Black Phosphorous Mediates Surface Charge Redistribution of CoSe<sub>2</sub> for Electrochemical H<sub>2</sub>O<sub>2</sub> Production in Acidic Electrolytes
Ya‐Rong Zheng, Shao‐Jin Hu, Xiaolong Zhang, Huanxin Ju, Zhenbin Wang, Pengju Tan, Rui Wu, Fei‐Yue Gao, Tao‐Tao Zhuang, Xiao Zheng, Junfa Zhu, Min‐Rui Gao, Shu‐Hong Yu
Abstract
Abstract Electrochemical generation of hydrogen peroxide (H 2 O 2 ) by two‐electron oxygen reduction offers a green method to mitigate the current dependence on the energy‐intensive anthraquinone process, promising its on‐site applications. Unfortunately, in alkaline environments, H 2 O 2 is not stable and undergoes rapid decomposition. Making H 2 O 2 in acidic electrolytes can prevent its decomposition, but choices of active, stable, and selective electrocatalysts are significantly limited. Here, the selective and efficient two‐electron reduction of oxygen toward H 2 O 2 in acid by a composite catalyst that is composed of black phosphorus (BP) nailed chemically on the metallic cobalt diselenide (CoSe 2 ) surface is reported. It is found that this catalyst exhibits a 91% Faradic efficiency for H 2 O 2 product at an overpotential of 300 mV. Moreover, it can mediate oxygen to H 2 O 2 with a high production rate of ≈1530 mg L −1 h −1 cm −2 in a flow‐cell reactor. Spectroscopic and computational studies together uncover a BP‐induced surface charge redistribution in CoSe 2 , which leads to a favorable surface electronic structure that weakens the HOO* adsorption, thus enhancing the kinetics toward H 2 O 2 formation.