One-Pot Synthesis of CHA/ERI-Type Zeolite Intergrowth from a Single Multiselective Organic Structure-Directing Agent
Name
KwonBello-JuradoIkonnikova - One-Pot Synthesis of CHAERI-Type Zeolite Intergrowth from a Single M....pdf
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Accepted version
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Author(s)
Kwon, Soonhyoung
Bello-Jurado, Estefanía
Ikonnikova, Evgeniia
Lee, Hwajun
Schwalbe-Koda, Daniel
Corma, Avelino
Willhammar, Tom
Olivetti, Elsa A
Gomez-Bombarelli, Rafael
Moliner, Manuel
Date Issued
March 13, 2024
Journal
ACS Applied Materials & Interfaces
Publisher
American Chemical Society
Citation
Soonhyoung Kwon, Estefanía Bello-Jurado, Evgeniia Ikonnikova, Hwajun Lee, Daniel Schwalbe-Koda, Avelino Corma, Tom Willhammar, Elsa A. Olivetti, Rafael Gomez-Bombarelli, Manuel Moliner, and Yuriy Román-Leshkov.
ACS Applied Materials & Interfaces 2024 16 (12), 14661-14668.
Version
Author's final manuscript
Abstract
We report the one-pot synthesis of a chabazite (CHA)/erionite (ERI)-type zeolite intergrowth structure characterized by adjustable extents of intergrowth enrichment and Si/Al molar ratios. This method utilizes readily synthesizable 6-azaspiro[5.6]dodecan-6-ium as the exclusive organic structure-directing agent (OSDA) within a potassium-dominant environment. High-throughput simulations were used to accurately determine the templating energy and molecular shape, facilitating the selection of an optimally biselective OSDA from among thousands of prospective candidates. The coexistence of the crystal phases, forming a distinct structure comprising disk-like CHA regions bridged by ERI-rich pillars, was corroborated via rigorous powder X-ray diffraction and integrated differential-phase contrast scanning transmission electron microscopy (iDPC S/TEM) analyses. iDPC S/TEM imaging further revealed the presence of single offretite layers dispersed within the ERI phase. The ratio of crystal phases between CHA and ERI in this type of intergrowth could be varied systematically by changing both the OSDA/Si and K/Si ratios. Two intergrown zeolite samples with different Si/Al molar ratios were tested for the selective catalytic reduction (SCR) of NOx with NH3, showing competitive catalytic performance and hydrothermal stability compared to that of the industry-standard commercial NH3-SCR catalyst, Cu-SSZ-13, prevalent in automotive applications. Collectively, this work underscores the potential of our approach for the synthesis and optimization of adjustable intergrown zeolite structures, offering competitive alternatives for key industrial processes.
MIT Department
Massachusetts Institute of Technology. Department of Chemical Engineering
Massachusetts Institute of Technology. Department of Materials Science and Engineering
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DOI of Published Version
https://doi.org/10.1021/acsami.3c15810
