Journal
ACS ENERGY LETTERS
Volume 7, Issue 10, Pages 3695-3702Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsenergylett.2c02053
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In this study, a unified explanation for the function of Mo HER catalysts was derived through various methods on a range of Mo-based catalysts. The formation of Mo3+ at cathodic potentials close to the thermodynamic HER onset drives activity, and the ease of reduction from Mo4+ to Mo3+ determines the activity of different catalysts.
Mo-based catalysts constitute a significant portion of active non-noble H2 evolution reaction (HER) catalysts, but the role of Mo in conferring this activity remains debated. In this study, we utilize electrochemical, physical, functional, and computational approaches on a range of Mo -based catalysts to derive a unified explanation for Mo HER catalyst function. Across all catalysts studied, the formation of Mo3+ at cathodic potentials close to the thermodynamic HER onset drives activity, and activity between catalysts is therefore heavily determined by the ease of reduction from Mo4+ to Mo3+. As such, surface oxidation is detrimental to HER activity as it makes Mo3+ formation less facile. This theory provides a cohesive explanation for the origin of activity in Mo-based HER catalysts, emphasizing the specific role of Mo atoms in forming hydrides and carrying out the HER from Mo3+, with implications for future Mo catalyst design.
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