TY - JOUR
T1 - Al-containing Ge-rich IWV
T2 - rapid synthesis via interzeolite transformation and application in Baeyer-Villiger oxidation
AU - Jiao, Meichen
AU - Jia, Chunmin
AU - Xu, Hao
AU - Wu, Peng
AU - Zhang, Xian Ming
N1 - Publisher Copyright:
© Science China Press 2024.
PY - 2024/7
Y1 - 2024/7
N2 - 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, 29Si and 27Al MAS NMR, FTIR, and N2 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 extra-framework 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. (Figure presented.)
AB - 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, 29Si and 27Al MAS NMR, FTIR, and N2 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 extra-framework 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. (Figure presented.)
KW - Al assistance
KW - Baeyer-Villiger oxidation
KW - Ge-rich IWV
KW - interzeolite transformation
UR - https://www.scopus.com/pages/publications/85195468277
U2 - 10.1007/s11426-023-1992-3
DO - 10.1007/s11426-023-1992-3
M3 - 文章
AN - SCOPUS:85195468277
SN - 1674-7291
VL - 67
SP - 2282
EP - 2291
JO - Science China Chemistry
JF - Science China Chemistry
IS - 7
ER -