不同方法制备的铈锰固溶体及其催化醇胺偶联反应
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O643.36

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国家自然科学基金项目(面上项目,重点项目,重大项目)


Preparation methods of cerium-manganese solid solutions for catalyzing N-alkylation of amines with alcohols
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The National Natural Science Foundation of China (General Program, Key Program, Major Research Plan)

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    摘要:

    为了研究不同制备方法对铈锰固溶体形貌、结构及其表面物种等的影响,阐明铈锰固溶体结构与其催化性能之间的关系,该文通过纳米铸型法、水热法、共沉淀法、热分解法制备出一系列理论掺锰量为15%的铈锰固溶体〔Ce0.85Mn0.15Ox,n(Ce)∶n(Mn)=0.85∶0.15〕。采用XRD、FESEM、TEM、N2-吸附脱附、ICP-OES、XPS等方法对催化剂进行物化性质表征,并以醇胺偶联反应为探针反应来评估其催化性能。结果表明,以纳米铸型法制备的铈锰固溶体催化剂具有最佳的催化活性,其苯胺转化率达到了67.9%,N-苄叉苯胺的选择性为99.4%,时空产率为0.56 mmol/(gcat·h)。与其他3种制备方法相比,纳米铸型法制备的铈锰固溶体具有较大的表面积、特定的介孔结构,催化剂表面拥有较高相对含量的Ce3+、Mn3+,有利于吸附和活化氧分子,这些因素均有利于催化醇胺偶联反应。

    Abstract:

    In order to explore the influence of different preparation methods on the morphologies, structures and surface species of cerium-manganese solid solutions, as well as clarify the relationship between the structures and their catalytic performances, four kinds of cerium-manganese solid solutions〔containing 15% manganese in theory, n(Ce)∶n(Mn)=0.85∶0.15〕were prepared by the nano-casting method, hydrothermal method, co-precipitation method and thermal decomposition method, respectively. The physical and chemical properties of the catalysts were characterized by XRD, FESEM, TEM, N2 adsorption-desorption, ICP-OES and XPS. The catalytic performances of catalysts were evaluated by the selective catalytic synthesis of N-benzylideneaniline from benzyl alcohol and aniline under air atmosphere. The results showed that the catalyst prepared by nano-casting method possessed the best catalytic activity with highest aniline conversion of 67.9%, N-benzylideneaniline selectivity of 99.4% and time space yield of 0.56 mmol/(gcat·h). Compared with the other three preparation methods, the best performance of cerium-manganese solid solution prepared by nano-casting method could be attributed to its larger surface area, specific mesoporous structure and richer content of surface Ce3+ and Mn3+.

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符淑钗,刘鹏,祝德兴,吴华杰,程高,余林.不同方法制备的铈锰固溶体及其催化醇胺偶联反应[J].精细化工,2020,37(6):

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  • 收稿日期:2019-12-29
  • 最后修改日期:2020-02-20
  • 录用日期:2020-02-26
  • 在线发布日期: 2020-04-13
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