Efficient and Ultrastable Iodide Oxidation Reaction Over Defect-Passivated Perovskite Photoanode for Unassisted Solar Fuel Production

Abstract

Recently, lead halide perovskites have emerged as promising photoanode materials for efficient hydrogen production. However, the sluggish kinetics of the oxygen evolution reaction (OER) and interfacial defect-mediated charge accumulation inevitably result in efficiency loss and degradation of perovskite photoanodes. Herein, a defect-passivated electron transport layer-based perovskite photoanode combined with a catalyst layer favorable is introduced for iodide oxidation reaction bearing a small thermodynamic barrier and rapid kinetics compared to OER for efficient solar fuel generation. The resulting perovskite photoanode revealed a saturated photocurrent density of 22.4 mA cm-2 at 0.3 V versus the reversible hydrogen electrode (VRHE) with an impressive onset potential of -0.2 VRHE as well as durability for 225 h in a neutral electrolyte. In addition, an unbiased hydrogen-production device comprising a perovskite photoanode and Pt coil electrocatalyst is demonstrated, achieving a remarkable solar-to-chemical conversion efficiency of 11.45% and stable operation for 25 h. Moreover, a wireless artificial leaf-structured device realizing solar-driven hydrogen generation in natural sea water under outdoor sunlight is presented.,The introduction of 4-methoxyphenethyl-amine at the PSK/SnO2 interface, combined with IOR and Co-Ni3S2 catalyst on the perovskite photoanode, demonstrates the remarkable onset potential of -0.2 VRHE and stability of 225 h, maintaining approximate to 90% of the initial photocurrent density. The efficient unbiased hydrogen production is successfully achieved with a simple PEC-EC configuration with a high SCC efficiency of 11.45% and long-term stability of 25 h. image,