TY - JOUR
T1 - Thermal Alteration in Adsorption Sites over SAPO-34 Zeolite
AU - Li, Guangchao
AU - Yoskamtorn, Tatchamapan
AU - Chen, Wei
AU - Foo, Christopher
AU - Zheng, Jianwei
AU - Tang, Chiu
AU - Day, Sarah
AU - Zheng, Anmin
AU - Li, Molly Meng-Jung
AU - Tsang, Shik Chi Edman
N1 - Funding Information:
The diffraction, NMR, DRIFT, and refinement works were performed at the University of Oxford, UK with financial support from the IUK-EPSRC grant (55872-383337). The SXRD was measured at the I11 station with the beamtimes allocated by Diamond Synchrotron Light Source, UK. Part of NMR studies was conducted at UCEA of PolyU with funding from GDSTC grant (2021A1515010021) and RGC Hong Kong (PolyU P0033541). Modeling support was provided by the Wuhan Institute of Physics and Mathematics with fundings from the National Natural Science Foundation of China (Nos. 22125304, 22032005, 22002174, 21991092, and 21991090) and the National Key Research and Development Program of China (2021YFA1502600).
Funding Information:
The diffraction, NMR, DRIFT, and refinement works were performed at the University of Oxford, UK with financial support from the IUK‐EPSRC grant (55872‐383337). The SXRD was measured at the I11 station with the beamtimes allocated by Diamond Synchrotron Light Source, UK. Part of NMR studies was conducted at UCEA of PolyU with funding from GDSTC grant (2021A1515010021) and RGC Hong Kong (PolyU P0033541). Modeling support was provided by the Wuhan Institute of Physics and Mathematics with fundings from the National Natural Science Foundation of China (Nos. 22125304, 22032005, 22002174, 21991092, and 21991090) and the National Key Research and Development Program of China (2021YFA1502600).
Publisher Copyright:
© 2022 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.
PY - 2022/4
Y1 - 2022/4
N2 - Zeolites have found tremendous applications in the chemical industry. However, the dynamic nature of their active sites under the flow of adsorbate molecules for adsorption and catalysis is unclear, especially in operando conditions, which could be different from the as-synthesized structures. In the present study, we report a structural transformation of the adsorptive active sites in SAPO-34 zeolite by using acetone as a probe molecule under various temperatures. The combination of solid-state nuclear magnetic resonance, in situ variable-temperature synchrotron X-ray diffraction, and in situ diffuse-reflectance infrared Fourier-transform spectroscopy allow a clear identification and quantification that the chemisorption of acetone can convert the classical Brønsted acid site adsorption mode to an induced Frustrated Lewis Pairs adsorption mode at increasing temperatures. Such facile conversion is also supported by the calculations of ab-initio molecular-dynamics simulations. This work sheds new light on the importance of the dynamic structural alteration of active sites in zeolites with adsorbates at elevated temperatures.
AB - Zeolites have found tremendous applications in the chemical industry. However, the dynamic nature of their active sites under the flow of adsorbate molecules for adsorption and catalysis is unclear, especially in operando conditions, which could be different from the as-synthesized structures. In the present study, we report a structural transformation of the adsorptive active sites in SAPO-34 zeolite by using acetone as a probe molecule under various temperatures. The combination of solid-state nuclear magnetic resonance, in situ variable-temperature synchrotron X-ray diffraction, and in situ diffuse-reflectance infrared Fourier-transform spectroscopy allow a clear identification and quantification that the chemisorption of acetone can convert the classical Brønsted acid site adsorption mode to an induced Frustrated Lewis Pairs adsorption mode at increasing temperatures. Such facile conversion is also supported by the calculations of ab-initio molecular-dynamics simulations. This work sheds new light on the importance of the dynamic structural alteration of active sites in zeolites with adsorbates at elevated temperatures.
KW - Active Sites
KW - Frustrated Lewis Pair
KW - Solid-State Nuclear Magnetic Resonance
KW - Synchrotron X-Ray Diffraction
KW - Zeolites
UR - http://www.scopus.com/inward/record.url?scp=85130062194&partnerID=8YFLogxK
U2 - 10.1002/anie.202204500
DO - 10.1002/anie.202204500
M3 - Journal article
C2 - 35471635
AN - SCOPUS:85130062194
SN - 1433-7851
VL - 61
JO - Angewandte Chemie - International Edition
JF - Angewandte Chemie - International Edition
IS - 27
M1 - e202204500
ER -