Issue 20, 2019

POM-FLPs: [Mo IV3]n-polyoxometalate bifunctional catalysis by [Mo IV3]n–Om Lewis pairs frustrated by triangular MoIV–MoIV bonds

Abstract

Lewis acid and Lewis base pairs combined in a single system are emerging as one of the most active frontier areas in bifunctional catalysis. To serve as efficient Lewis acid and Lewis base bifunctional catalysts, more reduced MoIVn-polyoxometalates having multiple MoIV–(μ2-O) Lewis pairs are necessary. The new mixed solvent pyridine/DMF/H2O and heterometal oxide (GeO2) have been introduced into the solvothermal partial oxidation system of [Mo3O2(O2CCH3)6(H2O)3]ZnCl4 to yield two novel [MoIV3]n-POM family members, H4[Mo@MoIV6MoV6MoVI8O54(OH)4py6] ({Mo@Mo20}-1) and [Ge@MoIV6MoVI10Zn0.5Ge1.5O47.5(H2O)0.5py6] ({Ge@Mo16Ge1.5Zn0.5}-2), providing two new important routes to extend the POM-FLP system and allowing for a systematic investigation into their reasonable syntheses, diverse molecular and electronic structures, and their influence on the catalytic efficiency. The POM-FLP system exhibits excellent selectivity (>97%) and structure-dependent conversion dominated by the HOMO MoIV percentage, and the number and linkage of [MoIV3]n–(μ2-O)m FLPs in the hydrazine transfer hydrogenation reduction of nitrobenzene to aniline, which is helpful to achieve optimal catalysis performance of the POM-FLP system in transfer hydrogenation or other catalysis reactions that are yet to be developed.

Graphical abstract: POM-FLPs: [MoIV3]n-polyoxometalate bifunctional catalysis by [MoIV3]n–Om Lewis pairs frustrated by triangular MoIV–MoIV bonds

Supplementary files

Article information

Article type
Paper
Submitted
06 Mar 2019
Accepted
15 Apr 2019
First published
16 Apr 2019

Dalton Trans., 2019,48, 6892-6898

POM-FLPs: [MoIV3]n-polyoxometalate bifunctional catalysis by [MoIV3]n–Om Lewis pairs frustrated by triangular MoIV–MoIV bonds

B. Luo and L. Xu, Dalton Trans., 2019, 48, 6892 DOI: 10.1039/C9DT00983C

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