Analysis of H2S Tolerance of Pd-Cu Alloy Hydrogen Separation Membranes

doi:10.1016/S1004-9541(14)60069-0

Chinese Journal of Chemical Engineering ›› 2014, Vol. 22 ›› Issue (5): 503-508.DOI: 10.1016/S1004-9541(14)60069-0

• 催化、动力学与反应工程 • 上一篇下一篇

Analysis of H₂S Tolerance of Pd-Cu Alloy Hydrogen Separation Membranes

高会元, 王岭

College of Chemical Engineering, Hebei United University, Tangshan 063009, China

收稿日期:2012-07-17 修回日期:2012-10-05 出版日期:2014-05-28 发布日期:2014-05-06
通讯作者: GAO Huiyuan,E-mail: hygao@heuu.edu.cn
基金资助:
Supported by the National Natural Science Foundation of China (50972038), the National Natural Science Foundation of Hebei Province (B2009000739, B2014209258), Science and Technology Support Program of Hebei Province (09215142D).

Analysis of H₂S Tolerance of Pd-Cu Alloy Hydrogen Separation Membranes

GAO Huiyuan, WANG Ling

College of Chemical Engineering, Hebei United University, Tangshan 063009, China

Received:2012-07-17 Revised:2012-10-05 Online:2014-05-28 Published:2014-05-06
Supported by:
Supported by the National Natural Science Foundation of China (50972038), the National Natural Science Foundation of Hebei Province (B2009000739, B2014209258), Science and Technology Support Program of Hebei Province (09215142D).

摘要/Abstract

摘要： The presence of a limited amount of H₂S in H₂-rich feed adversely affects the Pd-Cu membrane permeation performance due to the sulphidization of the membrane surface. A theoretical model was proposed to predict the S-tolerant performance of the Pd-Cu membranes in presence of H₂S under the industrial water-gas-shift (WGS) reaction conditions. The ideas of surface coverage and competitive adsorption thermodynamics of H₂S and H₂ on Pd-Cu surface were introduced in the model. The surface sulphidization of the Pd-Cu membranes mainly depended on the pressure ratio of H₂S to H₂, temperature and S-adsorbed surface coverage, i.e., the occurrence of sulphidization on the surface was not directly related with the bulk compositions and structures [body centered cubic and face centered cubic (bcc or fcc)] of Pd-Cu alloy membranes because of the surface segregation phenomena. The resulting equilibrium equations for the H₂S adsorption/sulphidization reactions were solved to calculate the pressure ratio of H₂S to H₂ over a wide range of temperatures. A validation of the model was performed through a comparison between lots of literature data and the model calculations over a rather broad range of operating conditions. An extremely good agreement was obtained in the different cases, and thus, the model can serve to guide the development of S-resistant Pd alloy membrane materials for hydrogen separation.

关键词: surface coverage, Pd-Cu alloy membranes, H₂S tolerance, theoretical model, hydrogen separation

Abstract: The presence of a limited amount of H₂S in H₂-rich feed adversely affects the Pd-Cu membrane permeation performance due to the sulphidization of the membrane surface. A theoretical model was proposed to predict the S-tolerant performance of the Pd-Cu membranes in presence of H₂S under the industrial water-gas-shift (WGS) reaction conditions. The ideas of surface coverage and competitive adsorption thermodynamics of H₂S and H₂ on Pd-Cu surface were introduced in the model. The surface sulphidization of the Pd-Cu membranes mainly depended on the pressure ratio of H₂S to H₂, temperature and S-adsorbed surface coverage, i.e., the occurrence of sulphidization on the surface was not directly related with the bulk compositions and structures [body centered cubic and face centered cubic (bcc or fcc)] of Pd-Cu alloy membranes because of the surface segregation phenomena. The resulting equilibrium equations for the H₂S adsorption/sulphidization reactions were solved to calculate the pressure ratio of H₂S to H₂ over a wide range of temperatures. A validation of the model was performed through a comparison between lots of literature data and the model calculations over a rather broad range of operating conditions. An extremely good agreement was obtained in the different cases, and thus, the model can serve to guide the development of S-resistant Pd alloy membrane materials for hydrogen separation.

Key words: surface coverage, Pd-Cu alloy membranes, H₂S tolerance, theoretical model, hydrogen separation

高会元, 王岭. Analysis of H₂S Tolerance of Pd-Cu Alloy Hydrogen Separation Membranes[J]. Chinese Journal of Chemical Engineering, 2014, 22(5): 503-508.

GAO Huiyuan, WANG Ling. Analysis of H₂S Tolerance of Pd-Cu Alloy Hydrogen Separation Membranes[J]. Chin.J.Chem.Eng., 2014, 22(5): 503-508.

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Analysis of H₂S Tolerance of Pd-Cu Alloy Hydrogen Separation Membranes

Analysis of H₂S Tolerance of Pd-Cu Alloy Hydrogen Separation Membranes

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