Low-Coordinated Conductive ZnCu Metal-Organic Frameworks for Highly Selective H₂O₂ Electrosynthesis

Direct 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.