TY - JOUR
T1 - A Stable Extra-Large Pore and High-Silica Zeolite Derived from Ge-Rich Precursor
AU - Zhao, Yuhong
AU - Wu, Shitao
AU - Wang, Jilong
AU - Peng, Mingming
AU - Xu, Hao
AU - Jiang, Jingang
AU - Ma, Yanhang
AU - Wu, Peng
N1 - Publisher Copyright:
© 2024 Wiley-VCH GmbH.
PY - 2024/3/4
Y1 - 2024/3/4
N2 - A multidimensional extra-large pore zeolite with highly hydrothermal stability, denoted as −IRT−HS, has been developed successfully, starting from Ge-rich germanosilicate precursor hydrothermally directed by a small and commercially available piperidinium-type organic structure-directing agent (OSDA). −IRT−HS, with the supermicropores, is structurally analogues to 28-membered ring −IRT topology as confirmed by various spectroscopic techniques. And it is the high-silica (Si/Ge=58) zeolite with the largest pore size as well. Notably, using acid-washed as-made Ge-rich −IRT precursor as the silicon source is crucial to restore partially collapsed structure into a stable framework by OSDA-assisted recrystallization. The calcined −IRT−HS maintains a high crystallinity, even when stored in a humid environment for extended periods or directly exposed to water. Additionally, high silica Al-containing analogue is also readily synthesized, serving as an active solid-acid catalyst in 1,3,5-triisopropylbenzene cracking reaction, yielding an impressive initial conversion up to 76.1 % much higher than conventional large-pore Beta zeolite (30.4 %). This work will pave the way for the designed synthesis of targeted high-silica zeolites with stable and extra-large pore frameworks, mimicking the structures of existing Ge-rich counterparts.
AB - A multidimensional extra-large pore zeolite with highly hydrothermal stability, denoted as −IRT−HS, has been developed successfully, starting from Ge-rich germanosilicate precursor hydrothermally directed by a small and commercially available piperidinium-type organic structure-directing agent (OSDA). −IRT−HS, with the supermicropores, is structurally analogues to 28-membered ring −IRT topology as confirmed by various spectroscopic techniques. And it is the high-silica (Si/Ge=58) zeolite with the largest pore size as well. Notably, using acid-washed as-made Ge-rich −IRT precursor as the silicon source is crucial to restore partially collapsed structure into a stable framework by OSDA-assisted recrystallization. The calcined −IRT−HS maintains a high crystallinity, even when stored in a humid environment for extended periods or directly exposed to water. Additionally, high silica Al-containing analogue is also readily synthesized, serving as an active solid-acid catalyst in 1,3,5-triisopropylbenzene cracking reaction, yielding an impressive initial conversion up to 76.1 % much higher than conventional large-pore Beta zeolite (30.4 %). This work will pave the way for the designed synthesis of targeted high-silica zeolites with stable and extra-large pore frameworks, mimicking the structures of existing Ge-rich counterparts.
KW - extra-large pore
KW - germanosilicate
KW - high-silica zeolite
KW - small OSDAs
KW - solid-acid catalyst
UR - https://www.scopus.com/pages/publications/85183690227
U2 - 10.1002/anie.202318298
DO - 10.1002/anie.202318298
M3 - 文章
C2 - 38240576
AN - SCOPUS:85183690227
SN - 1433-7851
VL - 63
JO - Angewandte Chemie - International Edition
JF - Angewandte Chemie - International Edition
IS - 10
M1 - e202318298
ER -