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快速筛选基于铜的双金属电催化剂:镁修饰铜上 CO 高效电催化还原为 C 产物。

Fast Screening for Copper-Based Bimetallic Electrocatalysts: Efficient Electrocatalytic Reduction of CO to C Products on Magnesium-Modified Copper.

机构信息

State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, National Engineering Laboratory for Green Chemical Productions of Alcohols, Ethers and Esters, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, Fujian, P. R. China.

Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), Xiamen, 361005, Fujian, P. R. China.

出版信息

Angew Chem Int Ed Engl. 2022 Dec 19;61(51):e202213423. doi: 10.1002/anie.202213423. Epub 2022 Nov 22.

Abstract

Electroreduction of CO (CO RR) into high value-added chemicals is an attractive route to achieve carbon neutrality. However, the development of an efficient catalyst for CO RR is still largely by trial-and-error and is very time-consuming. Herein, we built an electrocatalyst testing platform featuring a home-built automatic flow cell to accelerate the discovery of efficient catalysts. A fast screening of 109 Cu-based bimetallic catalysts in only 55 h identifies Mg combined with Cu as the best electrocatalyst for CO to C products. The thus designed Mg-Cu catalyst achieves a Faradaic efficiency (FE) of C products up to 80 % with a current density of 1.0 A cm at -0.77 V versus reversible hydrogen electrode (RHE). Systematic experiments with in situ spectroelectrochemistry analyses show that Mg species stabilize Cu sites during CO RR and promote the CO activation, thus enhancing the *CO coverage to promote C-C coupling.

摘要

电还原 CO(CO RR)为高附加值化学品是实现碳中和的一条有吸引力的途径。然而,高效 CO RR 催化剂的开发在很大程度上仍然是通过反复试验,非常耗时。在此,我们构建了一个具有内置自动流动池的电催化剂测试平台,以加速高效催化剂的发现。仅在 55 小时内对 109 种基于铜的双金属催化剂进行快速筛选,确定 Mg 与 Cu 结合为 CO 至 C 产物的最佳电催化剂。所设计的 Mg-Cu 催化剂在 -0.77 V 相对于可逆氢电极 (RHE) 的电流密度为 1.0 A cm 时,C 产物的法拉第效率(FE)高达 80%。通过原位光谱电化学分析的系统实验表明,Mg 物种在 CO RR 过程中稳定 Cu 位并促进 CO 的活化,从而提高*CO 覆盖度以促进 C-C 偶联。

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