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三唑类过渡金属配合物的合成、结构和性质表征

Syntheses, Structures and Properties of Transition Metal Compounds with Triazole Derivatives as Ligands

【作者】 李娜

【导师】 高胜利;

【作者基本信息】 西北大学 , 无机化学, 2007, 硕士

【摘要】 燃速催化剂是固体推进剂配方中关键的功能材料,是调节固体推进剂燃烧性能不可缺少的组分之一。传统的双基推进剂通常采用铅化合物作为燃速催化剂,铅化合物能够有效的提高推进剂燃速,降低压力指数;但是,这种推进剂的能量有限并且会对环境和从业人员造成极大危害。三唑衍生物与过渡金属离子形成的含能配合物由于高含氮量、高密度和热焓高等特点可以用作固体推进剂中的燃速催化剂。本文分别以1,2,4-三唑-5-酮和3-氨基-1,2,4-三唑为配体,合成了13种不含铅的金属配合物,并制备了其中九个配合物的单晶,对其热稳定性进行了研究并用X-射线单晶衍射仪对其结构进行了测定。结构测试发现,配体1,2,4-三唑-5-酮可以以双齿或单齿的形式与金属配位,其配位点分别为羰基上的氧原子和三唑环上二位的氮原子;配体3-氨基-1,2,4-三唑以质子化的形式与金属离子配位,其配位点为三唑环上一位的氮原子。高氯酸铵(AP)是固体火箭推进剂中的主要成分,常用作固体推进剂中的氧化剂和高能组分。其特性对火箭推进剂的总体性能有重要影响。本文在AP中添加少量的含能配合物(1/4)来研究配合物对AP热分解的影响。研究发现其中12个配合物与AP的混合体系在高温段的热分解温度比AP本身低,同时这12个混合体系高温热分解的能量大于AP本身高温段热分解的能量。

【Abstract】 Burning rate modifier is the critical function material in the double base propellants. Conventional double base propellants often utilize lead-based compounds as component of burning rate modifiers, which are hazardous to environment and the energy is limited. Many attentions were paid to find eco-friendly and energetic burning rate modifiers. The metal complexes with 1, 2, 4-triazole derivatives because of high nitrogen composition, high enthalpy of formation and high densities can be used as a new generation of burning rate modifiers.In this work, 13 new coordination compounds were synthesized using ligands 1, 2, 4-triazole-5-one and 3-amido-1, 2, 4-triazole and were characterized by elemental analysis, IR spectrum, DSC and TG-DTG techniques. Nine single crystals among the 13 coordination compounds were prepared and characterized by X-ray single crystal diffraction. The X-ray structure analysis revealed that the 1, 2, 4-triazole-5-one is a monodentate or didentate ligand in its coordination compounds, and the 3-amido-1, 2, 4-triazole is a monodentate ligand in its coordination compounds.Ammonium perchlorate (AP) is the most common oxidizer and energetic composition in double based propellants. Its thermal decomposition characteristics influence the combustion behavior of the propellant significantly. In this work, the energetic coordination compounds that we prepared were added to AP in order to evaluate their effect on the thermolysis of AP. This study revealed that the decomposition temperatures (Tonset) of the mixtures shift to lower temperature and the energy of most mixtures are much greater than AP itself.

  • 【网络出版投稿人】 西北大学
  • 【网络出版年期】2007年 05期
  • 【分类号】O641.4
  • 【被引频次】3
  • 【下载频次】418
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