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

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.

SUBMITTER: Wu X

PROVIDER: S-EPMC7844229 | biostudies-literature | 2021 Jan

REPOSITORIES: biostudies-literature

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Fast operando spectroscopy tracking in situ generation of rich defects in silver nanocrystals for highly selective electrochemical CO<sub>2</sub> reduction.

Wu Xinhao X Guo Yanan Y Sun Zengsen Z Xie Fenghua F Guan Daqin D Dai Jie J Yu Fengjiao F Hu Zhiwei Z Huang Yu-Cheng YC Pao Chih-Wen CW Chen Jeng-Lung JL Zhou Wei W Shao Zongping Z

Nature communications 20210128 1

Electrochemical CO<sub>2</sub> 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 condit ...[more]

PMID: 33510153

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Project description:Since nanoparticles are frequently used in commercial applications, there is a huge demand to obtain deeper insights into processes at the nanoscale. Especially, catalysis, chemical and electrochemical reaction dynamics are still poorly understood. Thus, simultaneous and coupled opto-and spectro-electrochemical dark-field microscopy is used to study in situ and operando the electrochemically driven dissolution mechanism of single silver nanoparticles in the presence of nitrate ions as non-complexing counter-ions, herein. Hyperspectral imaging is used to probe the intrinsic localized surface plasmon resonance of individual silver nanospheres before, during and after their electrochemical oxidation on a transparent indium tin oxide (ITO) electrode. Furthermore, optical video imaging was performed for additional information. Based on the complete loss of spectral information and intensity, a dissolution of the particles during the reaction was concluded. This way it is revealed that the dissolution of individual particles proceeds over several seconds, indicating a hindrance by the nitrate ions. Only electrochemical analysis does not provide this insight as the measured current does not allow distinguishing between successive fast dissolution of one particle after another or slow dissolution of several particles in a concerted manner. For comparison, experiments were performed in the presence of chloride ions. It was observed that the silver chloride formation is an instantaneous process. Thus, it is possible to study and define the reaction dynamics on the single nanoparticle level in various electrochemical systems and electrolyte solutions. Accordingly, operando opto- and spectro-electrochemical studies allow us to conclude, that the oxidation of silver to solvated silver cations is a kinetically slow process, while the oxidation to silver chloride is fast. We propose this approach as a new method to study electrocatalyst materials, their transformation and degradation under operando conditions.

Dataset Information

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

Publications

Fast operando spectroscopy tracking in situ generation of rich defects in silver nanocrystals for highly selective electrochemical CO<sub>2</sub> reduction.

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

Publications

Fast operando spectroscopy tracking in situ generation of rich defects in silver nanocrystals for highly selective electrochemical CO<sub>2</sub> reduction.

Similar Datasets

OmicsDI is part of the ELIXIR infrastructure

Tweets

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