Nitrogen-doping boosts ∗CO utilization and H2O activation on copper for improving CO2 reduction to C2+ products

• Published in: Green energy & environment 2024-09, Vol.9 (9), p.1459-1465
• Main Authors: Yang, Yisen, Tan, Zhonghao, Zhang, Jianling, Yang, Jie, Zhang, Renjie, Wang, Sha, Song, Yi, Su, Zhuizhui
• Format: Article
• Language: English
• Subjects: Carbon dioxide; Carbon monoxide; Catalysts; Copper; Copper catalyst; Doping; Electrocatalytic CO2 reduction reaction; Electrodes; In situ Raman measurement; Multi-carbon products; Nanoparticles; Nitrogen; Oxidation; Raman spectra; Raman spectroscopy; Scanning electron microscopy; Spectrum analysis; Synergistic effect
• ISSN: 2468-0257; 2096-2797; 2468-0257
• DOI: 10.1016/j.gee.2023.09.002

To improve the electrocatalytic transformation of carbon dioxide (CO2) to multi-carbon (C2+) products is of great importance. Here we developed a nitrogen-doped Cu catalyst, by which the maximum C2+ Faradaic efficiency can reach 72.7% in flow-cell system, with the partial current density reaching 0.62 A cm−2. The in situ Raman spectra demonstrate that the ∗CO adsorption can be strengthened on such a N-doped Cu catalyst, thus promoting the ∗CO utilization in the subsequent C–C coupling step. Simultaneously, the water activation can be well enhanced by N doping on Cu catalyst. Owing to the synergistic effects, the selectivity and activity for C2+ products over the N-deoped Cu catalyst are much improved. N-doped Cu exhibited remarkable efficiency in the electrocatalytic conversion of CO2-to-C2+ products. At a high current density of 0.85 A cm−2, the Faradaic efficiency of C2+ products reached 72.7%. This exceptional catalyst performance can primarily come from the improved ∗CO utilization and H2O activation by N doping. [Display omitted] •N-doped Cu showed a good electrocatalytic performance in converting CO2 to for multi-carbon products.•The N-doped Cu catalyst was synthesized by a electrolyis route for Cu3N precatalyst.•The performance improvement originates from the enhanced ∗CO utilization and H2O activation by N doping.