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Solid-State Synthesis of Aluminophosphate Zeotypes by Calcination of Amorphous Precursors
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2023-02-15 , DOI: 10.1021/jacs.3c00258 Shuo Tao 1 , Zhili Wang 2, 3 , Lei Wang 4 , Xiaolei Li 1 , Xue Li 1 , Yujie Wang 1 , Bo Wang 1 , Wenwen Zi 1 , Ying Wei 5 , Kuizhi Chen 2 , Zhijian Tian 2 , Guangjin Hou 2
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2023-02-15 , DOI: 10.1021/jacs.3c00258 Shuo Tao 1 , Zhili Wang 2, 3 , Lei Wang 4 , Xiaolei Li 1 , Xue Li 1 , Yujie Wang 1 , Bo Wang 1 , Wenwen Zi 1 , Ying Wei 5 , Kuizhi Chen 2 , Zhijian Tian 2 , Guangjin Hou 2
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Because of the growing interest in the applications of zeolitic materials and the various challenges associated with traditional synthesis methods, the development of novel synthesis approaches remains of fundamental importance. Herein, we report a general route for the synthesis of aluminophosphate (AlPO) zeotypes by simple calcination of amorphous precursors at moderate temperatures (250–450 °C) for short reaction times (3–60 min). Accordingly, highly crystalline AlPO zeotypes with various topologies of AST, SOD, LTA, AEL, AFI, and -CLO, ranging from ultra-small to extra-large pores, have been successfully synthesized. Multinuclear multidimensional solid-state NMR techniques combined with complementary operando mass spectrometry (MS), powder X-ray diffraction, high-resolution transmission electron microscopy, and Raman characterizations reveal that covalently bonded fluoride in the intermediates catalyze the bond breaking and remaking processes. The confined organic structure-directing agents with high thermal stability direct the ordered rearrangement. This novel synthesis strategy not only shows excellent synthesis efficiency in terms of a simple synthesis procedure, a fast crystallization rate, and a high product yield, but also sheds new light on the crystallization mechanism of zeolitic materials.
中文翻译：
通过无定形前体的煅烧固态合成磷酸铝 Zeotypes
由于对沸石材料应用的兴趣日益浓厚，以及与传统合成方法相关的各种挑战，开发新型合成方法仍然至关重要。在此，我们报告了通过在中等温度 (250–450 °C) 下短反应时间 (3–60 分钟) 简单煅烧无定形前体来合成磷酸铝 (AlPO) 沸石的一般途径。因此，具有AST、SOD、LTA、AEL、AFI和-CLO各种拓扑结构的高度结晶的 AlPO 类沸石，从超小孔到超大孔，已经成功合成。多核多维固态核磁共振技术与互补原位质谱 (MS)、粉末 X 射线衍射、高分辨率透射电子显微镜和拉曼表征相结合表明，中间体中的共价键合氟化物催化了键断裂和重建过程。具有高热稳定性的受限有机结构导向剂指导有序重排。这种新颖的合成策略不仅在合成过程简单、结晶速率快、产品收率高方面表现出优异的合成效率，而且为分子筛材料的结晶机理提供了新的思路。
更新日期：2023-02-15
中文翻译：
通过无定形前体的煅烧固态合成磷酸铝 Zeotypes
由于对沸石材料应用的兴趣日益浓厚，以及与传统合成方法相关的各种挑战，开发新型合成方法仍然至关重要。在此，我们报告了通过在中等温度 (250–450 °C) 下短反应时间 (3–60 分钟) 简单煅烧无定形前体来合成磷酸铝 (AlPO) 沸石的一般途径。因此，具有AST、SOD、LTA、AEL、AFI和-CLO各种拓扑结构的高度结晶的 AlPO 类沸石，从超小孔到超大孔，已经成功合成。多核多维固态核磁共振技术与互补原位质谱 (MS)、粉末 X 射线衍射、高分辨率透射电子显微镜和拉曼表征相结合表明，中间体中的共价键合氟化物催化了键断裂和重建过程。具有高热稳定性的受限有机结构导向剂指导有序重排。这种新颖的合成策略不仅在合成过程简单、结晶速率快、产品收率高方面表现出优异的合成效率，而且为分子筛材料的结晶机理提供了新的思路。
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