Abstract
The presented report focuses on an in-depth detailed characterization of immobilized methyltrioxorhenium (MTO), giving catalysts with a wide spectra of utilization. The range of mesoporous materials with different SiO2/Al2O3 ratios, namely mesoporous alumina (MA), aluminosilicates type Siral (with Al content 60%–90%) and MCM-41, were used as supports for immobilization of MTO. The tested support materials (aluminous/siliceous) exhibited high surface area, well-defined regular structure and narrow pore size distribution of mesopores, and therefore represent excellent supports for the active components. Some of the supports were modified by zinc chloride in order to obtain catalysts with higher activities for instance in metathesis reactions. The immobilization of MTO was optimized using these supports and it was successful using all supports. The success of the immobilization of MTO and the properties of the prepared heterogeneous catalysts were characterized using X-ray Fluorescence (XRF), atomic absorption spectroscopy (AAS), X-ray powder diffraction (XRD), scanning electron microscopy (SEM), physical adsorption of N2, ultraviolet-visible spectroscopy (UV-Vis), infrared spectroscopy (FTIR), Fourier Transform Infrared Spectroscopy (FTIR) using pyridine as a probe molecule and X-ray photoelectron spectroscopy (XPS). Furthermore, the catalytic activity of the immobilized MTO on the tested supports was demonstrated on metathesis reactions of various substrates.
Highlights
Methyltrioxorhenium (MTO) was described by Hermann et al more than 30 years ago as the first organometallic rhenium oxide [1,2,3]
The heterogenization of MTO is necessary for the successful performance of the metathesis reaction [10], since it is well known that metathesis reactions are initialized by metallocarbene present in the catalyst
MTO immobilized on materials with different physico-chemical properties were tested for various metathesis reactions in the presented research
Summary
Methyltrioxorhenium (MTO) was described by Hermann et al more than 30 years ago as the first organometallic rhenium oxide [1,2,3]. From the point of view of previous studies [16,17] in the field of MTO utilization (metathesis and olefin epoxidation), we would like to focus on the immobilization of MTO on inorganic alumina, silica and aluminosilicate supports. In this paper we provide a deep insight into the immobilization of MTO on various inorganic supports, namely MCM-41, mesoporous aluminas and aluminosilicates (type Siral). All these materials exhibit a high surface area, well-defined regular architecture and narrow pore size distribution of mesopores and represent excellent supports for the active components. A comparison of their loading ability and broad characterization is given These catalysts have possible applications in olefin metathesis and in olefin epoxidation. MTO on various supports is demonstrated on the various metathesis reactions in the presented paper
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