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

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.

Authors:
; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Institute for Atom-efficient Chemical Transformations (IACT); Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1307612
DOE Contract Number:  
AC02-06CH11357
Resource Type:
Journal Article
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 138; Journal Issue: 13; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Beletskiy, Evgeny V., Hou, Xianliang, Shen, Zhongliang, Gallagher, James R., Miller, Jeffrey T., Wu, Yuyang, Li, Tiehu, Kung, Mayfair C., and Kung, Harold H. Supported Tetrahedral Oxo-Sn Catalyst: Single Site, Two Modes of Catalysis. United States: N. p., 2016. Web. doi:10.1021/jacs.5b13436.
Beletskiy, Evgeny V., Hou, Xianliang, Shen, Zhongliang, Gallagher, James R., Miller, Jeffrey T., Wu, Yuyang, Li, Tiehu, Kung, Mayfair C., & Kung, Harold H. Supported Tetrahedral Oxo-Sn Catalyst: Single Site, Two Modes of Catalysis. United States. doi:10.1021/jacs.5b13436.
Beletskiy, Evgeny V., Hou, Xianliang, Shen, Zhongliang, Gallagher, James R., Miller, Jeffrey T., Wu, Yuyang, Li, Tiehu, Kung, Mayfair C., and Kung, Harold H. Thu . "Supported Tetrahedral Oxo-Sn Catalyst: Single Site, Two Modes of Catalysis". United States. doi:10.1021/jacs.5b13436.
@article{osti_1307612,
title = {Supported Tetrahedral Oxo-Sn Catalyst: Single Site, Two Modes of Catalysis},
author = {Beletskiy, Evgeny V. and Hou, Xianliang and Shen, Zhongliang and Gallagher, James R. and Miller, Jeffrey T. and Wu, Yuyang and Li, Tiehu and Kung, Mayfair C. and Kung, Harold H.},
abstractNote = {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.},
doi = {10.1021/jacs.5b13436},
journal = {Journal of the American Chemical Society},
issn = {0002-7863},
number = 13,
volume = 138,
place = {United States},
year = {2016},
month = {3}
}