Metal–Organic Framework‐Derived ZnO/ZnS Heteronanostructures for Efficient Visible‐Light‐Driven Photocatalytic Hydrogen Production

Abstract Developing highly active, recyclable, and inexpensive photocatalysts for hydrogen evolution reaction (HER) under visible light is significant for the direct conversion of solar energy into chemical fuels for various green energy applications. For such applications, it is very challenging but vitally important for a photocatalyst to simultaneously enhance the visible‐light absorption and suppress photogenerated electron–hole recombination, while also to maintain high stability and recyclability. Herein, a metal–organic framework (MOF)‐templated strategy has been developed to prepare heterostructured nanocatalysts with superior photocatalytic HER activity. Very uniquely, the synthesized photocatalytic materials can be recycled easily after use to restore the initial photocatalytic activity. It is shown that by controlling the calcination temperature and time with MOF‐5 as a host and guest thioacetamide as a sulfur source, the chemical compositions of the formed heterojunctions of ZnO/ZnS can be tuned to further enhance the visible‐light absorption and photocatalytic activity. The nanoscale heterojunction ZnO/ZnS structural feature serves to reduce the average free path of charge carriers and improve the charge separation efficiency, thus leading to significantly enhanced HER activity under visible‐light irradiation (λ > 420 nm) with high stability and recyclability without any cocatalyst.