Enhanced multi-carbon alcohol electroproduction from CO via modulated hydrogen adsorption

作者：Jun Li, Ao-Ni Xu, Fengwang Li, ZiYun Wang, Chengqin Zou, Christine M. Gabardo, Yuhang Wang, A. Ozden, Yi Xu, Dae-Hyun Nam, Yanwei Lum, Joshua Wicks, Bin Chen, Zhiqiang Wang, Jiatang Chen, Yunzhou Wen, Taotao Zhuang, Mingchuan Luo, Xiwen Du, T. Sham, Bo Zhang, E. Sargent, D. Sinton · 发表于：Nature Communications · 年份：2020 · DOI：10.1038/s41467-020-17499-5 · 被引用次数：117 · 研究领域：Chemistry、Medicine

Multi-carbon alcohols such as ethanol are valued as fuels in view of their high energy density and ready transport. Unfortunately, the selectivity toward alcohols in CO2/CO electroreduction is diminished by ethylene production, especially when operating at high current densities (>100 mA cm−2). Here we report a metal doping approach to tune the adsorption of hydrogen at the copper surface and thereby promote alcohol production. Using density functional theory calculations, we screen a suite of transition metal dopants and find that incorporating Pd in Cu moderates hydrogen adsorption and assists the hydrogenation of C2 intermediates, providing a means to favour alcohol production and suppress ethylene. We synthesize a Pd-doped Cu catalyst that achieves a Faradaic efficiency of 40% toward alcohols and a partial current density of 277 mA cm−2 from CO electroreduction. The activity exceeds that of prior reports by a factor of 2. The electrocatalytic upgrading of CO to higher-value fuels provides a promising route to multi-carbon alcohol products. Here, the authors show that high alcohol selectivity and activity can be achieved by incorporating palladium in copper.