A Mo2-ZnP molecular device that mimics photosystem I for solar-chemical energy conversion
| Autor: | Yingning Tan, Chun Y. Liu, Junpeng Zhou, Xiaoli Chen, Guang Yuan Zhu, Shaoyang Su, Tao Cheng, Miao Meng, Junhua Wei, Yi Yang Wu, Xiao Liu, Dai-Bin Kuang, Yuli Zhou |
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| Rok vydání: | 2021 |
| Předmět: |
Flavin adenine dinucleotide
Hydride Process Chemistry and Technology 02 engineering and technology Nicotinamide adenine dinucleotide 010402 general chemistry 021001 nanoscience & nanotechnology Photochemistry Photosystem I Solar fuel 01 natural sciences Catalysis 0104 chemical sciences chemistry.chemical_compound Solar chemical chemistry NAD+ kinase 0210 nano-technology General Environmental Science Photosystem |
| Zdroj: | Applied Catalysis B: Environmental. 286:119836 |
| ISSN: | 0926-3373 |
| Popis: | Bioinspired solar-chemical energy conversion has long been challenged by chemists with searching for effective synthetic photocatalysts. Herein we show that powered by visible light, molecular photocatalysts developed by integrating zinc porphyrin (ZnP) with a quadruply-bonded Mo2 unit enables hydrogen evolution from water in high yields up to 200 mmol g−1 with TON = 640. Remarkably, this unimolecular Mo2-ZnP device catalyzes efficiently photoreduction of nicotinamide adenine dinucleotide (NAD+) to NADH, the reducing equivalent for enzymatic reduction of CO2 in natural photosynthesis. Evidently, this Mo2-ZnP photosystem has the capability of accumulating up to four electrons and two protons for two-electron reduction. Mechanistic investigations reveal that the photoreduced zinc phlorin and chlorin-phlorin anions are the catalytic intermediates for hydride transfer to the substrates, which mimics functionally the hydroquinone state of flavin adenine dinucleotide in photosystem I. The understandings gained in this study are valuable for engineering photocatalysts for solar fuel production. |
| Databáze: | OpenAIRE |
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