Influence of crystalline phase of Li-Al-O oxides on the activity of Wacker-type catalysts in dimethyl carbonate synthesis

Abstract

The catalysts supported on LiAl₅O₈ (spinel) for vapor phase synthesis of dimethyl carbonate (DMC) from methyl nitrite (MN) have been studied. Their catalytic activities on supports prepared by different methods were evaluated in a continuous reactor. The samples were characterized by powder X-ray diffraction, N₂ adsorption-desorption isotherms, fourier transform infrared spectroscopy and temperature-programmed reduction of H₂. Li/Al molar ratio and calcination temperature greatly influence the structure of crystalline phase of Li-Al-O oxides. Desirable LiAl₅O₈ (spinel) was formed at 800°C, while LiAl₅O₈ (primitive cube) formed at 900°C is undesirable for the reaction. A high Li/Al molar ratio, which was related with LiAlO₂, also slowed the reaction rate. The electron transfer ability and the interaction with active component are the important properties of the spinel-based supports. The CuCl₂-PdCl₂/LiAl₅O₈ (spinel) with better electron transfer ability and low Pd²⁺ reduction temperature exhibited a better catalytic ability.

Keywords

Wacker-type catalyst / dimethyl carbonate / methyl nitrite / spinel

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