Origin of electrolyte-dopant dependent sulfur poisoning of SOFC anodes

Literature Information

Publication Date 2013-03-14
DOI 10.1039/C3CP51099A
Impact Factor 3.676
Authors

ZhenHua Zeng, Mårten E. Björketun, Sune Ebbesen, Mogens B. Mogensen, Jan Rossmeisl


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Abstract

The mechanisms governing the sulfur poisoning of the triple phase boundary (TPB) of Ni–XSZ (X2O3 stabilized zirconia) anodes have been investigated using density functional theory. The calculated sulfur adsorption energies reveal a clear correlation between the size of the cation dopant X3+ and the sulfur tolerance of the Ni–XSZ anode; the smaller the ionic radius, the higher the sulfur tolerance. The mechanistic study shows that the size of X3+ strongly influences XSZ's surface energy, which in turn determines the adhesion of Ni to XSZ. The Ni–XSZ interaction has a direct impact on the Ni–S interaction and on the relative stability of reconstructed and pristine Ni(100) facets at the TPB. Together, these two effects control the sulfur adsorption on the Ni atoms at the TPB. The established relationships explain experimentally observed dopant-dependent anode performances and provide a blueprint for the future search for and preparation of highly sulfur tolerant anodes.

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Source Journal

Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics
CiteScore: 5.5
Self-citation Rate: 10.3%
Articles per Year: 3036

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.

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