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氧化铜网状图案对高晶面铜表面选择性电还原一氧化碳制乙醇的协同效应。

Synergistic Effect of Cu O Mesh Pattern on High-Facet Cu Surface for Selective CO Electroreduction to Ethanol.

作者信息

Kim Ju Ye, Kim Gukbo, Won Hyeonsik, Gereige Issam, Jung Woo-Bin, Jung Hee-Tae

机构信息

Department of Chemical and Biomolecular Engineering (BK-21 four), Korea Advanced Institute of Science and Technology (KAIST), 291 Daehak-ro, Yuseong-gu, Daejeon, 34141, South Korea.

Chemical and Process Technology Division, Korea Research Institute of Chemical Technology (KRICT), 141 Gajeong-ro, Yuseong-gu, Daejeon, 34114, South Korea.

出版信息

Adv Mater. 2022 Jan;34(3):e2106028. doi: 10.1002/adma.202106028. Epub 2021 Nov 24.

Abstract

Although the electroconversion of carbon dioxide (CO ) into ethanol is considered to be one of the most promising ways of using CO , the ethanol selectivity is less than 50% because of difficulties in designing an optimal catalyst that arise from the complicated pathways for the electroreduction of CO to ethanol. Several approaches including the fabrication of oxide-derived structures, atomic surface control, and the Cu /Cu interfaces have been primarily used to produce ethanol from CO . Here, a combined structure with Cu and high-facets as electrocatalysts is constructed by creating high-facets of wrinkled Cu surrounded by Cu O mesh patterns. Using chemical vapor deposition graphene growth procedures, the insufficiently grown graphene is used as an oxidation-masking material, and the high-facet wrinkled Cu is simultaneously generated during the graphene growth synthesis. The resulting electrocatalyst shows an ethanol selectivity of 43% at -0.8 V versus reversible hydrogen electrode, which is one of the highest ethanol selectivity values reported thus far. This is attributed to the role of Cu in enhancing CO binding strength, and the high-facets, which favor C-C coupling and the ethanol pathway. This method for generating the combined structure can be widely applicable not only for electrochemical catalysts but also in various fields.

摘要

尽管将二氧化碳(CO₂)电转化为乙醇被认为是利用CO₂最有前景的方法之一,但由于将CO₂电还原为乙醇的途径复杂,难以设计出最佳催化剂,导致乙醇选择性低于50%。包括制备氧化物衍生结构、原子表面控制和Cu₂O/Cu界面等几种方法已主要用于从CO₂生产乙醇。在此,通过创建被Cu₂O网状图案包围的皱纹状Cu的高晶面,构建了一种以Cu和高晶面作为电催化剂的复合结构。利用化学气相沉积石墨烯生长程序,将生长不足的石墨烯用作氧化掩蔽材料,并在石墨烯生长合成过程中同时生成高晶面皱纹状Cu。所得电催化剂在相对于可逆氢电极-0.8 V时显示出43%的乙醇选择性,这是迄今为止报道的最高乙醇选择性值之一。这归因于Cu在增强CO结合强度方面的作用,以及有利于C-C偶联和乙醇生成途径的高晶面。这种生成复合结构的方法不仅可广泛应用于电化学催化剂,还可应用于各个领域。

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