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DOI10.1038/s41467-021-20960-8
Fast operando spectroscopy tracking in situ generation of rich defects in silver nanocrystals for highly selective electrochemical CO2 reduction
Wu X.; Guo Y.; Sun Z.; Xie F.; Guan D.; Dai J.; Yu F.; Hu Z.; Huang Y.-C.; Pao C.-W.; Chen J.-L.; Zhou W.; Shao Z.
发表日期2021
ISSN2041-1723
卷号12期号:1
英文摘要Electrochemical CO2 reduction (ECR) is highly attractive to curb global warming. The knowledge on the evolution of catalysts and identification of active sites during the reaction is important, but still limited. Here, we report an efficient catalyst (Ag-D) with suitable defect concentration operando formed during ECR within several minutes. Utilizing the powerful fast operando X-ray absorption spectroscopy, the evolving electronic and crystal structures are unraveled under ECR condition. The catalyst exhibits a ~100% faradaic efficiency and negligible performance degradation over a 120-hour test at a moderate overpotential of 0.7 V in an H-cell reactor and a current density of ~180 mA cm−2 at −1.0 V vs. reversible hydrogen electrode in a flow-cell reactor. Density functional theory calculations indicate that the adsorption of intermediate COOH could be enhanced and the free energy of the reaction pathways could be optimized by an appropriate defect concentration, rationalizing the experimental observation. © 2021, The Author(s).
语种英语
scopus关键词carbon dioxide; nanocrystal; potassium bicarbonate; silver nanoparticle; carbon dioxide; catalyst; crystal structure; electrochemical method; in situ measurement; nanoparticle; reduction; silver; spectroscopy; tracking; Article; catalyst; controlled study; crystal structure; density functional theory; electrochemical analysis; extended X ray absorption fine structure spectroscopy; gas diffusion; greenhouse effect; micromorphology; reaction analysis; X ray absorption near edge structure spectroscopy; X ray absorption spectroscopy
来源期刊Nature Communications
文献类型期刊论文
条目标识符http://gcip.llas.ac.cn/handle/2XKMVOVA/250776
作者单位State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering, Nanjing Tech University, Nanjing, China; Max Planck Institute for Chemical Physics of Solids, Dresden, Germany; Department of Electrophysics, National Chiao Tung University, Hsinchu, Taiwan; National Synchrotron Radiation Research Center, Hsinchu, Taiwan; Department of Chemical Engineering, Curtin University, Perth, WA, Australia
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Wu X.,Guo Y.,Sun Z.,et al. Fast operando spectroscopy tracking in situ generation of rich defects in silver nanocrystals for highly selective electrochemical CO2 reduction[J],2021,12(1).
APA Wu X..,Guo Y..,Sun Z..,Xie F..,Guan D..,...&Shao Z..(2021).Fast operando spectroscopy tracking in situ generation of rich defects in silver nanocrystals for highly selective electrochemical CO2 reduction.Nature Communications,12(1).
MLA Wu X.,et al."Fast operando spectroscopy tracking in situ generation of rich defects in silver nanocrystals for highly selective electrochemical CO2 reduction".Nature Communications 12.1(2021).
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