Reactivity of Methoxy Species toward CO on Keggin 12-H3PW12O40: A Study with Solid State NMR
Full article
| Общее |
Language:
Английский,
Genre:
Full article,
Status:
Published,
Source type:
Original
|
| Journal |
The Journal of Physical Chemistry C
ISSN: 1932-7447
, E-ISSN: 1932-7455
|
| Output data |
Year: 2009,
Volume: 113,
Number: 45,
Pages: 19639-19644
Pages count
: 6
DOI:
10.1021/jp906888m
|
| Authors |
Luzgin Mikhail V.
1,2
,
Kazantsev Maxim S.
2
,
Wang Wei
3
,
Stepanov Alexander G.
1,2
|
| Affiliations |
| 1 |
Boreskov Institute of Catalysis, Siberian Branch of Russian Academy of Sciences, Prospekt Akademika Lavrentieva 5, Novosibirsk 630090, Russia
|
| 2 |
Department of Natural Sciences, Novosibirsk State University, Pirogova Street 2, Novosibirsk 630090, Russia
|
| 3 |
State Key Laboratory of Applied Organic Chemistry, College of Chemistry and Chemical Engineering, Lanzhou University, Gansu 730000, People’s Republic of China
|
|
Funding (2)
|
1
|
Russian Foundation for Basic Research
|
08-03-92210
|
|
2
|
National Natural Science Foundation of China
|
20602016
|
By using 13C solid-state NMR, monitoring the reactivity of methoxy species with carbon monoxide has been performed on 12-tungstophosphoric acid, H3PW12O40, at 423−473 K. Surface methoxy species have been selectively prepared from methanol at 293−423 K. Almost quantitative conversion of surface methoxy species into acetyl groups bound to the Keggin anion and acetic acid has been observed at 473 K. These data provide unambiguous evidence for the role of methoxy species as the intermediate of methanol and dimethyl ether carbonylation on solid H3PW12O40. The formation of a trimethyloxonium ion has been detected on the surface of heteropolyacid for the first time. The carbonylation of trimethyloxonium proceeds via the analogous mechanism through the methoxy species intermediate.