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Proton proximity – New key parameter controlling adsorption, desorption and activity in propene oligomerization over H-ZSM-5 zeolites
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SYSNO ASEP 0464693 Document Type J - Journal Article R&D Document Type Journal Article Subsidiary J Článek ve WOS Title Proton proximity – New key parameter controlling adsorption, desorption and activity in propene oligomerization over H-ZSM-5 zeolites Author(s) Bernauer, Milan (UFCH-W) ORCID, RID
Tabor, Edyta (UFCH-W) RID, ORCID
Pashkova, Veronika (UFCH-W) RID, ORCID
Kaucký, Dalibor (UFCH-W) RID, ORCID
Sobalík, Zdeněk (UFCH-W) RID
Wichterlová, Blanka (UFCH-W) RID
Dědeček, Jiří (UFCH-W) RID, ORCIDSource Title Journal of Catalysis. - : Elsevier - ISSN 0021-9517
Roč. 344, DEC 2016 (2016), s. 157-172Number of pages 16 s. Language eng - English Country US - United States Keywords ZSM-5 ; Al siting ; Single Al Subject RIV CF - Physical ; Theoretical Chemistry R&D Projects GA15-13876S GA ČR - Czech Science Foundation (CSF) LM2015073 GA MŠMT - Ministry of Education, Youth and Sports (MEYS) Institutional support UFCH-W - RVO:61388955 UT WOS 000390182800016 EID SCOPUS 84991660817 DOI 10.1016/j.jcat.2016.09.025 Annotation The proximity of protons (∼5 Å) derived from the distribution of Al atoms in the H-ZSM-5 framework has been shown to substantially affect the rate of propene oligomerization. Two sets of H-ZSM-5 zeolites (Si/Al 13–30) greatly differing in the occurrence of Al pairs (AlSiSiAl sequences in 6MRs) or distant Al atoms in the framework (both located prevailingly at the channel intersections) were synthesized to analyze the effect of the proton proximity. Propene adsorption and formation of oligomeric alkoxides is faster over distant isolated protons, while the close (5 Å) positive charges of proximate protons result in faster olefin(s) release from H-bonded propene and oligomeric alkoxides. As the steady-state TOF of propene oligomerization to C4–C9 olefins at 473–533 K over close protons exceeds 2–10 fold (with increasing Si/Al) those over isolated protons, the release of olefins from alkoxides is suggested to be an important reaction step. The distribution of framework Al atoms determining the mutual distances of protons represents a new parameter for evaluating rates of acid-catalyzed reactions and individual steps over H-zeolites. Workplace J. Heyrovsky Institute of Physical Chemistry Contact Michaela Knapová, michaela.knapova@jh-inst.cas.cz, Tel.: 266 053 196 Year of Publishing 2017
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