Lyu Zhiheng, Zhu Shangqian, Xie Minghao, Zhang Yu, Chen Zitao, Chen Ruhui, Tian Mengkun, Chi Miaofang, Shao Minhua, Xia Younan
School of Chemistry and Biochemistry, Georgia Institute of Technology, Atlanta, GA, 30332, USA.
Department of Chemical and Biological Engineering, and Hong Kong Branch of the Southern Marine Science and Engineering Guangdong Laboratory, The Hong Kong University of Science and Technology, Clear Water Bay, Kowloon, Hong Kong, P. R. China.
Angew Chem Int Ed Engl. 2021 Jan 25;60(4):1909-1915. doi: 10.1002/anie.202011956. Epub 2020 Nov 20.
Copper nanostructures are promising catalysts for the electrochemical reduction of CO because of their unique ability to produce a large proportion of multi-carbon products. Despite great progress, the selectivity and stability of such catalysts still need to be substantially improved. Here, we demonstrate that controlling the surface oxidation of Cu nanowires (CuNWs) can greatly improve their C selectivity and stability. Specifically, we achieve a faradaic efficiency as high as 57.7 and 52.0 % for ethylene when the CuNWs are oxidized by the O from air and aqueous H O , respectively, and both of them show hydrogen selectivity below 12 %. The high yields of C products can be mainly attributed to the increase in surface roughness and the generation of defects and cavities during the electrochemical reduction of the oxide layer. Our results also indicate that the formation of a relatively thick, smooth oxide sheath can improve the catalytic stability by mitigating the fragmentation issue.
铜纳米结构因其独特的能力,能够大量生产多碳产物,是用于电化学还原CO的有前景的催化剂。尽管取得了巨大进展,但这类催化剂的选择性和稳定性仍需大幅提高。在这里,我们证明控制铜纳米线(CuNWs)的表面氧化可以极大地提高其碳选择性和稳定性。具体而言,当CuNWs分别被空气中的O和水溶液中的H₂O氧化时,我们实现了乙烯的高达57.7%和52.0%的法拉第效率,并且它们两者的氢选择性均低于12%。碳产物的高产率主要可归因于在氧化物层的电化学还原过程中表面粗糙度的增加以及缺陷和空洞的产生。我们的结果还表明,形成相对较厚、光滑的氧化鞘层可以通过减轻破碎问题来提高催化稳定性。