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- Title
Unprecedented {Fe<sub>14</sub>}/{Fe<sub>10</sub>} Polyoxotungstate-Based Nanoclusters with Efficient Photocatalytic H<sub>2</sub> Evolution Activity: Synthesis, Structure, Magnetism, and Electrochemistry.
- Authors
Singh, Vikram; Chen, Zhiyuan; Ma, Pengtao; Zhang, Dongdi; Drew, Michael G. B.; Niu, Jingyang; Wang, Jingping
- Abstract
Novel Fe10 and Fe14 clusters [Rb9Cs4H37Fe10O34(A-α-PW9O31)3(OH)3] ⋅36 H2O ( 1) and [H3Rb3Fe14(OH)12(PO4)6(B-α-PW9O34)2] ⋅21 H2O ( 2) were synthesized and characterized in the solid state by single-crystal X-ray diffraction, IR spectroscopy, thermogravimetric analysis (TGA), and magnetic studies, and in solution by electrochemistry. Cluster 1 is a decameric FeIII polyanionic cluster encapsulating a cesium atom in the center. Cluster 2 is a unique tetradecanuclear FeIII sandwich structure with phosphate-linked units featuring two quasicubic Fe4O4 moieties. Apparently, 2 has the highest nuclearity of all known FeIII sandwich-type polyoxometalate clusters. Clusters 1 and 2 also act as photocatalysts with platinum as cocatalyst for H2 evolution from light-driven water splitting. Changes in the cyclovoltammetric patterns with variations in pH were observed for 1 and 2, most likely due to intermolecular interactions among the high-nuclearity FeIII cluster cores and subsequent changes in the acid-base properties of the two reduced POMs. Magnetic studies provide evidence of antiferromagnetic interactions in 1 and 2. TGA showed that complexes 1 and 2 decompose between 580 and 590 °C.
- Subjects
POLYOXOTUNGSTATES; PHOTOCATALYTIC oxidation; ELECTROCHEMISTRY; MAGNETISM; X-ray diffraction
- Publication
Chemistry - A European Journal, 2016, Vol 22, Issue 31, p10983
- ISSN
0947-6539
- Publication type
Article
- DOI
10.1002/chem.201601453