Xiong Likun, Zhang Xiang, Yuan Hao, Wang Juan, Yuan Xuzhou, Lian Yuebin, Jin Huidong, Sun Hao, Deng Zhao, Wang Dan, Hu Jiapeng, Hu Huimin, Choi Jinho, Li Jiong, Chen Yufeng, Zhong Jun, Guo Jun, Rümmerli Mark H, Xu Lai, Peng Yang
Soochow Institute for Energy and Material Innovations (SIEMIS), College of Energy, Soochow University, P. R. China.
Key Laboratory for Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu Province, Soochow University, Suzhou, Jiangsu, P. R. China.
Angew Chem Int Ed Engl. 2021 Feb 1;60(5):2508-2518. doi: 10.1002/anie.202012631. Epub 2020 Nov 27.
Electrocatalytic conversion of carbon dioxide into high-value multicarbon (C ) 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 CO 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, C H 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 C H generation, of which direct CO dimerization is energetically favored.
将二氧化碳电催化转化为高价值的多碳（C）化学原料，为使化学工业摆脱对化石资源的依赖并最终闭合人为碳循环提供了一条很有前景的途径，但却因缺乏高性能催化剂而受到严重阻碍。为打破中间体吸附的线性比例关系并最小化CO还原反应的动力学势垒，制备了三元Cu-Au/Ag纳米框架，以解耦CO生成和C-C偶联的功能，其中前者由合金化的Ag/Au基底促进，而后者则由高度应变且带正电的Cu域促进。因此，在H型电解槽和流动电解槽中生成C₂H₄的法拉第效率分别高达69±5%和77±2%，同时还具有良好的电催化稳定性和材料耐久性。原位红外光谱和密度泛函理论计算揭示了生成C₂H₄的两条竞争途径，其中直接CO二聚在能量上更有利。
