Halogen/Nitrogen Codoped Carbon Encapsulated Ni Nanoparticles for Efficient CO<sub>2</sub> Electroreduction and High-Performance Zn-CO<sub>2</sub> Batteries.

Wang, Jigang; Sun, Yinggang; Li, Meiyin; Yi, Yuxiang; Liu, Qiang; Li, Zhongfang; Wang, Likai · Nano Lett · 2025

basic_science · Level V

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Abstract

Electroreduction of CO<sub>2</sub> (ECR) to CO or syngas is an effective approach to alleviating greenhouse gas emissions. Herein, nickel nanoparticles coated with halogen/nitrogen codoped carbon were prepared (X-Ni/NC-a). Cl-Ni/NC-a can obtain three important syngas compositions (CO:H<sub>2</sub>) under different voltages, such as 0.97, 0.51, and 0.32, which are the ratios for hydroformylation, methanol, and ethanol synthesis, respectively. For Br-Ni/NC-a, the CO Faraday efficiency (FE<sub>co</sub>) can exceed 96%, with a CO partial current density (<i>j</i><sub>co</sub>) of 48 mA cm<sup>-2</sup>. Additionally, Br-Ni/NC-a is used in a Zn-CO<sub>2</sub> battery (ZCB); the power density can reach 2.6 mW cm<sup>-2</sup>, and the charge-discharge stability can reach 110 h. DFT calculations revealed that the strong interaction between nickel nanoparticles and halogen/nitrogen codoped carbon regulates the electronic structure of the catalyst, affecting the adsorption/desorption of intermediates. This study provides a feasible scheme for halogen doping to modulate the selectivity of ECR and the potential application of catalysts in ZCB.