Synthesis, Structural Elucidation, and Application of a Pyrazolylpyridine-Molybdenum Oxide Composite as a Heterogeneous Catalyst for Olefin Epoxidation
authors Figueiredo, S; Gomes, AC; Neves, P; Amarante, TR; Paz, FAA; Soares, R; Lopes, AD; Valente, AA; Pillinger, M; Goncalves, IS
nationality International
journal INORGANIC CHEMISTRY
keywords STATE COORDINATION CHEMISTRY; ORGANIC/INORGANIC HYBRID MATERIAL; HYDROTHERMAL SYNTHESIS; CRYSTAL-STRUCTURES; POLYOXOMOLYBDATE CLUSTERS; CARBOXYLATE COORDINATION; LIGAND INFLUENCES; SUBUNITS; COMPLEXES; CHAINS
abstract The reaction of [MoO2Cl2(pypzEA)] (1) (pypzEA = ethyl[3-(pyridin-2-yl)-1H-pyrazol-1-yl]acetate) with water in a Teflon-lined stainless steel autoclave (100 degrees C) or in an open reflux system leads to the isolation of the molybdenum oxide/pyrazolylpyridine composite material [Mo2O6(HpypzA)] (2; HpypzA = [3-(pyridinium-2-yl)-1H-pyrazol-1-yl]-acetate). The solid state structure of 2 was solved through single crystal and powder X-ray diffraction analyses in conjunction with information derived from FT-IR and C-13 CP MAS NMR spectroscopies and elemental analyses. In the asymmetric unit of 2, two crystallographically distinct Mo6+ centers are bridged by a syn,syn-carboxylate group of HpypzA. The periodic repetition of these units along the a axis of the unit cell leads to the formation of a one-dimensional composite polymer, (1)(infinity)[Mo2O6(HpypzA)]. The outstretched pyrazolylpyridine groups of adjacent polymers interdigitate to form a zipper-like motif, generating strong onset pi-pi contacts between adjacent rings of coordinated HpypzA molecules. The composite oxide 2 is a stable heterogeneous catalyst for liquid-phase olefin epoxidation.
publisher AMER CHEMICAL SOC
issn 0020-1669
year published 2012
volume 51
issue 15
beginning page 8629
ending page 8635
digital object identifier (doi) 10.1021/ic301405r
web of science category Chemistry, Inorganic & Nuclear
subject category Chemistry
unique article identifier WOS:000307134700081

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