Methane reacts with heteropolyacids chemisorbed on silica to produce acetic acid under soft conditions

Miao Sun, Edy Abou-Hamad, Aaron J. Rossini, Jizhe Zhang, Anne Lesage, Haibo Zhu, Jeremie Pelletier, Lyndon Emsley, Valerie Caps, Jean-Marie Basset

Research output: Contribution to journalArticlepeer-review

17 Scopus citations

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, H 4SiW12O40, H3PW12O 40, H4SiMo12O40, and H 3PMo12O40 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. © 2012 American Chemical Society.
Original languageEnglish (US)
Pages (from-to)804-810
Number of pages7
JournalJournal of the American Chemical Society
Volume135
Issue number2
DOIs
StatePublished - Jan 3 2013

ASJC Scopus subject areas

  • Biochemistry
  • Colloid and Surface Chemistry
  • Chemistry(all)
  • Catalysis

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