Supported Tetrahedral Oxo-Sn Catalyst: Single Site, Two Modes of Catalysis

Evgeny V. Beletskiy; Xianliang Hou; Zhongliang Shen; James R. Gallagher; Jeffrey T. Miller; Yuyang Wu; Tiehu Li; Mayfair C. Kung; Harold H. Kung

doi:10.1021/jacs.5b13436

Supported Tetrahedral Oxo-Sn Catalyst: Single Site, Two Modes of Catalysis

Evgeny V. Beletskiy, Xianliang Hou, Zhongliang Shen, James R. Gallagher, Jeffrey T. Miller, Yuyang Wu, Tiehu Li, Mayfair C. Kung, Harold H. Kung

School of Materials Sience and Engineering

Research output: Contribution to journal › Article › peer-review

29 Scopus citations

Abstract

Mild calcination in ozone of a (POSS)-Sn-(POSS) complex grafted on silica generated a heterogenized catalyst that mostly retained the tetrahedral coordination of its homogeneous precursor, as evidenced by spectroscopic characterizations using EXAFS, NMR, UV-vis, and DRIFT. The Sn centers are accessible and uniform and can be quantified by stoichiometric pyridine poisoning. This Sn-catalyst is active in hydride transfer reactions as a typical solid Lewis acid. However, the Sn centers can also create Brønsted acidity with alcohol by binding the alcohol strongly as alkoxide and transferring the hydroxyl H to the neighboring Sn-O-Si bond. The resulting acidic silanol is active in epoxide ring opening and acetalization reactions.

Original language	English
Pages (from-to)	4294-4297
Number of pages	4
Journal	Journal of the American Chemical Society
Volume	138
Issue number	13
DOIs	https://doi.org/10.1021/jacs.5b13436
State	Published - 20 Apr 2016

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abstract = "Mild calcination in ozone of a (POSS)-Sn-(POSS) complex grafted on silica generated a heterogenized catalyst that mostly retained the tetrahedral coordination of its homogeneous precursor, as evidenced by spectroscopic characterizations using EXAFS, NMR, UV-vis, and DRIFT. The Sn centers are accessible and uniform and can be quantified by stoichiometric pyridine poisoning. This Sn-catalyst is active in hydride transfer reactions as a typical solid Lewis acid. However, the Sn centers can also create Br{\o}nsted acidity with alcohol by binding the alcohol strongly as alkoxide and transferring the hydroxyl H to the neighboring Sn-O-Si bond. The resulting acidic silanol is active in epoxide ring opening and acetalization reactions.",

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T1 - Supported Tetrahedral Oxo-Sn Catalyst

T2 - Single Site, Two Modes of Catalysis

AU - Beletskiy, Evgeny V.

AU - Hou, Xianliang

AU - Shen, Zhongliang

AU - Gallagher, James R.

AU - Miller, Jeffrey T.

AU - Wu, Yuyang

AU - Li, Tiehu

AU - Kung, Mayfair C.

AU - Kung, Harold H.

PY - 2016/4/20

Y1 - 2016/4/20

N2 - Mild calcination in ozone of a (POSS)-Sn-(POSS) complex grafted on silica generated a heterogenized catalyst that mostly retained the tetrahedral coordination of its homogeneous precursor, as evidenced by spectroscopic characterizations using EXAFS, NMR, UV-vis, and DRIFT. The Sn centers are accessible and uniform and can be quantified by stoichiometric pyridine poisoning. This Sn-catalyst is active in hydride transfer reactions as a typical solid Lewis acid. However, the Sn centers can also create Brønsted acidity with alcohol by binding the alcohol strongly as alkoxide and transferring the hydroxyl H to the neighboring Sn-O-Si bond. The resulting acidic silanol is active in epoxide ring opening and acetalization reactions.

AB - Mild calcination in ozone of a (POSS)-Sn-(POSS) complex grafted on silica generated a heterogenized catalyst that mostly retained the tetrahedral coordination of its homogeneous precursor, as evidenced by spectroscopic characterizations using EXAFS, NMR, UV-vis, and DRIFT. The Sn centers are accessible and uniform and can be quantified by stoichiometric pyridine poisoning. This Sn-catalyst is active in hydride transfer reactions as a typical solid Lewis acid. However, the Sn centers can also create Brønsted acidity with alcohol by binding the alcohol strongly as alkoxide and transferring the hydroxyl H to the neighboring Sn-O-Si bond. The resulting acidic silanol is active in epoxide ring opening and acetalization reactions.

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Supported Tetrahedral Oxo-Sn Catalyst: Single Site, Two Modes of Catalysis

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