球磨-再晶化法合成磷酸铝分子筛

Synthesis of Aluminophosphate Molecular Sieves by Ball Milling and Recrystallization

以热稳定性较差的二维层状磷酸铝AlPO-IM([C_3H_5N_2]_2[Al_3P_4O_(16)H])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MgAPOCJ73b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CSh M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.

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.