Tracing catalytic conversion on single zeolite crystals in 3D with nonlinear spectromicroscopy

Autor:	Domke, K.F., Riemer, T.A., Rago, G., Parvulescu, A.N., Bruijnincx, P.C.A., Enejder, A., Weckhuysen, B.M., Bonn, M., Inorganic Chemistry and Catalysis, Sub Inorganic Chemistry and Catalysis
Rok vydání:	2011
Předmět:	chemistry.chemical_classification Chemistry Reaction step Alkene Ether General Chemistry Carbocation Photochemistry Biochemistry Catalysis chemistry.chemical_compound Colloid and Surface Chemistry Reagent Reactivity (chemistry) Zeolite
Zdroj:	Journal of the American Chemical Society, 134(2), 1124. American Chemical Society
ISSN:	1520-5126 0002-7863
Popis:	The cost- and material-efficient development of next-generation catalysts would benefit greatly from a molecular-level understanding of the interaction between reagents and catalysts in chemical conversion processes. Here, we trace the conversion of alkene and glycol in single zeolite catalyst particles with unprecedented chemical and spatial resolution. Combined nonlinear Raman and two-photon fluorescence spectromicroscopies reveal that alkene activation constitutes the first reaction step toward glycol etherification and allow us to determine the activation enthalpy of the resulting carbocation formation. Considerable inhomogeneities in local reactivity are observed for micrometer-sized catalyst particles. Product ether yields observed on the catalyst are ca. 5 times higher than those determined off-line. Our findings are relevant for other heterogeneous catalytic processes and demonstrate the immense potential of novel nonlinear spectromicroscopies for catalysis research.
Databáze:	OpenAIRE
Externí odkaz:	https://explore.openaire.eu/search/publication?articleId=doi_dedup___::3740dc46ed9f83700d246ac473a73d5f https://pubmed.ncbi.nlm.nih.gov/22118571 Zobrazit plný text záznamu