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Study on condensation performance between methyl propionate and formaldehyde catalyzed by Cs/SiO2-ZrO2
Received date: 2024-03-01
Online published: 2024-11-27
The preparation of Methyl Methacrylate（MMA） by condensation of methyl propionate with formaldehyde hydroxyl aldehyde is currently the cleanest process route，and the key lies in the development of high-performance catalysts.A series of SiO2-ZrO2 composite oxides were prepared by coprecipitation and employed as carrier to load Cs2CO3 with an incipient wetness impregnation method.The physiochemical properties of the obtained SiO2-ZrO2 composite oxides and Cs/SiO2-ZrO2 catalysts were characterized by multiple techniques including XRD，Raman，ICP-OES，BET，NH3-TPD and CO2-TPD，and correlated to their performances in the condensation reaction of methyl propionate with formaldehyde.Special attention had been paid to the influence of carrier surface acidity and alkalinity on the activity of Cs/SiO2-ZrO2 catalysts towards the condensation reaction.The results indicated a transformation of zirconia from m-ZrO2 to t-ZrO2 with increasing the SiO2 content，suggesting t-ZrO2 was more stable in the SiO2-ZrO2 composites with higher SiO2 contents.Introduction of Cs2CO3 onto SiO2-ZrO2 composites changed greatly the distribution of surface acid-base sites，as well as the catalyst structure.The weakly basic sites on the catalyst surface were suitable active centers，and there existed an optimal interval between the number of weakly basic and total basic sites on the surface of catalysts with high catalytic activity，in which the reduction of medium-strongly basic sites and the elimination of acidic sites were favourable to the increase of catalytic activity.The 10Cs/60SiO2-40ZrO2 catalyst with 60% SiO2 and 10% Cs2CO3 exhibited the best catalytic performances，yielding the conversion of methyl propionate and the selectivity of methyl methacrylate（MMA） up to 30.77% and 97.89%，respectively，under the optimal reaction conditions of 370 ℃，0.2 MPa，and a space velocity of 1.0 h-1.
DU Haigang , WANG Xingyong , SUN Peiyong , CHEN He , FU Songbao , YAO Zhilong . Study on condensation performance between methyl propionate and formaldehyde catalyzed by Cs/SiO2-ZrO2[J]. Inorganic Chemicals Industry, 2024 , 56(11) : 165 -174 . DOI: 10.19964/j.issn.1006-4990.2024-0114
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