基于1H-苯并咪唑-2-羧酸的三个镧系超分子化合物的结构、热分解动力学和荧光性质

doi:10.3866/PKU.WHXB201210122

物理化学学报 >> 2012, Vol. 28 >> Issue (12): 2783-2789.doi: 10.3866/PKU.WHXB201210122

基于1H-苯并咪唑-2-羧酸的三个镧系超分子化合物的结构、热分解动力学和荧光性质

段林强¹, 乔成芳^1,2, 魏青¹, 夏正强¹, 陈三平¹, 张国春², 周春生², 高胜利^1,2

1 西北大学化学与材料科学学院, 合成与天然功能分子化学教育部重点实验室,西安 710069;
2 商洛学院化学与化学工程系, 陕西省尾矿资源综合利用重点实验室, 陕西商洛 726000

收稿日期:2012-07-25 修回日期:2012-10-11 发布日期:2012-11-14
通讯作者: 魏青, 陈三平 E-mail:weiqq@126.com; sanpingchen@126.com
基金资助:
国家自然科学基金(21173168, 21073142, 21127004)和陕西省教育厅科研基金(2010JK882, 2010JQ2007, 11JS110, 11JK0578)资助项目

Structures, Thermodecomposition Kinetics and Luminescence Properties of Three Lanthanide-Based Supramolecular Compounds with 1H-Benzimidazole-2-carboxylic Acid

DUAN Lin-Qiang¹, QIAO Cheng-Fang^1,2, WEI Qing¹, XIA Zheng-Qiang¹, CHEN San-Ping¹, ZHANG Guo-Chun², ZHOU Chun-Sheng², GAO Sheng-Li^1,2

1 Key Laboratory of Synthetic and Natural Functional Molecule Chemistry of Ministry of Education, College of Chemistry and Materials Science, Northwest University, Xi'an 710069, P. R. China;
2 Department of Chemistry and Chemical Engineering, Shaanxi Key Laboratory of Comprehensive Utilization of Tailing Resources, Shangluo University, Shangluo 726000, Shaanxi Province, P. R. China

Received:2012-07-25 Revised:2012-10-11 Published:2012-11-14
Supported by:
The project was supported by the National Natural Science Foundation of China (21173168, 21073142, 21127004) and Science Research Projects of Educational Department of Shaanxi Province, China (2010JK882, 2010JQ2007, 11JS110, 11JK0578).

摘要/Abstract

摘要：

在水热条件下合成了三个镧系超分子化合物[Ln(HBIC)₃]_n [Ln=Sm (1), Ho (2), Yb (3); H₂BIC=1H-苯并咪唑-2-羧酸], 其中化合物1、2呈单晶态, 化合物3则为粉末样品; 借助单晶X射线衍射(XRD)、粉末衍射、元素分析、红外(IR)光谱、热分析等手段对化合物进行了表征. 结构分析表明, 1-3为同构化合物, 都呈现二维的平面结构, 其中每一个镧系金属中心与来自五个HBIC^-配体的三个氮原子和五个氧原子以两种新的配位模式配位形成一个轻微扭曲的双帽三棱柱几何构型, 相邻的二维(2D)平面进一步通过强的氢键作用形成了一个三维(3D)的超分子结构. 热重分析结果表明, 化合物1-3在360 ℃前均保持稳定, 呈现出良好的热稳定性. 基于Kissinger和Ozawa-Doyle两种方法, 通过差示扫描量热(DSC)技术研究得到了化合物1热分解的动力学参数(指前因子A_K=1.286×10⁸ s^-1; 活化能E_K=199.3 kJ·mol^-1, E_O=205.2 kJ·mol^-1). 另外, 也研究了室温下化合物1和3的固态发光性能, 结果表明, 化合物1和3分别在可见光区和近红外光区呈现出相应镧系金属离子的特征发射.

关键词: 镧系配合物, 1H-苯并咪唑-2-羧酸, 结构分析, 发光, 热分析动力学

Abstract:

Three lanthanide-based supramolecular compounds, [Ln(HBIC)₃]_n[Ln=Sm (1), Ho (2), Yb (3); H₂BIC=1H-benzimidazole-2-carboxylic acid], were hydrothermally synthesized and structurally characterized by X-ray single crystal diffraction (compounds 1 and 2), powder X-ray diffraction (XRD) (compound3), elemental analysis, infrared (IR) spectroscopy, and thermal analysis. Structural analyses reveal that compounds 1-3 are isomorphous and display a two-dimensional (2D) plane, in which each lanthanide center is coordinated by three N and five O atoms from five flexible HBIC^- ligands with two kinds of new coordination modes, giving rise to a slightly distorted two-capped triangle prism geometry. The 2D square networks are further assembled into a three-dimensional (3D) supramolecular framework through strong hydrogen-bonding interactions. Thermogravimetry analyses (TG) indicate that compounds 1-3 exhibit good thermostability and could be stable up to 360℃. By means of differential scanning calorimetry (DSC) techniques, the thermoanalysis kinetics parameters of the thermodecomposition of compound 1 were calculated by the Kissinger's and Ozawa-Doyle's methods; the pre-exponential factor A_K was 1.286×108 s^-1 and the apparent activation energy E_K and E_O were determined to be 199.3 and 205.2 kJ·mol^-1, respectively. In addition, the luminescent properties of compounds 1 and 3 were also studied at room temperature in the solid state. The results reveal that compounds 1 and 3 exhibit characteristic emission bands of the corresponding lanthanide ions in the visible and near-infrared regions, respectively.

Key words: Lanthanide coordination compound, 1H-Benzimidazole-2-carboxylic acid, Structure analysis, Luminescence, Thermoanalysis kinetics

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段林强, 乔成芳, 魏青, 夏正强, 陈三平, 张国春, 周春生, 高胜利. 基于1H-苯并咪唑-2-羧酸的三个镧系超分子化合物的结构、热分解动力学和荧光性质[J]. 物理化学学报, 2012, 28(12), 2783-2789. doi: 10.3866/PKU.WHXB201210122

DUAN Lin-Qiang, QIAO Cheng-Fang, WEI Qing, XIA Zheng-Qiang, CHEN San-Ping, ZHANG Guo-Chun, ZHOU Chun-Sheng, GAO Sheng-Li. Structures, Thermodecomposition Kinetics and Luminescence Properties of Three Lanthanide-Based Supramolecular Compounds with 1H-Benzimidazole-2-carboxylic Acid[J]. Acta Phys. -Chim. Sin. 2012, 28(12), 2783-2789. doi: 10.3866/PKU.WHXB201210122

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB201210122

https://www.whxb.pku.edu.cn/CN/Y2012/V28/I12/2783

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基于1H-苯并咪唑-2-羧酸的三个镧系超分子化合物的结构、热分解动力学和荧光性质

Structures, Thermodecomposition Kinetics and Luminescence Properties of Three Lanthanide-Based Supramolecular Compounds with 1H-Benzimidazole-2-carboxylic Acid

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