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Permanent link (DOI): https://doi.org/10.7939/R3XT1W

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Coke and sulfur resistant solid oxide fuel cells: development, test and novel applications Open Access

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Other title
Subject/Keyword
Novel applications
Coke and sulfur resistant
Solid oxide fuel cells
Type of item
Thesis
Degree grantor
University of Alberta
Author or creator
Yan, Ning
Supervisor and department
Luo, Jingli (Department of Chemical and Materials Engineering)
Examining committee member and department
McDermott, Mark (Department of Chemistry)
Prasad, Vinay (Department of Chemical and Materials Engineering)
Cadien, Ken (Department of Chemical and Materials Engineering)
Irvine, John (School of Chemistry, University of St Andrews)
Department
Department of Chemical and Materials Engineering
Specialization
Materials Engineering
Date accepted
2013-12-17T14:02:41Z
Graduation date
2014-06
Degree
Doctor of Philosophy
Degree level
Doctoral
Abstract
Solid oxide fuel cells (SOFC) can be fuelled with external-reformed natural gas or directly with raw natural gas which usually contains significant amount of H2S to reduce the system complexity. The anode catalyst as well as the current collector employed in those environments must have excellent coke and sulfur resistances in addition to the general requirements. The coke-sulfur tolerant SOFC serving as a reactor could co-generate power and value-added chemical products, which promises to drastically minimize the energy waste and increase the efficiency. To address the coking issues in fuel cells fed by syngas or pretreated natural gas, Ni-P coated Ni foam is fabricated via electroless plating as the coke resistant current collector. The coated Ni foam with a surface composition of Ni3P + Ni (P > 6.5 wt%) exhibits excellent coking resistance in 24 h treatment in syngas at 750 oC and an essentially identical current collecting capability during the fuel cells application test. The developed Ni-Sx catalyst obtained through in-situ H2S passivation shows superior balance between high activity and good carbon resistance during 200 h test in dry syngas. The discovered H2 selective oxidation effect using this catalyst has been employed in the novel application of SOFC. To deal with the coking and sulfur deactivation issues in SOFC fuelled directly by sour natural gas with H2S concentration up to 0.5%, a Pd-CeO2/La0.3Sr0.7O3-δ composite anode catalyst has been studied and is applied to the fuel cells via infiltration method. Maximum power densities of 642 mW cm-2 and 274 mW cm-2 have been achieved in H2 and in 0.5% H2S + CH4 at 850 oC, respectively. The Pd particles catalyze the electrochemical conversion of the fuels and are proved to be thermodynamically stable, whereas CeO2 promotes their thermal stability on the electrolyte matrix. The electronically conductive titanate can also serve as the current collecting material in sour natural gas. In the application of the coke/sulfur tolerant fuel cells for the co-generation of electricity and CO from syngas, the developed proton-conduction SOFC is able to reach a maximum power density of 812 mW cm-2 at 750 oC and up to 23.4 % H2 is removed in the stream without oxidizing CO. Novel H2 electrocatalytic selective oxidation in syngas using O-2-conducting SOFC is also studied. The Ni-S anode catalyst shows up to 92% H2 selectivity through selective surface diffusion mechanism in 10% H2 + CO.
Language
English
DOI
doi:10.7939/R3XT1W
Rights
Permission is hereby granted to the University of Alberta Libraries to reproduce single copies of this thesis and to lend or sell such copies for private, scholarly or scientific research purposes only. Where the thesis is converted to, or otherwise made available in digital form, the University of Alberta will advise potential users of the thesis of these terms. The author reserves all other publication and other rights in association with the copyright in the thesis and, except as herein before provided, neither the thesis nor any substantial portion thereof may be printed or otherwise reproduced in any material form whatsoever without the author's prior written permission.
Citation for previous publication
N. Yan, X. Z. Fu, J. L. Luo, K. T. Chuang, A. R. Sanger, “Ni–P coated Ni foam as coking resistant current collector for solid oxide fuel cells fed by syngas”, Journal of Power Sources, 198(2012), 164-169.N. Yan, X. Z. Fu, J. L. Luo, K. T. Chuang, “Insights into high temperature CO poisoning in proton-conducting solid oxide fuel cells” Journal of Power Sources (accepted)N. Yan, X. Z. Fu, J. L. Luo, K. T. Chuang, “Co-generation of electricity and CO from syngas via proton-conducting solid oxide fuel cells”, ECS Trans. 57(2013), 2977-2985.

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