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Carbonylation of dimethyl ether on solid Rh-promoted Cs-salt of Keggin 12-H3PW12O40: A solid-state NMR study of the reaction mechanism
Luzgin, MV; Kazantsev, MS; Volkova, GG; Wang, W(王为); Stepanov, AG; Stepanov, AG (reprint author), Russian Acad Sci, Siberian Branch, Boreskov Inst Catalysis, Prospekt Akad Lavrentieva 5, Novosibirsk 630090, Russia.
2011-01-03
Source PublicationJOURNAL OF CATALYSIS   Impact Factor & Quartile
ISSN0021-9517
Volume277Issue:1
AbstractThe carbonylation of dimethyl ether (DME) with carbon monoxide on Rh-promoted cesium salt of 12-tungstophosphoric acid, Rh/Cs2HPW12O40 (HPA), has been studied with C-13 solid-state NMR. The bifunctional character of Rh/Cs2HPW12O40 catalyst in halide-free carbonylation of DME has been directly demonstrated. The activation of the C-O bond of DME proceeds on Bronsted acid sites of HPA with the formation of the methyl group attached to the surface of HPA (methoxy species), whereas the role of rhodium consists in trapping carbon monoxide from gaseous phase and a transfer of CO to the center of DME activation, acidic OH-group of the catalyst, in the form of rhodium carbonyls. The lattice of Cs2HPW12O40 makes it possible to locate these two different active centers in close proximity to each other, e.g., on two adjacent oxygen atoms, terminal and bridging, of one Keggin anion, thus facilitating the insertion of carbon monoxide from rhodium carbonyl into the C-O bond of methoxy-group to produce the acetate group bound to the Keggin anion. The latter offers finally methyl acetate under the interaction with DME, the intermediate surface methoxy-groups being restored. (C) 2010 Elsevier Inc. All rights reserved.
KeywordDimethyl ether Carbon monoxide Carbonylation Mechanism 12-Tungstophosphoric acid Methoxy species Rhodium carbonyls Solid-state NMR
Subject AreaChemistry ; Engineering
PublisherELSEVIER
DOI10.1016/j.jcat.2010.10.015
Publication PlaceSAN DIEGO
Indexed BySCIE ; EI
Language英语
First Inst
Funding Project国家自然科学基金项目 ; 高等学校学科创新引智计划(111计划)
Project NumberRussian Foundation for Basic Research [08-03-92210] ; Federal Target Program (FTP) "Science, Academic and Teaching Staff of Innovative Russia" [P253] ; National Natural Science Foundation of China [20602016] ; 111 project
WOS IDWOS:000286700300008
Funding OrganizationRussian Foundation for Basic Research [08-03-92210]; Federal Target Program (FTP) "Science, Academic and Teaching Staff of Innovative Russia" [P253]; National Natural Science Foundation of China [20602016]; 111 project ; NSFC ; SAFEA ; MOE
SubtypeArticle
EI ID20105113499524
Department[Luzgin, Mikhail V.;
Kazantsev, Maxim S.;
Volkova, Galina G.;
Stepanov, Alexander G.] Russian Acad Sci, Siberian Branch, Boreskov Inst Catalysis, Novosibirsk 630090, Russia;
[Wang, Wei] Lanzhou Univ, Coll Chem & Chem Engn, State Key Lab Appl Organ Chem, Lanzhou 730000, Gansu, Peoples R China;
[Luzgin, Mikhail V.;
Kazantsev, Maxim S.;
Stepanov, Alexander G.] Novosibirsk State Univ, Dept Nat Sci, Novosibirsk 630090, Russia
Citation statistics
Cited Times:33[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttps://ir.lzu.edu.cn/handle/262010/75847
Collection化学化工学院
兰州大学
Corresponding AuthorStepanov, AG (reprint author), Russian Acad Sci, Siberian Branch, Boreskov Inst Catalysis, Prospekt Akad Lavrentieva 5, Novosibirsk 630090, Russia.
Recommended Citation
GB/T 7714
Luzgin, MV,Kazantsev, MS,Volkova, GG,et al. Carbonylation of dimethyl ether on solid Rh-promoted Cs-salt of Keggin 12-H3PW12O40: A solid-state NMR study of the reaction mechanism[J]. JOURNAL OF CATALYSIS,2011,277(1).
APA Luzgin, MV,Kazantsev, MS,Volkova, GG,Wang, W,Stepanov, AG,&Stepanov, AG .(2011).Carbonylation of dimethyl ether on solid Rh-promoted Cs-salt of Keggin 12-H3PW12O40: A solid-state NMR study of the reaction mechanism.JOURNAL OF CATALYSIS,277(1).
MLA Luzgin, MV,et al."Carbonylation of dimethyl ether on solid Rh-promoted Cs-salt of Keggin 12-H3PW12O40: A solid-state NMR study of the reaction mechanism".JOURNAL OF CATALYSIS 277.1(2011).
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