Single-site gallium centers on the surface of silica are prepared grafting of [Ga(OSi(OBu))(THF)] on SiO followed by a thermolysis step. The resulting surface species corresponds to well-defined tetra-coordinate gallium single-sites, [([triple bond, length as m-dash]SiO)Ga(XOSi[triple bond, length as m-dash])] (X = -H or [triple bond, length as m-dash]Si) according to IR, X-ray absorption near-edge structure and extended X-ray absorption fine structure analysis. These gallium sites show high activity, selectivity and stability for propane dehydrogenation with an initial turnover frequency of 20 per h per gallium center, propylene selectivity of ≥93% and remarkable stability over 20 h. The stability of the catalyst probably results from site-isolation of the active site on a non-reducible support such as silica, diminishing facile reduction typical of GaO-based catalysts.
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http://www.ncbi.nlm.nih.gov/pmc/articles/PMC5433511 | PMC |
http://dx.doi.org/10.1039/c6sc05178b | DOI Listing |
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