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Self-Assembled Monolayers of Molybdenum Sulfide Clusters on Au Electrode as Hydrogen Evolution Catalyst for Solar Water Splitting

1
Department of Chemistry and Biochemistry, University of Alabama, Tuscaloosa, AL 35487, USA
2
Department of Chemistry, Tulane University, New Orleans, LA 70118, USA
*
Author to whom correspondence should be addressed.
Authors with equal contribution; Stephanie Spring is The Research Experiences for Undergraduates (REU) student of summer 2018 at The University of Alabama.
Inorganics 2019, 7(6), 79; https://doi.org/10.3390/inorganics7060079
Received: 1 May 2019 / Revised: 18 June 2019 / Accepted: 21 June 2019 / Published: 25 June 2019
(This article belongs to the Special Issue Inorganic Materials for Solar Energy Conversion)
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Abstract

Hydrogen evolution reaction (HER) activities of self-assembled monolayers (SAMs) of [Mo3S7(S2CNMe2)3] and several other MoSx molecular clusters are presented on planer Au electrode. Our study suggests that such Mo-S clusters are unstable under HER reaction conditions of a strongly acidic electrolyte. The [Mo3S7(S2CNEt2)3]I monolayer prepared from DMF showed greater stability among all the studied precursors. The X-ray photoelectron spectroscopy (XPS) analysis on a monolayer of [Mo3S7(S2CNMe2)3]I in THF assembled on Au/ITO suggested sulfur-rich composition with S:Mo ratio of 2.278. The Mo-S monolayer clusters resulting from [Mo3S7(S2CNMe2)3]I in THF showed a Tafel slope of 75.74 mV dec−1 and required a lower overpotential of 410 mV to reach a high HER catalytic current density of 100 mA cm−2 compared to the other studied precursors. Surface coverage of the Mo-S clusters on the Au surface was confirmed by cyclic voltammetry (CV) curves from K3Fe(CN)6 and anodization of Au surface. Further, the rotating ring-disk electrode (RRDE) measurements were performed for the monolayer of [Mo3S7(S2CNMe2)3]I prepared in THF to study its reaction kinetics. The HER catalytic activity of such monolayer Mo-S clusters can further be improved by controlling the sulfur vacancy. View Full-Text
Keywords: hydrogen evolution reaction; self-assembled monolayer; rotating ring disc electrode hydrogen evolution reaction; self-assembled monolayer; rotating ring disc electrode
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Spring, S.; Shinde, P.S.; Fontenot, P.R.; Donahue, J.P.; Pan, S. Self-Assembled Monolayers of Molybdenum Sulfide Clusters on Au Electrode as Hydrogen Evolution Catalyst for Solar Water Splitting. Inorganics 2019, 7, 79.

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