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Cited by 265

The DOI matches its Crossref record; 10 of the 10 references it cites were found in a registry or an index.

Evidence from in Situ X-ray Absorption Spectroscopy for the Involvement of Terminal Disulfide in the Reduction of Protons by an Amorphous Molybdenum Sulfide Electrocatalyst

Open access
Lassalle-Kaiser, Benedikt, Merki, Daniel, Vrubel, Heron, Gul, Sheraz, Yachandra, Vittal K., Hu, Xile, Yano, Junko·2015·Journal of the American Chemical Society

Abstract

The reduction of protons into dihydrogen is important because of its potential use in a wide range of energy applications. The preparation of efficient and cheap catalysts for this reaction is one of the issues that need to be tackled to allow the widespread use of hydrogen as an energy carrier. In this paper, we report the study of an amorphous molybdenum sulfide (MoSx) proton reducing electrocatalyst under functional conditions, using in situ X-ray absorption spectroscopy. We probed the local and electronic structures of both the molybdenum and sulfur elements for the as prepared material as well as the precatalytic and catalytic states. The as prepared material is very similar to MoS3 and remains unmodified under functional conditions (pH = 2 aqueous HNO3) in the precatalytic state (+0.3 V vs RHE). In its catalytic state (-0.3 V vs RHE), the film is reduced to an amorphous form of MoS2 and shows spectroscopic features that indicate the presence of terminal disulfide units. These units are formed concomitantly with the release of hydrogen, and we suggest that the rate-limiting step of the HER is the reduction and protonation of these disulfide units. These results show the implication of terminal disulfide chemical motifs into HER driven by transition-metal sulfides and provide insight into their reaction mechanism.

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Metadata

Authors
Lassalle-Kaiser, B., Merki, D., Vrubel, H., Gul, S., Yachandra, V. K., Hu, X., & Yano, J.
Venue
Journal of the American Chemical Society
Published
2014-12-19
Volume
137
Issue
1
Pages
314-321
ISSN
  • 0002-7863 (ISSN-L)
  • 1520-5126
OpenAlex
W1991415947
Cited by
265
References
10
FWCI
7.42
Type
journal article
Language
en
Open access
hybrid

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