Wu Zhitan, Meng Nannan, Yang Rong, Chen Maoxin, Pan Jinhui, Chi Sijia, Wu Chao, Xi Shibo, Liu Yuan, Ou Yingqing, Wu Wenya, Han Shuhe, Zhang Bin, Yang Quan-Hong, Ping Loh Kian
Joint School of National University of Singapore and Tianjin University, International Campus of Tianjin University, Binhai New City, Fuzhou 350207, China.
Department of Chemistry, National University of Singapore, 3 Science Drive 3, Singapore, 117543, Singapore.
Angew Chem Int Ed Engl. 2025 Feb 17;64(8):e202420283. doi: 10.1002/anie.202420283. Epub 2024 Dec 23.
The electrosynthesis of multi-carbon (C) alcohols, specifically ethanol and n-propanol through CO electroreduction (CORR) in HO, presents a sustainable pathway for intermittent renewable energy storage and a low-carbon economy. However, achieving high selectivity for alcohol production at industrial current densities is kinetically hampered by side reactions such as ethylene generation and hydrogen evolution reaction, which result from competing adsorption of *CO and *H. In this study, we developed a Cu/Zn alloy catalyst to simultaneously enhance the activity and selectivity for alcohol production by increasing CO capture capacity and enriching active hydrogen on Cu sites. Our findings demonstrate that the Cu/5Zn alloy with a molar ratio of Cu to Zn of 95 : 5 exhibits a Faradaic efficiency of 50 % for the selective electrosynthesis of C alcohols during ampere-level CO electrolysis. Mechanistic investigations revealed that the Cu/Zn alloy promotes polarized Cu sites, enhancing CO adsorption while facilitating the spillover of hydrogen atoms from Zn to Cu sites, contributing to selective alcohol formation.
通过在水中进行CO电还原（CORR）来电合成多碳（C）醇，特别是乙醇和正丙醇，为间歇性可再生能源存储和低碳经济提供了一条可持续途径。然而，在工业电流密度下实现高选择性的醇类生产在动力学上受到诸如乙烯生成和析氢反应等副反应的阻碍，这些副反应是由CO和H的竞争吸附导致的。在本研究中，我们开发了一种Cu/Zn合金催化剂，通过提高CO捕获能力和在Cu位点上富集活性氢，同时增强醇类生产的活性和选择性。我们的研究结果表明，在安培级CO电解过程中，Cu与Zn摩尔比为95∶5的Cu/5Zn合金对于C醇的选择性电合成表现出50%的法拉第效率。机理研究表明，Cu/Zn合金促进了极化的Cu位点，增强了CO吸附，同时促进了氢原子从Zn向Cu位点的溢流，有助于选择性地形成醇类。
