Fabrication, permeation, and corrosion stability measurements of silica membranes for HI decomposition in the thermochemical iodine-sulfur process

Myagmarjav, O.; Shibata, Ai*; Tanaka, Nobuyuki; Noguchi, Hiroki; Kubo, Shinji; Nomura, Mikihiro*; Takegami, Hiroaki

International Journal of Hydrogen Energy, 46(56), p.28435 - 28449, 2021/08

https://doi.org/10.1016/j.ijhydene.2021.06.079

Performance tests of catalysts for the safe conversion of hydrogen inside the nuclear waste containers in Fukushima Daiichi

Reinecke, E.-A.*; Takenaka, Keisuke*; Ono, Hitomi*; Kita, Tomoaki*; Taniguchi, Masashi*; Nishihata, Yasuo; Hino, Ryutaro; Tanaka, Hirohisa*

International Journal of Hydrogen Energy, 46(23), p.12511 - 12521, 2021/03

https://doi.org/10.1016/j.ijhydene.2020.08.262

The safe decommissioning as well as decontamination of the radioactive waste resulting from the nuclear accident in Fukushima Daiichi represents a huge task for the next decade. At present, research and development on long-term safe storage containers has become an urgent task with international cooperation in Japan. One challenge is the generation of hydrogen and oxygen in significant amounts by means of radiolysis inside the containers, as the nuclear waste contains a large portion of sea water. The generation of radiolysis gases may lead to a significant pressure build-up inside the containers and to the formation of flammable gases with the risk of ignition and the loss of integrity. In the framework of the project "R&D on technology for reducing concentration of flammable gases generated in long-term waste storage containers" funded by the Japanese Ministry of Education, Culture, Sports, Science and Technology of Japan (MEXT), the potential application of catalytic recombiner devices inside the storage containers is investigated. In this context, a suitable catalyst based on the so-called intelligent automotive catalyst for use in a recombiner is under consideration. The catalyst is originally developed and mass-produced for automotive exhaust gas purification, and is characterized by having a self-healing function of precious metals (Pd, Pt and Rh) dissolved as a solid solution in the perovskite type oxides. The basic features of this catalyst have been tested in an experimental program. The test series in the REKO-4 facility has revealed the basic characteristics of the catalyst required for designing the recombiner system.

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

https://doi.org/10.1016/j.ijhydene.2020.02.229

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 oxidation reaction. As a result, the cell overvoltage for the membrane Bunsen reaction was significantly reduced to 0.21 V at 200 mA/cm, 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.

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

https://doi.org/10.1016/j.ijhydene.2019.09.132

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

https://doi.org/10.1016/j.ijhydene.2018.11.121

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.

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

https://doi.org/10.1016/j.ijhydene.2017.10.043

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 -alumina layer. The silica membranes formed on -alumina-coated -alumina tubes displayed a higher H permeance than that formed directly on an -alumina tube. A silica membrane based on a 1.5 m-thick -alumina layer fabricated under deposition conditions of 450C, 1200 s, and a N carrier gas velocity of 0.044 m s exhibited a high H permeance of 9.4 10 mol Pa m s while maintaining an H/N selectivity of over 80.0. The performance of a membrane reactor based on an HTMOS-derived silica membrane was evaluated at 400C by measuring the HI conversion and H flow rates. The conversion was approximately 0.48 when the HI flow rate was 9.7 mL min.

X-ray absorption spectroscopy study on water formation reaction of palladium metal nanoparticle catalysts

Matsumura, Daiju; Taniguchi, Masashi*; Tanaka, Hirohisa*; Nishihata, Yasuo

International Journal of Hydrogen Energy, 42(11), p.7749 - 7754, 2017/03

https://doi.org/10.1016/j.ijhydene.2016.08.189

Characteristics of flow field and pressure fluctuation in complex turbulent flow in the third elbow of a triple elbow piping with small curvature radius in three-dimensional layout

Ebara, Shinji*; Takamura, Hiroyuki*; Hashizume, Hidetoshi*; Yamano, Hidemasa

International Journal of Hydrogen Energy, 41(17), p.7139 - 7145, 2016/05

https://doi.org/10.1016/j.ijhydene.2016.02.068

In this study, a flow visualization and pressure measurement were conducted by using an experimental setup including test sections of 1/7-scale models of the cold-leg piping of Japan sodium-cooled reactor with high Reynolds number region up to about one million. Regarding the flow field, flow separation appeared in the intrados of the third elbow. However, the separation region was smaller than that observed in the first elbow in the direction normal to the mean flow and was larger in the streamwise direction. This can be considered because of the swirling flow generated downstream of the second elbow which flowed into the third elbow with a little reduction. From the pressure fluctuation test, it was found that prominent frequencies of the pressure fluctuation appeared at about 0.4 in Strouhal number, which corresponds to a nondimensional frequency, in the region from 0 D to 0.4 D downstream of the elbow outlet, where D is the diameter of the piping. And weak peaks of about 0.7 in Strouhal number were observed in the region far 0.75 D downstream of the outlet.

Hydrogenation of a TiFe-based alloy at high pressures and temperatures

Endo, Naruki*; Saita, Itoko*; Nakamura, Yumiko*; Saito, Hiroyuki; Machida, Akihiko

International Journal of Hydrogen Energy, 40(8), p.3283 - 3287, 2015/03

https://doi.org/10.1016/j.ijhydene.2015.01.015

Effect of sulfuric acid on electro-electrodialysis of HIx solution

Tanaka, Nobuyuki; Onuki, Kaoru; Kubo, Shinji

International Journal of Hydrogen Energy, 39(1), p.86 - 89, 2014/01

https://doi.org/10.1016/j.ijhydene.2013.10.103

The effect of sulfuric acid on the concentration of HIx solution by electro-electrodialysis (EED) was examined for the thermochemical water-splitting iodine-sulfur process. Presence of sulfuric acid in the anolyte HIx solution did not affect the concentration behavior. However, sulfuric acid in the catholyte solution caused side reaction(s) producing whitish precipitates, which indicates that the sulfur compound should be removed prior to the EED operation.