Stabilizing highly active atomically dispersed NiN₄Cl sites by Cl‐doping for CO₂ electroreduction

Abstract Nickel‐nitrogen‐carbon single‐atom catalysts have attracted widespread interest for CO 2 electroreduction but they suffer from poor stability. Herein, we report on the preparation of Cl‐ and N‐doped porous carbon nanosheets with atomically dispersed NiN 4 Cl active sites (NiN Cl‐ClNC) through a molten‐salt‐assisted pyrolysis strategy. The optimized Cl‐ClNC catalyst delivers exceptional conversion activity outstanding stability over 220 h at −0.7 V versus RHE high Faradaic efficiency 98.7% partial current density 12.4 mA cm ‒2 . Moreover, displays remarkable approximately 349.4 −2 in flow‐cell, meeting requirements industrial applications. Operando attenuated total reflectance surface‐enhanced infrared absorption spectroscopy functional theory calculations are used to understand Results reveal that introduced axial Ni‐Cl bond Ni center Cl─C support synergetically induce electronic delocalization, which not only stabilizes against leaching also facilitates formation COOH* intermediate is found be rate‐determining step.