Homogeneous visible light-driven hydrogen evolution by the molecular molybdenum sulfide model [Mo2S12]2−

Abstract

The visible light-driven hydrogen evolution reaction by the molecular molybdenum sulfide anion [Mo₂S₁₂]²⁻ is reported. When coupled with the photosensitizer [Ru(bpy)₃]²⁺ (bpy = 2,2′-bipyridine) and the electron/proton donor ascorbic acid, turnover numbers > 1600 and turnover frequencies > 700 h⁻¹ are observed. Comparison with the prototype HER catalyst [Mo₃S₁₃]²⁻ shows remarkable reactivity differences which are explored by initial mechanistic studies under reaction conditions.