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Synergistic Effects between Acid and Base Sites and Kinetic for Synthesis of Methylacrolein on the Cs-P/γ-Al2O3 Catalyst
Industrial & Engineering Chemistry Research ( IF 3.8 ) Pub Date : 2020-09-17 , DOI: 10.1021/acs.iecr.0c03337 Gang Wang 1 , Guangming Cai 1
Industrial & Engineering Chemistry Research ( IF 3.8 ) Pub Date : 2020-09-17 , DOI: 10.1021/acs.iecr.0c03337 Gang Wang 1 , Guangming Cai 1
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Methylacrolein (MAL) is traditionally synthesized from propanal and formaldehyde via the Mannich reaction instead of the aldol reaction in homogeneous catalytic systems due to the undesired self-condensation of propanal. Herein, the direct synthesis of MAL from propanal and trioxane via the aldol reaction was realized on an acid–base bifunctional Cs-P/γ-Al2O3 catalyst, which exhibited good catalytic stability and could be prepared in a large scale with 54.5% yield and 100% selectivity. The influence of P elements on the structure and acid–base properties of Cs-P/γ-Al2O3 and even on the selectivity of MAL, compared with Cs/γ-Al2O3, was elucidated through FT-IR, XRD, XPS, and CO2- and NH3-TPD characterizations in combination with catalytic activity evaluation. The synergistic effects between acid and base sites on MAL production were unveiled where the decomposition of trioxane into a formaldehyde unit followed by condensation between the formaldehyde monomer and propanal proceeded on the acid and base sites. Kinetics studies revealed that the trioxane decomposition into formaldehyde was zero-order-dependent on trioxane concentration and the condensation step conformed to the Langmuir–Hinshelwood mechanism, with activation barriers of 72 ± 0.2 and 65 ± 0.5 kJ/mol, respectively.
中文翻译：
酸碱站点和动力学为在CS-P /γ-Al系甲基丙烯醛的合成的协同作用2 ö 3催化剂
甲基丙烯醛（MAL）传统上是由丙醛和甲醛通过曼尼希反应而不是在均相催化体系中的醛醇缩合反应合成的，这是由于丙烯不希望的自缩合而产生的。这里，MAL的从丙醛和三恶烷的直接合成通过醛醇缩合反应是在酸-碱官能铯-P /γ-Al系实现2 ö 3催化剂，其表现出良好的催化稳定性，并可能在大规模与54.5来制备％产率和100％选择性。P个元素的上铯-P的结构和酸-碱特性/γ-Al系的影响2 ö 3，甚至在MAL的选择性，与CS /γ-Al系相比2 ö 3通过FT-IR，XRD，XPS和CO 2-和NH 3 -TPD表征与催化活性评估相结合进行了阐明。揭示了酸和碱位之间对MAL产生的协同作用，其中三恶烷分解成甲醛单元，然后甲醛单体和丙醛之间的缩合在酸和碱位上进行。动力学研究表明，三恶烷分解成甲醛是零级依赖于三恶烷浓度的，并且缩合步骤符合Langmuir-Hinshelwood机理，活化势垒分别为72±0.2和65±0.5 kJ / mol。
更新日期：2020-10-07
中文翻译：
酸碱站点和动力学为在CS-P /γ-Al系甲基丙烯醛的合成的协同作用2 ö 3催化剂
甲基丙烯醛（MAL）传统上是由丙醛和甲醛通过曼尼希反应而不是在均相催化体系中的醛醇缩合反应合成的，这是由于丙烯不希望的自缩合而产生的。这里，MAL的从丙醛和三恶烷的直接合成通过醛醇缩合反应是在酸-碱官能铯-P /γ-Al系实现2 ö 3催化剂，其表现出良好的催化稳定性，并可能在大规模与54.5来制备％产率和100％选择性。P个元素的上铯-P的结构和酸-碱特性/γ-Al系的影响2 ö 3，甚至在MAL的选择性，与CS /γ-Al系相比2 ö 3通过FT-IR，XRD，XPS和CO 2-和NH 3 -TPD表征与催化活性评估相结合进行了阐明。揭示了酸和碱位之间对MAL产生的协同作用，其中三恶烷分解成甲醛单元，然后甲醛单体和丙醛之间的缩合在酸和碱位上进行。动力学研究表明，三恶烷分解成甲醛是零级依赖于三恶烷浓度的，并且缩合步骤符合Langmuir-Hinshelwood机理，活化势垒分别为72±0.2和65±0.5 kJ / mol。
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