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One-pot synthesis of glycerol carbonate from glycerol using three-dimensional mesoporous silicates of K/TUD-1 under environmentally benign conditions
Molecular Catalysis ( IF 4.6 ) Pub Date : 2020-09-10 , DOI: 10.1016/j.mcat.2020.111188
Shivali Arora , Vijayalakshmi Gosu , Verraboina Subbaramaiah

In the present study, a series of potassium (K) incorporated three-dimensional mesoporous silica material (K/TUD-1) has been synthesized for the one-pot synthesis of glycerol carbonate through transesterification of glycerol with dimethyl carbonate (DMC). The synthesized catalyst (K/TUD-1) has been characterized to confirm porosity by nitrogen adsorption-desorption isotherm, X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and transmission electron microscopy (TEM). Small-angle XRD revealed that TUD-1 is mesostructure in nature. Morphology study revealed that TUD-1 exhibited a 3D structure without any agglomeration. The surface area of bare TUD-1 significantly declined with the incorporation of active metal from 632 m2/g to 430 m2/g. However, the basicity of K/TUD-1 improved, which is a highly desired property for the transesterification reaction. Batch experimental results have been concluded that 7% K/TUD-1 has better catalytic activity for the conversion of glycerol to glycerol carbonate. Further investigation has been conducted on the influence of reaction parameters such as reaction temperature, reaction time, catalyst dosage, and DMC/glycerol molar ratio. Under optimized conditions the maximum glycerol carbonate yield (∼91.50 %) was observed with catalyst dose of 6 wt.% (of glycerol mass), DMC/glycerol molar ratio of 5, reaction temperature of 90 °C in 2.5 h. Further, catalyst feasibility was also conducted at optimized conditions, and it sustains activity up to 4 cycles. The kinetics of the reaction was studied using the ODE 15 s solver in MATLAB.



中文翻译:

在环境良好的条件下,使用K / TUD-1的三维介孔硅酸盐从甘油一锅法合成甘油碳酸酯

在本研究中,已经合成了一系列掺入钾(K)的三维介孔二氧化硅材料(K / TUD-1),用于通过甘油与碳酸二甲酯(DMC)的酯交换反应一锅法合成碳酸甘油酯。合成的催化剂(K / TUD-1)已通过氮气吸附-解吸等温线,X射线衍射(XRD),X射线光电子能谱(XPS)和透射电子显微镜(TEM)确认孔隙率。小角X射线衍射表明TUD-1本质上是介观结构。形态学研究表明,TUD-1呈现3D结构,没有任何团聚。随着活性金属的掺入,裸TUD-1的表面积从632 m 2 / g显着下降至430 m 2/G。但是,提高了K / TUD-1的碱度,这是酯交换反应的高度期望的性质。批处理实验结果表明,7%K / TUD-1具有更好的催化活性,可将甘油转化为碳酸甘油酯。已经对反应参数如反应温度,反应时间,催化剂用量和DMC /甘油摩尔比的影响进行了进一步研究。在最佳条件下,催化剂用量为甘油重量的6 wt。%,DMC /甘油摩尔比为5,反应温度为90℃,在2.5小时内,观察到最大碳酸甘油酯收率(约91.50%)。此外,催化剂的可行性也在最优化的条件下进行,并且可以维持多达4个循环的活性。使用MATLAB中的ODE 15 s求解器研究了反应动力学。

更新日期:2020-09-11
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