Silver Single-Atom Catalyst for Efficient Electrochemical CO2 Reduction Synthesized from Thermal Transformation and Surface Reconstruction

Ningqiang Zhang; Xinxin Zhang; Lei Tao; Peng Jiang; Chenliang Ye; Rui Lin; Zhiwei Huang; Ang Li; Dawei Pang; Han Yan; Yu Wang; Peng Xu; Sufeng An; Qinghua Zhang; Licheng Liu; Shixuan Du; Xiaodong Han; Dingsheng Wang; Yadong Li

doi:10.1002/anie.202014718

Silver Single-Atom Catalyst for Efficient Electrochemical CO₂ Reduction Synthesized from Thermal Transformation and Surface Reconstruction

Angew Chem Int Ed Engl. 2021 Mar 8;60(11):6170-6176. doi: 10.1002/anie.202014718. Epub 2021 Jan 29.

Authors

Ningqiang Zhang¹, Xinxin Zhang², Lei Tao³, Peng Jiang¹, Chenliang Ye¹, Rui Lin¹, Zhiwei Huang⁴, Ang Li⁵, Dawei Pang⁵, Han Yan¹, Yu Wang⁶, Peng Xu⁷, Sufeng An⁸, Qinghua Zhang³, Licheng Liu², Shixuan Du³, Xiaodong Han⁵, Dingsheng Wang¹, Yadong Li¹

Affiliations

¹ Department of Chemistry, Tsinghua University, Beijing, 100084, P. R. China.
² Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, Qingdao, 266101, P. R. China.
³ Institute of Physics, Chinese Academy of Sciences, Beijing, 100190, P. R. China.
⁴ Department of Environmental Science & Engineering, Huaqiao University, Xiamen, 361021, P. R. China.
⁵ Beijing Key Laboratory of Microstructure and Property of Advanced Materials, Beijing University of Technology, Beijing, 100124, P. R. China.
⁶ Shanghai Synchrotron Radiation Facilities, Shanghai Institute of Applied Physics, Chinese Academy of Science, Shanghai, P. R. China.
⁷ CAS Key Laboratory of Standardization and Measurement for Nanotechnology, National Center for Nanoscience and Technology, Beijing, 100190, P. R. China.
⁸ State Key Laboratory of Fine Chemicals, PSU-DUT Joint Center for Energy Research, School of Chemical Engineering, Dalian University of Technology, Dalian, 116024, P. R. China.

PMID: 33274797
DOI: 10.1002/anie.202014718

Abstract

We report an Ag₁ single-atom catalyst (Ag₁ /MnO₂ ), which was synthesized from thermal transformation of Ag nanoparticles (NPs) and surface reconstruction of MnO₂ . The evolution process of Ag NPs to single atoms is firstly revealed by various techniques, including in situ ETEM, in situ XRD and DFT calculations. The temperature-induced surface reconstruction process from the MnO₂ (211) to (310) lattice plane is critical to firmly confine the existing surface of Ag single atoms; that is, the thermal treatment and surface reconstruction of MnO₂ is the driving force for the formation of single Ag atoms. The as-obtained Ag₁ /MnO₂ achieved 95.7 % Faradic efficiency at -0.85 V vs. RHE, and coupled with long-term stability for electrochemical CO₂ reduction reaction (CO₂ RR). DFT calculations indicated single Ag sites possessed high electronic density close to Fermi Level and could act exclusively as the active sites in the CO₂ RR. As a result, the Ag₁ /MnO₂ catalyst demonstrated remarkable performance for the CO₂ RR, far surpassing the conventional Ag nanosized catalyst (Ag_NP /MnO₂ ) and other reported Ag-based catalysts.

Keywords: CO2 reduction reaction; anti-Ostwald ripening; silver; surface reconstruction.

Abstract

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