Zhong Yang, Xu Yan, Ma Jun, Wang Cheng, Sheng Siyu, Cheng Congtian, Li Mengxuan, Han Lu, Zhou Linlin, Cai Zhao, Kuang Yun, Liang Zheng, Sun Xiaoming
State Key Laboratory of Chemical Resource Engineering, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, 100029, China.
Electrical Engineering and Automation, Shandong University of Science and Technology, Tsingtao, 266590, China.
Angew Chem Int Ed Engl. 2020 Oct 19;59(43):19095-19101. doi: 10.1002/anie.202005522. Epub 2020 Aug 31.
In this work, an artificial electrode/electrolyte (E/E) interface, made by coating the electrode surface with a quaternary ammonium cation (R N ) surfactant, was successfully developed, leading to a change in the CO reduction reaction (CO RR) pathway. This artificial E/E interface, with high CO permeability, promotes CO transportation and hydrogenation, as well as suppresses the hydrogen evolution reaction (HER). Linear and branched surfactants facilitated formic acid and CO production, respectively. Molecular dynamics simulations show that the artificial interface provided a facile CO diffusion pathway. Moreover, density-functional theory (DFT) calculations revealed the stabilization of the key intermediate, OCHO*, through interactions with R N . This strategy might also be applicable to other electrocatalytic reactions where gas consumption is involved.
在这项工作中，通过用季铵阳离子（RN）表面活性剂涂覆电极表面成功开发了一种人工电极/电解质（E/E）界面，这导致了一氧化碳还原反应（CO RR）途径的改变。这种具有高CO渗透性的人工E/E界面促进了CO的传输和氢化，同时抑制了析氢反应（HER）。线性和支化表面活性剂分别促进了甲酸和CO的生成。分子动力学模拟表明，人工界面提供了一条便捷的CO扩散途径。此外，密度泛函理论（DFT）计算揭示了关键中间体OCHO*通过与RN相互作用而得到稳定。该策略也可能适用于其他涉及气体消耗的电催化反应。
