First-principles investigation of H2S adsorption and dissociation on titanium carbide surfaces

Literature Information

Publication Date 2017-09-25
DOI 10.1039/C7CP05756C
Impact Factor 3.676
Authors

Shiyan Wang, Xilin Zhang, Yanxing Zhang, Jianjun Mao


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Abstract

The adsorption and dissociation reactions of H2S on TiC(001) are investigated using first-principles density functional theory calculations. The geometric and electronic structures of the adsorbed S-based species (including H2S, SH and S) on TiC(001) are analyzed in detail. It is found that the H2S is bound weakly, while SH and atomic S are bound strongly on the TiC(001) surface. The transition state calculations show that the formation of SH from H2S (H2S → SH + H) is very easy, while the presence of a co-adsorbed H will inhibit the further dissociation of SH (SH + H → S + H + H). In contrast, the hydrogenation of the adsorbed SH is rather easy (SH + H → H2S). Therefore, the dissociative SH can be removed via the hydrogenation reaction. It is concluded that it is difficult for H2S to dissociate completely to form atomic S and poison the TiC surface. The results will further provide understanding of the mechanism of the sulfur tolerance of the TiC anode of proton exchange membrane fuel cells (PEMFCs).

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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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