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论文类型：期刊论文

发表时间：2017-10-30

发表刊物：SCIENTIFIC REPORTS

收录刊物：SCIE、PubMed、Scopus

卷号：7

期号：1

页面范围：14347

ISSN号：2045-2322

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, 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 H-2 evolution, with the turnover number (TON) and turnover frequency (TOF) reaching 400 and 100 moles H-2 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 redoxactive NADH mimic dihydropyridine amido moieties within the ligands played an important role in photocatalytic proton reduction process.