Selective hydrogenation of methyl 3-hydroxypropionate over zirconium-modified Cu/SiO2 catalysts
A series of the zirconium(Zr)-modified Cu/SiO2 catalysts were synthesized by ammonia-evaporation method and applied in the gas-phase hydrogenation of methyl 3-hydroxypropionate(3-HMP)to 1,3-propanediol(1,3-PDO).N2 adsorption-desorption,XRD,ICP-OES,H2-TPR,NH3-TPD,CO2-TPD,FTIR,TG-DTG,HRTEM,XPS and AES techniques were used for detailed characterizations.Introduction of the Zr species results in a strong interactions between the Cu and Zr species,leading to the generation of more copper phyllosilicate,and thus increasing the specific surface area of the catalyst as well as reducing the particle sizes of the copper species.The addition of Zr also made the copper species better be dispersed over the SiO2 support,increased the Cu+ content and enhanced the electronic absorption of the substrate 3-HMP by the acyl and methoxide groups.Compared with the unmodified Cu/SiO2 catalyst,the Zr-added(0.5%)Cu/SiO2 catalyst showed better catalytic performance.The conversion of 3-HMP as 96.0%was achieved along with the 1,3-PDO selectivity of 84.3%,Resulting in a total yield of 80.9%for 1,3-PDO.These were the best results obtained currently at a high liquid hourly space velocity(LHSV)of 0.10h-1.
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