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Tytuł:
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Coke Formation in a Zeolite Crystal During the Methanol-to-Hydrocarbons Reaction as Studied with Atom Probe Tomography.
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Autorzy:
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Schmidt JE; Debye Institute for Nanomaterials Science, Utrecht University, Universiteitsweg 99, 3584, CG, Utrecht, The Netherlands.
Poplawsky JD; Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, TN, 37831, USA.
Mazumder B; Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, TN, 37831, USA.
Attila Ö; Debye Institute for Nanomaterials Science, Utrecht University, Universiteitsweg 99, 3584, CG, Utrecht, The Netherlands.
Fu D; Debye Institute for Nanomaterials Science, Utrecht University, Universiteitsweg 99, 3584, CG, Utrecht, The Netherlands.
de Winter DA; Structural Geology & EM, Utrecht University, Postbus 80.021, 3508, TA, Utrecht, The Netherlands.
Meirer F; Debye Institute for Nanomaterials Science, Utrecht University, Universiteitsweg 99, 3584, CG, Utrecht, The Netherlands.
Bare SR; SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA, 94025, USA. .
Weckhuysen BM; Debye Institute for Nanomaterials Science, Utrecht University, Universiteitsweg 99, 3584, CG, Utrecht, The Netherlands. .
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Źródło:
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Angewandte Chemie (International ed. in English) [Angew Chem Int Ed Engl] 2016 Sep 05; Vol. 55 (37), pp. 11173-7. Date of Electronic Publication: 2016 Aug 03.
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Typ publikacji:
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Journal Article; Research Support, Non-U.S. Gov't
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Język:
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English
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Imprint Name(s):
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Publication: <2004-> : Weinheim : Wiley-VCH
Original Publication: Weinheim/Bergstr. : New York, : Verlag Chemie ; Academic Press, c1962-
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References:
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Contributed Indexing:
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Keywords: Al zoning; atom probe tomography; carbon deposits; methanol to hydrocarbons; zeolites
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Entry Date(s):
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Date Created: 20160804 Date Completed: 20180806 Latest Revision: 20210109
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Update Code:
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20240104
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PubMed Central ID:
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PMC6681177
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DOI:
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10.1002/anie.201606099
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PMID:
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27485276
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Understanding the formation of carbon deposits in zeolites is vital to developing new, superior materials for various applications, including oil and gas conversion processes. Herein, atom probe tomography (APT) has been used to spatially resolve the 3D compositional changes at the sub-nm length scale in a single zeolite ZSM-5 crystal, which has been partially deactivated by the methanol-to-hydrocarbons reaction using (13) C-labeled methanol. The results reveal the formation of coke in agglomerates that span length scales from tens of nanometers to atomic clusters with a median size of 30-60 (13) C atoms. These clusters correlate with local increases in Brønsted acid site density, demonstrating that the formation of the first deactivating coke precursor molecules occurs in nanoscopic regions enriched in aluminum. This nanoscale correlation underscores the importance of carefully engineering materials to suppress detrimental coke formation.
(© 2016 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA.)
