Yanan Liu, Chengxiang Shi*, Zhensheng Shen, Lun Pan, Li Wang, Xiangwen Zhang and Ji-Jun Zou*,
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And then, we explored the effect of the integration manner of metal–acid catalysts on performance. A series of catalysts composed of Pd and HUSY with different proximities initially exhibited similar carbon yields of target products (bi- and tricyclic compounds generated via C–C coupling reactions), reaching 91.37% for 0.2Pd/Y (Pd supported on HUSY), 91.17% for 0.2Pd/Al|Y (grinding and granulation of Pd/Al<sub>2</sub>O<sub>3</sub> with the HUSY powder), and 88.53% for 0.2Pd/Al–Y (physical mixture of Pd/Al<sub>2</sub>O<sub>3</sub> granules with HUSY granules). However, their deactivation rates varied over time on stream. Among them, Pd/Al|Y exhibited the best stability. Furthermore, the influences of the metal-to-acid ratio and reaction conditions on catalytic performance were also investigated. In addition, the substrates were expanded from phenol to guaiacol, 2,6-dimethoxyphenol, eugenol, and two mimics of real lignin oil. 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引用次数: 0
摘要
从可再生木质素油中生产喷气燃料范围的环烷烃是替代石油基喷气燃料和减少温室气体排放的一种有前途的方法。最近的研究主要集中在使用金属-酸双功能催化剂将木质素衍生的酚类转化为循环喷气燃料,主要是在间歇反应器中。本文报道了在固定床反应器中,以木质素衍生的酚类化合物和环己酮为原料,以Pd和HUSY组成的金属-酸双功能催化剂为催化剂,在H2条件下连续合成双环和三环喷气燃料前驱体。首先,研究了苯酚-环己酮体系中酸催化C-C偶联反应的反应网络。在此基础上,探讨了金属-酸催化剂的整合方式对催化剂性能的影响。由不同邻域Pd和HUSY组成的一系列催化剂最初表现出相似的目标产物(通过C-C偶联反应生成的双环和三环化合物)的碳收率,0.2Pd/Y (HUSY负载Pd)达到91.37%,0.2Pd/Al|Y(用HUSY粉末研磨和制粒Pd/Al2O3)达到91.17%,0.2Pd/Al - Y (Pd /Al2O3颗粒与HUSY颗粒的物理混合物)达到88.53%。然而,它们的失活率随着时间的推移而变化。其中,Pd/Al|Y的稳定性最好。此外,还考察了金属酸比和反应条件对催化性能的影响。此外,底物从苯酚扩展到愈创木酚、2,6-二甲氧基酚、丁香酚和两种木质素油的模拟物。总之,本研究为木质素衍生的酚类化合物和环己酮高效合成多环喷气燃料提供了一种可行的方法。
Continuous Synthesis of Cyclic Jet Fuel Precursors from Phenolics and Cyclohexanone
Producing jet fuel-range cycloalkanes from renewable lignin oil is a promising way to replace petroleum-based jet fuels and reduce greenhouse gas emissions. Recent studies have focused on converting lignin-derived phenolics into cyclic jet fuels using metal–acid bifunctional catalysts, primarily in batch reactors. Here, we report the continuous synthesis of bi- and tricyclic jet fuel precursors using lignin-derived phenolics and cyclohexanone, catalyzed by metal–acid bifunctional catalysts composed of Pd and HUSY under H2 in a fixed-bed reactor. First, we investigated the reaction network of acid-catalyzed C–C coupling reactions in the system of phenol and cyclohexanone. And then, we explored the effect of the integration manner of metal–acid catalysts on performance. A series of catalysts composed of Pd and HUSY with different proximities initially exhibited similar carbon yields of target products (bi- and tricyclic compounds generated via C–C coupling reactions), reaching 91.37% for 0.2Pd/Y (Pd supported on HUSY), 91.17% for 0.2Pd/Al|Y (grinding and granulation of Pd/Al2O3 with the HUSY powder), and 88.53% for 0.2Pd/Al–Y (physical mixture of Pd/Al2O3 granules with HUSY granules). However, their deactivation rates varied over time on stream. Among them, Pd/Al|Y exhibited the best stability. Furthermore, the influences of the metal-to-acid ratio and reaction conditions on catalytic performance were also investigated. In addition, the substrates were expanded from phenol to guaiacol, 2,6-dimethoxyphenol, eugenol, and two mimics of real lignin oil. Overall, this study presents a viable method for the efficient synthesis of polycyclic jet fuels from lignin-derived phenolics and cyclohexanone.
期刊介绍:
ndustrial & Engineering Chemistry, with variations in title and format, has been published since 1909 by the American Chemical Society. Industrial & Engineering Chemistry Research is a weekly publication that reports industrial and academic research in the broad fields of applied chemistry and chemical engineering with special focus on fundamentals, processes, and products.