| 新型三维开放骨架磷酸铝[C4H14N2][Al4P5O19OH]的合成、表征及结构导向研究 |
| Synthesis and Characterization of a New Three-Dimensional Open-Framework Aluminophosphate [C4H14N2][Al4P5O19OH] and Investigation of the Structure-Directing Effect |
| 作者 | 单位 | E-mail | | 仝晓强 | 吉林大学无机制备与合成国家重点实验室, 吉林大学化学学院, 长春 130012 | | | 卢慧英 | 吉林大学无机制备与合成国家重点实验室, 吉林大学化学学院, 长春 130012 | | | 黄湃 | 吉林大学无机制备与合成国家重点实验室, 吉林大学化学学院, 长春 130012 | | | 闫文付 | 吉林大学无机制备与合成国家重点实验室, 吉林大学化学学院, 长春 130012 | yanw@jlu.edu.cn | | 于吉红 | 吉林大学无机制备与合成国家重点实验室, 吉林大学化学学院, 长春 130012 | | | 徐如人 | 吉林大学无机制备与合成国家重点实验室, 吉林大学化学学院, 长春 130012 | |
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| 摘要: 以1,4-丁二胺(BDA, C4H12N2)为结构导向剂,在水热条件下合成了一例新型三维阴离子开放骨架磷酸铝化合物[C4H14N2][Al4P5O19OH](AlPO-BDA),用单晶X-射线衍射确定了其结构,并用X-射线粉末衍射(XRD)、扫描电子显微镜(SEM),热重以及元素分析等进行了表征。该开放骨架在[100]和[010]方向上分别具有8和12元环的椭圆形孔道,并相互交叉形成联通的二维孔道系统。以1,6-己二胺(HDA)、1,5-戊二胺(PDA)或2-甲基1,5-戊二胺(MPMD)为结构导向剂,在水热条件下也可得到与AlPO-BDA非常类似的开放骨架拓扑结构,表明这些有机胺在一定的条件下和1,4-丁二胺具有相同的拓扑结构导向作用,但有机胺的尺寸和形状对开放骨架的结晶学对称性及孔道形状有显著的影响,有机胺分子中N-N之间的距离同开放骨架的理论表面积和孔自由体积存在明确的相关性。 |
| 关键词: 沸石 磷酸铝 结构导向作用 |
| 基金项目: 国家自然科学基金(No.21171063);优秀青年基金(No.21222103);国家重点基础研究发展规划项目(2011CB808703)和高等学校博士学科点专项科研基金资助课题资助项目。 |
| Abstract: A new three-dimensional (3D) anionic open-framework aluminophosphate [C4H14N2][Al4P5O19OH] (AlPO-BDA) was hydrothermally synthesized by using 1,4-diaminobutane (BDA, C4H12N2) as a structure directing agent. The structure was determined by single-crystal X-ray diffraction structural analysis. AlPO-BDA was further characterized by powder X-ray diffraction (XRD), scanning electron microscope (SEM), elemental (CHN) and thermogravimetric (TG) analyses. The open-framework of AlPO-BDA contains 12-ring (12R) channels along [010] direction which are intersected with 8-ring (8R) channels running along [100] direction. In the presence of 1, 6-hexanediamine (HDA), 1, 5-pentanediamine (PDA), or 2-methylpentamethylenediamine (MPMD) and under hydrothermal condition, anionic open-frameworks with similar topology of AlPO-BDA can be obtained, which are denoted AlPO-HDA, AlPO-PDA, and AlPO-MPMD, respectively. However, their crystallographic symmetry and the shape of the channels are different. These results suggest that these amines have the same topological structure-directing effect but different structure-directing effect in the formation of these open-frameworks. The correlation between the calculated free volume and surface of the open-frameworks and the N-N distance of the diamines is observed. CCDC: 947284 |
| Keywords: zeolite aluminophosphate structure-direct effect |
| 投稿时间：2013-02-01 修订日期：2013-04-25 |
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| 仝晓强,卢慧英,黄湃,闫文付,于吉红,徐如人.新型三维开放骨架磷酸铝[C4H14N2][Al4P5O19OH]的合成、表征及结构导向研究[J].无机化学学报,2013,29(8):1639-1644. |
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