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Selected Works of Aaron Rossini
Article
Methane Reacts with Heteropolyacids Chemisorbed on Silica to Produce Acetic Acid under Soft Conditions
Journal of the American Chemical Society (2013)
  • Miao Sun, King Abdullah University of Science and Technology
  • Edy Abou-Hamad, King Abdullah University of Science and Technology
  • Aaron J. Rossini, Université de Lyon
  • Jizhe Zhang, King Abdullah University of Science and Technology
  • Anne Lesage, University of Lyon
  • Haibo Zhu, King Abdullah University of Science and Technology
  • Jeremie D.A. Pelletier, King Abdullah University of Science and Technology
  • Lyndon Emsley, University of Lyon
  • Valerie Caps, King Abdullah University of Science and Technology
  • Jean-Marie Basset, King Abdullah University of Science and Technology
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Abstract
Selective functionalization of methane at moderate temperature is of crucial economic, environmental, and scientific importance. Here, we report that methane reacts with heteropolyacids (HPAs) chemisorbed on silica to produce acetic acid under soft conditions. Specially, when chemisorbed on silica, H4SiW12O40, H3PW12O40, H4SiMo12O40, and H3PMo12O40 activate the primary C–H bond of methane at room temperature and atmospheric pressure. With these systems, acetic acid is produced directly from methane, in a single step, in the absence of Pd and without adding CO. Extensive surface characterization by solid-state NMR spectroscopy, IR spectroscopy, cyclic voltammetry, and X-ray photoelectron spectroscopy suggests that C–H activation of methane is triggered by the protons in the HPA–silica interface with concerted reduction of the Keggin cage, leading to water formation and hydration of the interface. This is the simplest and mildest way reported to date to functionalize methane.
Disciplines
Publication Date
December 26, 2013
DOI
10.1021/ja309966j
Publisher Statement
Reprinted (adapted) with permission from Journal of the American Chemical Society, 135(2); 804-810. Doi: 10.1021/ja309966j. Copyright 2013 America Chemical Society.
Citation Information
Miao Sun, Edy Abou-Hamad, Aaron J. Rossini, Jizhe Zhang, et al.. "Methane Reacts with Heteropolyacids Chemisorbed on Silica to Produce Acetic Acid under Soft Conditions" Journal of the American Chemical Society Vol. 135 Iss. 2 (2013) p. 804 - 810
Available at: http://works.bepress.com/aaron-rossini/18/