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Fast operando spectroscopy tracking in situ generation of rich defects in silver nanocrystals for highly selective electrochemical CO2 reduction

Xinhao Wu, Yanan Guo, Zengsen Sun, Fenghua Xie, Daqin Guan, Jie Dai, Fengjiao Yu, Zhiwei Hu, Yu-Cheng Huang, Chih-Wen Pao, Jeng-Lung Chen, Wei Zhou () and Zongping Shao ()
Additional contact information
Xinhao Wu: Nanjing Tech University
Yanan Guo: Nanjing Tech University
Zengsen Sun: Nanjing Tech University
Fenghua Xie: Nanjing Tech University
Daqin Guan: Nanjing Tech University
Jie Dai: Nanjing Tech University
Fengjiao Yu: Nanjing Tech University
Zhiwei Hu: Max Planck Institute for Chemical Physics of Solids
Yu-Cheng Huang: National Chiao Tung University
Chih-Wen Pao: National Synchrotron Radiation Research Center
Jeng-Lung Chen: National Synchrotron Radiation Research Center
Wei Zhou: Nanjing Tech University
Zongping Shao: Nanjing Tech University

Nature Communications, 2021, vol. 12, issue 1, 1-11

Abstract: Abstract 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.

Date: 2021
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Persistent link: https://EconPapers.repec.org/RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-20960-8

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DOI: 10.1038/s41467-021-20960-8

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