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钾掺杂调节铜位点与中间体之间的相互作用实现将CO电还原为乙醇的法拉第效率超过70%。

Over 70 % Faradaic Efficiency for CO Electroreduction to Ethanol Enabled by Potassium Dopant-Tuned Interaction between Copper Sites and Intermediates.

作者信息

Ding Lianchun, Zhu Nannan, Hu Yan, Chen Zheng, Song Pin, Sheng Tian, Wu Zhengcui, Xiong Yujie

机构信息

Key Laboratory of Functional Molecular Solids, Ministry of Education, Anhui Key Laboratory of Molecule-Based Materials, Anhui Provincial Engineering Laboratory of New-Energy Vehicle Battery Energy-Storage Materials, Anhui Engineering Research Center of Carbon Neutrality, College of Chemistry and Materials Science, Anhui Normal University, Wuhu, 241002, P. R. China.

School of Chemistry and Materials Science, Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, 230026, P. R. China.

出版信息

Angew Chem Int Ed Engl. 2022 Sep 5;61(36):e202209268. doi: 10.1002/anie.202209268. Epub 2022 Jul 28.

Abstract

It is highly desired yet challenging to steer the CO electroreduction reaction (CO ER) toward ethanol with high selectivity, for which the evolution of reaction intermediates on catalytically active sites holds the key. Herein, we report that K doping in Cu Se nanosheets array on Cu foam serves as a versatile way to tune the interaction between Cu sites and reaction intermediates in CO ER, enabling highly selective production of ethanol. As revealed by characterization and simulation, the electron transfer from K to Se can stabilize Cu species which facilitate the adsorption of linear *CO and bridge *CO intermediates to promote C-C coupling during CO ER. As a result, the optimized K -Cu Se nanosheets array can catalyze CO ER to ethanol as a single liquid product with high selectivity in a potential area from -0.6 to -1.2 V. Notably, it offers a Faradaic efficiency of 70.3 % for ethanol production at -0.8 V with as is stable for 130 h.

摘要

将CO电还原反应(CO ER)高选择性地导向乙醇是非常理想的,但也具有挑战性,其中反应中间体在催化活性位点上的演化是关键。在此,我们报道了在泡沫铜上的Cu Se纳米片阵列中掺杂K是一种调节CO ER中Cu位点与反应中间体之间相互作用的通用方法,能够高选择性地生产乙醇。表征和模拟结果表明,从K到Se的电子转移可以稳定Cu物种,这有助于线性CO和桥式CO中间体的吸附,从而在CO ER过程中促进C-C偶联。结果,优化后的K -Cu Se纳米片阵列可以在-0.6至-1.2 V的电位范围内将CO ER催化为单一液体产物乙醇,具有高选择性。值得注意的是,在-0.8 V下,它对乙醇生产的法拉第效率为70.3%,并且可以稳定130小时。

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