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Atomically Dispersed Silver-Cobalt Dual-Metal Sites Synergistically Promoting Photocatalytic Hydrogen Evolution |
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| Authors: | Yazi Liu Yue Sun En Zhao Weiwei Yang Jingkai Lin Qiang Zhong Haifeng Qi Aixin Deng Shaogui Yang Huayang Zhang Huan He Shaomin Liu Zupeng Chen Shaobin Wang |
| Affiliation: | 1. School of Environment, Nanjing Normal University, Jiangsu Engineering Lab of Water and Soil Eco-Remediation, Nanjing, 210023 P. R. China
School of Chemical Engineering, The University of Adelaide, Adelaide, SA, 5005 Australia State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing, 210023 P. R. China Department of Chemical Engineering, Curtin University, GPO Box U1987, Perth, WA, 6845 Australia;2. School of Environment, Nanjing Normal University, Jiangsu Engineering Lab of Water and Soil Eco-Remediation, Nanjing, 210023 P. R. China;3. Jiangsu Co-Innovation Center of Efficient Processing and Utilization of Forest Resources, International Innovation Center for Forest Chemicals and Materials, Nanjing Forestry University, Nanjing, 210037 P. R. China;4. School of Materials and Chemistry, University of Shanghai for Science and Technology, Shanghai, 200093 P. R. China;5. School of Chemical Engineering, The University of Adelaide, Adelaide, SA, 5005 Australia;6. Leibniz-Institut für Katalyse e.V., Albert-Einstein-Str. 29a, 18059 Rostock, Germany;7. School of Environment, Nanjing Normal University, Jiangsu Engineering Lab of Water and Soil Eco-Remediation, Nanjing, 210023 P. R. China Department of Municipal Engineering, School of Civil Engineering, Southeast University, Nanjing, Jiangsu, 210096 P. R. China;8. Department of Chemical Engineering, Curtin University, GPO Box U1987, Perth, WA, 6845 Australia State Key Laboratory of Separation Membranes and Membrane Processes, School of Textile Science and Engineering, Tiangong University, Tianjin, 300387 China |
| Abstract: | Regulating the coordination environment of single-atom sites is of high necessity to promote the catalytic performances of the photocatalysts. Herein, the preparation of atomically dispersed Co-Ag dual-metal sites anchored on P-doped carbon nitride (Co1Ag1-PCN) via supramolecular and solvothermal approaches is reported, which demonstrates desirable performance for photocatalytic H2 evolution from water splitting. The optimal Co1Ag1-PCN catalyst achieves a remarkable hydrogen production rate of 1190 µmol g−1 h−1 with an apparent quantum yield (AQY) of 1.49% at 365 nm, superior to most of the newly reported metal-N-coordinated photocatalysts. Systematic experimental characterizations and density functional theoretic studies attribute the enhanced photocatalytic activity to the synergistic effect of Co-Ag dual sites with exclusive coordination configuration of Co-N6 and Ag-N2C2, which enhances the charge density and promotes oriented electrons transport to the metal centers with reduced free energy barriers by facilitating the formation of H* intermediates as the key step in hydrogen evolution. This study reveals a versatile strategy to tailor the electronic structures of dual-metal sites with synergies by engineering the neighboring coordination environment. |
| Keywords: | carbon nitride coordination environment dual-metal sites photocatalytic H 2 production synergistic effect |