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

ABSTRACT

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 Mo3S x 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.