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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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Zimmermann, Tobias1, Autor           
Bilke, Marius1, Autor           
Soorholtz, Mario2, Autor           
Schüth, Ferdi1, Autor           
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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Schlagwörter: methane functionalization; natural gas; platinum; product protection; selective oxidation
 Zusammenfassung: 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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Sprache(n): eng - English
 Datum: 2018-05-152018-08-272018-10-05
 Publikationsstatus: Online veröffentlicht
 Seiten: 7
 Ort, Verlag, Ausgabe: -
 Inhaltsverzeichnis: -
 Art der Begutachtung: Expertenbegutachtung
 Identifikatoren: DOI: 10.1021/acscatal.8b01878
 Art des Abschluß: -

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Titel: ACS Catalysis
  Kurztitel : ACS Catal.
Genre der Quelle: Zeitschrift
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Affiliations:
Ort, Verlag, Ausgabe: Washington, DC : ACS
Seiten: - Band / Heft: 8 (10) Artikelnummer: - Start- / Endseite: 9262 - 9268 Identifikator: ISSN: 2155-5435
CoNE: https://pure.mpg.de/cone/journals/resource/2155-5435