DHPA-Containing Cobalt-Based Redox Metal-Organic Cyclohelicates as Enzymatic Molecular Flasks for Light-Driven H2 Production.

作者: Liang Zhao , Jian Wang , Pengyan Wu , Cheng He , Xiangyang Guo

DOI: 10.1038/S41598-017-14728-8

关键词:

摘要: The supramolecular assembly of predesigned organic and inorganic building blocks is an excellent tool for constructing well-defined nanosized molecular cavities that catalyse specific chemical transformations. By incorporating a reduced nicotinamide adenine dinucleotide (NADH) mimic within the ligand backbone, redox-active cobalt-based macrocycle was developed as redox vehicle construction artificial photosynthesis (AP) system. cyclohelicate can encapsulate fluorescein its cavity light-driven H2 evolution, with turnover number (TON) frequency (TOF) reaching 400 100 moles per mole catalyst hour, respectively. Control experiments demonstrated reactions were potentially occurred cyclohelicates which inhibited in presence adenosine triphosphate (ATP), NADH dihydropyridine amido moieties ligands played important role photocatalytic proton reduction process.

参考文章(52)
Casey J. Brown, F. Dean Toste, Robert G. Bergman, Kenneth N. Raymond, Supramolecular Catalysis in Metal–Ligand Cluster Hosts Chemical Reviews. ,vol. 115, pp. 3012- 3035 ,(2015) , 10.1021/CR4001226
Wolfgang Lubitz, William Tumas, Hydrogen: an overview. Chemical Reviews. ,vol. 107, pp. 3900- 3903 ,(2007) , 10.1021/CR050200Z
Yonggang Zhao, Dong Guo, Yang Liu, Cheng He, Chunying Duan, A mixed-valence (FeII)2(FeIII)2 square for molecular expression of quantum cellular automata Chemical Communications. pp. 5725- 5727 ,(2008) , 10.1039/B811061A
Zhiji Han, Luxi Shen, William W. Brennessel, Patrick L. Holland, Richard Eisenberg, Nickel Pyridinethiolate Complexes as Catalysts for the Light-Driven Production of Hydrogen from Aqueous Solutions in Noble-Metal-Free Systems Journal of the American Chemical Society. ,vol. 135, pp. 14659- 14669 ,(2013) , 10.1021/JA405257S
Sven Rau, Dirk Walther, Johannes G. Vos, Inspired by nature: light driven organometallic catalysis by heterooligonuclear Ru(ii) complexes Dalton Transactions. pp. 915- 919 ,(2007) , 10.1039/B615987G
Feng Wang, Wen-Guang Wang, Xiao-Jun Wang, Hong-Yan Wang, Chen-Ho Tung, Li-Zhu Wu, A highly efficient photocatalytic system for hydrogen production by a robust hydrogenase mimic in an aqueous solution. Angewandte Chemie. ,vol. 50, pp. 3193- 3197 ,(2011) , 10.1002/ANIE.201006352
Marcetta Y. Darensbourg, Ryan D. Bethel, Merging the old with the new Nature Chemistry. ,vol. 4, pp. 11- 13 ,(2012) , 10.1038/NCHEM.1228
Musiri M. Balakrishnarajan, Roald Hoffmann, Electron-deficient bonding in rhomboid rings. Journal of the American Chemical Society. ,vol. 126, pp. 13119- 13131 ,(2004) , 10.1021/JA0467420