Low‐Coordinated Conductive ZnCu Metal‐Organic Frameworks for Highly Selective H<sub>2</sub>O<sub>2</sub> Electrosynthesis
Zhihao Pei, Yunxiang Li, Guilan Fan, Yan Guo, Deyan Luan, Xiaojun Gu, Xiong Wen Lou
Abstract
Abstract Direct electrosynthesis of hydrogen peroxide (H 2 O 2 ) with high production rate and high selectivity through the two‐electron oxygen reduction reaction (2e − ORR) offers a sustainable alternative to the energy‐intensive anthraquinone technology but remains a challenge. Herein, a low‐coordinated, 2D conductive Zn/Cu metal‐organic framework supported on hollow nanocube structures (ZnCu‐MOF (H)) is rationally designed and synthesized. The as‐prepared ZnCu‐MOF (H) catalyst exhibits substantially boosted electrocatalytic kinetics, enhanced H 2 O 2 selectivity, and ultra‐high Faradaic efficiency for 2e − ORR process in both alkaline and neutral conditions. Electrochemical measurements, operando/quasi in situ spectroscopy, and theoretical calculation demonstrate that the introduction of Cu atoms with low‐coordinated structures induces the transformation of active sites, resulting in the beneficial electron transfer and the optimized energy barrier, thereby improving the electrocatalytic activity and selectivity.