Efficient solar fuel production enabled by an iodide oxidation reaction on atomic layer deposited MoS2

Abstract

AbstractOxygen evolution reaction (OER) as a half‐anodic reaction of water splitting hinders the overall reaction efficiency owing to its thermodynamic and kinetic limitations. Iodide oxidation reaction (IOR) with low thermodynamic barrier and rapid reaction kinetics is a promising alternative to the OER. Herein, we present a molybdenum disulfide (MoS2) electrocatalyst for a high‐efficiency and remarkably durable anode enabling IOR. MoS2 nanosheets deposited on a porous carbon paper via atomic layer deposition show an IOR current density of 10 mA cm–2 at an anodic potential of 0.63 V with respect to the reversible hydrogen electrode owing to the porous substrate as well as the intrinsic iodide oxidation capability of MoS2 as confirmed by theoretical calculations. The lower positive potential applied to the MoS2‐based heterostructure during IOR electrocatalysis prevents deterioration of the active sites on MoS2, resulting in exceptional durability of 200 h. Subsequently, we fabricate a two‐electrode system comprising a MoS2 anode for IOR combined with a commercial Pt@C catalyst cathode for hydrogen evolution reaction. Moreover, the photovoltaic–electrochemical hydrogen production device comprising this electrolyzer and a single perovskite photovoltaic cell shows a record‐high current density of 21 mA cm–2 at 1 sun under unbiased conditions.