Improved Fe/Mg-Al hydrotalcite catalyst for Baeyer-Villiger oxidation of ketones with molecular oxygen and benzaldehyde

Autor: Naoko Fujisaki, Tsuneji Sano, Tomonori Kawabata, Kiyoshi Nomura, Katsuomi Takehira, Tetsuya Shishido
Jazyk: angličtina
Rok vydání: 2006
Předmět:
Zdroj: JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL. 253(1-2):279-289
ISSN: 1381-1169
Popis: Metal (Me: Fe, Co, Ni or Cu) containing Mg-Al hydrotalcite-type anionic clay catalysts have been prepared by adopting the “memory effect” of hydrotalcite and tested for Baeyer–Villiger oxidation of ketones. Mg-Al hydrotalcite was calcined to the mixed oxide and dipped in an aqueous solution of metal (Me) salt; metal species was incorporated by “memory effect” to form Me/Mg-Al hydrotalcite as the active phase on the surface of the Mg-Al mixed oxide. The activity and the structure of these catalysts have been compared with those of metal supported catalysts prepared by coprecipitation and impregnation. Among the metals tested, iron was the most effective and use of Fe(NH 4 ) 2 (SO 4 ) 2 ·6H 2 O as the metal salt resulted in the highest activity. The activity of the catalyst was higher than those prepared by coprecipitation from the nitrates of Mg, Fe and Al. Judging from Mossbauer and Fe K-edge XAFS spectra, Fe species possess the Fe 3+ valence state, are mainly octahedrally coordinated and form Fe O Fe cluster-type structure on the Mg-Al mixed oxides. This clearly indicates that the Fe 3+ O Fe 3+ cluster-type compounds are more active for the Baeyer–Villiger oxidation than well dispersed Fe 3+ species formed on the hydrotalcite prepared by coprecipitation. Six-membered cyclic ketones, such as cyclohexanone, 2-norbornone and 2-adamantanone, were effectively oxidized to the corresponding lactones by using O 2 /benzaldehyde as an oxidizing agent.
Databáze: OpenAIRE