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Silver Single Atom in Carbon Nitride Catalyst for Highly Efficient Photocatalytic Hydrogen Evolution
Authors:Xun-Heng Jiang  Dr. Long-Shuai Zhang  Hai-Yan Liu  Prof. Dai-She Wu  Fei-Yao Wu  Lei Tian  Ling-Ling Liu  Prof. Jian-Ping Zou  Prof. Sheng-Lian Luo  Bing-Bing Chen
Affiliation:1. Key Laboratory of Jiangxi Province for Persistent Pollutants Control and Resources Recycle, Nanchang Hangkong University, Nanchang, Jiangxi, 330063 P. R. China

Key Laboratory of Poyang Lake Environment and Resource Utilization of Ministry of Education, School of Resources Environmental and Chemical Engineering, Nanchang University, Nanchang, Jiangxi, 330031 P. R. China

These authors contributed equally to this work.;2. Key Laboratory of Jiangxi Province for Persistent Pollutants Control and Resources Recycle, Nanchang Hangkong University, Nanchang, Jiangxi, 330063 P. R. China

These authors contributed equally to this work.;3. Key Laboratory of Jiangxi Province for Persistent Pollutants Control and Resources Recycle, Nanchang Hangkong University, Nanchang, Jiangxi, 330063 P. R. China;4. Key Laboratory of Poyang Lake Environment and Resource Utilization of Ministry of Education, School of Resources Environmental and Chemical Engineering, Nanchang University, Nanchang, Jiangxi, 330031 P. R. China;5. Key Laboratory of Jiangxi Province for Persistent Pollutants Control and Resources Recycle, Nanchang Hangkong University, Nanchang, Jiangxi, 330063 P. R. China

Key Laboratory of Poyang Lake Environment and Resource Utilization of Ministry of Education, School of Resources Environmental and Chemical Engineering, Nanchang University, Nanchang, Jiangxi, 330031 P. R. China;6. Department of Energy Science and Engineering, Nanjing Tech University, Nanjing, Jiangsu, 210009 P. R. China

Abstract:Single atom catalysts (SACs) with the maximized metal atom efficiency have sparked great attention. However, it is challenging to obtain SACs with high metal loading, high catalytic activity, and good stability. Herein, we demonstrate a new strategy to develop a highly active and stable Ag single atom in carbon nitride (Ag-N2C2/CN) catalyst with a unique coordination. The Ag atomic dispersion and Ag-N2C2 configuration have been identified by aberration-correction high-angle-annular-dark-field scanning transmission electron microscopy (AC-HAADF-STEM) and extended X-ray absorption. Experiments and DFT calculations further verify that Ag-N2C2 can reduce the H2 evolution barrier, expand the light absorption range, and improve the charge transfer of CN. As a result, the Ag-N2C2/CN catalyst exhibits much better H2 evolution activity than the N-coordinated Ag single atom in CN (Ag-N4/CN), and is even superior to the Pt nanoparticle-loaded CN (PtNP/CN). This work provides a new idea for the design and synthesis of SACs with novel configurations and excellent catalytic activity and durability.
Keywords:co-coordination  electron transfer  photocatalysis  single-atom catalyst
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