微波辅助溶剂热条件下烟酸锌配位聚合物的合成
摘要
本论文主要研究烟酸锌金属-有机配位聚合物的微波合成与结构表征,旨在研究微波加热与传统加热方式相比的高效性。本论文首次利用微波辅助溶剂热法在10min的时间内合成出形貌规则的烟酸锌配合物,并对所合成配合物进行了性质的表征。同时讨论了温度、反应时间、反应物初始浓度、加热方式以及溶剂对产物结晶情况的影响。
微波辅助溶剂热法虽具有晶体成核均匀、对产物具有很好选择性等一系列优点,但由于反应时间短,导致产物的晶粒度较小。本文尝试采用微波溶剂热与传统溶剂热相结合的方法进行烟酸锌配位聚合物的合成。首先由微波溶剂热法制取晶种,接着在传统溶剂热条件下实现晶体的二次生长。所合成产物既具备了微波加热的各种优点,同时又在较短的反应时间里生成了较大的单晶体,这对于新结构及新产物的确定具有非常重要的意义。
Coordination polymers is one of top topics in the field of materials chemistry due to their applications in a large number of different aspects, such as electrical, optical, magnetic, catalytic and adsorption-desorption. As we known that the structure of coordination polymers determines the characteristic performance, therefore, it is a great challenge for scientific workers to fastly synthesize the coordination polymers for required functionality. Most of zinc complexes have good photoluminescence and nonlinear optical properties, so the study of zinc complexes will have a great significance.
At present, hydro(solvo)thermal method is widely used in synthesis of coordination polymers which have high stability. But the conventional hydro(solvo)thermal method requires so much time that it extends the reaction periods. In recent years, microwave technology is widely used in preparing products quickly, so it could overcome this shortcoming. Microwave heating not only shorten the reaction time significantly and improve the yield and purity of product, but also has good reproducibility and stability of the amplification. Therefore, our laboratory use microwave as the heating means. We were succeeded in synthesis of bis(nicotinate)zinc under microwave-assisted solvothermal condition. Also, we obtained bis(nicotinate)zinc which has particle size of about 0.5mm by the combination of microwave-assisted solvothermal method and conventional solvothermal method. The specific descriptions are as follows:
We used nicotinic acid as the ligand to coordinate with zinc(Ⅱ) to build the 2D chiral coordination polymer of [Zn(nicotinate)2]n under microwave-assisted solvothermal condition, while dimethylformamide (DMF) was used as the solvent, and the reaction time was only 10min. This method not only shortened the reaction time significantly, but also decreased the temperature of the reaction. The compound were characterized by means of X-ray powder diffraction (XRD), polarized light microscopy, scanning electron microscopy (SEM), fluorescent spectrometry and TG-DTA. The complex has strong fluorescence emission property at room temperature, also the complex has high thermal stability, while TG-DTA showed that the complex has onset decomposition temperature of 400℃.
In addition, we also disscussed the influences of reaction time, temperature, solvent, substrate concentration and heating method on the crystallization of the complexes. It was found that the particle size of the crystal would be gradually larger and the shape of the crystal would transit from plate to octahedral when reaction conditions were changed, such as the extension of reaction time, the increase of temperature and substrate concentration. In contrast to conventional solvothermal method, we found that microwave heating can obtain pure [Zn(nicotinate)2]n in 10min, while conventional solvothermal method obtain the mixture of [Zn(nicotinate)2]n and other products. That was noted that microwave heating can not only reduce the reaction time, but also have a better selectivity for the reaction. When we used other solvents, the reaction could not take place under the same reaction conditions, it was noted that DMF was irreplaceable for this reaction.
Although microwave-assisted solvothermal method have many advantages, the partical size of crystals obtained from microwave heating was always so small that we couldn’t get the structure information of the crystal. So we combined the microwave-assisted solvothermal method and the conventional solvothermal method. Firstly the crystal quickly nucleated under microwave-assisted solvothermal condition; secondly the nucleus got secondary growth under conventional solvothermal condition. The product we obtained not only has the advantages of microwave heating, but also has a larger partical size that suitable for structural analysis. This successful attempt for new synthesis method will have great significance on the synthesis of new compound and the determination of new structure.
微波辅助溶剂热法虽具有晶体成核均匀、对产物具有很好选择性等一系列优点,但由于反应时间短,导致产物的晶粒度较小。本文尝试采用微波溶剂热与传统溶剂热相结合的方法进行烟酸锌配位聚合物的合成。首先由微波溶剂热法制取晶种,接着在传统溶剂热条件下实现晶体的二次生长。所合成产物既具备了微波加热的各种优点,同时又在较短的反应时间里生成了较大的单晶体,这对于新结构及新产物的确定具有非常重要的意义。
Coordination polymers is one of top topics in the field of materials chemistry due to their applications in a large number of different aspects, such as electrical, optical, magnetic, catalytic and adsorption-desorption. As we known that the structure of coordination polymers determines the characteristic performance, therefore, it is a great challenge for scientific workers to fastly synthesize the coordination polymers for required functionality. Most of zinc complexes have good photoluminescence and nonlinear optical properties, so the study of zinc complexes will have a great significance.
At present, hydro(solvo)thermal method is widely used in synthesis of coordination polymers which have high stability. But the conventional hydro(solvo)thermal method requires so much time that it extends the reaction periods. In recent years, microwave technology is widely used in preparing products quickly, so it could overcome this shortcoming. Microwave heating not only shorten the reaction time significantly and improve the yield and purity of product, but also has good reproducibility and stability of the amplification. Therefore, our laboratory use microwave as the heating means. We were succeeded in synthesis of bis(nicotinate)zinc under microwave-assisted solvothermal condition. Also, we obtained bis(nicotinate)zinc which has particle size of about 0.5mm by the combination of microwave-assisted solvothermal method and conventional solvothermal method. The specific descriptions are as follows:
We used nicotinic acid as the ligand to coordinate with zinc(Ⅱ) to build the 2D chiral coordination polymer of [Zn(nicotinate)2]n under microwave-assisted solvothermal condition, while dimethylformamide (DMF) was used as the solvent, and the reaction time was only 10min. This method not only shortened the reaction time significantly, but also decreased the temperature of the reaction. The compound were characterized by means of X-ray powder diffraction (XRD), polarized light microscopy, scanning electron microscopy (SEM), fluorescent spectrometry and TG-DTA. The complex has strong fluorescence emission property at room temperature, also the complex has high thermal stability, while TG-DTA showed that the complex has onset decomposition temperature of 400℃.
In addition, we also disscussed the influences of reaction time, temperature, solvent, substrate concentration and heating method on the crystallization of the complexes. It was found that the particle size of the crystal would be gradually larger and the shape of the crystal would transit from plate to octahedral when reaction conditions were changed, such as the extension of reaction time, the increase of temperature and substrate concentration. In contrast to conventional solvothermal method, we found that microwave heating can obtain pure [Zn(nicotinate)2]n in 10min, while conventional solvothermal method obtain the mixture of [Zn(nicotinate)2]n and other products. That was noted that microwave heating can not only reduce the reaction time, but also have a better selectivity for the reaction. When we used other solvents, the reaction could not take place under the same reaction conditions, it was noted that DMF was irreplaceable for this reaction.
Although microwave-assisted solvothermal method have many advantages, the partical size of crystals obtained from microwave heating was always so small that we couldn’t get the structure information of the crystal. So we combined the microwave-assisted solvothermal method and the conventional solvothermal method. Firstly the crystal quickly nucleated under microwave-assisted solvothermal condition; secondly the nucleus got secondary growth under conventional solvothermal condition. The product we obtained not only has the advantages of microwave heating, but also has a larger partical size that suitable for structural analysis. This successful attempt for new synthesis method will have great significance on the synthesis of new compound and the determination of new structure.
引文
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[1]禹良才,梁宏,周春山等.四水二异烟酸锌(Ⅱ)的合成及其晶体结构[J].合成化学,2005,13(5):504-506.
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[3]唐雯霞,祝世彤,戴安邦.配位化学近期进展[J].化学通报,1991,11: 1-5.
[4] Basolo著,高忆慈等译.无机化学前沿[M].兰州大学出版社,1989.
[5] Li H, Eddaoudi M, Groy T L, et al. Establishing Microporosity in Open Metal-Organic Frameworks: Gas Sorption Isotherms for Zn(BDC)(BDC= 1,4-Benzene dicarboxylate) [J]. J. Am. Chem. Soc., 1998, 120: 8571-8572.
[6] Mooibroek T J, Gamez P. The s-triazine ring, a remarkable unit to generate supramolecular interactions [J]. Inorg. Chim. Acta, 2007, 360: 381-404.
[7] Hagrman P J, Hagrman D, Zubieta J. Organic-Inorganic Hybrid Materials: From“Simple”Coordination Polymers to Organodiamine-Templated Molybdenum Oxides [J]. Angew. Chem. Int. Ed., 1999, 38: 2638-2684.
[8] James S L. Metal-organic frameworks [J]. Chem. Soc. Rev., 2003, 32: 276-288.
[9]王磊.1,2,4-苯三酸及巯基多氮杂环构筑的配位聚合物水热合成、结构与性质表征[D].吉林:吉林大学化学学院,2006.
[10] Hunter C A. Self-Assembly of Molecular-Sized Boxes [J]. Angew. Chem. Int. Ed. Engl., 1995, 34: 1079-1081.
[11] Férey G, Serpaggi F. Scale of the dimensions of the pores as a function of time [J]. Chem. Mater., 2001, 13: 3084-3098.
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