Yi Li, Yanghan Chen, Tao Chen, Guoqiang Shi, Lin Zhu, Ye Sun* and Miao Yu*,
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引用次数: 1
摘要
乙醇(C2H5OH)是电化学还原CO2过程中经济理想的C2产物。然而,CO2-to-C2H5OH的转化率一直很低,在大多数情况下,潜在的催化机制仍然模糊或未被探索。本文通过在Cu纳米片上均匀修饰Cu2S纳米晶体,将Cu (Cuδ+)较高的局部正电荷、Cuδ+与零价Cu0之间丰富的界面以及催化剂表面非扁平阶梯式的三个理想特征整合到电催化剂中,从而提高了*CO的亲和力,降低了*COCO的形成屏障,并在热力学上倾向于* ch2cho到-*CH3CHO的转化。结果表明,在含有0.1 M KHCO3溶液的h电池中,在- 1.2 V vs可逆氢电极下,C2H5OH的偏电流密度高达~20.7 mA cm-2,法拉第效率为46%。这项工作提出了一种高效的策略,用于高产量的二氧化碳到c2h5oh的转化,强调了工业生产酒精和相关产品从二氧化碳的承诺。
Insight into the Electrochemical CO2-to-Ethanol Conversion Catalyzed by Cu2S Nanocrystal-Decorated Cu Nanosheets
Ethanol (C2H5OH) is an economically ideal C2 product in electrochemical CO2 reduction. However, the CO2-to-C2H5OH conversion yield has been rather low and the underlying catalytic mechanism remains vague or unexplored in most cases. Herein, by decorating small Cu2S nanocrystals uniform ly on Cu nanosheets, three desirable features are integrated into the electrocatalyst, including a relatively high positive local charge on Cu (Cuδ+), abundant interfaces between Cuδ+ and zero-valence Cu0, and a non-flat, stepped catalyst surface, leading to the promoted affinity of *CO, decreased *COCO formation barrier, and thermodynamically preferred *CH2CHO-to-*CH3CHO conversion. As a result, a high partial current density of ~20.7 mA cm–2 and a Faraday efficiency of 46% for C2H5OH are delivered at ?1.2 V vs reversible hydrogen electrode in an H-cell containing a 0.1 M KHCO3 solution. This work proposes an efficient strategy for the high-yield CO2-to-C2H5OH conversion, emphasizing the promise for the industrial production of alcohol and related products from CO2.
期刊介绍:
ACS Applied Materials & Interfaces is a leading interdisciplinary journal that brings together chemists, engineers, physicists, and biologists to explore the development and utilization of newly-discovered materials and interfacial processes for specific applications. Our journal has experienced remarkable growth since its establishment in 2009, both in terms of the number of articles published and the impact of the research showcased. We are proud to foster a truly global community, with the majority of published articles originating from outside the United States, reflecting the rapid growth of applied research worldwide.