Wang Yiyong, Cheng Yingying, Liu Shiqiang, Yin Yaoyu, Yang Jiahao, Wang Hengan, Li Ke, Zhou Meng, Jiao Jiapeng, Zhang Pei, Qian Qingli, Zhu Qinggong, Sun Xiaofu, Xu Yi, 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.
Angew Chem Int Ed Engl. 2025 Feb 24;64(9):e202420661. doi: 10.1002/anie.202420661. Epub 2025 Jan 16.
Modulating the surface microenvironment of electrodes stands as a pivotal aspect in enhancing the electrocatalytic performance for CO electroreduction. Herein, we propose an innovative approach by incorporating a small amount of linear oligomer, polyethylene glycol (PEG), into CuO catalysts during the preparation of the Cu electrode. The Faradaic efficiency (FE) toward multicarbon products (C) increases from 69.3 % over Cu electrode without PEG to 90.3 % over Cu electrode at 500 mA cm in 1 M KOH in a flow cell. In situ investigations and theoretical calculations reveal that PEG molecules significantly modify the microenvironment on the Cu surface through hydrogen bond interactions. This modification leads to the relaxation of Nafion, increasing the availability of active sites and enhancing the adsorption of *CO and *OH, which in turn promotes C-C coupling. Concurrently, the reconstructed hydrogen bond network reduces the presence of active hydrogen species, thereby inhibiting the hydrogen evolution reaction.
调节电极的表面微环境是提高CO电还原电催化性能的关键环节。在此，我们提出了一种创新方法，即在制备铜电极的过程中，将少量线性低聚物聚乙二醇（PEG）引入到CuO催化剂中。在流动池中，于1 M KOH溶液中，在500 mA cm的电流密度下，对多碳产物（C）的法拉第效率（FE）从不含PEG的铜电极上的69.3%提高到含PEG的铜电极上的90.3%。原位研究和理论计算表明，PEG分子通过氢键相互作用显著改变了铜表面的微环境。这种改变导致Nafion的松弛，增加了活性位点的可用性，并增强了CO和OH的吸附，进而促进了C-C偶联。同时，重构的氢键网络减少了活性氢物种的存在，从而抑制了析氢反应。
