Pentadecanuclear Fe-Containing Polyoxometalate Catalyst for Visible-Light-Driven Generation of Hydrogen
Autor: | Xikui Fang, Lin Qin, Huijie Li, Hongjin Lv, Tingting Cui, Fangyu Fu, Xing Xin |
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Rok vydání: | 2021 |
Předmět: |
010405 organic chemistry
Chemistry Electron donor 010402 general chemistry 01 natural sciences 0104 chemical sciences Catalysis Inorganic Chemistry chemistry.chemical_compound Triethanolamine Hexafluorophosphate Polymer chemistry Polyoxometalate medicine Photocatalysis Physical and Theoretical Chemistry Luminescence Hydrogen production medicine.drug |
Zdroj: | Inorganic Chemistry. 60:4124-4132 |
ISSN: | 1520-510X 0020-1669 |
Popis: | The structurally new, carbon-free pentadecanuclear Fe-containing polyoxometalate, Na21[NaFe15(OH)12(PO4)4(A-α-SiW9O34)4]·85H2O (Na21-Fe15P4(SiW9)4), was synthesized using a facile one-pot, solution-based synthetic approach and systematically characterized by various spectroscopic techniques. Single-crystal X-ray diffraction reveals that the title complex is composed of two [Fe4(A-α-SiW9O34)] fragments and two [Fe3.5(A-α-SiW9O34)] fragments stabilized by four PO4 linkers in a tetrameric style with idealized Td point group symmetry. When coupling with (4,4'-ditert-butyl-2,2'-dipyridyl)-bis(coumarin)-iridium(III) hexafluorophosphate ([Ir(coumarin)2(dtbbpy)][PF6]) photosensitizer and triethanolamine (TEOA) sacrificial electron donor, polyoxoanion Fe15P4(SiW9)4 effectively catalyzed hydrogen production with a minimally optimized TON of 986, which represents, to our knowledge, one of the highest values among known Fe-substituted POM-catalyzed hydrogen production systems. Both a mercury-poisoning test and FT-IR characterizations proved the structural stability of Fe15P4(SiW9)4 catalyst under photocatalytic conditions. The photocatalytic mechanism of the present hydrogen-evolving system was investigated by time-solved luminescence and static emission quenching measurements. |
Databáze: | OpenAIRE |
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