| 宁东红石湾煤大分子模型构建及量子化学计算 |
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| 引用本文： | 李壮楣,王艳美,李平,李和平,白红存,郭庆杰.宁东红石湾煤大分子模型构建及量子化学计算[J].化工学报,2018,69(5):2208-2216. |
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| 作者姓名： | 李壮楣 王艳美 李平 李和平 白红存 郭庆杰 |
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| 作者单位： | 1. 省部共建煤炭高效利用与绿色化工国家重点实验室(宁夏大学), 宁夏 银川 750021;
2. 宁夏大学化学化工学院, 宁夏 银川 750021 |
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| 基金项目： | 宁夏自然科学基金面上项目（NZ17008）；宁夏科技厅对外交流合作项目（2015年）；宁夏高等学校一流学科建设项目（化学工程与技术学科，NXYLXK2017A04）；宁夏大学研究生创新项目（GIP2017029）。 |
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| 摘 要： | 使用工业分析、元素分析、固体核磁（13C NMR）、X射线光电子能谱（XPS）、傅里叶变换红外光谱（FT-IR）对宁东红石湾（HSW）煤样进行表征，获得煤样中元素赋存的种类、价态、化学键环境等物质微观结构的关键参数。结果表明HSW煤结构以芳香族为主，占75.96%，桥接芳碳与周碳比为0.315，可知其结构中以萘为主，苯和蒽为辅。氧原子主要以醚氧基（C-O）、羰基（C=O）和羧基（-COO）的形式存在，其中C-O占53.57%。氮原子以吡啶和吡咯的形式存在。苯环的连接方式以三、四取代为主，分别占47.77%、32.97%，脂肪族中环烷烃或脂肪烃-CH3占优势。确定HSW煤的分子式为C221H148O28N2，分子量为3142.32。在此基础上结合计算机辅助实现了二维和三维大分子模型构筑。应用量子化学计算对HSW煤大分子模型进行了优化及核磁共振、红外光谱模拟，验证了所建模型的合理性。最终实现了HSW煤的微观分子结构的实验与量子化学描述。
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| 关 键 词： | 煤 模型 计算化学 结构优化 分子模拟 光谱模拟 |
| 收稿时间： | 2018-01-05 |
| 修稿时间： | 2018-01-10 |
Macromolecular model construction and quantum chemical calculation of Ningdong Hongshiwan coal |
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| LI Zhuangmei,WANG Yanmei,LI Ping,LI Heping,BAI Hongcun,GUO Qingjie.Macromolecular model construction and quantum chemical calculation of Ningdong Hongshiwan coal[J].Journal of Chemical Industry and Engineering(China),2018,69(5):2208-2216. |
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| Authors: | LI Zhuangmei WANG Yanmei LI Ping LI Heping BAI Hongcun GUO Qingjie |
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| Affiliation: | 1. State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering, Ningxia University, Yinchuan 750021, Ningxia, China;
2. College of Chemistry and Chemical Engineering, Ningxia University, Yinchuan 750021, Ningxia, China |
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| Abstract: | Hongshiwan (HSW) coal from Ningdong China was characterized to determine key microstructural parameters of materials, such as elements, valence and chemical bonding, with proximate and ultimate analyses, solid state 13C nuclear magnetic resonance (13C NMR), X ray photoelectron spectroscopy (XPS) and Fourier transform infrared spectroscopy (FT-IR). The results revealed that main structure of HSW coal was 75.96%(mass) aromatic skeleton and 0.315 ratio of aromatic bridge carbon to aromatic peripheral carbon, indicating more naphthalene than benzene and anthracene in coal. Oxygen predominantly presented in the form of ether (C-O), carbonyl (C=O) and carboxyl (-COO), which C-O was accounted for 53.57%. Nitrogen presented in the form of pyridine and pyrrole. Tri-and tetra-substituents were mainly located on benzene ring at 47.77% and 32.97%, respectively. Methyl (-CH3) group was predominant in cyclic and aliphatic hydrocarbons. Thus, coal molecular formula was defined as C221H148O28N2 with molecular weight of 3142.32. Based on these results, macromolecular 2D and 3D model of HSW coal was built with computer-aided modelling. The model was optimized and further verified by FT-IR and 13C NMR spectra simulation by quantum chemical calculations. Therefore, molecular microstructures of HSW coal have been depicted from both experimental and quantum chemical approaches. |
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| Keywords: | coal model computational chemistry structural optimization molecular simulation spectral simulation |
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