Cargando…

Silica-supported isolated gallium sites as highly active, selective and stable propane dehydrogenation catalysts

Single-site gallium centers on the surface of silica are prepared via grafting of [Ga(OSi(OtBu)(3))(3)(THF)] on SiO(2–700) 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)(3)Ga(XOSi[...

Descripción completa

Detalles Bibliográficos
Autores principales: Searles, Keith, Siddiqi, Georges, Safonova, Olga V., Copéret, Christophe
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Royal Society of Chemistry 2017
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5433511/
https://www.ncbi.nlm.nih.gov/pubmed/28553501
http://dx.doi.org/10.1039/c6sc05178b
Descripción
Sumario:Single-site gallium centers on the surface of silica are prepared via grafting of [Ga(OSi(OtBu)(3))(3)(THF)] on SiO(2–700) 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)(3)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 Ga(2)O(3)-based catalysts.