Wang Jigang, Sun Yinggang, Li Meiyin, Yi Yuxiang, Liu Qiang, Li Zhongfang, Wang Likai
School of Chemistry and Chemical Engineering, Shandong University of Technology, Zibo, Shandong 255049, China.
Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, Qingdao, Shandong 266101, China.
Nano Lett. 2025 May 21;25(20):8168-8175. doi: 10.1021/acs.nanolett.5c01034. Epub 2025 May 7.
Electroreduction of CO (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) 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) can exceed 96%, with a CO partial current density () of 48 mA cm. Additionally, Br-Ni/NC-a is used in a Zn-CO battery (ZCB); the power density can reach 2.6 mW cm, 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.
将一氧化碳电还原（ECR）为一氧化碳或合成气是减轻温室气体排放的有效方法。在此，制备了包覆有卤素/氮共掺杂碳的镍纳米颗粒（X-Ni/NC-a）。Cl-Ni/NC-a在不同电压下可获得三种重要的合成气组成（CO:H），分别为0.97、0.51和0.32，这分别是氢甲酰化、甲醇和乙醇合成的比例。对于Br-Ni/NC-a，一氧化碳的法拉第效率（FE）可超过96%，一氧化碳的分电流密度（）为48 mA cm。此外，Br-Ni/NC-a用于锌-一氧化碳电池（ZCB）；功率密度可达到2.6 mW cm，充放电稳定性可达到110小时。密度泛函理论计算表明，镍纳米颗粒与卤素/氮共掺杂碳之间的强相互作用调节了催化剂的电子结构，影响了中间体的吸附/脱附。本研究为卤素掺杂调节ECR的选择性以及催化剂在ZCB中的潜在应用提供了可行方案。
