Cyclohexene oxidation with h 2 o 2 over metal-organic framework mil-125(Ti): The effect of protons on reactivity

Nataliya Maksimchuk, Ji Sun Lee, Artem Ayupov, Jong San Chang, Oxana Kholdeeva

Результат исследования: Научные публикации в периодических изданияхстатья

5 Цитирования (Scopus)

Аннотация

The catalytic performance of the titanium-based metal-organic framework MIL-125 was evaluated in the selective oxidation of cyclohexene (CyH) with environmentally friendly oxidants, H 2 O 2 and t BuOOH. The catalytic activity of MIL-125 as well as the oxidant utilization efficiency and selectivity toward epoxide and epoxide-derived products can be greatly improved by acid additives (HClO 4 or CF 3 SO 3 H). In the presence of 1 molar equivalent (relative to Ti) of a proton source, the total selectivity toward CyH epoxide and trans-cyclohexane-1,2-diol reached 75-80% at 38-43% alkene conversion after 45 min of reaction with 1 equivalent of 30% H 2 O 2 at 50 °C. With 50% H 2 O 2 as the oxidant, the total selectivity toward heterolytic oxidation products increased up to 92% at the same level of alkene conversion. N 2 adsorption, powder X-ray diffraction (PXRD), and infrared (IR) spectroscopy studies before and after the catalytic oxidations confirmed the absence of structural changes in the Metal-organic framework (MOF) structure. MIL-125 was stable toward titanium leaching, behaved as a truly heterogeneous catalyst, and could easily be recovered and reused several times without any loss of the catalytic properties.

Язык оригиналаанглийский
Номер статьи324
Число страниц14
ЖурналCatalysts
Том9
Номер выпуска4
DOI
СостояниеОпубликовано - 1 апр 2019

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