Zhou Jun-Hao, Yuan Chen-Yue, Zheng Ya-Li, Yin Hai-Jing, Yuan Kun, Sun Xiao-Chen, Zhang Ya-Wen
Beijing National Laboratory for Molecular Sciences, College of Chemistry and Molecular Engineering, Peking University No. 5 Yiheyuan Road, Haidian District Beijing 100871 China
RSC Adv. 2021 Nov 29;11(61):38486-38494. doi: 10.1039/d1ra07507a.
Tandem catalysis, in which a CO-to-C process is divided into a CO-to-CO/*CO step and a CO/*CO-to-C step, is promising for enhancing the C product selectivity when using Cu-based electrochemical CO reduction catalysts. In this work, a nanoporous hollow Au/CuO-CuO tandem catalyst was used for catalyzing the eCORR, which exhibited a C product FE of 52.8% at -1.0 V RHE and a C product partial current density of 78.77 mA cm at -1.5 V RHE. In addition, the C product FE stably remained at over 40% over a wide potential range, from -1.0 V to -1.5 V. This superior performance was attributed to good matching in terms of the optimal working potential and charge-transfer resistance between CO/*CO-production sites (Au/CuO) and CO/*CO-reduction sites (CuO). This site pair matching effect ensured sufficient supplies of CO/*CO and electrons at CuO sites at the working potentials, thus dramatically enhancing the formation rate of C products.
串联催化是将CO到C的过程分为CO到CO/*CO步骤和CO/*CO到C步骤,在使用铜基电化学CO还原催化剂时,有望提高C产物的选择性。在这项工作中,一种纳米多孔中空Au/CuO-CuO串联催化剂被用于催化电化学CO还原反应(eCORR),在-1.0 V(相对于可逆氢电极,RHE)时,其C产物的法拉第效率(FE)为52.8%,在-1.5 V(相对于可逆氢电极,RHE)时,C产物的分电流密度为78.77 mA cm²。此外,在-1.0 V至-1.5 V的宽电位范围内,C产物的FE稳定保持在40%以上。这种优异的性能归因于CO/*CO生成位点(Au/CuO)和CO/*CO还原位点(CuO)在最佳工作电位和电荷转移电阻方面的良好匹配。这种位点对匹配效应确保了在工作电位下CuO位点有足够的CO/*CO和电子供应,从而显著提高了C产物的生成速率。