Product Yield Increasing More Than 20 Times Achieved by Reducing Water Poisoning for Direct Diethyl Carbonate Synthesis.

Abstract

Diethyl carbonate (DEC) synthesis from CO2 and ethanol is a typical green chemical route for sustainable development and cleaner production. However, the bottleneck problem of a low DEC yield is still not solved at present. The DEC yield still maintains 0.5-5.0% unless expensive third additives are added. Compared to the cheap price of DEC, the third additives are generally more expensive. It is not advisible to use expensive chemicals to prepare cheap chemicals. In this work, the (ZrO2)1.0/(Fe2O3)1.0 catalyst was prepared by a novel template-precipitation method and the DEC yield of the DEC direct synthetic reaction only from CO2 and ethanol without third additives obtained 1.95%. After a series of supported catalysts were prepared, the DEC yield reached up to 46.1% for the (ZrO2)1.0/(Fe2O3)1.0@3A-CaO-CaC2 catalyst. This carrier can also be applied to other catalyst systems. CO2-TPD, NH3-TPD, and XRD were measured to analyze the microstructure and catalytic mechanism. Active center site theory was proposed to explain the intrinsic mechanism of catalyst activity. This new discovery of the mechanism and the DEC yield removed obstacles for the application of this reaction.