Ultrathin Nitrogen‐Doped Carbon Encapsulated Ni Nanoparticles for Highly Efficient Electrochemical CO2 Reduction and Aqueous Zn‐CO2 Batteries

Electrochemical CO₂ reduction reaction (CO₂ RR), powered by renewable electricity, has attracted great attention for producing high value-added fuels and chemicals, as well as feasibly mitigating CO₂ emission problem. Here, this work reports a facile hard template strategy to prepare the Ni@N-C catalyst with core-shell structure, where nickel nanoparticles (Ni NPs) are encapsulated by thin nitrogen-doped carbon shells (N-C shells). The Ni@N-C catalyst has demonstrated a promising industrial current density of 236.7 mA cm^-2 with the superb FE_CO of 97% at -1.1 V versus RHE. Moreover, Ni@N-C can drive the reversible Zn-CO₂ battery with the largest power density of 1.64 mW cm^-2 , and endure a tough cycling durability. These excellent performances are ascribed to the synergistic effect of Ni@N-C that Ni NPs can regulate the electronic microenvironment of N-doped carbon shells, which favor to enhance the CO₂ adsorption capacity and the electron transfer capacity. Density functional theory calculations prove that the binding configuration of N-C located on the top of Ni slabs (Top-Ni@N-C) is the most thermodynamically stable and possess a lowest thermodynamic barrier for the formation of COOH^* and the desorption of CO. This work may pioneer a new method on seeking high-efficiency and worthwhile electrocatalysts for CO₂ RR and Zn-CO₂ battery.