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Facet Design Promotes Electroreduction of Carbon Dioxide to Carbon Monoxide on Palladium Nanocrystals
Chemical Engineering Science ( IF 4.7 ) Pub Date : 2019-02-01 , DOI: 10.1016/j.ces.2018.03.029
Hao Dong , Lei Zhang , Piaoping Yang , Xiaoxia Chang , Wenjin Zhu , Xiaohong Ren , Zhi-Jian Zhao , Jinlong Gong

Abstract Highly selective electrochemical carbon dioxide reduction to valuable chemical products is a crucial approach to alleviate the energy crisis. To date, some noble metal based heterogeneous catalysts such as Pd exhibit high activity for electrochemical carbon dioxide reduction. However, few systematic studies of the active reaction site of these catalysts have been reported. This paper describes the facet effect on Pd nanocrystals with the same size for CO2 electroreduction. The surface structure of Pd catalysts enclosed with {3 1 0}, {1 0 0} and {1 1 1} facets can be precisely controlled. The Pd concave cubes enclosed with high-index {3 1 0} facets show the highest CO Faradaic efficiency (FE) of 90.6%, compared with Pd cubes enclosed with {1 0 0} facets and Pd octahedrons enclosed with {1 1 1} facets. Density functional theory calculations reveal that the {3 1 0} facets of concave cubes boost the catalytic activity by facilitating the COOH∗ formation and the desorption of CO∗.

中文翻译:

刻面设计促进钯纳米晶体上二氧化碳电还原为一氧化碳

摘要 高选择性电化学二氧化碳还原为有价值的化学产品是缓解能源危机的重要途径。迄今为止,一些基于贵金属的非均相催化剂如 Pd 对电化学二氧化碳还原表现出很高的活性。然而,关于这些催化剂的活性反应位点的系统研究鲜有报道。本文描述了对相同尺寸的 Pd 纳米晶体进行 CO2 电还原的刻面效应。可以精确控制由{3 1 0}、{1 0 0}和{1 1 1}面包围的Pd催化剂的表面结构。与由 {1 0 0} 面包围的 Pd 立方体和由 {1 1 1} 面包围的 Pd 八面体相比,由高指数 {3 1 0} 面包围的 Pd 凹面立方体显示出最高的 CO 法拉第效率 (FE),为 90.6%方面。
更新日期:2019-02-01
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