Silver Single‐Atom Catalyst for Efficient Electrochemical CO<sub>2</sub> 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
Abstract
Abstract We report an Ag 1 single‐atom catalyst (Ag 1 /MnO 2 ), which was synthesized from thermal transformation of Ag nanoparticles (NPs) and surface reconstruction of MnO 2 . 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 MnO 2 (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 MnO 2 is the driving force for the formation of single Ag atoms. The as‐obtained Ag 1 /MnO 2 achieved 95.7 % Faradic efficiency at −0.85 V vs. RHE, and coupled with long‐term stability for electrochemical CO 2 reduction reaction (CO 2 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 CO 2 RR. As a result, the Ag 1 /MnO 2 catalyst demonstrated remarkable performance for the CO 2 RR, far surpassing the conventional Ag nanosized catalyst (Ag NP /MnO 2 ) and other reported Ag‐based catalysts.