Yin Yaoyu, Ling Zhongnan, Liu Shiqiang, Jiao Jiapeng, Wang Yiyong, Peng Yaguang, Tong Xing, Zhou Meng, Feng Rongjuan, Xing Xueqing, Xu Yi, Zhu Qinggong, Sun Xiaofu, Luo Mingchuan, Kang Xinchen, Han Buxing
Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Centre for Excellence in Molecular Sciences, Centre for Carbon Neutral Chemistry, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China.
School of Chemistry, University of Chinese Academy of Sciences, Beijing 100049, China.
J Am Chem Soc. 2025 Jul 23;147(29):25584-25591. doi: 10.1021/jacs.5c06402. Epub 2025 Jul 11.
The electroreduction of CO to CH offers a promising avenue for advancing carbon neutrality and promoting sustainable chemical manufacturing. In acidic environments, while long-term operational stability and CO utilization efficiency are enhanced, the formation of C-C bonds is hindered due to the weak adsorption of *CO intermediates and the competing hydrogen evolution reaction (HER). Theoretical studies suggest that K cations with reduced bound water content can strengthen the adsorption of the critical *CO intermediate, and that elevated K concentrations on the Cu electrode surface significantly facilitate CO electroreduction to CH. In this work, a catalyst termed Cu was developed by strategically modifying the Nafion ionomer distribution within the catalyst layer. This structural adjustment effectively lowers the bound water associated with K cations and concurrently elevates the surface concentration of K on the Cu electrode, thereby promoting C-C coupling for CH formation while suppressing HER. Consequently, Cu achieves a Faradaic efficiency of 70.2% for CH production, accompanied by a high partial current density of 561.6 mA cm in an acidic electrolyte (pH = 1).
将CO电还原为CH为推进碳中和和促进可持续化学制造提供了一条有前景的途径。在酸性环境中，虽然长期运行稳定性和CO利用效率得到了提高，但由于CO中间体的弱吸附和竞争性析氢反应（HER），C-C键的形成受到阻碍。理论研究表明，结合水含量降低的K阳离子可以增强关键CO中间体的吸附，并且Cu电极表面上较高的K浓度显著促进了CO电还原为CH。在这项工作中，通过策略性地改变催化剂层内Nafion离聚物的分布，开发了一种名为Cu的催化剂。这种结构调整有效地降低了与K阳离子相关的结合水，并同时提高了Cu电极上K的表面浓度，从而促进C-C偶联以形成CH，同时抑制HER。因此，Cu在酸性电解质（pH = 1）中实现了70.2%的CH生成法拉第效率，同时伴随着561.6 mA cm的高部分电流密度。
