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- Title
[{Ni<sub>4</sub>(OH)<sub>3</sub>AsO<sub>4</sub>}<sub>4</sub>( B-α-PW<sub>9</sub>O<sub>34</sub>)<sub>4</sub>]<sup>28−</sup>: A New Polyoxometalate Structural Family with Catalytic Hydrogen Evolution Activity.
- Authors
Lv, Hongjin; Chi, Yingnan; van Leusen, Jan; Kögerler, Paul; Chen, Zheyuan; Bacsa, John; Geletii, Yurii V.; Guo, Weiwei; Lian, Tianquan; Hill, Craig L.
- Abstract
A new structural polyoxometalate motif, [{Ni4(OH)3AsO4}4( B-α-PW9O34)4]28−, which contains the highest nuclearity structurally characterized multi-nickel-containing polyanion to date, has been synthesized and characterized by single-crystal X-ray diffraction, temperature-dependent magnetism and several other techniques. The unique central {Ni16(OH)12O4(AsO4)4} core shows dominant ferromagnetic exchange interactions, with maximum χm T of 69.21 cm3 K mol−1 at 3.4 K. Significantly, this structurally unprecedented complex is an efficient, water-compatible, noble-metal-free catalyst for H2 production upon visible light irradiation (photosensitizer=[Ir(ppy)2(dtbbpy)][PF6]; sacrificial electron donor=triethylamine or triethanolamine). The highest turnover number of approximately 580, corresponding to a best quantum yield of approximately 4.07 %, is achieved when using triethylamine as electron donor in the presence of water. The mechanism of this photodriven process has been probed by time-solved luminescence and by static emission quenching.
- Subjects
CATALYSIS research; HYDROGEN; METALATION; PHOTOSENSITIZERS; POLYANIONS
- Publication
Chemistry - A European Journal, 2015, Vol 21, Issue 48, p17363
- ISSN
0947-6539
- Publication type
Article
- DOI
10.1002/chem.201503010