n‐ZrS3/p‐ZrOS Photoanodes with NiOOH/FeOOH Oxygen Evolution Catalysts for Photoelectrochemical Water Oxidation

Abstract Photoelectrochemical water splitting offers a promising approach for carbon neutrality, but its commercial prospects are still hampered by a lack of efficient and stable photoelectrodes with earth‐abundant materials. Here, we report a strategy to construct an efficient photoanode with a coaxial nanobelt structure, comprising a buried‐ZrS 3 /ZrOS n−p junction, for photoelectrochemical water splitting. The p‐type ZrOS layer, formed on the surface of the n‐type ZrS 3 nanobelt through a pulsed‐ozone‐treatment method, acts as a hole collection layer for hole extraction and a protective layer to shield the photoanode from photocorrosion. The resulting ZrS 3 /ZrOS photoanode exhibits light harvesting with good photo‐to‐current efficiencies across the whole visible region to over 650 nm. By further employing NiOOH/FeOOH as the oxygen evolution reaction cocatalyst, the ZrS 3 /ZrOS/NiOOH/FeOOH photoanode yields a photocurrent density of ~9.3 mA cm −2 at 1.23 V versus the reversible hydrogen electrode with an applied bias photon‐to‐current efficiency of ~3.2 % under simulated sunlight irradiation in an alkaline solution (pH=13.6). The conformal ZrOS layer enables ZrS 3 /ZrOS/NiOOH/FeOOH photoanode operation over 1000 hours in an alkaline solution without obvious performance degradation. This study, offering a promising approach to fabricate efficient and durable photoelectrodes with earth‐abundant materials, advances the frontiers of photoelectrochemical water splitting.