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dc.contributor.authorYue, Yuanyuan
dc.contributor.authorFu, Jing
dc.contributor.authorWang, Chuanming
dc.contributor.authorYuan, Pei
dc.contributor.authorBao, Xiaojun
dc.contributor.authorXie, Zailai
dc.contributor.authorBasset, Jean-Marie
dc.contributor.authorZhu, Haibo
dc.date.accessioned2021-01-13T12:40:35Z
dc.date.available2021-01-13T12:40:35Z
dc.date.issued2021-01
dc.date.submitted2020-06-04
dc.identifier.citationYue, Y., Fu, J., Wang, C., Yuan, P., Bao, X., Xie, Z., … Zhu, H. (2021). Propane Dehydrogenation Catalyzed by Single Lewis Acid Site in Sn-Beta Zeolite. Journal of Catalysis. doi:10.1016/j.jcat.2020.12.019
dc.identifier.issn0021-9517
dc.identifier.doi10.1016/j.jcat.2020.12.019
dc.identifier.urihttp://hdl.handle.net/10754/666890
dc.description.abstractThe gap between supply and demand of propylene has become more and more evident, because of a large consumption of the downstream products derived from propylene. Propane dehydrogenation (PDH) constitutes an important alternative for the production of propylene, and thus considerable attention has been paid to the development of eco-friendly and cost-efficient catalysts for this process. Herein, we discover that the Sn-Beta zeolite with Lewis acid sites can activate the C-H bond, and exhibits high catalytic performance in the PDH. XRD, STEM, and XPS characterizations confirm that Sn species are incorporated into the zeolite framework, and H2-TPR suggests that there is a strong interaction between Sn species and zeolite framework. It is found that the Lewis acid is the active site for dehydrogenation reaction, and the Brønsted acid is responsible for cracking reaction. The dehydrogenation rate/cracking rate is positively proportional to the L/B ratio, and a high L/B ratio is beneficial for the propane dehydrogenation reaction. The Na-Sn-Beta-30 catalyst possessing the highest amount of Lewis acid but the lowest Brønsted/Lewis ratio, exhibits the best performance in the PDH, which delivers propane conversion of 40% and propylene selectivity of 92%. Most importantly, these Sn-Beta zeolites are extremely stable without any detectable deactivation under the harsh reaction condition for 72 hours. Density functional theory calculations reveal that both Sn and adjacent O atom or OH group cooperatively act as the active sites. The PDH occurs through the direct reaction mechanism in which hydrogen molecule is produced by the direct coupling of H atom of primary C3H7 motif with the Brønsted proton in closed sites or the proton of water in open sites. It seems that open sites are more reactive than the closed ones, and the intrinsic enthalpy barriers are calculated to be 242 ∼ 301 kJ/mol depending on the hydroxylation extents. These efficient Sn-Beta zeolites could provide a new possibility for the development of a new generation of PDH catalysts with a high stability for the production of propylene.
dc.publisherElsevier BV
dc.relation.urlhttps://linkinghub.elsevier.com/retrieve/pii/S002195172030511X
dc.rightsNOTICE: this is the author’s version of a work that was accepted for publication in Journal of Catalysis. Changes resulting from the publishing process, such as peer review, editing, corrections, structural formatting, and other quality control mechanisms may not be reflected in this document. Changes may have been made to this work since it was submitted for publication. A definitive version was subsequently published in Journal of Catalysis, [, , (2021-01)] DOI: 10.1016/j.jcat.2020.12.019 . © 2021. This manuscript version is made available under the CC-BY-NC-ND 4.0 license http://creativecommons.org/licenses/by-nc-nd/4.0/
dc.titlePropane Dehydrogenation Catalyzed by Single Lewis Acid Site in Sn-Beta Zeolite
dc.typeArticle
dc.contributor.departmentChemical Science Program
dc.contributor.departmentKAUST Catalysis Center (KCC)
dc.contributor.departmentPhysical Science and Engineering (PSE) Division
dc.identifier.journalJournal of Catalysis
dc.rights.embargodate2022-01-01
dc.eprint.versionPost-print
dc.contributor.institutionNational Engineering Research Center of Chemical Fertilizer Catalyst, School of Chemical Engineering, Fuzhou University, Fuzhou 350002, China.
dc.contributor.institutionState Key Laboratory of Green Chemical Engineering and Industrial Catalysis, Sinopec Shanghai Research Institute of Petrochemical Technology, Shanghai 201208, China.
dc.contributor.institutionState Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou 350002, China.
kaust.personBasset, Jean-Marie
dc.date.accepted2020-12-20
refterms.dateFOA2021-01-13T12:43:15Z


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