Chuai Hongyuan, Yang Haibei, Zhang Sheng
School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China.
ACS Appl Mater Interfaces. 2024 May 15;16(19):24823-24830. doi: 10.1021/acsami.4c04318. Epub 2024 May 6.
Ni single-atom-decorated nitrogen-doped carbon materials (Ni-N-C) have demonstrated high efficiency in the electrochemical reduction of CO (CORR) to CO. In this study, Ni-N-C active sites were embedded within a carbon membrane via an electrospinning and pyrolysis process. The resulting self-supported carbon membrane hosting Ni-N-C sites could be directly utilized as an electrode for the CORR. To enhance the CORR performance of the carbon membrane, the porous structure of the carbon membrane was fine-tuned by incorporating a pore-forming agent. The optimized porous carbon membrane electrode, K-Ni-NC, achieved an impressive CO faradaic efficiency (FE) of over 90% within a wide potential range from -0.8 to -1.6 V vs RHE for CORR. Additionally, it maintained an FE of above 90% at -0.8 V vs RHE throughout a 30 h durability test in an H-cell. Further analysis has revealed that the porous structure of the carbon membrane not only facilitates the mass transport of CO but also increases the level of exposure of active sites during the CORR.
镍单原子修饰的氮掺杂碳材料（Ni-N-C）在将CO电化学还原为CO（CORR）方面已展现出高效性。在本研究中，通过静电纺丝和热解过程将Ni-N-C活性位点嵌入碳膜中。所得负载Ni-N-C位点的自支撑碳膜可直接用作CORR的电极。为提高碳膜的CORR性能，通过加入造孔剂对碳膜的多孔结构进行微调。优化后的多孔碳膜电极K-Ni-NC在相对于可逆氢电极（RHE）为-0.8至-1.6 V的宽电位范围内，CORR的CO法拉第效率（FE）超过90%，令人印象深刻。此外，在H型电解池中进行的30小时耐久性测试中，在相对于RHE为-0.8 V时，其FE保持在90%以上。进一步分析表明，碳膜的多孔结构不仅有助于CO的传质，还增加了CORR过程中活性位点的暴露程度。
