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Cage-defining Ring: A Molecular Sieve Structural Indicator for Light Olefin Product Distribution from the Methanol-to-Olefins Reaction

Kang, Jong Hun and Alshafei, Faisal H. and Zones, Stacey I. and Davis, Mark E. (2019) Cage-defining Ring: A Molecular Sieve Structural Indicator for Light Olefin Product Distribution from the Methanol-to-Olefins Reaction. ACS Catalysis, 9 (7). pp. 6012-6019. ISSN 2155-5435. https://resolver.caltech.edu/CaltechAUTHORS:20190412-081340826

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Abstract

The methanol-to-olefins (MTO) process produces high-value-added light olefins from nonpetroleum sources. Acidic zeotypes containing cages bounded by 8-ring (small-pore) windows can effectively catalyze the MTO reaction, since their cages can accommodate the necessary aromatic intermediates that produce the light olefin products that escape. While progress on the mechanisms of the MTO reaction continues, zeotype structure–reaction property relationships have yet to be elucidated. Here, we report MTO reaction results from various small-pore, cage-containing silicoaluminophosphate/metalloaluminophosphates (SAPO/MAPOs) and zeolites under the same reaction conditions. The MTO behaviors of microporous materials having the following topologies are investigated: LEV, ERI, CHA, AFX, SFW, AEI, DDR, RTH, ITE, SAV, LTA, RHO, KFI, and UFI. The previous observation that light olefin product distributions from a series of small-pore, cage-containing zeolites can be classified into four structural categories is further supported by the results shown here from zeolite structures not investigated in the previous study and SAPO and MAPO materials with isostructural frameworks to all the zeolites. Additionally, these data reveal that light olefin product distributions are very similar over a given topology independent of framework composition. To develop a structure–property relationship between the framework topology and the MTO light olefin product distribution, the concept of the cage-defining ring size is introduced. The cage-defining ring size is defined as the minimum number of tetrahedral atoms of the ring encircling the center of the framework cages in the molecular sieve topology. It is shown that the cage-defining ring size correlates with MTO light olefin product distribution.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1021/acscatal.9b00746DOIArticle
ORCID:
AuthorORCID
Kang, Jong Hun0000-0002-4197-9070
Davis, Mark E.0000-0001-8294-1477
Additional Information:© 2019 American Chemical Society. Received: February 19, 2019; Revised: April 5, 2019; Published: April 11, 2019. The Chevron Energy and Technology Company provided financial support for this research. J.H.K. would like to thank the Samsung Scholarship for financial support for his graduate studies. The authors declare no competing financial interest.
Funders:
Funding AgencyGrant Number
Chevron Energy and Technology CompanyUNSPECIFIED
Samsung ScholarshipUNSPECIFIED
Subject Keywords:zeolite, SAPO, MAPO, structure−property relationships, solid acid catalysis
Issue or Number:7
Record Number:CaltechAUTHORS:20190412-081340826
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20190412-081340826
Official Citation:Cage-Defining Ring: A Molecular Sieve Structural Indicator for Light Olefin Product Distribution from the Methanol-to-Olefins Reaction. Jong Hun Kang, Faisal H. Alshafei, Stacey I. Zones, and Mark E. Davis. ACS Catalysis 2019 9 (7), 6012-6019. DOI: 10.1021/acscatal.9b00746
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:94679
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:12 Apr 2019 15:47
Last Modified:03 Oct 2019 21:06

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