Highly Active and Stable Cu-Cd Bimetallic Oxides for Enhanced Electrochemical CO2 Reduction.

IF 3.9 2区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Chemistry - A European Journal Pub Date : 2025-01-14 Epub Date: 2024-11-25 DOI:10.1002/chem.202403261
Guoliang Mei, Yanling Zhai, Weiwei Guo, Doudou Liu, Zijian Fang, Guixian Xie, Zongxia Duan, Xianzhen Lang, Zhijun Zhu, Xiaoquan Lu, Jianguo Tang
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Abstract

Electrochemical reduction of carbon dioxide (CO2) can produce value-added chemicals such as carbon monoxide (CO) and multicarbon (C2+). However, the complex reaction pathways of CO2 electro-reduction reaction (CO2RR) greatly limit the product selectivity and conversion efficiency. Herein, the Cu-Cd bimetallic oxides catalyst was designed and applied for the CO2RR. The optimized 4.73 %Cd-CuO exhibits remarkable electrocatalytic CO2RR activity for selective CO production in H-cell using 0.5 M 1-butyl-3-methylimidazolium hexafluorophosphate ([Bmim]PF6)/MeCN as electrolyte. The Faradaic efficiency of CO (FE(CO)) can be maintained above 90 % over a wide potential range of -2.0 to -2.4 V vs. Ag/Ag+. Particularly, the catalyst achieves an impressive FE(CO) of 96.3 % with a current density of 60.7 mA cm-2 at -2.2 V vs. Ag/Ag+. Furthermore, scaling up the 4.73 %Cd-CuO catalyst into a flow cell can reach 56.64 % FE of C2+ products (ethylene, ethanol and n-propanol) with a current density as high as 600 mA cm-2 steadily. The excellent CO2RR performance of the as-synthesized 4.73 %Cd-CuO can be mainly attributed to the introduction of CdO to improve the ability of CuO to activate CO2, the electronic interactions between Cu and Cd can boost the activation and conversion the key intermediates of CO2RR and ensure the continuous stability of the 4.73 %Cd-CuO in electrolysis process.

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用于增强电化学二氧化碳还原的高活性、高稳定性铜镉双金属氧化物。
二氧化碳(CO2)的电化学还原反应可以生产一氧化碳(CO)和多碳(C2+)等高附加值化学品。然而,二氧化碳电还原反应(CO2RR)复杂的反应途径极大地限制了产品的选择性和转化效率。本文设计了 Cu-Cd 双金属氧化物催化剂,并将其应用于 CO2RR 反应。优化后的 4.73%Cd-CuO 在以 0.5 M 1-butyl-3-methylimidazolium hexafluorophosphate ([Bmim]PF6)/MeCN 为电解质的 H-cell 中选择性生产 CO2 时表现出显著的电催化 CO2RR 活性。在相对于 Ag/Ag+ 的 -2.0 至 -2.4 V 的宽电位范围内,一氧化碳的法拉第效率(FE(CO))可保持在 90% 以上。特别是在 -2.2 V(相对于 Ag/Ag+)的电流密度为 60.7 mA cm-2 时,催化剂的 FE(CO) 效率达到了 96.3%,令人印象深刻。此外,将 4.73%Cd-CuO 催化剂放大到流动池中,C2+ 产物(乙烯、乙醇和正丙醇)的 FE 可达到 56.64%,电流密度稳定在 600 mA cm-2 左右。所合成的 4.73%Cd-CuO 具有优异的 CO2RR 性能,主要归功于 CdO 的引入提高了 CuO 活化 CO2 的能力,Cu 和 Cd 之间的电子相互作用促进了 CO2RR 关键中间产物的活化和转化,并确保了 4.73%Cd-CuO 在电解过程中的持续稳定性。
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来源期刊
Chemistry - A European Journal
Chemistry - A European Journal 化学-化学综合
CiteScore
7.90
自引率
4.70%
发文量
1808
审稿时长
1.8 months
期刊介绍: Chemistry—A European Journal is a truly international journal with top quality contributions (2018 ISI Impact Factor: 5.16). It publishes a wide range of outstanding Reviews, Minireviews, Concepts, Full Papers, and Communications from all areas of chemistry and related fields. Based in Europe Chemistry—A European Journal provides an excellent platform for increasing the visibility of European chemistry as well as for featuring the best research from authors from around the world. All manuscripts are peer-reviewed, and electronic processing ensures accurate reproduction of text and data, plus short publication times. The Concepts section provides nonspecialist readers with a useful conceptual guide to unfamiliar areas and experts with new angles on familiar problems. Chemistry—A European Journal is published on behalf of ChemPubSoc Europe, a group of 16 national chemical societies from within Europe, and supported by the Asian Chemical Editorial Societies. The ChemPubSoc Europe family comprises: Angewandte Chemie, Chemistry—A European Journal, European Journal of Organic Chemistry, European Journal of Inorganic Chemistry, ChemPhysChem, ChemBioChem, ChemMedChem, ChemCatChem, ChemSusChem, ChemPlusChem, ChemElectroChem, and ChemistryOpen.
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