Hybrid Polyoxotungstate/MIL-101 Materials: Synthesis, Characterization, and Catalysis of H2O2-Based Alkene Epoxidation Full article
| Journal |
Inorganic Chemistry
ISSN: 0020-1669 , E-ISSN: 1520-510X |
||||
|---|---|---|---|---|---|
| Output data | Year: 2010, Volume: 49, Number: 6, Pages: 2920-2930 Pages count : 11 DOI: 10.1021/ic902459f | ||||
| Tags | METAL-ORGANIC FRAMEWORKS; HETEROPOLY ACID H3PW12O40; HYDROGEN-PEROXIDE; TUNGSTOPHOSPHORIC ACID; OXIDATION CATALYSTS; SELECTIVE EPOXIDATION; OLEFIN EPOXIDATION; TERMINAL OLEFINS; ALLYLIC ALCOHOLS; SILICA | ||||
| Authors |
|
||||
| Affiliations |
|
Funding (4)
| 1 | Russian Foundation for Basic Research | 09-03-12112 |
| 2 | Russian Foundation for Basic Research | 09-03-93109 |
| 3 | Russian Foundation for Basic Research | 09-03-93113 |
| 4 | Siberian Branch of the Russian Academy of Sciences | 107 |
Abstract:
Polyoxotungstates [PW4O24]3− (PW4) and [PW12O40]3− (PW12) have been inserted into nanocages of the metal organic framework MIL-101. The hybrid materials PWx/MIL-101 (x = 4 or 12) containing 5−14 wt % of polyoxotungstate have been obtained and characterized by elemental analysis, N2 adsorption, FT-IR, Raman, and 31P NMR MAS spectroscopic techniques. Their catalytic performance was assessed in the selective oxidation of alkenes with aqueous hydrogen peroxide under mild reaction conditions ([H2O2] = 0.1−0.2 M, 50 °C, MeCN). PWx/MIL-101 enclosing 5 wt % of polyoxotungstate demonstrated fairly good catalytic activities in the epoxidation of various alkenes (3-carene, limonene, α-pinene, cyclohexene, cyclooctene, 1-octene), the turnover frequencies (TOF) and alkene conversions were close to the corresponding parameters achieved with homogeneous PWx. For the oxidation of substrates with aromatic groups (styrene, cis- and trans-stilbenes), a higher level of olefin conversion was attained using PW12/MIL-101. Moreover, confinement of PW12 within MIL-101 nanocages allowed us to reach higher epoxide selectivities at higher alkene conversions. The hybrid PWx/MIL-101 materials were stable to leaching, behaved as true heterogeneous catalysts, were easily recovered by filtration, and reused several times with the maintenance of the catalytic performance.
Cite:
Maksimchuk N.V.
, Kovalenko K.A.
, Arzumanov S.S.
, Chesalov Y.A.
, Melgunov M.S.
, Stepanov A.G.
, Fedin V.P.
, Kholdeeva O.A.
Hybrid Polyoxotungstate/MIL-101 Materials: Synthesis, Characterization, and Catalysis of H2O2-Based Alkene Epoxidation
Inorganic Chemistry. 2010. V.49. N6. P.2920-2930. DOI: 10.1021/ic902459f WOS Scopus РИНЦ ANCAN PMID OpenAlex
Hybrid Polyoxotungstate/MIL-101 Materials: Synthesis, Characterization, and Catalysis of H2O2-Based Alkene Epoxidation
Inorganic Chemistry. 2010. V.49. N6. P.2920-2930. DOI: 10.1021/ic902459f WOS Scopus РИНЦ ANCAN PMID OpenAlex
Dates:
| Submitted: | Dec 11, 2009 |
| Published online: | Feb 18, 2010 |
| Published print: | Mar 15, 2010 |
Identifiers:
| Web of science: | WOS:000275164900044 |
| Scopus: | 2-s2.0-77949389624 |
| Elibrary: | 15335659 |
| Chemical Abstracts: | 2010:213109 |
| Chemical Abstracts (print): | 152:381776 |
| PMID: | 20166742 |
| OpenAlex: | W1974312340 |