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Issue 5, 2018
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Understanding homogeneous hydrogen evolution reactivity and deactivation pathways of molecular molybdenum sulfide catalysts

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Abstract

Molybdenum sulfides are highly active hydrogen evolution reaction (HER) catalysts based on earth abundant elements. Here, the molybdenum sulfide anion [Mo3S13]2− is used as a molecular model to rationalize HER reactivity of Mo–S-catalysts. For the first time, homogeneous, visible light-driven HER activity of [Mo3S13]2− is reported and high reactivity is observed (turnover number TON ∼23 000, maximum turnover frequency TOFmax ∼156 min−1). Experimental and theoretical studies shed light on the catalytic role of terminal disulfide ligands (S22−) and show that these ligands modulate catalyst redox-activity and electron transfer in solution. Partial substitution of the terminal disulfides with water ligands leads to the most active catalytic species, e.g. [Mo3S11(H2O)2]. In contrast, complete substitution of the terminal disulfides results in a significant loss of reactivity. These results could lay the foundations for the knowledge-based development of homogeneous and heterogeneous molybdenum sulfide catalysts.

Graphical abstract: Understanding homogeneous hydrogen evolution reactivity and deactivation pathways of molecular molybdenum sulfide catalysts

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Publication details

The article was received on 15 Dec 2017, accepted on 01 Mar 2018 and first published on 01 Mar 2018


Article type: Paper
DOI: 10.1039/C7SE00599G
Citation: Sustainable Energy Fuels, 2018,2, 1020-1026
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    Understanding homogeneous hydrogen evolution reactivity and deactivation pathways of molecular molybdenum sulfide catalysts

    M. Dave, A. Rajagopal, M. Damm-Ruttensperger, B. Schwarz, F. Nägele, L. Daccache, D. Fantauzzi, T. Jacob and C. Streb, Sustainable Energy Fuels, 2018, 2, 1020
    DOI: 10.1039/C7SE00599G

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