Direct Anchoring of Molybdenum Sulfide Molecular Catalysts on Antimony Selenide Photocathodes for Solar Hydrogen Production

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Molybdenum sulfide serves as an effective nonprecious metal catalyst for hydrogen evolution, primarily active at edge sites with unsaturated molybdenum sites or terminal disulfides. To improve the activity at a low loading density, two molybdenum sulfide clusters, [Mo3S4]4+ and [Mo3S13]2–, were investigated. The Mo3Sx molecular catalysts were heterogenized on Sb2Se3 with a simple soaking treatment, resulting in a thin catalyst layer of only a few nanometers that gave up to 20 mA cm–2 under one sun illumination. Both [Mo3S4]4+ and [Mo3S13]2– exhibit catalytic activities on Sb2Se3, with [Mo3S13]2– emerging as the superior catalyst, demonstrating enhanced photovoltage and an average faradaic efficiency of 100% for hydrogen evolution. This superiority is attributed to the effective loading and higher catalytic activity of [Mo3S13]2– on the Sb2Se3 surface, validated by X-ray photoelectron and Raman spectroscopy.