Atomically precise Au25(GSH)18 nanoclusters versus plasmonic Au nanocrystals: Evaluating charge impetus in solar water oxidation |
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| Institution: | 1. College of Materials Science and Engineering, Fuzhou University, New Campus, Minhou 350108, China;2. Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China, Fuzhou 350108, China;1. Key Lab for Anisotropy and Texture of Materials (MoE), School of Materials Science and Engineering, Northeastern University, Shenyang 110819, China;2. Institute for Frontier Technologies of Low-Carbon Steelmaking, Shenyang 110819, China;1. College of Environmental Science and Engineering, Hunan University and Key Laboratory of Environmental Biology and Pollution Control, Ministry of Education (Hunan University), Changsha 410082, China;2. School of Design, Hunan University, Changsha 410082, China;3. School of Resources and Environment, Hunan University of Technology and Business, Changsha 410205, China;4. Department of Chemical and Materials Engineering, University of Alberta, Edmonton, Alberta T6G 1H9, Canada;1. College of Physics and Center of Quantum Materials and Devices, Chongqing University, Chongqing 401331, China;2. College of Material Science and Engineering, Chongqing University, Chongqing 400044, China;3. Beijing Key Laboratory of Microstructure and Property of Advanced Materials, Beijing University of Technology, Beijing 100024, China;1. Department of Chemistry, Institutes of Biomedical Sciences, and Shanghai Stomatological Hospital, Fudan University, Shanghai 200000, China;2. Changhai Hospital, The Naval Military Medical University, Shanghai 200433, China;1. Key Laboratory of Poyang Lake Environment and Resource Utilization of Ministry of Education, School of Resources & Environment, Nanchang University, Nanchang 330031, China;2. Key Laboratory of Jiangxi Province for Persistent Pollutants Control and Resources Recycle, Nanchang Hangkong University, Nanchang 330063, China;3. School of Chemistry & Molecular Engineering, East China University of Science and Technology, Shanghai 200237, China |
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| Abstract: | Atomically precise metal nanoclusters (NCs) have been deemed as an emerging class of metal nanomaterials owing to fascinating size-dependent physicochemical properties, discrete energy band structure, and quantum confinement effect, which are distinct from conventional metal nanoparticles (NPs). Nevertheless, metal NCs suffer from photoinduced self-oxidative aggregation accompanied by in-situ transformation to metal NPs, markedly reducing the photosensitization of metal NCs. Herein, maneuvering the generic instability of metal NCs, we perform the charge transport impetus comparison between atomically precise metal NCs and plasmonic metal NPs counterpart obtained from in-situ self-transformation of metal NCs in photoelectrochemical (PEC) water splitting reaction. For conceptual demonstration, we proposed two quintessential heterostructures, which include TNTAs-Au25 heterostructure fabricated by electrostatically depositing glutathione (GSH)-protected Au25(GSH)18 NCs on the TiO2 nanotube arrays (TNTAs) substrate, and TNTAs-Au heterostructure constructed by triggering self-transformation of Au25(GSH)18 NCs to plasmonic Au NPs in TNTAs-Au25 via calcination. The results indicate that photoelectrons produced over Au25 NCs are superior to hot electrons of plasmonic Au NPs in stimulating the interracial charge transport toward solar water oxidation. This is mainly ascribed to the significantly accelerated carrier transport kinetics, prolonged carrier lifespan, and substantial photosensitization effect of Au25 NCs compared with plasmonic Au NPs, resulting in the considerably enhanced PEC water splitting performance of TNTAs-Au25 relative to plasmonic TNTAs-Au counterpart under visible light irradiation. Our work would provide important implications for rationally designing atomically precise metal NCs-based photosystems toward solar energy conversion. |
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