In Situ Observation of Hot Carrier Transfer at Plasmonic Au/Metal-Organic Frameworks (MOFs) Interfaces |
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Authors: | Dr Shuobo Wang Lei Wu Prof Dr Jikun Li Chaoyuan Deng Jing Xue Daojian Tang Prof Dr Hongwei Ji Prof Dr Chuncheng Chen Prof Dr Yuchao Zhang Prof Dr Jincai Zhao |
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Institution: | 1. Key Laboratory of Photochemistry CAS Research/Education Center for Excellence in Molecular Sciences Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190 P. R. China;2. Key Laboratory of Photochemistry CAS Research/Education Center for Excellence in Molecular Sciences Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190 P. R. China
University of Chinese Academy of Sciences, Beijing, 100049 P. R. China |
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Abstract: | Constructing heterostructures have been demonstrated as an ideal strategy for boosting charge separation on plasmonic photocatalysts, but the detailed interface charge transfer mechanism remains elusive. Herein, that authors fabricate plasmonic Au and metal-organic frameworks (MOFs, NH2−MIL-125 and MIL-125 used in this work) heterostructures and explore the interface charge transfer mechanism by in situ electron paramagnetic resonance (EPR) spectroscopy and electrochemical measurements. The plasmon-excited hot electrons on Au can transfer across the Au/MOF interface and be captured by the coordinatively unsaturated sites of secondary building units (Ti8O8(OH)4 cluster) of the MOF structure, and the plasmon-excited hot holes on Au tend to transfer to and be trapped at the functionalized organic ligand (1,4-benzenedicarboxylate−NH2). The spatially separated hot electrons and holes exhibit boosted the photocatalytic activity for chromium (VI) reduction and selective benzyl alcohol oxidation. This work illustrates the advantage of the versatile functionalization of MOF structures enabling molecular-level manipulation of interface charge transfer on plasmonic photocatalysts. |
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Keywords: | charge transfer EPR spectroscopy metal-organic frameworks photocatalysis surface plasmon resonance |
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