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用于选择性和稳定的CO电还原的具有三明治状C/Cu/C催化剂的表面重构

Surface Reconstruction with a Sandwich-like C/Cu/C Catalyst for Selective and Stable CO Electroreduction.

作者信息

Ni Wei, Yixiang Zhou, Yao Yebo, Wang Xiaoxuan, Zhao Rui, Yang Zhiyu, Li Xin, Yan Yi-Ming

机构信息

State Key Lab of Organic-Inorganic Composites, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing 100029, People's Republic of China.

School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing 100081, People's Republic of China.

出版信息

ACS Appl Mater Interfaces. 2022 Mar 23;14(11):13261-13270. doi: 10.1021/acsami.1c23662. Epub 2022 Mar 8.

Abstract

For the steady electroreduction of carbon dioxide (CORR) to value-added chemicals with high efficiency, the uncontrollable surface reconstruction under highly reducing conditions is a critical issue in electrocatalyst design. Herein, we construct a catalyst model with a sandwich-like structure composed of highly reactive metallic Cu nanosheet that is confined in thin carbon layers (denoted as C/Cu/C nanosheet). The sandwich-like C/Cu/C nanosheet avoids the oxidation of the active site of metallic Cu at an ambient atmosphere owing to the protective coating of the carbon layer, which inhibits the surface reconstruction that occurs via the dissolution of copper oxides and redeposition of dissolved Cu ions. The as-prepared C/Cu/C nanosheet exhibits a prominent Faradaic efficiency (FE) of 47.8% for CH products at -1.0 V with a current density of 20.3 mA·cm and stable production of CH during 12 h operation with negligible selectivity loss. Our findings provide an effective strategy of restraining surface reconstruction for the design of selective and stable electrocatalysts toward CORR.

摘要

为了将二氧化碳高效稳定地电还原为高附加值化学品,在高还原条件下无法控制的表面重构是电催化剂设计中的一个关键问题。在此,我们构建了一种具有三明治结构的催化剂模型,该结构由被限制在薄碳层中的高活性金属铜纳米片组成(表示为C/Cu/C纳米片)。由于碳层的保护涂层,这种三明治状的C/Cu/C纳米片在环境气氛中避免了金属铜活性位点的氧化,从而抑制了通过氧化铜溶解和溶解的铜离子再沉积而发生的表面重构。所制备的C/Cu/C纳米片在-1.0 V时对CH产物表现出47.8%的显著法拉第效率(FE),电流密度为20.3 mA·cm ,在12小时的运行过程中CH产量稳定,选择性损失可忽略不计。我们的研究结果为设计用于二氧化碳电还原反应的选择性和稳定电催化剂提供了一种抑制表面重构的有效策略。

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