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

Abstract Electrochemical CO 2 reduction reaction (CO 2 RR), powered by renewable electricity, has attracted great attention for producing high value‐added fuels and chemicals, as well as feasibly mitigating CO 2 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‐CO 2 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 CO 2 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 CO 2 RR and Zn‐CO 2 battery.