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Acc. Chem. Res上最新光催化综述：通过分子组装来提高光催化还原质子产氢效率
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Enhancement of the Efficiency of Photocatalytic Reduction of Protons to Hydrogen via Molecular Assembly 全文9页，参考文献35篇。 Li-Zhu Wu received her B.S. degree in chemistry from Lanzhou University in 1990, and got her Ph.D. degree from the Institute of Photographic Chemistry, the Chinese Academy of Sciences, under the supervision of Professor Chen-Ho Tung in 1995. From 1995−1998, she worked at the Institute of Photographic Chemistry as an associate professor. After a postdoctoral stay (1997−1998) at the University of Hong Kong working with Professor Chi-Ming Che, she returned to the Technical Institute of Physics and Chemistry, the Chinese Academy of Sciences, as a full professor. Her research interests are focused on photochemical conversion, including artificial photosynthesis, visible light catalysis for organic transformation, and photoinduced electron transfer, energy transfer and chemical reactions in supramolecular systems. Biography Bin Chen received her B.S. degree in chemistry from Southwest China Normal University in 1994, and obtained her Ph.D. degree from Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, under the supervision of Professor Chen-Ho Tung in 2007. She is currently a professor in the Technical Institute of Physics and Chemistry. Her research interests are focused on photoinduced electron transfer and energy transfer in supramolecular systems, and selectivity in photochemical reactions. Biography Zhi-Jun Li received his B.S. degree in chemistry from Lanzhou University in 2008, and his Ph.D. degree in organic chemistry at the Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, under the supervision of Professor Li-Zhu Wu and Professor Chen-Ho Tung in 2013. Then, he started to work as an assistant professor at the same Institute. His work is focused on the artificial photosynthesis, particularly photocatalytic water splitting. Biography Chen-Ho Tung graduated from the polymer chemistry department of the University of Science and Technology of China in 1963, and was awarded a Ph.D. degree in 1983 from Columbia University in New York City, under the supervision of Professor Nicholas J. Turro. He attended the Institute of Photographic Chemistry, the Chinese Academy of Sciences, and is currently a full professor at the Technical Institute of Physics and Chemistry, and an academician of the Chinese Academy of Sciences. His research interests include photochemical reactions, photoinduced electron transfer and energy transfer in supramolecular systems. One of the best solutions for meeting future energy demands is the conversion of water into hydrogen fuel using solar energy. The splitting of water into molecular hydrogen (H2) and oxygen (O2) using light involves two half-reactions: the oxidation of water to O2 and the reduction of protons to H2. To take advantage of the full range of the solar spectrum, researchers have extensively investigated artificial photosynthesis systems consisting of two photosensitizers and two catalysts with a Z-configuration: one photosensitizer-catalyst pair for H2 evolution and the other for O2 evolution. This type of complete artificial photosynthesis system is difficult to build and optimize; therefore, researchers typically study the reductive half-reaction and the oxidative half-reaction separately. To study the two half-reactions, researchers use a sacrificial electron donor to provide electrons for the reductive half-reaction, and a sacrificial electron acceptor to capture electrons for the oxidative half-reaction. After optimization, they can eliminate the added donors and acceptors as the two half reactions are coupled to a complete photocatalytic water spitting system. Most photocatalytic systems for the H2 evolution half-reaction consist of a photosensitizer, a catalyst, and a sacrificial electron donor. To promote photoinduced electron transfer and photocatalytic H2 production, these three components should be assembled together in a controlled manner. Researchers have struggled to design a photocatalytic system for H2 evolution that uses earth-abundant materials and is both efficient and durable. This Account reviews advances our laboratory has made in the development of new systems for photocatalytic H evolution that uses earth-abundant materials and is both efficient and durable. We used organometallic complexes and quantum-confined semiconductor nanocrystals (QDs) as photosensitizers, and [FeFe]-H2ase mimics and inorganic transition metal salts as catalysts to construct photocatalytic systems with sacrificial electron donors. Covalently linked Re(I) complex-[FeFe]-H2ase mimic dyads and ferrocene-Re(I) complex-[FeFe]-H2ase mimic triads could photocatalyze H2 production in organic solutions, but these photocatalytic systems tended to decompose. We also constructed several assemblies of CdTe and CdSe QDs as photosensitizers with [FeFe]-H2ase mimics as catalysts. These assemblies produced H2 in aqueous solutions photocatalytically and efficiently, with turnover numbers (TONs) up to tens of thousands. Assemblies of 3-mercaptopropionic acid (MPA)-capped CdTe QDs with Co2+ ions formed Coh-CdTe hollow nanospheres, and MPA capped-CdSe QDs with Ni+ ions produced Nih-CdSe/CdS core/shell hybrids in situ in aqueous solutions upon irradiation. The resulting photocatalytic systems proved robust for H2 evolution. These systems showed excellent activity and impressive durability in the photocatalytic reaction, suggesting that they can serve as a valuable part of an overall water splitting system.  图片1.jpg |
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