【作者】 李春生；

【导师】 秦志宏；

【作者基本信息】 中国矿业大学 ， 化学工程与技术， 2015， 硕士

【摘要】 为研究煤嵌布结构模型中有关大分子组分和中型分子组分所构成的骨架结构的平均分子特征,以童亭煤全组分族分离所得重质组、疏中质组、密中质组和轻质组为对象,通过四级溶剂分级萃取抽提出各自的可溶小分子后,对其不溶物进行FTIR、XPS和13C NMR等测试与分析,获得各族组分骨架结构的特征信息,在此基础上构建了童亭煤各族组分的骨架结构分子模型;通过Gaussian09W软件对各模型进行了结构最优化计算并得到了相应的IR谱图;利用GC/MS和FTIR分析了各族组分可溶小分子的组成与结构特征。结果表明:重质组、疏中质组和密中质组骨架结构中的碳原子均以芳香单元及其取代烷烃形式为主,其含量(物质的量分数,下同)分别为69.20%、79.86%和85.44%,其次为酚碳或醚碳;有机氧原子以羟基和醚氧键形式为主,含量分别为51.69%、47.48和41.83%,其次为羧基和羰基;氮的赋存形式以吡咯型氮为主,含量分别为64.29%、59.41%和52.50%,其次为吡啶型氮;有机硫以噻吩型硫为主,含量分别为31.50%、47.07%和40.00%,其次为砜型硫和硫醇硫醚型硫。重质组、疏中质组和密中质组骨架结构的芳香度分别为64.7%、67.2%和67.8%,脂肪碳含量分别为26.3%、21.7%和22.8%,脂氢与芳氢之比分别为1.75、1.96和2.25,芳香桥碳与周碳之比分别为0.28、0.24和0.23;芳香结构单元均以2-3环的缩合芳环为主,4环为辅;所构建结构模型的分子式分别为C246H186O15N4、C216H183O5N5S和C195H179O4N3S,相对分子质量分别为3434、2957和2657。经能量最小化和频率计算后所得IR谱图与实验谱图吻合良好。溶剂可溶小分子在重质组中以芳族和C-O化合物为主,在疏中质组中以芳族化合物为主,在密中质组中以脂族化合物为主。轻质组全部为溶剂可溶,并以含N、O杂原子化合物为主。论文最后构建了童亭煤的嵌布结构模型。更多还原

【Abstract】 Tongting coal was separated to four group components, i.e.heavy component, light component, loose medium component and dense medium component, to study the average molecular characteristics of the framework structure of macromolecule and medium molecular components, the department of the Embedded Structure Model. We performed the fractional and multiple extraction of group components and get the residues by extracting the soluble small molecule, the undissolved matters were analyzed via FTIR, XPS and 13 C NMR to get the feature information of group components framework structure. The structure model of Tongting coal group components were constructed based on the information we get. Using Gaussian 09 W software to simulate the optimization structure and calculated the IR spectra of the framework structure model. The dissolved matters were tested via GC/MS and FTIR, and analysis of the distribution and dissolution regularities of small soluble molecules. The results indicated that:Carbon atoms of heavy component, light component, loose medium component and dense medium component framework structure are mainly for C=C and C- H forms, and their contents(amount of substance fraction, the same below) are 69.20%, 79.86% and 85.44%, followed by C-O; The oxygen atoms existed as the form of hydroxyl and ether oxygen bond, their contents are 51.69%, 47.48% and 41.83%; secondly for COO- and C=O; Pyrrole-type nitrogen is the main form of nitrogen atorm in each group component, their contents are 64.29%, 59.41% and 52.50%, then Pyridine-type nitrogen; Thiophenic sulfur is the main form of organic sulfur, their contents are 31.50%, 47.07% and 40.00%, followed by sulfone type sulfur and mercaptan sulfur ether type sulfur.The aromaticity of heavy component, light component, loose medium component and dense medium component framework structure are 64.7%, 67.2% and 67.8%, aliphatic carbon content are 26.3%, 21.7% and 22.8%, aliphatic hydrogen and aromatic hydrogen ratio are 1.75, 1.96 and 2.25, and the XBP are 0.28, 0.24 and 0.23. Aromatic unit mainly for 2-3 ring-condensed polycyclic aromatic and the subsidiary role of four-ring, The structural formulas of group components framework structure model are C246H186O15N4, C216H183O5N5 S, and C195H179O4N3 S, and the relative molecular mass are 3434, 2957 and 2657. The calculated IR spectrogram is well consistent with that of the experimental results after energy minimization andfrequency calculaton.The solvent soluble small molecule of heavy components are mainly for aromatic and C-O components, aromatic components is the main form of soluble small molecule in light component, and in dense medium component the soluble small molecular is mainly for aliphatic components. All the light component were dissolved by solvent, and it`s soluble small molecule is mainly composed by heteroatom component with N and O.Construct of the embedded structure model of Tongting coal in the end of this thesis.更多还原