Highly Selective H2O2-Based Oxidation of Alkylphenols to p-Benzoquinones over MIL-125 Metal-Organic Frameworks
Научная публикация
| Общее |
Язык:
Английский,
Жанр:
Статья (Full article),
Статус опубликования:
Опубликована,
Оригинальность:
Оригинальная
|
| Журнал |
European Journal of Inorganic Chemistry
ISSN: 1434-1948
, E-ISSN: 1099-0682
|
| Вых. Данные |
Год: 2014,
Том: 2014,
Номер: 1,
Страницы: 132-139
Страниц
: 8
DOI:
10.1002/ejic.201301098
|
| Ключевые слова |
Heterogeneous catalysis, Hydrogen peroxide, Metal-organic framework, Oxidation, Titanium |
| Авторы |
Ivanchikova Irina D.
1
,
Lee Ji Sun
2,3
,
Maksimchuk Natalia V.
1
,
Shmakov Alexander N.
1
,
Chesalov Yurii A.
1
,
Ayupov Artem B.
1
,
Hwang Young Kyu
2
,
Jun Chul-Ho
3
,
Chang Jong-San
2,4
,
Kholdeeva Oxana A.
1
|
| Организации |
| 1 |
Boreskov Institute of Catalysis, Pr. Akademika Lavrentieva 5, Novosibirsk 630090, Russia
|
| 2 |
Korea Research Institute of Chemical Technology (KRICT), P. O. Box 107, Gajeongro 141, Yuseong, Daejeon 305-600, Republic of Korea
|
| 3 |
Department of Chemistry and Center for Bioactive Molecular Hybrid, Yonsei University, Seoul 120-749, Republic of Korea
|
| 4 |
Department of Chemistry, Sungkyunkwan University, Suwon 440-476, Republic of Korea
|
|
Информация о финансировании (2)
|
1
|
Российский фонд фундаментальных исследований
|
13-03-00413
|
|
2
|
Korea Research Institute of Chemical Technology
|
SK-1301
|
The titanium-based metal–organic framework MIL-125 and its amine-functionalized analog, MIL-125_NH2, have been synthesized and characterized by elemental analysis, XRD, SEM, TEM, N2 adsorption measurements, and spectroscopic techniques, including FTIR, Raman, and DR UV/Vis spectroscopy. Catalytic properties of MIL-125 and MIL-125_NH2 were evaluated in the selective oxidation of two representative alkyl-substituted phenols, 2,3,6-trimethylphenol and 2,6-di-tert-butylphenol, with the clean oxidant H2O2. With both MIL-125 and MIL-125_NH2, the selectivity toward the corresponding p-benzoquinones was 100 %. Samples of MIL-125 with different sizes of crystallites (0.5, 1.5, and 5 μm) demonstrated similar reaction rates, thus indicating the absence of diffusion limitations. The efficiency of the oxidant utilization and stability of the MIL-125 structure increased upon decreasing the amount of water in the reaction mixture. Even if the structural integrity of MIL-125 was destroyed by the reaction medium, the metal–organic framework acted as a precursor for the highly active, selective, and recyclable catalyst. The MIL-125-derived materials were stable toward titanium leaching, behaved as true heterogeneous catalysts, and could easily be recovered by filtration and reused several times without the loss of the catalytic properties.