TY - JOUR
T1 - Probing the Design Rationale of a High-Performing Faujasitic Zeotype Engineered to have Hierarchical Porosity and Moderated Acidity
AU - Chapman, Stephanie
AU - Carravetta, Marina
AU - Miletto, Ivana
AU - Doherty, Cara M.
AU - Dixon, Hannah
AU - Taylor, James D.
AU - Gianotti, Enrica
AU - Yu, Jihong
AU - Raja, Robert
N1 - Publisher Copyright:
© 2020 The Authors. Published by Wiley-VCH GmbH
PY - 2020/10/26
Y1 - 2020/10/26
N2 - Porosity and acidity are influential properties in the rational design of solid-acid catalysts. Probing the physicochemical characteristics of an acidic zeotype framework at the molecular level can provide valuable insights in understanding intrinsic reaction pathways, for affording structure–activity relationships. Herein, we employ a variety of probe-based techniques (including positron annihilation lifetime spectroscopy (PALS), FTIR and solid-state NMR spectroscopy) to demonstrate how a hierarchical design strategy for a faujasitic (FAU) zeotype (synthesized for the first time, via a soft-templating approach, with high phase-purity) can be used to simultaneously modify the porosity and modulate the acidity for an industrially significant catalytic process (Beckmann rearrangement). Detailed characterization of hierarchically porous (HP) SAPO-37 reveals enhanced mass-transport characteristics and moderated acidity, which leads to superior catalytic performance and increased resistance to deactivation by coking, compared to its microporous counterpart, further vindicating the interplay between porosity and moderated acidity.
AB - Porosity and acidity are influential properties in the rational design of solid-acid catalysts. Probing the physicochemical characteristics of an acidic zeotype framework at the molecular level can provide valuable insights in understanding intrinsic reaction pathways, for affording structure–activity relationships. Herein, we employ a variety of probe-based techniques (including positron annihilation lifetime spectroscopy (PALS), FTIR and solid-state NMR spectroscopy) to demonstrate how a hierarchical design strategy for a faujasitic (FAU) zeotype (synthesized for the first time, via a soft-templating approach, with high phase-purity) can be used to simultaneously modify the porosity and modulate the acidity for an industrially significant catalytic process (Beckmann rearrangement). Detailed characterization of hierarchically porous (HP) SAPO-37 reveals enhanced mass-transport characteristics and moderated acidity, which leads to superior catalytic performance and increased resistance to deactivation by coking, compared to its microporous counterpart, further vindicating the interplay between porosity and moderated acidity.
KW - acid catalysis
KW - heterogeneous catalysis
KW - hierarchical porosity
KW - probe-based techniques
KW - structure–activity relationships
UR - http://www.scopus.com/inward/record.url?scp=85089784117&partnerID=8YFLogxK
U2 - 10.1002/anie.202005108
DO - 10.1002/anie.202005108
M3 - Article
SN - 1433-7851
VL - 59
SP - 19561
EP - 19569
JO - Angewandte Chemie - International Edition
JF - Angewandte Chemie - International Edition
IS - 44
ER -