Sarawalee Thanasilp, J. Schwank, V. Meeyoo, S. Pengpanich, M. Hunsom
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引用次数: 3
摘要
在间歇式反应器中,采用负载型硅钨酸(SiW)催化剂催化甘油液相氧化脱水制丙烯酸。考察了氧化剂浓度(H2O2)、反应温度(70℃和90℃)、载体类型(HZSM-5、SiO2和Al2O3)和SiW负载(根据载体不同,负载比例为20 ~ 60 wt.%)对转化率和产率的影响。H2O2和负载SiW催化剂的加入对甘油转化率和丙烯酸收率以及其他期望产物(乙醇酸、甲酸、乙酸、丙烯醛和丙烯酸)产生了显著的协同正效应。高的反应温度能够提高高的甘油转化率,使所有期望产物的产率相同。负载型SiW催化剂的BET表面积对甘油氧化脱水活性的影响比催化剂的酸度更显著。在负载SiW催化剂中,SiW/HZSM-5在负载SiW为30 wt.%时,甘油转化率最高(85.54%),在2.74 M H2O2条件下,在90°C条件下的丙烯酸收率为30.57%。研究了负载型SiW催化剂上甘油转化为所需产物的动力学。
Liquid Phase Oxydehydration of Glycerol to Acrylic Acid over Supported Silicotungstic Acid Catalyst: Influence of Reaction Parameters
The liquid phase catalytic oxydehydration of glycerol to acrylic acid over supported silicotungstic acid (SiW) catalysts was carried out in the batch reactor. The effect of oxidizing agent concentration (H2O2), reaction temperatures (70 and 90 °C), types of supports (HZSM-5, SiO2 and Al2O3) and SiW loading (20-60 wt.% based on support) on the conversion and product yield were investigated. The addition of H2O2 and supported SiW catalysts significantly conducted the synergetic positive effects on glycerol conversion and acrylic acid yields as well as other desired products including glycolic acid, formic acid, acetic acid, acrolein and acrylic acid. High reaction temperature was able to enhance high glycerol conversion as the same yield of all desired products. The BET surface area of supported SiW catalysts played much more important role in the activities of oxydehydration of glycerol that this oxydehydration was more remarkable than the acidity of catalysts. Among all supported SiW catalysts, the SiW/HZSM-5 with SiW loading of 30 wt.% exhibited the highest glycerol conversion (85.54%) with the production acrylic acid yield of 30.57 % over 2.74 M H2O2 at 90 °C. The kinetics of glycerol conversion to desired products over supported SiW catalyst was explored.