Methane Reacts with Heteropolyacids Chemisorbed on Silica to Produce Acetic Acid under Soft Conditions - Archive ouverte HAL Accéder directement au contenu
Article Dans Une Revue Journal of the American Chemical Society Année : 2013

Methane Reacts with Heteropolyacids Chemisorbed on Silica to Produce Acetic Acid under Soft Conditions

Miao Sun
  • Fonction : Auteur
Anne Lesage
Haibo Zhu
  • Fonction : Auteur
Lyndon Emsley
  • Fonction : Auteur
  • PersonId : 925398
Valérie Caps
Jean-Marie Basset
  • Fonction : Auteur
  • PersonId : 925394

Résumé

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.
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Dates et versions

hal-00799220 , version 1 (11-03-2013)

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Citer

Miao Sun, Edy Abou-Hamad, Aaron J. Rossini, Jizhe Zhang, Anne Lesage, et al.. Methane Reacts with Heteropolyacids Chemisorbed on Silica to Produce Acetic Acid under Soft Conditions. Journal of the American Chemical Society, 2013, 135 (2), pp.804-810. ⟨10.1021/ja309966j⟩. ⟨hal-00799220⟩
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