Crown ether functionalization boosts CO2 electroreduction to ethylene on copper-based MOFs†

IF 4.3 2区化学 Q2 CHEMISTRY, MULTIDISCIPLINARY

Chemical Communications Pub Date : 2025-01-14 DOI:10.1039/d4cc06719c

Xuan Zheng , Siheng Yang , Dingwen Chen , Yuxuan Kong , Tianhua Cui , Xueli Zheng , Haiyan Fu , Weichao Xue , Shuang Li , Chong Cheng , Hua Chen , Ruixiang Li , Jiaqi Xu

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Abstract

The electroconversion of CO₂ into ethylene (C₂H₄) offers a promising solution to environmental and energy challenges. Crown ether (CE) modification significantly enhances the C₂H₄ selectivity of copper-based MOFs, improving C₂H₄ faradaic efficiency (FE) in CuBTC, CuBDC, and CuBDC-NH₂ by 3.1, 1.7, and 2.4 times, respectively. Among these, CuBTC achieves the highest FE for C₂H₄, reaching ca. 52% at 120 mA cm⁻². Control experiments and in situ Fourier transform infrared spectroscopy (FTIR) reveal that CE stabilizes Cu⁺ during the catalyst's in situ reconstruction, promoting the formation of Cu₂O, which is more favorable for C₂H₄ production. Furthermore, CE increases the local concentration of K⁺ at the catalyst–electrolyte interface, enhancing *CO adsorption and facilitating C–C coupling reactions. This process promotes the formation of key intermediates, such as *CO*CO, *CO*COH and *COCHO, ultimately boosting C₂H₄ production.

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冠醚功能化促进铜基mof上CO2电还原成乙烯

二氧化碳电转化为乙烯（C2H4）为解决环境和能源挑战提供了一个有前途的解决方案。冠醚（CE）改性显著提高了铜基mof对C2H4的选择性，使CuBTC、CuBDC和CuBDC- nh2中的C2H4法达化效率（FE）分别提高了3.1倍、1.7倍和2.4倍。其中，cutc对C2H4的FE最高，在120 mA cm−2时达到约52%。控制实验和原位傅里叶变换红外光谱（FTIR）结果表明，CE在催化剂原位重构过程中稳定Cu+，促进Cu2O的生成，更有利于C2H4的生成。此外，CE增加了催化剂-电解质界面处K+的局部浓度，增强了*CO的吸附，促进了C-C偶联反应。这一过程促进了*CO*CO、*CO*COH和*COCHO等关键中间体的形成，最终促进了C2H4的生成。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Chemical Communications 化学-化学综合

CiteScore

8.60

自引率

4.10%

发文量

2705

审稿时长

1.4 months

期刊介绍： ChemComm (Chemical Communications) is renowned as the fastest publisher of articles providing information on new avenues of research, drawn from all the world''s major areas of chemical research.