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Kinetic investigations of styrene carbonate synthesis from styrene oxide and CO2 using a continuous flow tube-in-tube gas-liquid reactor
Journal of CO2 Utilization ( IF 7.2 ) Pub Date : 2018-03-15 , DOI: 10.1016/j.jcou.2018.02.001
Abdul Rehman , Ana María López Fernández , M.F.M. Gunam Resul , Adam Harvey

A continuous method of styrene carbonate (SC) synthesis from styrene oxide (SO) and carbon dioxide (CO2) is reported, using a semipermeable Teflon® AF-2400-based tube-in-tube gas-liquid reactor. The reaction was performed in the presence of and tetrabutylammonium bromide (TBAB) and zinc bromide (ZnBr2), acting as a highly efficient and economical homogeneous binary catalyst system. The exceptionally high permeation of CO2 through the membrane, combined with the high surface area to volume ratio in such continuous flow reactors resulted in complete SO conversion (100%) in a significantly reduced reaction time (tR) of 45 min at 120 °C and 6 bar of CO2 pressure. The effect of various operating conditions such as reaction temperature, CO2 pressure, residence time and catalyst molar ratio (ZnBr2/TBAB) was determined. Moreover, a detailed kinetic study of SC synthesis was carried out to determine the corresponding kinetic values (k and Ea) and activation parameters (ΔH, ΔS and ΔG). Based on the experimental data, the reaction was found to be first-order in SO, TBAB and CO2 concentrations. The activation energy of SC synthesis in the presence of TBAB catalyst alone was calculated to be 55 kJ mol−1 over a temperature range of (90–120 °C), which was reduced to 32 kJ mol−1 as a result of using ZnBr2 as a co-catalyst.



中文翻译:

连续流管-管式气液反应器由环氧乙烷和CO 2合成碳酸苯乙烯的动力学研究

据报道,使用基于AF-2400的半渗透性的管中管式气液反应器,由氧化苯乙烯(SO)和二氧化碳(CO 2)合成碳酸苯乙烯(SC)的连续方法。该反应在四丁基溴化铵(TBAB)和溴化锌(ZnBr 2)的存在下进行,作为高效且经济的均相二元催化剂体系。在这种连续流反应器中,CO 2极高的透过膜渗透性,再加上高的表面积/体积比,导致120%的反应时间(t R)大大缩短了反应时间(t R),从而实现了完全的SO转化(100%)。C和6 bar的CO 2压力。确定了各种操作条件的影响,例如反应温度,CO 2压力,停留时间和催化剂摩尔比(ZnBr 2 / TBAB)。此外,对SC合成进行了详细的动力学研究,以确定相应的动力学值(k和E a)和活化参数(ΔH ,ΔS 和ΔG )。根据实验数据,发现该反应在SO,TBAB和CO 2浓度上是一级反应。在90-120°C的温度范围内,仅在TBAB催化剂存在下,SC合成的活化能经计算为55 kJ mol -1,降低到32 kJ mol使用ZnBr 2作为助催化剂的结果是-1

更新日期:2018-03-15
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