铝离子在beta沸石晶化过程中对多形体A富集的影响

摘要

Using tetraethylammonium hydroxide as the organic structure-directing agent and in the presence of fluoride, polymorph A-enriched silica beta zeolite was synthesized under concentrated hydro-thermal conditions. The introduction of Al species into the same starting mixture resulted in a de-crease in the degree of enrichment of polymorph A in beta zeolite and an Al-incorporated beta zeo-lite resulted. The crystallized polymorph A-enriched silica beta zeolite and the Al-incorporated beta zeolite and their crystallization processes were investigated by X-ray diffractometry, elemental analysis, thermogravimetric analysis-differential thermal analysis, nitrogen adsorption, scanning electron microscopy, and solid-state magic angle spinning nuclear magnetic resonance. The intro-duction of Al species accelerated crystallization and reduced the crystal size of Al-incorporated beta zeolite. The intermediate of five-coordinated Al species accounted for a decrease in the degree of enrichment of polymorph A in the crystallization of Al-incorporated beta zeolite.%以四乙基氢氧化铵为有机结构导向剂，采用超浓水热方法，从氟离子体系合成出手性多形体A(简称A形体)富集的全硅beta沸石。在同样的初始混合物中引入铝源后，所合成的beta沸石中A形体含量明显降低，产物为普通的硅铝beta沸石。用粉末X射线衍射、元素分析、热重-差热分析、氮气吸附、扫描电子显微镜和固体魔角自旋核磁共振等表征手段对全硅beta沸石和硅铝beta沸石进行了详细的表征，并研究了其晶化过程。结果表明，铝源的引入可以加速beta沸石的晶化，得到的硅铝beta沸石晶体粒径明显减小。在硅铝beta沸石的晶化过程中生成了五配位铝物种，五配位铝物种可能是导致产物中A形体含量降低的原因。