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First-principles studies of H₂S adsorption and dissociation on metal surfaces

Journal Article · · Surface Science

Density functional theory calculations were employed to investigate the molecular and dissociative adsorption of H₂S on the closed packed surfaces of a number of important noble metals (Ag(1 1 1), Au(1 1 1) and Cu(1 1 1)) and transition metals (Ir(1 1 1), Ni(1 1 1), Pd(1 1 1) and Pt(1 1 1)). Energy minima corresponding to adsorbed states were identified with H₂S binding preferentially at the top sites. The adsorption of other S moieties (SH and S) was also examined. SH and S were found to prefer bridge sites and hollow sites, respectively. The binding of H₂S and its S-containing dissociated species is stronger on the transition metals. The elementary reactions of abstraction of H from H₂S to form a surface SH intermediate and abstraction of H from SH to form a surface S intermediate as model pathways for the dissociation of H₂S were examined. Our results suggest that H₂S decomposition on the aforementioned transition metal surfaces is more facile, both thermodynamically and kinetically.

Research Organization:
National Energy Technology Laboratory - In-house Research
Sponsoring Organization:
USDOE Assistant Secretary for Fossil Energy (FE-1)
OSTI ID:
1012228
Report Number(s):
NETL-TPR3492
Journal Information:
Surface Science, Journal Name: Surface Science Journal Issue: 16 Vol. 602; ISSN 0039-6028
Publisher:
Elsevier
Country of Publication:
United States
Language:
English

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