Abstract

AbstractConstructing rich defect active site structure for material design is still a great challenge. Herein, a simple surface engineering strategy is demonstrated to construct one‐unit‐cell ZnIn2S4 atomic layers with the modulated surface energy of S vacancy. Rich surface energy can regulate and control the rich S vacancy, which ensures rich active sites, higher charge density and effective carrier transport. As a result, the ZnIn2S4 atomic layers with rich surface energy affords an obvious enhancement in H2O2 productive rate of 1592.04 µmol g−1 h−1, roughly 14.58 times superior to that with poor surface energy. Moreover, the in situ infrared diffuse reflection spectrum indicates that S vacancy as the oxygen reduction reaction active site is responsible for the critical intermediate *O2− and *OOH, corresponding to two‐electron oxygen reduction reaction. This study provides a valuable insight and guidance for constructing controllably defects to achieve highly efficient H2O2 production.

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