; Nomura, Mikihiro*

International Journal of Hydrogen Energy, 42(9), p.6012 - 6023, 2017/03

 Times Cited Count:12 Percentile:43.52(Chemistry, Physical)

Journal Articles

IS process hydrogen production test for components and system made of industrial structural material, 2; H$$_{2}$$SO$$_{4}$$ decomposition, HI distillation, and HI decomposition section

Noguchi, Hiroki; Takegami, Hiroaki; Kamiji, Yu; Tanaka, Nobuyuki; Iwatsuki, Jin; Kasahara, Seiji; Kubo, Shinji

Proceedings of 8th International Topical Meeting on High Temperature Reactor Technology (HTR 2016) (CD-ROM), p.1029 - 1038, 2016/11

JAEA has been conducting R&D on the IS process for nuclear-powered hydrogen production. We have constructed a 100 NL/h-H$$_2$$-scale test apparatus made of industrial materials. At first, we investigated performance of components in this apparatus. In this paper, the test results of H$$_2$$SO$$_4$$ decomposition, HI distillation, and HI decomposition were shown. In the H$$_2$$SO$$_4$$ section, O$$_2$$ production rate is proportional to H$$_2$$SO$$_4$$ feed rate and SO$$_3$$ decomposition ratio was estimated about 80%. In HI distillation section, we confirmed to acquire a concentrated HI solution over azeotropic HI composition in the condenser. In HI decomposition section, H$$_2$$ could be produced stably by HI decomposer and decomposition ratio was about 18%. The H$$_2$$SO$$_4$$ decomposer, the HI distillation column, and the HI decomposer were workable. Based on the results added to that shown in Series I, we conducted a trial continuous operation and succeeded it for 8 hours.

Journal Articles

IS process hydrogen production test for components and system made of industrial structural material, 1; Bunsen and HI concentration section

Tanaka, Nobuyuki; Takegami, Hiroaki; Noguchi, Hiroki; Kamiji, Yu; Iwatsuki, Jin; Aita, Hideki; Kasahara, Seiji; Kubo, Shinji

Proceedings of 8th International Topical Meeting on High Temperature Reactor Technology (HTR 2016) (CD-ROM), p.1022 - 1028, 2016/11

Japan Atomic Energy Agency (JAEA) has manufactured 100 NL/h-H$$_2$$-scale hydrogen test apparatus. In advance to conduct the continuous operation, we investigated performance of the components in each section of the IS process. In this paper, the results of test of Bunsen and HI concentration sections was shown. In Bunsen reaction, section, we confirmed that outlet gas flow rate included no SO$$_{2}$$ gas, indicating that all the feed SO$$_{2}$$ gas was absorbed to the solution in the Bunsen reactor for the Bunsen reaction. On the basis of these results, we evaluated that Bunsen reactor was workable. In HI concentration section, HI concentration was conducted by EED stack. As a result, it can concentrate HI in HIx solution as theoretically predicted on the basis of the previous paper. Based on the results added to that shown in Series II, we have conducted a trial continuous operation and succeeded it for 8 hours.

JAEA Reports

Research and development on chemical reactors made of industrial structural materials and hydriodic acid concentration technique for thermochemical hydrogen production IS process

Kubo, Shinji; Iwatsuki, Jin; Takegami, Hiroaki; Kasahara, Seiji; Tanaka, Nobuyuki; Noguchi, Hiroki; Kamiji, Yu; Onuki, Kaoru

JAEA-Technology 2015-028, 32 Pages, 2015/10

JAEA-Technology-2015-028.pdf:23.69MB

JAEA has been conducting a study on IS process for thermochemical hydrogen production in order to develop massive hydrogen production technology for hydrogen society. Integrity of the chemical reactors and concentration technology of hydrogen iodide in HIx solution were studied. In the former study, the chemical reactors were trial-fabricated using industrial materials. A test of 30 times of thermal cycle test under circulating condition of the Bunsen reaction solution showed integrity of the Bunsen reactor made of fluororesin lined steel. Also, 100 hours of reaction tests showed integrity of the sulfuric acid decomposer made of silicon carbide and of the hydrogen iodide decomposer made of Hastelloy C-276. In the latter study, concerning electro-electrodialysis using cation-exchange membrane, sulfuric acid in the anolyte had little influence on the concentration performance. These results suggest the purification system of HIx solution can be simplified. Based on the Nernst-Planck equation and the Smoluchowski equation, proton transport number, water permeance, and IR drop of the cation exchange membrane were formulated. The derived equations enable quantitative estimation for the performance indexes of Nafion membrane and, also, of ETFE-St membranes made by radiation-induced graft polymerization method.

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