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Methanol-to-olefins catalysis on ERI-type molecular sieves: towards enhancing ethylene selectivity

Alshafei, Faisal H. and Park, Youngkyu and Zones, Stacey I. and Davis, Mark E. (2021) Methanol-to-olefins catalysis on ERI-type molecular sieves: towards enhancing ethylene selectivity. Journal of Catalysis, 404 . pp. 620-633. ISSN 0021-9517. doi:10.1016/j.jcat.2021.10.025. https://resolver.caltech.edu/CaltechAUTHORS:20211201-161242469

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Abstract

ERI-type molecular sieves (SSZ-98, UZM-12, ERI-type zeolite, SAPO-17) are synthesized with varying Si/Al = 5–9 and Si/T-atoms = 0.034–0.12 using several organic structure-directing agents (OSDAs), and evaluated as catalysts for the methanol-to-olefins (MTO) reaction. SAPO-34 (Si/T-atoms = 0.089) and SSZ-13 (Si/Al = 15) are also prepared and tested for comparison. The ERI-type zeolites gave improved ethylene-to-propylene ratios (E/P = 1.1–1.9) over SSZ-13 (E/P = 0.82) and SAPO-34 (E/P = 0.85). The SAPO-17 samples produced an E/P of 0.7–1.1 and a generally high C₄+ fraction. The differences observed in the olefins product distributions between the zeolites with low framework Si/Al (E/P > 1.5) and SAPO-17 with low Si/T-atom < 0.1 (E/P ≤ 1 and high C₄+) are the result of slower maturation of aromatic hydrocarbon-pool (HP) species and the presence of aromatics with bulky alkyl-groups (C₃-C₄) in the SAPO-17 samples. The rapid formation of cyclic intermediates and the shift in their composition towards less-methylated ((CH₃)_(n≤4)) methylbenzenes and methylnaphthalenes are found to be key to enhancing the ethylene selectivity in ERI-type molecular sieves.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1016/j.jcat.2021.10.025DOIArticle
ORCID:
AuthorORCID
Alshafei, Faisal H.0000-0003-1808-1374
Zones, Stacey I.0000-0002-3128-6481
Davis, Mark E.0000-0001-8294-1477
Additional Information:© 2021 Elsevier Inc. Received 1 August 2021, Revised 8 October 2021, Accepted 18 October 2021, Available online 25 October 2021. The Chevron Energy and Technology Company provided financial support for this research. The authors gratefully acknowledge Dr. Nathan Dalleska (Resnick Water and Environment Laboratory at the California Institute of Technology) for assistance with the GC-MS experiments, Dr. Sonjong Hwang for assistance with solid-state NMR, and Dr. Donglong Fu for valuable technical discussions. F.H.A. would like to thank Aramco R&D for financially supporting his graduate studies. Y.P. gratefully acknowledges financial support from Kwanjeong Educational Foundation. The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.
Funders:
Funding AgencyGrant Number
Chevron Energy Technology CompanyUNSPECIFIED
AramcoUNSPECIFIED
Kwanjeong Educational FoundationUNSPECIFIED
Subject Keywords:Erionite; Methanol-to-olefins; Small-pore zeolites; SAPOs
DOI:10.1016/j.jcat.2021.10.025
Record Number:CaltechAUTHORS:20211201-161242469
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20211201-161242469
Official Citation:Faisal H. Alshafei, Youngkyu Park, Stacey I. Zones, Mark E. Davis, Methanol-to-olefins catalysis on ERI-type molecular sieves: towards enhancing ethylene selectivity, Journal of Catalysis, Volume 404, 2021, Pages 620-633, ISSN 0021-9517, https://doi.org/10.1016/j.jcat.2021.10.025.
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:112129
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:01 Dec 2021 17:46
Last Modified:22 Dec 2021 21:45

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