催化剂酸碱性与催化酯醛缩合性能的关系
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1.北京石油化工学院 新材料与化工学院,北京 大兴 102617;2.恩泽生物质精细化工北京市重点实验室,北京 大兴 102617;3.中海油化工与新材料科学研究院北京有限公司

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TQ

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The effect of acid-base property of catalyst on condensation performance for ester aldehydes
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1.College of New Materials and Chemical Engineering, Beijing Institute of Petrochemical Technology, Daxing 102617, Beijing, China;2. Beijing Key Laboratory of Enze Biomass Fine Chemical, Daxing 102617, Beijing, China;3.CNOOC Research Institute of Chemical Engineering and New Materials Science (Beijing) Compony Limited, Changping 102209, Beijing, China

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    摘要:

    以γ-Al2O3和SiO2为载体,采用浸渍法引入不同含量Na、K和Cs碱金属制备了一系列酯醛气相缩合催化剂。利用XRD、BET、NH3-TPD和CO2-TPD等手段对催化剂结构和表面酸、碱性进行了表征,并以丙酸甲酯与甲醛为原料,考察了其催化酯醛气相缩合反应性能。结果表明,在0.2 MPa、370 ℃和质量空速为1.2 h-1的条件下,催化剂10% Cs/SiO2对丙酸甲酯转化率最高(41.03%),甲基丙烯酸甲酯选择性为99.20%。在有丰富碱活性中心的前提下,催化剂表面弱碱性位点比例与其催化酯醛气相缩合反应性能呈正相关关系,催化剂表面酸性位点和中强碱性位点的存在会导致催化剂催化活性和选择性的降低。

    Abstract:

    A series of catalysts with different contents of K, Na and Cs for vapor phase condensation of ester aldehydes were prepared by impregnation method using γ-Al2O3 and SiO2 as carriers. The structure, acid and basic sites of the catalysts were characterized by XRD, BET, NH3-TPD and CO2-TPD. The condensation performance of catalysts for methyl propionate and formaldehyde in vapor phase was investigated. The results showed that the activity of 10% Cs/SiO2 catalyst was better under the same reaction conditions (pressure 0.2 MPa, temperature 370 ℃, weight hourly space velocity 1.2 h-1), the conversion of methyl propionate was the highest (41.03%) and the selectivity was 99.20%. Under the premise of abundant alkali center, there was a positive correlation between the proportion of weakly basic sites on the surface of the catalyst and its catalytic performance for condensation of ester aldehydes in vapor phase. The presence of acidic and moderately strong alkaline sites of the catalyst could lead to a decrease in activity and selectivity of the catalyst.

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张伟,贾鑫,王兴永,孙培永,傅送保,姚志龙,张胜红,陈和,杜海岗.催化剂酸碱性与催化酯醛缩合性能的关系[J].精细化工,2024,41(3):

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  • 收稿日期:2023-04-04
  • 最后修改日期:2023-06-09
  • 录用日期:2023-06-28
  • 在线发布日期: 2024-03-07
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