Li Pengsong, Lu Xu, Wu Zishan, Wu Yueshen, Malpass-Evans Richard, McKeown Neil B, Sun Xiaoming, Wang Hailiang
State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing, 100029, P. R. China.
Department of Chemistry, Yale University, New Haven, CT, 06520, USA.
Angew Chem Int Ed Engl. 2020 Jun 26;59(27):10918-10923. doi: 10.1002/anie.202003093. Epub 2020 Apr 21.
Hybrid electrodes with improved O tolerance and capability of CO conversion into liquid products in the presence of O are presented. Aniline molecules are introduced into the pore structure of a polymer of intrinsic microporosity to expand its gas separation functionality beyond pure physical sieving. The chemical interaction between the acidic CO molecule and the basic amino group of aniline renders enhanced CO separation from O . Loaded with a cobalt phthalocyanine-based cathode catalyst, the hybrid electrode achieves a CO Faradaic efficiency of 71 % with 10 % O in the CO feed gas. The electrode can still produce CO at an O /CO ratio as high as 9:1. Switching to a Sn-based catalyst, for the first time O -tolerant CO electroreduction to liquid products is realized, generating formate with nearly 100 % selectivity and a current density of 56.7 mA cm in the presence of 5 % O .
本文介绍了一种具有改进的氧耐受性以及在有氧存在时将一氧化碳转化为液体产物能力的混合电极。将苯胺分子引入固有微孔聚合物的孔结构中，以将其气体分离功能扩展到纯物理筛分之外。酸性一氧化碳分子与苯胺碱性氨基之间的化学相互作用增强了一氧化碳与氧的分离。负载基于钴酞菁的阴极催化剂后，该混合电极在一氧化碳原料气中含10%氧气的情况下实现了71%的一氧化碳法拉第效率。该电极在氧/一氧化碳比高达9:1时仍能产生一氧化碳。切换到基于锡的催化剂后，首次实现了耐氧的一氧化碳电还原为液体产物，在存在5%氧气的情况下，以近100%的选择性生成甲酸盐，电流密度为56.7 mA/cm²。
