Superior catalytic properties in aerobic oxidation of olefins over Au nanoparticles on pyrrolidone-modified SBA-15

We report on our systematic investigation of Au nanoparticles highly dispersed in the mesopores of (s)-(–)-2-pyrrolidinone-5-carboxylic acid (Py)-modified SBA-15 (Au/SBA-15-Py) by using a series of modern techniques. 13C NMR and IR spectroscopies indicate that Py species are successfully grafted on the surface of mesopores in SBA-15; XRD patterns and N2 adsorption isotherms show that the sample mesostructures are well preserved; TEM images clearly confirm the uniform Au nanoparticles in the mesopores; and XPS suggests an interaction between Au nanoparticles with Py species. Interestingly, Au/SBA-15-Py catalysts always exhibit superior catalytic properties in the oxidation of cyclohexene and styrene by molecular oxygen at atmospheric pressure, compared with the pyrrolidone-free SBA-15 supported Au catalyst (Au/SBA-15-N). This phenomenon is reasonably related to the interaction between Au nanoparticles with Py species, which is consistent with results analyzed from our density-functional theory (DFT) calculations.

Graphical abstractAu nanoparticles highly dispersed in the mesopores of pyrrolidone (Py)-modified SBA-15 (Au/SBA-15-Py) are efficient and stable heterogeneous catalysts for oxidations of cyclohexene and styrene by molecular oxygen at atmospheric pressure. The interaction between Au nanoparticles with Py in Au/SBA-15-Py is supported by XPS characterization, in strong agreement with density-functional theory calculations.Figure optionsDownload full-size imageDownload high-quality image (107 K)Download as PowerPoint slideHighlights► Au nanoparticles are highly dispersed in the mesopores of pyrrolidone-modified SBA-15 ►. Au/SBA-15-Py has excellent catalytic properties in aerobic oxidation of olefins. ► There is an interaction between Au nanoparticles with Py species. ► The interaction was studied by density-functional theory calculations.