Tuning and mechanistic insights of metal chalcogenide molecular catalysts for the hydrogen-evolution reaction

James McAllister, Nuno A. G. Bandeira (), Jessica C. McGlynn, Alexey Y. Ganin, Yu-Fei Song (), Carles Bo () and Haralampos N. Miras ()
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James McAllister: University of Glasgow
Nuno A. G. Bandeira: The Barcelona Institute of Science and Technology
Jessica C. McGlynn: University of Glasgow
Alexey Y. Ganin: University of Glasgow
Yu-Fei Song: Beijing University of Chemical Technology
Carles Bo: The Barcelona Institute of Science and Technology
Haralampos N. Miras: University of Glasgow

Nature Communications, 2019, vol. 10, issue 1, 1-10

Abstract: Abstract The production of hydrogen through water splitting using earth-abundant metal catalysts is a promising pathway for converting solar energy into chemical fuels. However, existing approaches for fine stoichiometric control, structural and catalytic modification of materials by appropriate choice of earth abundant elements are either limited or challenging. Here we explore the tuning of redox active immobilised molecular metal-chalcoxide electrocatalysts by controlling the chalcogen or metal stoichiometry and explore critical aspects of the hydrogen evolution reaction (HER). Linear sweep voltammetry (LSV) shows that stoichiometric and structural control leads to the evolution of hydrogen at low overpotential with no catalyst degradation over 1000 cycles. Density functional calculations reveal the effect of the electronic and structural features and confer plausibility to the existence of a unimolecular mechanism in the HER process based on the tested hypotheses. We anticipate these findings to be a starting point for further exploration of molecular catalytic systems.

Date: 2019
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DOI: 10.1038/s41467-018-08208-4

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