Decoupling H2 and O2 Release in Particulate Photocatalytic Overall Water Splitting Using a Reversible O2 Binder

Abstract H 2 and O 2 evolutions occur simultaneously for conventional particulate photocatalytic overall water splitting (PPOWS), leading to a significant backward reaction and the formation of an explosive H 2 /O 2 gas mixture. This is an issue that must be addressed prior to industrialization of PPOWS. Here, a convenient, cost‐effective, and scalable concept is introduced to uncouple hydrogen and oxygen production for PPOWS. Based on this idea, a three‐component photocatalyst, Co(5 %)‐HPCN/(rGO/Pt), is constructed, consisting of a photoresponsive chip (HPCN), a H 2 evolution cocatalyst (rGO/Pt), and a cobalt complex capable of reversibly binding O 2 (Co), to achieve the decoupling of PPOWS under alternating UV and visible light irradiations. The asynchronous O 2 and H 2 evolution strategy have considerable flexibility regarding the photocatalyst structure and light sources suitable for PPOWS.