Title: Surface reaction and transport kinetics of hydrogen through palladium-based membranes under gas co-existing with hydrogen atmospheres

Authors: Atsushi Unemoto, Nobuyuki Hirai, Atsushi Kaimai, Kazuhisa Sato, Takanori Otake, Keiji Yashiro, Junichiro Mizusaki, Tatsuya Kawada, Tatsuya Tsuneki, Yoshinori Shirasaki, Yoshu Ota, Isamu Yasuda

Addresses: Graduate School of Environmental Studies, Tohoku University, 6–6 Aoba, Aramaki, Aoba-ku, Sendai 980–8579, Japan. ' Institute of Multidisciplinary Research for Advanced Materials, Tohoku University, 2–1–1 Katahira, Aoba-ku, Sendai 980–8577, Japan; Hydraulic Control System Group, Core Component Engineering Department, Engineering Division, AISIN AW Co., Ltd., 10 Takane, Fujii-cho, Anjo, Aichi 444–1192, Japan. ' Institute of Multidisciplinary Research for Advanced Materials, Tohoku University, 2–1–1 Katahira, Aoba-ku, Sendai 980–8577, Japan; Graduate School of Environmental Studies, Tohoku University, 6–6 Aoba, Aramaki, Aoba-ku, Sendai 980–8579, Japan. ' Institute of Multidisciplinary Research for Advanced Materials Tohoku University, 2–1–1 Katahira, Aoba-ku, Sendai 980–8577, Japan. ' Institute of Multidisciplinary Research for Advanced Materials, Tohoku University, 2–1–1 Katahira, Aoba-ku, Sendai 980–8577, Japan; Combustion and Materials Technology Group, Fundamental Research Department, Technical Research Institute, Toho Gas Co., Ltd., 507–2 Shinpo-Machi, Tokai, Aichi 476–8501, Japan. ' Institute of Multidisciplinary Research for Advanced Materials, Tohoku University, 2–1–1 Katahira, Aoba-ku, Sendai 980–8577, Japan; Nonmetallic Inorganic Materials, ETH Zurich, Wolfgang-Pauli-Strasse 10, 8093 Zurich, Switzerland. ' Institute of Multidisciplinary Research for Advanced Materials, Tohoku University, 2–1–1 Katahira, Aoba-ku, Sendai 980–8577, Japan. ' Graduate School of Environmental Studies, Tohoku University, 6–6 Aoba, Aramaki, Aoba-ku, Sendai 980–8579, Japan. ' Hydrogen System Team, Technology Research Institute, Fundamental Technology Department, Technology Development Division, Tokyo Gas Co., Ltd., 1–7–7 Suehiro-cho, Tsurumi-ku, Yokohama 230–0045, Japan. ' Hydrogen System Team, Technology Research Institute, Fundamental Technology Department, Technology Development Division, Tokyo Gas Co., Ltd., 1–7–7 Suehiro-cho, Tsurumi-ku, Yokohama 230–0045, Japan. ' Hydrogen System Team, Technology Research Institute, Fundamental Technology Department, Technology Development Division, Tokyo Gas Co., Ltd., 1–7–7 Suehiro-cho, Tsurumi-ku, Yokohama 230–0045, Japan. ' Hydrogen System Team, Technology Research Institute, Fundamental Technology Department, Technology Development Division, Tokyo Gas Co., Ltd., 1–7–7 Suehiro-cho, Tsurumi-ku, Yokohama 230–0045, Japan

Abstract: In order to understand how gas co-existing with hydrogen affects the hydrogen permeability of a silver 23wt%-palladium membrane, the surface reaction of hydrogen was evaluated from the continuity of the surface reaction rate and the bulk diffusion flux of hydrogen based on the results of hydrogen-permeation measurements. The interference effect of the co-existing species was quantified as a function of temperature, partial pressure and the components of the co-existing gas. In order to investigate the behaviour of the co-existing species on the membrane surface, in situ observation using the Polarisation Modulated Infrared Reflection Absorption Spectroscopy (PM-IRRAS) was carried out. An infrared absorption peak due to the adsorption of carbon monoxide on the membrane was observed under the atmosphere of 7.8% carbon monoxide – 2.3% water vapour – 89.9% hydrogen. From the dependence of the infrared absorption peak on temperature, co-existing carbon monoxide was found to adsorb onto the membrane surface irreversibly.

Keywords: palladium-silver membrane; hydrogen permeability; membrane reactors; surface reaction; co-existing gas; in situ observations; transport kinetics; hydrogen atmospheres; carbon monoxide.

DOI: 10.1504/IJNHPA.2009.023827

International Journal of Nuclear Hydrogen Production and Applications, 2009 Vol.2 No.1, pp.55 - 68

Published online: 13 Mar 2009 *

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