Reaction mechanism and kinetic modeling for the hydrodeoxygenation of triglycerides over alumina supported nickel catalyst

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• 作者：Sudhakara Reddy Yenumala ; Sunil K. Maity…
• 关键词：Triglyceride ; Hydrodeoxygenation ; Reaction mechanism ; Kinetics ; Nickel ; alumina
• 刊名：Reaction Kinetics, Mechanisms and Catalysis
• 出版年：2017
• 出版时间：February 2017
• 年：2017
• 卷：120
• 期：1
• 页码：109-128
• 全文大小：
• 刊物类别：Chemistry and Materials Science
• 刊物主题：Catalysis; Physical Chemistry; Industrial Chemistry/Chemical Engineering;
• 出版者：Springer Netherlands
• ISSN：1878-5204
• 卷排序：120

文摘

The present work provides a systematic study to delineate the reaction mechanism and develop a mechanistic kinetic model for the hydrodeoxygenation (HDO) of triglycerides (TG) over alumina supported nickel catalyst. The HDO of 1:2 molar mixtures of tripalmitin and tristearin was studied in a batch reactor over a wide range of process conditions. The results showed that TG instantaneously converted to respective fatty acids. The fatty acids further converted to the fatty aldehydes. The fatty aldehydes, then, rapidly converted to alkanes by two parallel reaction pathways. The decarbonylation of fatty aldehyde (RP-I) was the dominating route compared to the reduction of the fatty aldehyde to fatty alcohol followed by its dehydration and hydrogenation (RP-II). A mechanistic kinetic model was developed based on the observed reaction pathway to correlate the experimental results. The rate constants for the conversion of palmitic acid and stearic acid to alkanes were matched closely with each other thereby demonstrating that HDO is independent of fatty acid chain length. The developed kinetic model was further validated using experimental data at various hydrogen-to-nitrogen mole ratios in the gas phase. Furthermore, the rate constants obtained for various catalyst loadings were correlated by a linear equation with zero intercept.