Abstract

Silica-zirconia mixed oxide (SiO 2-ZrO 2) was synthesized by sol-gel method; with SiO 2-ZrO 2 as the support, CuCl 2/SiO 2-ZrO 2 catalyst was then prepared by ion-exchange and used in the liquid oxidative carbonylation of methanol to dimethyl carbonate (DMC). The results showed that the introduction of zirconium species into the amorphous silica leads to the formation of Si-O-Zr bonds and Brønsted acid sites. When the CuCl 2/SiO 2-ZrO 2 catalyst is calcined at 300–550°C in an inert atmosphere, CuCl 2 is dispersed and bounded on the surface of SiO 2-ZrO 2 support; CuCl 2 can be auto-reduced to CuCl, which is then ion-exchanged with the surface Brönsted acid sites of the SiO 2-ZrO 2 support to form Cu + species. As a result, most of copper remains to be highly dispersed on the surface of SiO 2-ZrO 2 and only a small amount of chlorine is left over. The CuCl 2/SiO 2-ZrO 2 catalyst calcined at 450°C exhibits excellent activity in the oxidative carbonylation of methanol; under the conditions of 140°C, 2.4 MPa and a CO/O 2 ratio of 2, the conversion of methanol and the selectivity to DMC reach 10.0% and 79.4%, respectively.

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