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酸碱处理对ZSM-5分子筛物化性质和反应性能的影响

吕江江 黄星亮 赵蕾蕾 孙仁山 胡龙旺 龚艳

吕江江, 黄星亮, 赵蕾蕾, 孙仁山, 胡龙旺, 龚艳. 酸碱处理对ZSM-5分子筛物化性质和反应性能的影响[J]. 燃料化学学报, 2016, 44(6): 732-737.
引用本文: 吕江江, 黄星亮, 赵蕾蕾, 孙仁山, 胡龙旺, 龚艳. 酸碱处理对ZSM-5分子筛物化性质和反应性能的影响[J]. 燃料化学学报, 2016, 44(6): 732-737.
LV Jiang-jiang, HUANG Xing-liang, ZHAO Lei-lei, SUN Ren-shan, HU Long-wang, GONG Yan. Effects of acid-alkali treatment on properties and reactivity of ZSM-5 catalyst[J]. Journal of Fuel Chemistry and Technology, 2016, 44(6): 732-737.
Citation: LV Jiang-jiang, HUANG Xing-liang, ZHAO Lei-lei, SUN Ren-shan, HU Long-wang, GONG Yan. Effects of acid-alkali treatment on properties and reactivity of ZSM-5 catalyst[J]. Journal of Fuel Chemistry and Technology, 2016, 44(6): 732-737.

酸碱处理对ZSM-5分子筛物化性质和反应性能的影响

基金项目: 

国家自然科学基金 51261012

和昆明理工大学分析测试基金 20140292

详细信息
  • 中图分类号: TE624.9

Effects of acid-alkali treatment on properties and reactivity of ZSM-5 catalyst

More Information
  • 摘要: 考察了碱处理、先碱后两步酸处理对HZSM-5分子筛物化性质以及苯与甲醇烷基化反应性能的影响。结果表明, 碱处理在脱除分子筛中非骨架硅的同时, 提高了晶孔的利用率, 也中和了分子筛的强酸中心, 使催化剂活化甲醇的能力减弱, 苯与甲醇反应活性降低; 先碱后两步酸处理既脱除了分子筛中的非骨架铝, 也恢复了一部分强酸中心, 提高了苯与甲醇的反应活性。进一步考察了先碱后两步酸处理中不同碱浓度的影响, 结果表明, 适宜浓度的碱处理后再两步酸处理, 一方面, 能脱除分子筛的非骨架硅铝物种, 使分子筛的颗粒粒径更加均匀; 另一方面, 分子筛的强酸中心有所减少, 降低了催化剂的积炭失活速率, 苯转化率提高15%以上。
  • 图  1  不同碱浓度处理的BAA-ZSM-5系列催化剂的SEM照片

    (a): HZSM-5; (b): B1AA-ZSM-5; (c): B2AA-ZSM-5; (d): B3AA-ZSM-5

    Figure  1.  SEM images of BAA-ZSM-5 series catalysts treated by different concentration of alkaline

    图  2  不同碱浓度处理的BAA-ZSM-5分子筛催化剂的XRD谱图

    Figure  2.  XRD patterns of BAA-ZSM-5 series catalysts treated by different alkalinity

    图  3  不同碱浓度处理的BAA-ZSM-5分子筛催化剂的N2吸附脱附谱图

    Figure  3.  N2 adsorbtion-desorption profrles of BAA-ZSM-5 series catalyst treated with alkaline of different concentration

    图  4  不同碱浓度处理的BAA-ZSM-5分子筛催化剂的孔径分布图

    Figure  4.  Pore diameter distribution of BAA-ZSM-5 series catalyst treated with alkaline of different concentration

    图  5  不同碱浓度处理的BAA-ZSM-5分子筛催化剂酸性质比较

    Figure  5.  NH3-TPD profiles of BAA-ZSM-5 catalysts treated by different alkalinity

    图  6  不同碱浓度处理的BAA-ZSM-5分子筛催化剂催化性能比较

    Figure  6.  Catalytic performance of BAA-ZSM-5 >catalysts treated by different alkalinity

    表  1  不同碱浓度处理的BAA-ZSM-5系列分子筛的粒径分布

    Table  1.   Particle size distribution of BAA-ZSM-5 series catalysts treated by different alkalinity

    CatalystParticle size d/μm
    ≤0.70.7-1.5≥1.5
    HZSM-526.663.79.7
    B1AA1371.415.6
    B2AA87616
    B3AA3.37026.7
    下载: 导出CSV

    表  2  酸碱处理后ZSM-5的XRF分析

    Table  2.   XRF results of ZSM-5 treated by alkaline and acid

    CatalystConcentration w/% SiO2/Al2O3
    SiO2Al2O3
    HZSM-594.105.9027.119
    AA94.125.8827.22
    B94.085.9227.027
    BAA94.095.9127.112
    A: 0.08mol/L HCl; B: 0.15mol/L Na2CO3
    下载: 导出CSV

    表  3  不同碱浓度处理的BAA-ZSM-5分子筛催化剂的结晶度

    Table  3.   Crystallinity of BAA-ZSM-5 catalysts treating by different alkalinity

    CatalystFMI peak areaCrystallinity
    HZSM-530615100
    B1AA2983797.46
    B2AA2913595.17
    B3AA2731889.23
    下载: 导出CSV

    表  4  不同碱浓度处理BAA-ZSM-5催化剂的BET表征

    Table  4.   BET results of BAA-ZSM-5 series catalysts treated by different alkalinity

    Catalyst ABET
    /(m2·g-1)
    Amica
    /(m2·g-1)
    vmica
    /(cm3·g-1)
    HZSM-53462500.120
    B1AA3112390.115
    B2AA3362560.123
    B3AA3142380.115
    a: t-plot method
    下载: 导出CSV
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出版历程
  • 收稿日期:  2015-12-02
  • 修回日期:  2016-03-29
  • 网络出版日期:  2021-01-23
  • 刊出日期:  2016-06-10

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