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Breaking the Linear Scaling Relationship by Compositional and Structural Crafting of Ternary Cu–Au/Ag Nanoframes for Electrocatalytic Ethylene Production
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2020-10-02 , DOI: 10.1002/anie.202012631 Likong Xiong 1 , Xiang Zhang 1 , Hao Yuan 2 , Juan Wang 3 , Xuzhou Yuan 1 , Yuebin Lian 1 , Huidong Jin 1 , Hao Sun 1 , Zhao Deng 1 , Dan Wang 1 , Jiapeng Hu 1 , Huiming Hu 1 , Jinho Choi 1 , Jiong Li 1 , Yufeng Chen 2 , Jun Zhong 2 , Jun Guo 4 , Mark H Rümmerli 1 , Lai Xu 2 , Yang Peng 5
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2020-10-02 , DOI: 10.1002/anie.202012631 Likong Xiong 1 , Xiang Zhang 1 , Hao Yuan 2 , Juan Wang 3 , Xuzhou Yuan 1 , Yuebin Lian 1 , Huidong Jin 1 , Hao Sun 1 , Zhao Deng 1 , Dan Wang 1 , Jiapeng Hu 1 , Huiming Hu 1 , Jinho Choi 1 , Jiong Li 1 , Yufeng Chen 2 , Jun Zhong 2 , Jun Guo 4 , Mark H Rümmerli 1 , Lai Xu 2 , Yang Peng 5
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Electrocatalytic conversion of carbon dioxide into high‐value multicarbon (C2+) chemical feedstocks offers a promising avenue to liberate the chemical industry from fossil‐resource dependence and eventually close the anthropogenic carbon cycle but is severely impeded by the lack of high‐performance catalysts. To break the linear scaling relationship of intermediate binding and minimize the kinetic barrier of CO2 reduction reactions, ternary Cu–Au/Ag nanoframes were fabricated to decouple the functions of CO generation and C−C coupling, whereby the former is promoted by the alloyed Ag/Au substrate and the latter is facilitated by the highly strained and positively charged Cu domains. Thus, C2H4 production in an H‐cell and a flow cell occurred with high Faradic efficiencies of 69±5 and 77±2 %, respectively, as well as good electrocatalytic stability and material durability. In situ IR and DFT calculations unveiled two competing pathways for C2H4 generation, of which direct CO dimerization is energetically favored.
中文翻译：
通过三元Cu-Au / Ag纳米骨架的组成和结构设计打破线性比例关系以生产电催化乙烯
将二氧化碳电催化转化为高价值的多碳（C 2+）化学原料，为将化学工业摆脱对化石资源的依赖并最终关闭人为碳循环提供了一条有希望的途径，但由于缺乏高性能催化剂而受到严重阻碍。为了打破中间键的线性比例关系并使CO 2还原反应的动力学障碍最小化，制造了三元Cu–Au / Ag纳米框架以解耦CO生成和C–C耦合的功能，由此前者通过合金化而得以促进高应变和带正电的Cu域促进了Ag / Au衬底和后者的生长。因此，C 2 H 4H电池和流通池的生产分别具有69±5％和77±2％的高Faradic效率，以及良好的电催化稳定性和材料耐久性。原位IR和DFT计算揭示了产生C 2 H 4的两种竞争途径，其中直接CO二聚强烈地受到青睐。
更新日期：2020-10-02
中文翻译：
通过三元Cu-Au / Ag纳米骨架的组成和结构设计打破线性比例关系以生产电催化乙烯
将二氧化碳电催化转化为高价值的多碳（C 2+）化学原料，为将化学工业摆脱对化石资源的依赖并最终关闭人为碳循环提供了一条有希望的途径，但由于缺乏高性能催化剂而受到严重阻碍。为了打破中间键的线性比例关系并使CO 2还原反应的动力学障碍最小化，制造了三元Cu–Au / Ag纳米框架以解耦CO生成和C–C耦合的功能，由此前者通过合金化而得以促进高应变和带正电的Cu域促进了Ag / Au衬底和后者的生长。因此，C 2 H 4H电池和流通池的生产分别具有69±5％和77±2％的高Faradic效率，以及良好的电催化稳定性和材料耐久性。原位IR和DFT计算揭示了产生C 2 H 4的两种竞争途径，其中直接CO二聚强烈地受到青睐。
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