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Reaction kinetics and pathways of crotonic acid conversion in sub- and supercritical water for renewable fuel production
Reaction Chemistry & Engineering ( IF 3.9 ) Pub Date : 2021-11-15 , DOI: 10.1039/d1re00435b
Diane Valenzuela Gubatanga 1 , Osamu Sawai 1, 2 , Teppei Nunoura 1, 2, 3
Affiliation  

Conversion of waste lipid biomass into renewable fuels using sub- and supercritical water provides an alternative green approach in contrast with the current treatment methods. However, the reaction network of unsaturated lipids in sub- and supercritical water has not been clarified. Unsaturated lipids are found abundantly in waste lipid biomass, making the establishment of their reaction network essential. In this study, the reaction of crotonic acid (CA) as a model unsaturated lipid in sub- and supercritical water was clarified through an in-depth study of its reaction pathways and kinetics. The experiments were conducted at temperatures from 300 to 415 °C, a pressure of 25 MPa, and residence times from 30 to 150 s in a continuous flow process. The main products in the initial stage of the reaction were butyric acid (BA) and propene. Based on the temperature dependence experiments, the CA conversion increased along with temperature and residence time. Based on the product distribution, two main decomposition pathways were identified in the initial stage of the CA reaction. The first is CA direct decarboxylation and the second is CA hydrogenation followed by BA decarbonylation. Examination of the kinetic rates revealed that the reaction mainly proceeds via CA direct decarboxylation, contrary to the results reported in previous studies. The findings demonstrated that the role of water can change according to the conditions and reactions employed. This was proven by the evident variation of kinetic rate constants under sub- and supercritical conditions and is reflected in the Arrhenius plot.

中文翻译:

用于可再生燃料生产的亚临界和超临界水中巴豆酸转化的反应动力学和途径

与当前的处理方法相比,使用亚临界和超临界水将废弃的脂质生物质转化为可再生燃料提供了一种替代的绿色方法。然而,不饱和脂质在亚临界和超临界水中的反应网络尚未阐明。在废弃的脂质生物质中大量发现不饱和脂质,因此建立它们的反应网络至关重要。本研究通过对其反应途径和动力学的深入研究,阐明了巴豆酸 (CA) 作为模型不饱和脂质在亚临界和超临界水中的反应。实验在 300 至 415 °C 的温度、25 MPa 的压力和 30 至 150 s 的连续流动过程中的停留时间下进行。反应初期的主要产物为丁酸(BA)和丙烯。基于温度依赖性实验,CA 转化率随着温度和停留时间的增加而增加。根据产物分布,在 CA 反应的初始阶段确定了两种主要的分解途径。第一个是 CA 直接脱羧,第二个是 CA 加氢,然后是 BA 脱羰。动力学速率的检查表明反应主要进行通过CA 直接脱羧,与先前研究报告的结果相反。研究结果表明,水的作用可以根据所采用的条件和反应而改变。亚临界和超临界条件下动力学速率常数的明显变化证明了这一点,并反映在阿伦尼乌斯图中。
更新日期:2021-12-01
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