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Al-containing Ge-rich IWV:rapid synthesis via interzeolite transformation and application in Baeyer-Villiger oxidation

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摘要 Ge-containing Lewis acidic zeolites are typically synthesized using a conventional hydrothermal strategy from amorphous silica sources,through a long time-and energy-consuming approach limiting their wide applications.This study reports a rapid synthesis strategy for a series of IWV aluminogermanosilicate zeolites(T-x-Al)with a wide range of Si/Ge molar ratios(5–15)by interzeolite transformation of dealuminated FAU(DA-FAU).Notably,Ge-rich IWV could be obtained with crystallization time as short as one day by the equimolecular Si/Ge ratio gel.The effect of synthetic parameters was investigated and the obtained T-x-Al samples were characterized by XRD,SEM,EDS,ICP,^(29)Si and^(27)Al MAS NMR,FTIR,and N_(2)physisorption analyses.Compared with a previously reported IWV germanosilicate(H-3),T-x-Al displayed a better catalytic activity in Baeyer-Villiger(BV)oxidation,attributed to the presence of the active framework Ge sites with the assistance of the extraframework Al species.The cyclic catalysis tests revealed that the presence of framework Al species contributed to the stability of the T-x-Al.Specifically,T-x-Al,with 14-membered ring(MR)supercages,outperformed the typical 12-MR Sn-beta catalyst in the BV oxidation of large ketone-like 2-admantanone,indicating a promising potential application in the macromolecular catalytic process.
出处 《Science China Chemistry》 SCIE EI CAS CSCD 2024年第7期2282-2291,共10页 中国科学(化学英文版)
基金 supported by the National Natural Science Foundation of China(22302116) the Natural Science Foundation of Shanxi Province(202203021212412)。
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