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

Abstract 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...

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Autores principales:	Liang Zhao, Jian Wang, Pengyan Wu, Cheng He, Xiangyang Guo, Chunying Duan
Formato:	article
Lenguaje:	EN
Publicado:	Nature Portfolio 2017
Materias:	Medicine R Science Q
Acceso en línea:	https://doaj.org/article/0a1f096ce5f048eca3fd6974577d23c8
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spelling	oai:doaj.org-article:0a1f096ce5f048eca3fd6974577d23c82021-12-02T11:40:58ZDHPA-Containing Cobalt-Based Redox Metal-Organic Cyclohelicates as Enzymatic Molecular Flasks for Light-Driven H2 Production10.1038/s41598-017-14728-82045-2322https://doaj.org/article/0a1f096ce5f048eca3fd6974577d23c82017-10-01T00:00:00Zhttps://doi.org/10.1038/s41598-017-14728-8https://doaj.org/toc/2045-2322Abstract 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, a redox-active cobalt-based macrocycle was developed as a redox vehicle for the construction of an artificial photosynthesis (AP) system. The cyclohelicate can encapsulate fluorescein within its cavity for light-driven H2 evolution, with the turnover number (TON) and turnover frequency (TOF) reaching 400 and 100 moles H2 per mole redox catalyst per hour, respectively. Control experiments demonstrated that the reactions were potentially occurred within the cavity of the cyclohelicates which were inhibited in the presence of adenosine triphosphate (ATP), and the redox-active NADH mimic dihydropyridine amido moieties within the ligands played an important role in photocatalytic proton reduction process.Liang ZhaoJian WangPengyan WuCheng HeXiangyang GuoChunying DuanNature PortfolioarticleMedicineRScienceQENScientific Reports, Vol 7, Iss 1, Pp 1-9 (2017)
institution	DOAJ
collection	DOAJ
language	EN
topic	Medicine R Science Q
spellingShingle	Medicine R Science Q Liang Zhao Jian Wang Pengyan Wu Cheng He Xiangyang Guo Chunying Duan DHPA-Containing Cobalt-Based Redox Metal-Organic Cyclohelicates as Enzymatic Molecular Flasks for Light-Driven H2 Production
description	Abstract 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, a redox-active cobalt-based macrocycle was developed as a redox vehicle for the construction of an artificial photosynthesis (AP) system. The cyclohelicate can encapsulate fluorescein within its cavity for light-driven H2 evolution, with the turnover number (TON) and turnover frequency (TOF) reaching 400 and 100 moles H2 per mole redox catalyst per hour, respectively. Control experiments demonstrated that the reactions were potentially occurred within the cavity of the cyclohelicates which were inhibited in the presence of adenosine triphosphate (ATP), and the redox-active NADH mimic dihydropyridine amido moieties within the ligands played an important role in photocatalytic proton reduction process.
format	article
author	Liang Zhao Jian Wang Pengyan Wu Cheng He Xiangyang Guo Chunying Duan
author_facet	Liang Zhao Jian Wang Pengyan Wu Cheng He Xiangyang Guo Chunying Duan
author_sort	Liang Zhao
title	DHPA-Containing Cobalt-Based Redox Metal-Organic Cyclohelicates as Enzymatic Molecular Flasks for Light-Driven H2 Production
title_short	DHPA-Containing Cobalt-Based Redox Metal-Organic Cyclohelicates as Enzymatic Molecular Flasks for Light-Driven H2 Production
title_full	DHPA-Containing Cobalt-Based Redox Metal-Organic Cyclohelicates as Enzymatic Molecular Flasks for Light-Driven H2 Production
title_fullStr	DHPA-Containing Cobalt-Based Redox Metal-Organic Cyclohelicates as Enzymatic Molecular Flasks for Light-Driven H2 Production
title_full_unstemmed	DHPA-Containing Cobalt-Based Redox Metal-Organic Cyclohelicates as Enzymatic Molecular Flasks for Light-Driven H2 Production
title_sort	dhpa-containing cobalt-based redox metal-organic cyclohelicates as enzymatic molecular flasks for light-driven h2 production
publisher	Nature Portfolio
publishDate	2017
url	https://doaj.org/article/0a1f096ce5f048eca3fd6974577d23c8
work_keys_str_mv	AT liangzhao dhpacontainingcobaltbasedredoxmetalorganiccyclohelicatesasenzymaticmolecularflasksforlightdrivenh2production AT jianwang dhpacontainingcobaltbasedredoxmetalorganiccyclohelicatesasenzymaticmolecularflasksforlightdrivenh2production AT pengyanwu dhpacontainingcobaltbasedredoxmetalorganiccyclohelicatesasenzymaticmolecularflasksforlightdrivenh2production AT chenghe dhpacontainingcobaltbasedredoxmetalorganiccyclohelicatesasenzymaticmolecularflasksforlightdrivenh2production AT xiangyangguo dhpacontainingcobaltbasedredoxmetalorganiccyclohelicatesasenzymaticmolecularflasksforlightdrivenh2production AT chunyingduan dhpacontainingcobaltbasedredoxmetalorganiccyclohelicatesasenzymaticmolecularflasksforlightdrivenh2production
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DHPA-Containing Cobalt-Based Redox Metal-Organic Cyclohelicates as Enzymatic Molecular Flasks for Light-Driven H2 Production

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