Influence of F- on the Structure-directing Effect of Organic Amines in the Synthesis of Open-framework Aluminophosphates†

doi:10.7503/cjcu20140894

Abstract

Abstract:

The significant influence of F^- on the structure-directing effect of ethylenediamine(en) and diethylenetriamine(deta) in the synthesis of open-framework aluminophosphates was investigated. For the system with ethylenediamine, in the absence of F^-, layered aluminophosphate Al₂P₂O₉·NH₃(CH₂)₂NH₃(UiO-13) was obtained from the initial mixture with n(Al₂O₃):n(P₂O₅):n(en):n(H₂O)=1.0:1.5:18.0:147 under hydrothermal condition, while layered aluminophosphate AlF(HPO₄)·NH₂(CH₂)₂NH₂(1) was obtained from the initial mixture with n(Al₂O₃):n(P₂O₅):n(en):n(HF):n(H₂O)=1.0:1.5:18.0:3.0:147. The results suggested that the F^- significantly affected the structure-directing effect of ethylenediamine. For the system with diethylenetriamine, a three-dimensional(3D) open-framework aluminophosphate Al₄P₅O₂₀(H₂O)₂·C₄N₃H₁₆(AlPO-CJ31) was synthesized from the initial mixture with n(Al₂O₃):n(P₂O₅):n(deta):n(H₂O)=1.0:4.0:3.0:153 under hydrothermal condition, while a one-dimensional(1D) aluminophosphate Al₂P₄O₁₀(OH)₃F·C₄N₃H₁₅(2) was crystallized from the similar initial mixture in the presence of F^-[n(Al₂O₃):n(P₂O₅):n(deta):n(HF):n(H₂O)=1.0:4.0:3.0:3.0:153]. The results indicated that the structure-directing effect of diethylenetriamine was significantly altered by F^-. The structural properties of open-framework aluminophosphates UiO-13, 1, AlPO-CJ31 and 2 were analyzed in detail and the influence of F^- on the structure-directing effect of ethylenediamine and diethylenetriamine was discussed.

Key words: Open-framework aluminophosphate, Fluoride, Ethylenediamine, Diethylenetriamine, Structure-directing effect

CLC Number:

O611.4

TrendMD:

TIAN Ye, WANG Shurong, YAN Wenfu, XU Ruren, WANG Yongrui, MU Xuhong. Influence of F^- on the Structure-directing Effect of Organic Amines in the Synthesis of Open-framework Aluminophosphates^†[J]. Chem. J. Chinese Universities, 2015, 36(3): 428.

Figures/Tables 4

Fig.1 Experimental(a) and simulated(b) powder X-ray diffraction patterns for compound UiO-13(A) and compound 1(B)

Fig.2 Structures of compound UiO-13(A) and compound 1(B) viewed along the [010] direction

Fig.3 Experimental(a) and simulated(b) powder X-ray diffraction patterns for compound AlPO-CJ31(A) and compound 2(B)

Fig.4 Structures of compound AlPO-CJ31(A) and compound 2(B) viewed along the [001] direction

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