Affiliation:
1. School of Chemistry Chemical Engineering and Biotechnology Nanyang Technological University 62 Nanyang Drive Singapore 637459 Singapore
2. Department of Chemistry City University of Hong Kong 83 Tat Chee Avenue Hong Kong Kowloon 999077 China
3. School of Chemistry and Chemical Engineering Inner Mongolia University Hohhot 010021 China
Abstract
AbstractDirect electrosynthesis of hydrogen peroxide (H2O2) 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 H2O2 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.