Jitjamnong Jakkrapong, Khongprom Parinya, Ratanawilai Thanate, Ratanawilai Sukritthira
Department of Chemical Engineering, Faculty of Engineering, Prince of Songkla University Hat Yai Songkhla 90110 Thailand
Air Pollution and Health Effect Research Center, Prince of Songkla University Songkhla 90110 Thailand.
RSC Adv. 2024 Feb 19;14(9):5941-5958. doi: 10.1039/d4ra00290c. eCollection 2024 Feb 14.
Waste crude glycerol was successfully enriched and utilized as an inexpensive source for producing value-added chemicals, such as glycerol carbonate (GC) - a valuable compound with extensive industrial applications. The Li/MCM-41 heterogeneous catalyst was synthesized and used for the transesterification of enriched glycerol and dimethyl carbonate (DMC) to produce GC. The catalyst's physicochemical properties were characterized using thermogravimetric, Hammett indicator, inductively coupled plasma-optical emission spectroscopy, nitrogen adsorption-desorption, X-ray diffractometry, scanning electron microscopy, and Fourier-transform infrared spectroscopy analyses. Reaction conditions were optimized using response surface methodology and analysis of variance, yielding an accurate quadratic model to predict the GC yield under different transesterification variables. The results revealed that 5%Li/MCM-41 served as the optimal catalyst, achieving the highest TOF of 4.72 h. The DMC: enriched glycerol molar ratio had the greatest impact on the GC yield, with an = 0.9743 and adjusted = 0.9502. The optimal GC yield (58.77%) with a final purity of 78% was attained at a 5.15 wt% catalyst loading relative to the initial amount of enriched glycerol, DMC: enriched glycerol molar ratio of 4.24 : 1, and a reaction temperature of 86 °C for 165 min. The 5%Li/MCM-41 heterogeneous catalyst could be reused for four cycles with a decreased GC yield from 58.77% to 45.72%. Thus, the Li/MCM-41 catalyst demonstrated a remarkable efficiency and potential as a heterogeneous catalyst for synthesizing GC. This method not only contributes to environmental sustainability by making use of a byproduct from biodiesel production but also aligns with the principles of a circular economy.
废弃粗甘油被成功富集并用作生产增值化学品的廉价原料,例如碳酸甘油酯(GC)——一种具有广泛工业应用价值的化合物。合成了Li/MCM-41非均相催化剂,并将其用于富集甘油与碳酸二甲酯(DMC)的酯交换反应以制备GC。通过热重分析、哈米特指示剂、电感耦合等离子体发射光谱、氮吸附-脱附、X射线衍射、扫描电子显微镜以及傅里叶变换红外光谱分析对催化剂的物理化学性质进行了表征。采用响应面法和方差分析对反应条件进行了优化,得到了一个准确的二次模型,用于预测不同酯交换变量下的GC产率。结果表明,5%Li/MCM-41为最佳催化剂,最高TOF为4.72 h。DMC与富集甘油的摩尔比对GC产率影响最大,相关系数R² = 0.9743,调整后的R² = 0.9502。相对于富集甘油的初始量,催化剂负载量为5.15 wt%、DMC与富集甘油的摩尔比为4.24 : 1、反应温度为86 °C并反应165 min时,可获得最佳GC产率(58.77%),最终纯度为78%。5%Li/MCM-41非均相催化剂可重复使用四个循环,GC产率从58.77%降至45.72%。因此,Li/MCM-41催化剂作为合成GC的非均相催化剂表现出显著的效率和潜力。该方法不仅通过利用生物柴油生产的副产物促进了环境可持续性,还符合循环经济的原则。