Pentadecanuclear Fe-Containing Polyoxometalate Catalyst for Visible-Light-Driven Generation of Hydrogen

Tingting Cui, Lin Qin, Fangyu Fu, Xing Xin, Huijie Li, Xikui Fang, Hongjin Lv*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

31 Citations (Scopus)

Abstract

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.

Original languageEnglish
Pages (from-to)4124-4132
Number of pages9
JournalInorganic Chemistry
Volume60
Issue number6
DOIs
Publication statusPublished - 15 Mar 2021

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