摘要
Background: Transformation of CO2-derived CO into alkyl carbonates becomes a very attractive route for CO2 utilization. Heterogeneous catalysis of the oxidative carbonylation using a halide-free solid catalyst offers a greener process by preventing corrosion issues and separation difficulties. Method: Copper-activated carbon (Cu/AC) hybrid materials were developed by using a facile aerosol-assisted synthetic approach for the heterogeneous catalysis of liquid-phase oxidative carbonylation of methanol and CO into dimethyl carbonate (DMC), an appealing alternative route for CO2 utilization. Significant Findings: Without using additional additives, promotors or solvents, high space-time yield (STYDMC, 1110.8 mg gcat -1 h-1) and high selectivity (93.6 %) toward DMC production can be achieved, showing the high potential of sustainability in the green chemical process by using the developed Cu/AC solid hybrid catalysts. Various factors, including metal loading (0-20 wt %), spraying condition (two-fluid, 3-fluid, metal-organic framework-templated), and calcination temperature (350-450 degrees C) were investigated. Results revealed a direct correlation between STYDMC and active metal surface area of the Cu/AC catalysts. The study demonstrates a sustainable route for the effective CO2 conversion into valuable chemicals with a significant improvement of the yield and high selectivity.