發(fā)布時(shí)間：2018-08-11 08:54

【摘要】：2-(二硝基亞甲基)-1,3-二氮雜環(huán)戊烷(DNDZ)是以FOX-7為原料合成出的,它是FOX-7親核反應(yīng)的一種重要的衍生物,是一類(lèi)新型的含能材料,表現(xiàn)出優(yōu)越的高能鈍感性能。本課題組以DNDZ為主配體,以有機(jī)胺類(lèi)溶液為輔助配體,與金屬(Cd、Zn)發(fā)生配位反應(yīng),在與甲胺溶液的反應(yīng)過(guò)程中DNDZ首次開(kāi)環(huán)形成N-(2-氨基乙基)-2,2-二硝基乙酰胺(ADNA)。本論文合成出五種配合物,其中兩種DNDZ的配合物,三種ADNA的配合物,培養(yǎng)出四種配合物的單晶。同時(shí),利用X-射線衍射儀測(cè)定了這些配合物的晶體結(jié)構(gòu)。并對(duì)數(shù)據(jù)進(jìn)行分析處理,進(jìn)而了解這些配合物的分子結(jié)構(gòu)、分子間的作用力和晶體的堆積情況。Cd(NH_3)_4(DNDZ)_2:單斜晶系；P_(21/c)空間群；[Cd(CH_3NH_2)_2(ADNA)_2]_n:三斜晶系；P_(-1)空間群；[Cd(C_2H_5NH_2)_2(ADNA)_2]_n:三斜晶系；P_(-1)空間群；Zn(NH_3)_2(DNDZ)_2:四方晶系；P_(4_12_12)空間群；在非等溫條件下,測(cè)定五種配合物的DSC和TG/DTG曲線,并研究了其熱分解行為,使用Kissinger法和Ozawa法計(jì)算得到了它們的熱分解動(dòng)力學(xué)參數(shù)。測(cè)定Cd(NH_3)_4(DNDZ)_2、[Cd(CH_3NH_2)_2(ADNA)_2]_n和Zn(NH_3)_2(DNDZ)_2的連續(xù)比熱容。在比熱容方程的基礎(chǔ)上,計(jì)算出配合物在298.15 K時(shí)的摩爾熱容分別為：642.0,608.6,636.6和521.3 J·mor1·K-1。并據(jù)此估算它們的絕熱至爆時(shí)間,計(jì)算結(jié)果分別為：59.4,22.7,48.6,64.3 s。測(cè)定配合物Cd(NH_3)_4(DNDZ)_2, [Cd(NH_3)_2(ADNA)_2]n, [Cd(CH_3NH_2)_2(ADNA)_2]_n, [Cd(C_2H_5NH_2)_2(ADNA)_2]_n和Zn(NH_3)_2(DNDZ)_2的撞擊感度來(lái)評(píng)價(jià)其熱安定性,其值分別為：20,18,17,11,15 J。
[Abstract]:2- (dinitromethylene) -1n 3-diazacyclopentane (DNDZ) is synthesized from FOX-7. It is an important derivative of FOX-7 nucleophilic reaction. It is a new type of energetic materials and has excellent high energy passivity. DNDZ was the main ligand and organic amine solution was used as auxiliary ligand to coordinate with metal (CD ~ (2 +) Zn). During the reaction with methylamine solution, DNDZ formed N- (2-aminoethyl) -2o _ 2-dinitroacetamide (ADNA). For the first time in the process of reaction with methylamine solution. In this paper, five complexes were synthesized, including two complexes of DNDZ and three complexes of ADNA, and the single crystals of four complexes were grown. At the same time, the crystal structure of these complexes was determined by X-ray diffractometer. The data are analyzed and processed to understand the molecular structure of these complexes, the intermolecular force and the stacking of crystals. CD (NH_3) 4 (DNDZ) 2: monoclinic S / S P _ (21 / c) space group; [CD (CH_3NH_2) _ 2 (ADNA) _ 2] n: triclinic system P _ (-1) space group; [CD (C_2H_5NH_2) _ 2 (ADNA) _ 2] n: triclinic crystal system P-1 space group; [CD (CH_3NH_2) _ 2 (ADNA) _ 2 (ADNA) _ 2]; [CD (C_2H_5NH_2) _ 2 (ADNA) _ 2] n: triclinic crystal system P _ (-1) space group; [CD (CH_3NH_2) 2 (ADNA) 2] n: P _ (-1) space group; The DSC and TG/DTG curves of the five complexes were measured under non-isothermal conditions, and their thermal decomposition behaviors were studied. The kinetic parameters of their thermal decomposition were calculated by Kissinger and Ozawa methods. The continuous specific heat capacity of CD (NH_3), [CD (CH_3NH_2) _ 2 (ADNA) _ 2] and Zn (NH_3) _ 2 (DNDZ) _ 2 was measured. On the basis of the specific heat capacity equation, the molar heat capacities of the complexes at 298.15 K were calculated to be: 642.0608.6636.6 and 521.3 J mor1 K-1, respectively. Their adiabatic time to explosion time is estimated, and the calculated results are respectively: 59.422.7 / 48.6 / 64.3s. The thermal stability of CD (NH_3), [CD (NH_3) _ 2 (ADNA) _ 2] n, [CD (CH_3NH_2) _ 2 (ADNA) _ 2] _ n, [CD (C_2H_5NH_2) _ 2 (ADNA) _ 2] _ S _ n and Zn (NH_3) _ 2 (DNDZ) _ 2 are measured to evaluate their thermal stability.
【學(xué)位授予單位】：西北大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2016
【分類(lèi)號(hào)】：TQ560.1;O641.4

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