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

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    Type
    Article
    Authors
    Sun, Miao
    Abou-Hamad, Edy cc
    Rossini, Aaron J.
    Zhang, Jizhe cc
    Lesage, Anne
    Zhu, Haibo
    Pelletier, Jeremie cc
    Emsley, Lyndon
    Caps, Valerie cc
    Basset, Jean-Marie cc
    KAUST Department
    Advanced Membranes and Porous Materials Research Center
    Biological and Environmental Sciences and Engineering (BESE) Division
    Chemical Science Program
    KAUST Catalysis Center (KCC)
    Physical Science and Engineering (PSE) Division
    Date
    2013-01-03
    Online Publication Date
    2013-01-03
    Print Publication Date
    2013-01-16
    Permanent link to this record
    http://hdl.handle.net/10754/562614
    
    Metadata
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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, 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.
    Citation
    Sun, M., Abou-Hamad, E., Rossini, A. J., Zhang, J., Lesage, A., Zhu, H., … Basset, J.-M. (2013). Methane Reacts with Heteropolyacids Chemisorbed on Silica to Produce Acetic Acid under Soft Conditions. Journal of the American Chemical Society, 135(2), 804–810. doi:10.1021/ja309966j
    Sponsors
    The authors acknowledge KAUST Nuclear Magnetic Resonance Core Lab and technical assistance of Dr. Kazuo Yamauchi (NMR). The authors also wish to thank Dr. Aram Amassian, Mr. Ahmed E. Mansour, and Mr. Guy Olivier NGONGANG NDJAWA for their kind help in XPS measurements. M.S. acknowledges support from Dr. Xin Liu in HPA structure drawing. A.J.R acknowledges support from an EU Marie-Curie IIF fellowship (PIIF-GA-2010-274574). This work was supported by funds from King Abdullah University of Science and Technology and SABIC (Saudi Basic Industries Corporation) company.
    Publisher
    American Chemical Society (ACS)
    Journal
    Journal of the American Chemical Society
    DOI
    10.1021/ja309966j
    PubMed ID
    23268596
    ae974a485f413a2113503eed53cd6c53
    10.1021/ja309966j
    Scopus Count
    Collections
    Articles; Biological and Environmental Science and Engineering (BESE) Division; Advanced Membranes and Porous Materials Research Center; Physical Science and Engineering (PSE) Division; Chemical Science Program; KAUST Catalysis Center (KCC)

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