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  Methane to Chloromethane by Mechanochemical Activation: A Selective Radical Pathway

Bilke, M., Losch, P., Vozniuk, O., Bodach, A., & Schüth, F. (2019). Methane to Chloromethane by Mechanochemical Activation: A Selective Radical Pathway. Journal of the American Chemical Society, 141(28), 11212-11218. doi:10.1021/jacs.9b04413.

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 Creators:
Bilke, Marius1, Author           
Losch, Pit2, Author           
Vozniuk, Olena1, Author           
Bodach, Alexander3, Author           
Schüth, Ferdi1, Author           
Affiliations:
1Research Department Schüth, Max-Planck-Institut für Kohlenforschung, Max Planck Society, ou_1445589              
2Research Group Schmidt, Max-Planck-Institut für Kohlenforschung, Max Planck Society, ou_1445618              
3Research Group Felderhoff, Max-Planck-Institut für Kohlenforschung, Max Planck Society, ou_3027887              

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 Abstract: State-of-the-art processes to directly convert methane into CH3Cl are run under corrosive conditions and typically yield a mixture of chloromethanes requiring subsequent separation. We report a mechanochemical strategy to selectively convert methane to chloromethane under overall benign conditions, employing trichloroisocyanuric acid (TCCA) as a cheap and noncorrosive solid chlorinating agent. TCCA is shown to release active chlorine species upon milling with Lewis acids such as alumina and ceria to functionalize methane at moderate temperatures (<150 °C). A thorough parameter optimization led to a maximum methane chlorination rate of 0.8 μmol(CH4,conv) (g(catalyst) s)−1. Findings were compared to the thermal reaction of methane with TCCA and evidenced that mechanochemical activation permitted significantly lower reaction temperatures (90 vs 200 °C) at a drastically improved CH3Cl selectivity (95% vs 66% at 30% conversion). Considering the characterization of the interaction between TCCA and Lewis acids as well as the in-depth analysis of byproducts, we suggest a plausible reaction mechanism and a possible regeneration of the chlorinating agent.

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Language(s): eng - English
 Dates: 2019-04-242019-06-202019-07-17
 Publication Status: Published in print
 Pages: 7
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1021/jacs.9b04413
 Degree: -

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Title: Journal of the American Chemical Society
  Other : J. Am. Chem. Soc.
  Abbreviation : JACS
Source Genre: Journal
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Publ. Info: Washington, DC : American Chemical Society
Pages: - Volume / Issue: 141 (28) Sequence Number: - Start / End Page: 11212 - 11218 Identifier: ISSN: 0002-7863
CoNE: https://pure.mpg.de/cone/journals/resource/954925376870