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High carbon utilization in CO2 reduction to multi-carbon products in acidic media

Xie Yi,Ou Pengfei,Wang Xue,Xu Zhanyou,Li Yuguang C.,Wang Ziyun,Huang Jianan Erick,Wicks Joshua,McCallum Christopher,Wang Ning,Wang Yuhang,Chen Tianxiang,Lo Benedict T. W.,Sinton David,Yu Jimmy C.,Wang Ying,Sargent Edward H.

Renewable electricity-powered CO 2 reduction to multi-carbon (C 2+ ) products offers a promising route to realization of low-carbon-footprint fuels and chemicals. However, a major fraction of input CO 2 (>85%) is consumed by the electrolyte through reactions with hydroxide to form carbonate/bicarbonate in both alkaline and neutral reactors. Acidic conditions offer a solution to overcoming this limitation, but also promote the hydrogen evolution reaction. Here we report a design strategy that suppresses hydrogen evolution reaction activity by maximizing the co-adsorption of CO and CO 2 on Cu-based catalysts to weaken H* binding. Using density functional theory studies, we found Pd–Cu promising for selective C 2+ production over C 1 , with the lowest ∆ G OCCOH* and ∆ G OCCOH* - ∆ G CHO* . We synthesized Pd–Cu catalysts and report a crossover-free system (liquid product crossover <0.05%) with a Faradaic efficiency of 89 ± 4% for CO 2 to C 2+ at 500 mA cm −2 , simultaneous with single-pass CO 2 utilization of 60 ± 2% to C 2+ .