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A novel single-step hydrogenation of 2-imidazolecarboxaldehyde to 2-methylimidazole over Pd-impregnated Al–Ti mixed oxide and kinetics
Reaction Chemistry & Engineering ( IF 3.4 ) Pub Date : 2020-06-16 , DOI: 10.1039/d0re00154f Devendra S. Pisal 1, 2, 3, 4 , Ganapati D. Yadav 1, 2, 3, 4
Reaction Chemistry & Engineering ( IF 3.4 ) Pub Date : 2020-06-16 , DOI: 10.1039/d0re00154f Devendra S. Pisal 1, 2, 3, 4 , Ganapati D. Yadav 1, 2, 3, 4
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2-Methyl imidazole (2MIMZ) is a very essential chemical feedstock and intermediate used in the manufacturing of pharmaceutical drugs, metal organic frameworks (MOFs), agricultural chemicals, pigments and dyes, and coating additives. The currently used processes for the synthesis of 2MIMZ include dehalogenation and dehydrogenation routes, which use homogeneous catalysts and hazardous chemicals such as CH3CN and aryl-halides leading to wastes, and ultimately increase the cost of production. Therefore, a green route was developed in this work using Al–Ti mixed oxide (ATMO) based catalysts, which were developed by co-precipitation and hydrothermal methods. ATMO was further doped with various metals (M = Ni, Cu, Fe and Pd) to give respective M/ATMO catalysts. These prepared M/ATMO catalysts were screened for selective hydrogenation of 2-imidazolecarboxaldehyde (IMZC) to give 2-methyl imidazole (2MIMZ). The order of activity was 2% Pd/ATMOCP > 5% Ni/ATMOCP > 2% Pd/Al2O3 > 5% Cu/ATMOCP > 5% Fe/ATMOCP > 2% Pd/TiO2. At 140 °C and 10 atm H2 pressure, there was >99% conversion of IMZC and 95% selectivity to 2MIMZ in 2 h. It is a consecutive reaction with 1H-imidazole-2-methanol (IMZ2MOL) as an intermediate, which on further hydrogenation gave 2MIMZ. The catalysts were characterized by sophisticated techniques such as FESEM, EDS, XRD, NH3-TPD, FTIR, BET analysis, HRTEM, XPS, TPR, and TGA. The Langmuir–Hinshelwood–Hougen–Watson (LHHW) dual-site reaction mechanism was found to be consistent with the experimental findings. The activation energies for the hydrogenation steps were 11.4 and 13.6 kcal mol−1, respectively. The catalysts were found to be robust, active and selective. Here, we unveil for the very first time a new route for the selective single-step hydrogenation of IMZC to 2MIMZ.
中文翻译：
Pd浸渍Al-Ti复合氧化物上2-咪唑甲醛甲醛一步加氢制备2-甲基咪唑的新方法和动力学
2-甲基咪唑（2MIMZ）是非常重要的化学原料和中间体，用于制造药物，金属有机骨架（MOF），农药，颜料和染料以及涂料添加剂。当前用于合成2MIMZ的方法包括脱卤和脱氢路线，该路线使用均相催化剂和危险化学品（例如CH 3）CN和芳基卤化物会导致浪费，并最终增加生产成本。因此，这项工作开发了一条绿色路线，使用的是Al-Ti混合氧化物（ATMO）基催化剂，该催化剂是通过共沉淀和水热法开发的。将ATMO进一步掺杂各种金属（M = Ni，Cu，Fe和Pd）以得到各自的M / ATMO催化剂。筛选这些制备的M / ATMO催化剂，以对2-咪唑甲醛（IMZC）进行选择性加氢，得到2-甲基咪唑（2MIMZ）。活性顺序为2％Pd / ATMO CP＞ 5％Ni / ATMO CP＞ 2％Pd / Al 2 O 3＞ 5％Cu / ATMO CP＞ 5％Fe / ATMO CP＞ 2％Pd / TiO 2。在140°C和10 atm H 2下在2小时内，IMZC的转化率> 99％，对2MIMZ的选择性达到95％。它是与1 H-咪唑-2-甲醇（IMZ2MOL）作为中间体的连续反应，进一步氢化后得到2MIMZ。催化剂的特征在于复杂的技术，例如FESEM，EDS，XRD，NH 3 -TPD，FTIR，BET分析，HRTEM，XPS，TPR和TGA。Langmuir-Hinshelwood-Hougen-Watson（LHHW）双位反应机制被发现与实验结果一致。氢化步骤的活化能分别为11.4和13.6kcal mol -1。发现该催化剂是坚固的，活性的和选择性的。在这里，我们首次公开了将IMZC选择性单步氢化为2MIMZ的新路线。
更新日期：2020-07-28
中文翻译：
Pd浸渍Al-Ti复合氧化物上2-咪唑甲醛甲醛一步加氢制备2-甲基咪唑的新方法和动力学
2-甲基咪唑（2MIMZ）是非常重要的化学原料和中间体，用于制造药物，金属有机骨架（MOF），农药，颜料和染料以及涂料添加剂。当前用于合成2MIMZ的方法包括脱卤和脱氢路线，该路线使用均相催化剂和危险化学品（例如CH 3）CN和芳基卤化物会导致浪费，并最终增加生产成本。因此，这项工作开发了一条绿色路线，使用的是Al-Ti混合氧化物（ATMO）基催化剂，该催化剂是通过共沉淀和水热法开发的。将ATMO进一步掺杂各种金属（M = Ni，Cu，Fe和Pd）以得到各自的M / ATMO催化剂。筛选这些制备的M / ATMO催化剂，以对2-咪唑甲醛（IMZC）进行选择性加氢，得到2-甲基咪唑（2MIMZ）。活性顺序为2％Pd / ATMO CP＞ 5％Ni / ATMO CP＞ 2％Pd / Al 2 O 3＞ 5％Cu / ATMO CP＞ 5％Fe / ATMO CP＞ 2％Pd / TiO 2。在140°C和10 atm H 2下在2小时内，IMZC的转化率> 99％，对2MIMZ的选择性达到95％。它是与1 H-咪唑-2-甲醇（IMZ2MOL）作为中间体的连续反应，进一步氢化后得到2MIMZ。催化剂的特征在于复杂的技术，例如FESEM，EDS，XRD，NH 3 -TPD，FTIR，BET分析，HRTEM，XPS，TPR和TGA。Langmuir-Hinshelwood-Hougen-Watson（LHHW）双位反应机制被发现与实验结果一致。氢化步骤的活化能分别为11.4和13.6kcal mol -1。发现该催化剂是坚固的，活性的和选择性的。在这里，我们首次公开了将IMZC选择性单步氢化为2MIMZ的新路线。
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