Low‐Coordinated CoNC on Oxygenated Graphene for Efficient Electrocatalytic H<sub>2</sub>O<sub>2</sub> Production
Haisheng Gong, Zengxi Wei, Zhichao Gong, Jingjing Liu, Gonglan Ye, Minmin Yan, Juncai Dong, Christopher S. Allen, Jianbin Liu, Kang Huang, Rui Liu, Guanchao He, Shuangliang Zhao, Huilong Fei
Abstract
Abstract Electrochemical H 2 O 2 production through the 2‐electron oxygen reduction reaction (ORR) is a promising alternative to the energy‐intensive anthraquinone process. Herein, by simultaneously regulating the coordination number of the atomically dispersed cobalt sites and the nearby oxygen functional groups via a one‐step microwave thermal shock, a highly selective and active CoNC electrocatalyst for H 2 O 2 electrosynthesis that exhibits a high H 2 O 2 selectivity (91.3%), outstanding mass activity (44.4 A g −1 at 0.65 V), and large kinetic current density (11.3 mA cm −2 at 0.65 V) in 0.1 m KOH is obtained. In strong contrast to the typical CoN 4 moieties for the 4‐electron ORR, the present CoNC catalyst possesses a low‐coordinated CoN 2 configuration and abundant epoxide groups, which work in synergy for promoting the 2‐electron ORR, as demonstrated by a series of control experiments and theoretical simulations. This study may provide an effective avenue to modulating the composition and structure of electrocatalysts at the atomic scale, leading to the development of new electrocatalysts with unprecedented reactivity.