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Mechanistic insights into C-C coupling in electrochemical CO reduction using gold superlattices  ( SCI-EXPANDED收录)  

文献类型:期刊文献

英文题名:Mechanistic insights into C-C coupling in electrochemical CO reduction using gold superlattices

作者:Yang, Xiaoju[1,2];Rong, Chao[3];Zhang, Li[1,2];Ye, Zhenkun[1,2];Wei, Zhiming[4];Huang, Chengdi[1,2];Zhang, Qiao[4];Yuan, Qing[1,2];Zhai, Yueming[4];Xuan, Fu-Zhen[3];Xu, Bingjun[5];Zhang, Bowei[3];Yang, Xuan[1,2]

机构:[1]Huazhong Univ Sci & Technol, Key Lab Mat Chem Energy Convers & Storage, Wuhan 430074, Peoples R China;[2]Huazhong Univ Sci & Technol, Sch Chem & Chem Engn, Hubei Key Lab Bioinorgan Chem & Mat Med, Wuhan 430074, Peoples R China;[3]East China Univ Sci & Technol, Sch Mech & Power Engn, Shanghai Key Lab Intelligent Sensing & Detect Tech, Shanghai 200237, Peoples R China;[4]Wuhan Univ, Inst Adv Studies, Wuhan 430072, Peoples R China;[5]Peking Univ, Coll Chem & Mol Engn, Beijing 100871, Peoples R China

年份:2024

卷号:15

期号:1

外文期刊名:NATURE COMMUNICATIONS

收录:;WOS:【SCI-EXPANDED(收录号:WOS:001150728500015)】;

基金:XiaojuY., L.Z., Z.Y., C.H., Q.Y., and XuanY. acknowledge the support from the National Natural Science Foundation of China (Grant. No. 22204054), HUST Academic Frontier Youth Team grant (Grant No. 2019QYTD11), Knowledge Innovation Program of Wuhan-Shuguang, and Wuhan Talented Youth Program. C.R. and B.Z. acknowledge the National Natural Science Foundation of China (Grant. No. 52105145, No. 12274124). Z.W., Q.Z., and Y.Z. acknowledge the support from the National Natural Science Foundation of China (No. 21974103) and the start-up funds of Wuhan University. Thanks to engineer Wei Xu in Optoelectronic Micro&Nano Fabrication and Characterizing Facility, Wuhan National Laboratory for Optoelectronics of Huazhong University of Science and Technology for the support in device fabrication.

语种:英文

摘要:Developing in situ/operando spectroscopic techniques with high sensitivity and reproducibility is of great importance for mechanistic investigations of surface-mediated electrochemical reactions. Herein, we report the fabrication of highly ordered rhombic gold nanocube superlattices (GNSs) as substrates for surface-enhanced infrared absorption spectroscopy (SEIRAS) with significantly enhanced SEIRA effect, which can be controlled by manipulating the randomness of GNSs. Finite difference time domain simulations reveal that the electromagnetic effect accounts for the significantly improved spectroscopic vibrations on the GNSs. In situ SEIRAS results show that the vibrations of CO on the Cu2O surfaces have been enhanced by 2.4 +/- 0.5 and 18.0 +/- 1.3 times using GNSs as substrates compared to those on traditional chemically deposited gold films in acidic and neutral electrolytes, respectively. Combined with isotopic labeling experiments, the reaction mechanisms for C-C coupling of CO electroreduction on Cu-based catalysts are revealed using the GNSs substrates. Developing operando spectroscopic techniques with high sensitivity and reproducibility is of great importance for mechanistic investigations of surface-mediated electrochemical reactions. Here the authors study reaction mechanism of CO electroreduction using highly ordered gold superlattices as substrate for surface-enhanced infrared absorption spectroscopy.

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