Boosting the Ni–Zn interplay via O/N dual coordination for high‐efficiency CO₂ electroreduction

Design of supportive atomic sites with a controllably adjusted coordinating environment is essential to advancing the reduction CO2 value-added fuels and chemicals achieving carbon neutralization. Herein, Ni (Zn) that are uniquely coordinated ternary Zn (Ni)/N/O ligands were successfully decorated on formamide-derived porous nanomaterials, possibly forming an structure Ni(N2O1)-Zn(N2O1), as studied by combining X-ray photoelectron spectroscopy absorption spectroscopy. With mediation additional O coordination, Ni–Zn dual site induces significantly decreased desorption molecular CO. The NiZn-NC rich Ni(N2O1)-Zn(N2O1) remarkably gained >97% CO Faraday efficiency over wide potential range ‒0.8 ‒1.1 V (relative reversible hydrogen electrode). Density functional theory computations suggest N/O coordination effectively modulates electronic duplex optimizes adsorption conversion properties subsequent intermediates. Different from conventional pathway using active in duplex, it found Ni-neighboring showed much lower energy barriers protonation step dehydroxylation step.