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One-step synthesis of glycidol from glycerol in a gas-phase packed-bed continuous flow reactor over HZSM-5 zeolite catalysts modified by CsNO3
Chemical Engineering Journal ( IF 15.1 ) Pub Date : 2020-04-06 , DOI: 10.1016/j.cej.2020.124945
Andrii Kostyniuk , David Bajec , Petar Djinović , Blaž Likozar

In this work we report the pioneering gas-phase conversion of glycerol into glycidol in one-step over Cs–ZSM-5 zeolite catalyst with SiO2/Al2O3 = 1500. The structure and catalytic performance of catalysts synthesized by wet impregnation method with different Cs loadings were studied. The catalysts were characterized by ICP–MS, XRD, N2 physisorption, STEM–EDX, SEM, pyridine-DRIFT, CO2–TPD, NH3–TPD, and TGA techniques. The reaction was carried out in a packed-bed continuous flow reactor under atmospheric pressure. The highest achieved glycidol yield was 40.4 mol% over 20wt% Cs–ZSM-5(1500) catalyst with 10 wt% glycerol in the feed at 350 °C reaction temperature and GHSVtotal = 1250 h-1. The glycidol selectivity was increasing steadily from 41.4 to 64.3 mol% during 27 h time-on-stream. This catalyst showed relatively high stability and selectivity, which was attributed to the presence of a suitable amount of basic sites and the strong CsNO3/HZSM-5 support synergetic interaction. Based on the identified reaction products, we propose the reaction mechanism of the catalytic glycerol conversion to glycidol over the tested catalysts.



中文翻译:

在CsNO 3改性的HZSM-5沸石催化剂上,在气相填充床连续流反应器中由甘油一步合成缩水甘油

在这项工作中,我们报告了在SiO 2 / Al 2 O 3 = 1500的Cs–ZSM-5沸石催化剂上一步一步将甘油气相转化为缩水甘油的过程。湿浸渍法合成的催化剂的结构和催化性能研究了具有不同Cs负载的情况。通过ICP-MS,XRD,N 2物理吸附,STEM-EDX,SEM,吡啶-DRIFT,CO 2 -TPD,NH 3 -TPD和TGA技术对催化剂进行了表征。该反应在填充床连续流反应器中在大气压下进行。在350°C反应温度和GHSV下,进料中20wt%Cs–ZSM-5(1500)催化剂中甘油含量为10 wt%时,最高缩水甘油产率为40.4 mol%总计= 1250h -1。在运行27小时后,缩水甘油的选择性从41.4 mol%稳定增加。该催化剂表现出相对较高的稳定性和选择性,这归因于存在适量的碱性位点和强的CsNO 3 / HZSM-5支持协同作用。基于确定的反应产物,我们提出了在测试的催化剂上催化甘油转化为缩水甘油的反应机理。

更新日期:2020-04-06
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