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  Influence of Catalyst Concentration on Activity and Selectivity in Selective Methane Oxidation with Platinum Compounds in Sulfuric Acid and Oleum

Zimmermann, T., Bilke, M., Soorholtz, M., & Schüth, F. (2018). Influence of Catalyst Concentration on Activity and Selectivity in Selective Methane Oxidation with Platinum Compounds in Sulfuric Acid and Oleum. ACS Catalysis, 8(10), 9262-9268. doi:10.1021/acscatal.8b01878.

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Item Permalink: http://hdl.handle.net/21.11116/0000-0002-95F5-1 Version Permalink: http://hdl.handle.net/21.11116/0000-0004-73F4-7
Genre: Journal Article

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 Creators:
Zimmermann, Tobias1, Author              
Bilke, Marius1, Author              
Soorholtz, Mario2, Author              
Schüth, Ferdi1, Author              
Affiliations:
1Research Department Schüth, Max-Planck-Institut für Kohlenforschung, Max Planck Society, ou_1445589              
2Research Group Palkovits, Max-Planck-Institut für Kohlenforschung, Max Planck Society, ou_1445615              

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Free keywords: methane functionalization; natural gas; platinum; product protection; selective oxidation
 Abstract: Direct catalytic functionalization of methane, a “dream reaction”, is typically characterized by poorly active catalysts and low product selectivity. Selectivity is particularly high for the “Periana system”, in which methane is oxidized to methyl bisulfate in sulfuric acid/oleum using a η2-(2,2′-bipyrimidyl)dichloroplatinum(II) ((bpym)PtCl2, 1) catalyst. Recently it was shown that well-chosen reaction conditions result in not only high selectivity but also remarkably high activity, previously considered to be the prohibiting factor regarding commercialization. The high activity apparently contradicts the original report. Detailed studies of the dependence of activity and selectivity on the catalyst concentration resolve this contradiction and reveal solubility, transformation of catalyst precursors, speciation, and solubility of methane as crucial factors for the observed reaction rates. Additionally, the selectivity pattern clearly discloses the consecutive nature of the reaction network.

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Language(s): eng - English
 Dates: 2018-05-152018-08-272018-10-05
 Publication Status: Published online
 Pages: 7
 Publishing info: -
 Table of Contents: -
 Rev. Method: Peer
 Identifiers: DOI: 10.1021/acscatal.8b01878
 Degree: -

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Title: ACS Catalysis
  Abbreviation : ACS Catal.
Source Genre: Journal
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Publ. Info: Washington, DC : ACS
Pages: - Volume / Issue: 8 (10) Sequence Number: - Start / End Page: 9262 - 9268 Identifier: ISSN: 2155-5435
CoNE: https://pure.mpg.de/cone/journals/resource/2155-5435