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从一氧化碳和甲醇原料中高效电子共电合成甲酸盐

Electron-Efficient Co-Electrosynthesis of Formates from CO and Methanol Feedstocks.

作者信息

Li Xin, Chen Qingsong, Sun Wei, He Chengchao, Wen Zhenhai

机构信息

State Key Laboratory of Structural Chemistry, Fujian Provincial Key Laboratory of Material and Techniques toward Hydrogen Energy, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, 350002, Fuzhou, Fujian, China.

College of Chemistry and Materials Science, Fujian Normal University, 350002, Fuzhou, Fujian, China.

出版信息

Angew Chem Int Ed Engl. 2024 Nov 4;63(45):e202412410. doi: 10.1002/anie.202412410. Epub 2024 Sep 17.

Abstract

The electrochemical conversion of CO into valuable chemicals using renewable electricity shows significant promise for achieving carbon neutrality and providing alternative energy storage solutions. However, its practical application still faces significant challenges, including high energy consumption, poor selectivity, and limited stability. Here, we propose a hybrid acid/alkali electrolyzer that couples the acidic CO reduction reaction (CORR) at the cathode with alkaline methanol oxidation reaction (MOR) at the anode. This dual electro-synthesis cell is implemented by developing Bi nanosheets as cathode catalysts and oxide-decorated CuSe nanoflowers as anode catalysts, enabling high-efficiency electron utilization for formate production with over 180 % coulombic efficiency and more than 90 % selectivity for both CORR and MOR conversion. The hybrid acid/alkali CORR-MOR cell also demonstrates long-term stability exceeding 90 hours of continuous operation, delivers a formate partial current density of 130 mA cm at a voltage of only 2.1 V, and significantly reduces electricity consumption compared to the traditional CO electrolysis system. This study illuminates an innovative electron-efficiency and energy-saving techniques for CO electrolysis, as well as the development of highly efficient electrocatalysts.

摘要

利用可再生电力将二氧化碳电化学转化为有价值的化学品,在实现碳中和和提供替代储能解决方案方面显示出巨大的前景。然而,其实际应用仍面临重大挑战,包括高能耗、选择性差和稳定性有限。在此,我们提出了一种混合酸/碱电解槽,它将阴极的酸性二氧化碳还原反应(CORR)与阳极的碱性甲醇氧化反应(MOR)耦合在一起。这种双电合成电池是通过开发铋纳米片作为阴极催化剂和氧化物修饰的硒化铜纳米花作为阳极催化剂来实现的,能够高效利用电子生产甲酸盐,库仑效率超过180%,CORR和MOR转化的选择性均超过90%。混合酸/碱CORR-MOR电池还展示了超过90小时连续运行的长期稳定性,在仅2.1V的电压下提供130mA cm的甲酸盐分电流密度,与传统的二氧化碳电解系统相比,显著降低了电力消耗。这项研究阐明了一种用于二氧化碳电解的创新电子效率和节能技术,以及高效电催化剂的开发。

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