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用于将CO高效稳定电还原为乙烯的超薄Al₂O₃在铜纳米晶体上的晶面选择性沉积

Facet-Selective Deposition of Ultrathin Al O on Copper Nanocrystals for Highly Stable CO Electroreduction to Ethylene.

作者信息

Li Hui, Yu Peiping, Lei Renbo, Yang Feipeng, Wen Peng, Ma Xiao, Zeng Guosong, Guo Jinghua, Toma Francesca M, Qiu Yejun, Geyer Scott M, Wang Xinwei, Cheng Tao, Drisdell Walter S

机构信息

Joint Center for Artificial Photosynthesis, Chemical Sciences Division, Lawrence Berkeley National Laboratory, 1 Cyclotron Road, Berkeley, California, 94720, USA.

Institute of Functional Nano and Soft Materials, Soochow University, Suzhou, 215123, China.

出版信息

Angew Chem Int Ed Engl. 2021 Nov 15;60(47):24838-24843. doi: 10.1002/anie.202109600. Epub 2021 Oct 13.

Abstract

Catalysts based on Cu nanocrystals (NCs) for electrochemical CO -to-C conversion with high activity have been a subject of considerable interest, but poor stability and low selectivity for a single C product remain obstacles for realizing sustainable carbon-neutral cycles. Here, we used the facet-selective atomic layer deposition (FS-ALD) technique to selectively cover the (111) surface of Cu NCs with ultrathin Al O to increase the exposed facet ratio of (100)/(111), resulting in a faradaic efficiency ratio of C H /CH for overcoated Cu NCs 22 times higher than that for pure Cu NCs. Peak performance of the overcoated catalyst (Cu NCs/Al O -10C) reaches a C H faradaic efficiency of 60.4 % at a current density of 300 mA cm in 5 M KOH electrolyte, when using a gas diffusion electrode flow cell. Moreover, the Al O overcoating effectively suppresses the dynamic mobility and the aggregation of Cu NCs, which explains the negligible activity loss and selectivity degradations of Cu NCs/Al O -10C shown in stability tests.

摘要

基于铜纳米晶体(NCs)的用于电化学CO转化为碳的高活性催化剂一直是备受关注的课题,但稳定性差和对单一碳产物的选择性低仍然是实现可持续碳中性循环的障碍。在此,我们使用面选择性原子层沉积(FS-ALD)技术,用超薄Al₂O₃选择性覆盖Cu NCs的(111)表面,以提高(100)/(111)的暴露面比率,使得包覆后的Cu NCs的C₂H₄/CH₄的法拉第效率比纯Cu NCs高22倍。当使用气体扩散电极流动池时,包覆催化剂(Cu NCs/Al₂O₃-10C)在5M KOH电解液中、电流密度为300 mA cm⁻²时的峰值性能达到C₂H₄法拉第效率60.4%。此外,Al₂O₃包覆有效地抑制了Cu NCs的动态迁移率和聚集,这解释了稳定性测试中Cu NCs/Al₂O₃-10C可忽略不计的活性损失和选择性降解。

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