Methane reacts with heteropolyacids chemisorbed on silica to produce acetic acid under soft conditions.
J Am Chem Soc
; 135(2): 804-10, 2013 Jan 16.
Article
em En
| MEDLINE
| ID: mdl-23268596
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(4)SiW(12)O(40), H(3)PW(12)O(40), H(4)SiMo(12)O(40), and H(3)PMo(12)O(40) 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.
Texto completo:
1
Coleções:
01-internacional
Base de dados:
MEDLINE
Idioma:
En
Revista:
J Am Chem Soc
Ano de publicação:
2013
Tipo de documento:
Article
País de afiliação:
Arábia Saudita