Methane reacts with heteropolyacids chemisorbed on silica to produce acetic acid under soft conditions
Type
ArticleAuthors
Sun, MiaoAbou-Hamad, Edy

Rossini, Aaron J.
Zhang, Jizhe

Lesage, Anne
Zhu, Haibo
Pelletier, Jeremie

Emsley, Lyndon
Caps, Valerie

Basset, Jean-Marie

KAUST Department
Advanced Membranes and Porous Materials Research CenterBiological and Environmental Sciences and Engineering (BESE) Division
Chemical Science Program
KAUST Catalysis Center (KCC)
Physical Science and Engineering (PSE) Division
Date
2013-01-03Online Publication Date
2013-01-03Print Publication Date
2013-01-16Permanent link to this record
http://hdl.handle.net/10754/562614
Metadata
Show full item recordAbstract
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/ja309966jSponsors
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)PubMed ID
23268596ae974a485f413a2113503eed53cd6c53
10.1021/ja309966j
Scopus Count
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