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通过设计丰富的供电子铜物种在接近理论电位下将CO电催化还原为乙醇

Electrocatalytic Reduction of CO to Ethanol at Close to Theoretical Potential via Engineering Abundant Electron-Donating Cu Species.

作者信息

Guo Chengying, Guo Yihe, Shi Yanmei, Lan Xianen, Wang Yuting, Yu Yifu, Zhang Bin

机构信息

Institute of Molecular Plus, Department of Chemistry, School of Science, Tianjin University, Tianjin, 300072, China.

College of Chemistry, Nankai University, Tianjin, 300071, China.

出版信息

Angew Chem Int Ed Engl. 2022 Aug 8;61(32):e202205909. doi: 10.1002/anie.202205909. Epub 2022 Jun 23.

Abstract

Electrochemical CO reduction to liquid multi-carbon alcohols provides a promising way for intermittent renewable energy reservation and greenhouse effect mitigation. Cu (0<δ<1) species on Cu-based electrocatalysts can produce ethanol, but the in situ formed Cu is insufficient and easily reduced to Cu . Here a Cu S catalyst with abundant Cu (0<δ<1) species is designedly synthesized and exhibited an ultralow overpotential of 0.19 V for ethanol production. The catalyst not only delivers an outstanding ethanol selectivity of 86.9 % and a Faradaic efficiency of 73.3 % but also provides a long-term stability of Cu , gaining an economic profit based on techno-economic analysis. The calculation and in situ spectroscopic results reveal that the abundant Cu sites display electron-donating ability, leading to the decrease of the reaction barrier in the potential-determining C-C coupling step and eventually making the applied potential close to the theoretical value.

摘要

将电化学CO还原为液态多碳醇为间歇性可再生能源储存和缓解温室效应提供了一条很有前景的途径。铜基电催化剂上的Cu(0<δ<1)物种可以产生乙醇,但原位形成的Cu不足且容易还原为Cu。在此,设计合成了一种具有丰富Cu(0<δ<1)物种的CuS催化剂,其在乙醇生产中表现出0.19 V的超低过电位。该催化剂不仅具有86.9%的出色乙醇选择性和73.3%的法拉第效率,还具有Cu的长期稳定性,基于技术经济分析获得了经济效益。计算和原位光谱结果表明,丰富的Cu位点具有给电子能力,导致在决定电位的C-C偶联步骤中反应势垒降低,最终使施加电位接近理论值。

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