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通过稳定的铜/铜界面实现直接OC-CHO偶联以实现高C产物选择性电还原。

Direct OC-CHO coupling towards highly C products selective electroreduction over stable Cu/Cu interface.

作者信息

Zhang Xin Yu, Lou Zhen Xin, Chen Jiacheng, Liu Yuanwei, Wu Xuefeng, Zhao Jia Yue, Yuan Hai Yang, Zhu Minghui, Dai Sheng, Wang Hai Feng, Sun Chenghua, Liu Peng Fei, Yang Hua Gui

机构信息

Key Laboratory for Ultrafine Materials of Ministry of Education, Shanghai Engineering Research Center of Hierarchical Nanomaterials, School of Materials Science and Engineering, East China University of Science and Technology, 130 Meilong Road, Shanghai, 200237, China.

State Key Laboratory of Chemical Engineering, School of Chemical Engineering, East China University of Science and Technology, 130 Meilong Road, Shanghai, 200237, China.

出版信息

Nat Commun. 2023 Nov 24;14(1):7681. doi: 10.1038/s41467-023-43182-6.

Abstract

Electroreduction of CO to valuable multicarbon (C) products is a highly attractive way to utilize and divert emitted CO. However, a major fraction of C selectivity is confined to less than 90% by the difficulty of coupling C-C bonds efficiently. Herein, we identify the stable Cu/Cu interfaces derived from copper phosphate-based (CuPO) electrocatalysts, which can facilitate C production with a low-energy pathway of OC-CHO coupling verified by in situ spectra studies and theoretical calculations. The CuPO precatalyst shows a high Faradaic efficiency (FE) of 69.7% towards CH in an H-cell, and exhibits a significant FE of 90.9% under industrially relevant current density (j = -350 mA cm) in a flow cell configuration. The stable Cu/Cu interface breaks new ground for the structural design of electrocatalysts and the construction of synergistic active sites to improve the activity and selectivity of valuable C products.

摘要

将CO电还原为有价值的多碳(C)产物是一种极具吸引力的利用和转移排放CO的方式。然而,由于有效耦合C-C键的困难,大部分C选择性被限制在90%以下。在此,我们确定了源自磷酸铜基(CuPO)电催化剂的稳定Cu/Cu界面,通过原位光谱研究和理论计算验证,该界面可以通过OC-CHO耦合的低能途径促进C产物的生成。CuPO预催化剂在H型电解池中对CH表现出69.7%的高法拉第效率(FE),在流动电解池配置下,在工业相关电流密度(j = -350 mA cm)下表现出90.9%的显著FE。稳定的Cu/Cu界面为电催化剂的结构设计和构建协同活性位点以提高有价值C产物的活性和选择性开辟了新途径。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/4279/10667242/4831b50d4c2f/41467_2023_43182_Fig1_HTML.jpg

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