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Cu/CuMgAlOx-Catalyzed Guaiacol Hydrodeoxygenation in Supercritical Methanol: A Modeling Mechanistic Insight for Lignin-Derivatives Upgrading
Energy & Fuels ( IF 5.2 ) Pub Date : 2020-12-30 , DOI: 10.1021/acs.energyfuels.0c03732 Xiangchen Kong 1 , Chao Liu 1 , Yue Han 1 , Ming Lei 1 , Yuyang Fan 1 , Ming Li 1 , Rui Xiao 1
Energy & Fuels ( IF 5.2 ) Pub Date : 2020-12-30 , DOI: 10.1021/acs.energyfuels.0c03732 Xiangchen Kong 1 , Chao Liu 1 , Yue Han 1 , Ming Lei 1 , Yuyang Fan 1 , Ming Li 1 , Rui Xiao 1
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The development of an economic and sustainable catalytic system was crucial for lignin-based biorefinery. Herein, we reported a low-cost Cu/CuMgAlOx catalyst with promising activity toward lignin hydrodeoxygenation (HDO) through a H2-free method. Supercritical methanol was used as the hydrogen donor, solvent, and reactant simultaneously. Guaiacol was employed as a representative lignin model compound to reveal the HDO mechanism of lignin derivatives. HDOs of guaiacol performed at 250, 275, 300, and 350 °C with durations ranging from 15 to 120 min indicated a high HDO efficiency of the catalytic system. The obtained liquid products were categorized to oxygen-containing unsaturated products (OUPs), oxygen-containing saturated products (OSPs), and cycloalkanes. A kinetic model based on a simplified reaction process containing the three following conversion steps was established: guaiacol transformed to OUPs through the initial HDO, then hydrogenated to OSPs (medium HDO), and eventually turned to cycloalkanes by the deep HDO. The deep HDO was the rate-determining step, and the apparent activation energies of the three steps were all lower than those in the literature. Phenol, 1,2-cyclohexanediol, anisole, and veratrole were the major intermediates, the HDOs of which were programed for pathway verification. Remarkably, catechol (the culprit of condensation) was not produced in this system. Overall, a detailed reaction network of guaiacol HDO was established, and the veil of Cu/CuMgAlOx-catalyzed lignin-derivatives HDO in supercritical methanol was revealed. This work paved the way for the application of Cu/CuMgAlOx catalyst in lignin-derivatives upgrading.
中文翻译：
Cu / CuMgAlO x催化的超临界甲醇中的愈创木酚加氢脱氧：木质素衍生物升级的建模机理研究。
经济和可持续的催化系统的发展对于木质素生物精炼厂至关重要。在本文中，我们报道了一种低成本的Cu / CuMgAlO X催化剂通过一个有前途的ħ朝向木质素加氢脱氧（HDO）活性2-free方法。超临界甲醇同时用作氢供体，溶剂和反应物。愈创木酚被用作代表性的木质素模型化合物，以揭示木质素衍生物的HDO机制。愈创木酚的HDO在250、275、300和350°C下进行，持续时间为15至120分钟，表明催化体系的HDO效率很高。将获得的液体产物分类为含氧不饱和产物（OUPs），含氧饱和产物（OSPs）和环烷烃。建立了基于简化反应过程的动力学模型，该过程包含以下三个转化步骤：愈创木酚通过初始HDO转化为OUP，然后氢化为OSP（中等HDO），并最终通过深HDO转化为环烷烃。深入的HDO是决定速率的步骤，并且这三个步骤的表观活化能均低于文献中的值。苯酚，1,2-环己二醇，苯甲醚和藜芦醇是主要中间体，其HDO被编程用于途径验证。值得注意的是，该系统中未产生邻苯二酚（冷凝的元凶）。总的来说，建立了愈创木酚HDO的详细反应网络，以及Cu / CuMgAlO的面纱揭示了在超临界甲醇中x催化的木质素衍生物HDO。这项工作为将Cu / CuMgAlO x催化剂应用于木质素衍生物的升级铺平了道路。
更新日期：2021-01-21
中文翻译：
Cu / CuMgAlO x催化的超临界甲醇中的愈创木酚加氢脱氧：木质素衍生物升级的建模机理研究。
经济和可持续的催化系统的发展对于木质素生物精炼厂至关重要。在本文中，我们报道了一种低成本的Cu / CuMgAlO X催化剂通过一个有前途的ħ朝向木质素加氢脱氧（HDO）活性2-free方法。超临界甲醇同时用作氢供体，溶剂和反应物。愈创木酚被用作代表性的木质素模型化合物，以揭示木质素衍生物的HDO机制。愈创木酚的HDO在250、275、300和350°C下进行，持续时间为15至120分钟，表明催化体系的HDO效率很高。将获得的液体产物分类为含氧不饱和产物（OUPs），含氧饱和产物（OSPs）和环烷烃。建立了基于简化反应过程的动力学模型，该过程包含以下三个转化步骤：愈创木酚通过初始HDO转化为OUP，然后氢化为OSP（中等HDO），并最终通过深HDO转化为环烷烃。深入的HDO是决定速率的步骤，并且这三个步骤的表观活化能均低于文献中的值。苯酚，1,2-环己二醇，苯甲醚和藜芦醇是主要中间体，其HDO被编程用于途径验证。值得注意的是，该系统中未产生邻苯二酚（冷凝的元凶）。总的来说，建立了愈创木酚HDO的详细反应网络，以及Cu / CuMgAlO的面纱揭示了在超临界甲醇中x催化的木质素衍生物HDO。这项工作为将Cu / CuMgAlO x催化剂应用于木质素衍生物的升级铺平了道路。
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