高等学校化学学报 ›› 2018, Vol. 39 ›› Issue (9): 1859-1866.doi: 10.7503/cjcu20180114

• 研究论文:无机化学 • 上一篇    下一篇

球磨-再晶化法合成磷酸铝分子筛

王双1, 于越1, 白璞1, 刘健聪1, 李霖1, 宋晓伟1,2()   

  1. 1. 吉林大学化学学院, 无机合成与制备化学国家重点实验室, 长春 130012
    2. 布拉格查尔斯大学理学院物理和高分子化学系, 布拉格 12843
  • 收稿日期:2018-02-07 出版日期:2018-09-07 发布日期:2018-08-03
  • 作者简介:

    联系人简介: 宋晓伟, 女, 博士, 副教授, 主要从事纳米孔功能材料分子工程学方面的研究. E-mail: xiaoweisong@jlu.edu.cn

  • 基金资助:
    国家自然科学基金(批准号: 21641004, 21621001)和高等学校学科创新引智计划(批准号: B17020)资助.

Synthesis of Aluminophosphate Molecular Sieves by Ball Milling and Recrystallization

WANG Shuang1, YU Yue1, BAI Pu1, LIU Jiancong1, LI Lin1, SONG Xiaowei1,2,*()   

  1. 1. State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun 130012, China
    2. Department of Physical and Macromolecular Chemistry, Faculty of Science, Charles University in Prague,12843 Prague 2, Czech Republic
  • Received:2018-02-07 Online:2018-09-07 Published:2018-08-03
  • Contact: SONG Xiaowei E-mail:xiaoweisong@jlu.edu.cn
  • Supported by:
    † Supported by the National Natural Science Foundation of China(Nos. 21641004, 21621001) and the “111” Project of China(No. B17020).

摘要:

以热稳定性较差的二维层状磷酸铝AlPO-IM([C3H5N2]2[Al3P4O16H])为前驱体, 经过球磨-再晶化快速合成出具有AWO拓扑结构的磷酸铝分子筛AlPO-CJ73a及具有LAU拓扑结构的磷酸铝分子筛MgAPO-CJ73b和ZnAPO-CJ73c. 通过对合成条件的详细研究, 发现金属杂原子在合成过程中对LAU结构的生成起到导向作用, 结合共振拉曼光谱和CShM值计算研究了相转变机制. 利用球磨-再晶化法不仅极大缩短了晶化时间, 而且可在无溶剂条件下将二维层状磷酸铝前驱体转变为三维分子筛, 实现了分子筛合成中对环境的零排放. 与传统的水热/溶剂热法相比, 该方法具有高效、 节能的特点, 拓展了磷酸铝分子筛的合成路线.

关键词: 球磨法, 磷酸铝, 结构转变, 绿色合成

Abstract:

A rapid synthetic strategy through ball milling and recrystallization was successfully developed. Aluminophosphate molecular sieve with AWO topology was prepared by the precursor of two-dimensional(2D) layered aluminophosphate AlPO-IM. Simultaneously, metal-containing aluminophosphate molecular sieves with LAU topology were synthesized by introducing the metal heteroatoms in the ball-milling process. The phase transformation mechanism was comprehensively analyzed by Raman spectroscopy and CShM calculation. The results show that metal heteroatoms have an inorganic structure-directing effect in the synthesis of LAU molecular sieves. The ball milling-recrystallization method not only greatly shortens the crystallization time, but also converts the 2D layered aluminophosphates into a 3D molecular sieve under solvent-free conditions. Compared with the traditional hydrothermal/solvothermal synthesis, the ball milling-recrystallization method has the characteristics of high efficiency and energy saving, which expands the synthetic route of aluminophosphate molecular sieves.

Key words: Ball milling, Aluminophosphate, Structural transformation, Green synthesis

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