A New Hexagonal Cobalt Nanosheet Catalyst for Selective CO 2 Conversion to Ethanal

作者：Jie Yin, Zhouyang Yin, Jing Jin, Mingzi Sun, Bolong Huang, Honghong Lin, Zhenhui Ma, Michelle Muzzio, Mengqi Shen, Chao Yu, Hong Zhang, Yong Peng, Pinxian Xi, Chun‐Hua Yan, Shouheng Sun · 发表于：Journal of the American Chemical Society · 年份：2021 · DOI：10.1021/jacs.1c06877 · 被引用次数：137 · 研究领域：CO2 Reduction Techniques and Catalysts、Carbon dioxide utilization in catalysis、Ammonia Synthesis and Nitrogen Reduction

We report a new form of catalyst based on ferromagnetic hexagonal-close-packed (hcp) Co nanosheets (NSs) for selective CO 2 RR to ethanal, CH 3 CHO. In all reduction potentials tested from −0.2 to −1.0 V (vs RHE) in 0.5 M KHCO 3 solution, the reduction yields ethanal as a major product and ethanol/methanol as minor products. At −0.4 V, the Faradaic efficiency (FE) for ethanal reaches 60% with current densities of 5.1 mA cm –2 and mass activity of 3.4 A g –1 (total FE for ethanal/ethanol/methanol is 82%). Density functional theory (DFT) calculations suggest that this high CO 2 RR selectivity to ethanal on the hcp Co surface is attributed to the unique intralayer electron transfer, which not only promotes [OC–CO]* coupling but also suppresses the complete hydrogenation of the coupling intermediates to ethylene, leading to highly selective formation of CH 3 CHO.