神府煤显微组分大分子及聚集态结构模型构建  

Construction of macromolecular and aggregate structure models of Shenfu coal macerals

作　　者：张怀青 周安宁[1,2] 李振 屈进州[1,2] 焦卫红 杨志远[1,2] ZHANG Huaiqing;ZHOU Anning;LI Zhen;QU Jinzhou;JIAO Weihong;YANG Zhiyuan(College of Chemistry and Chemical Engineering,Xi'an University of Science and Technology,Xi'an,Shaanxi 710054,China;Key Laboratory of Coal Resources Exploration and Comprehensive Utilization,Ministry of Natural Resources,Xi'an,Shaanxi 710021,China)

机构地区：[1]西安科技大学化学与化工学院,陕西西安710054 [2]自然资源部煤炭资源勘查与综合利用重点实验室,陕西西安710021

出　　处：《中国矿业大学学报》2023年第4期796-812,共17页Journal of China University of Mining & Technology

基　　金：国家自然科学基金-新疆联合基金(U2003133);陕西省煤炭联合基金项目(2019JLP-10);陕西省重点产业创新链(群)-工业领域项目(2017ZDCXL-GY-10-01-02);霍英东教育基金会高等院校青年教师基金项目(171102)。

摘　　要：为了深入解析神府煤的结构特征,促进其低碳高值化利用,采用X射线光电子能谱、固体核磁等表征手段,结合分子动力学计算,构建了神府煤(SFC)及其镜质体富集样(SFV)和惰质体富集样(SFI)的大分子和聚集态结构模型.结果表明:SFC,SFV和SFI大分子结构的分子式分别为C_(128)H_(106)N_(2)O_(11),C_(133)H_(114)N_(2)O_(12)和C_(137)H_(110)N_(2)O_(11).SFI的芳香度和不饱和度较大,芳环缩合程度高,氮主要以吡咯形式存在;SFV中含有相对丰富的羧基官能团,氮主要以吡啶形式存在.在模拟构建聚集态结构的过程中,大分子结构不断调整优化,非键能大幅降低.SFV的模拟密度为1.25 g/cm^(3),具有较高的表面积和丰富的孔隙结构,非键能为-105.59 kJ/mol;SFI的模拟密度为1.35 g/cm^(3),与周围周期性单元间重叠度高,非键能为2231.39 kJ/mol,结构稳定,分子间相互作用力强;SFC的模拟密度为1.30 g/cm^(3),非键能为1567.96 kJ/mol,介于两者之间.In order to deeply analyze the structural characteristics of Shenfu coal and promote its low-carbon and high-value utilization.The macromolecular and aggregated structural models of Shenfu coal sample(SFC)and its vitrinite enriched sample(SFV)and inertinite enriched sample(SFI)were constructed by methods of X-ray photoelectron spectroscopy,solid-state nuclear magnetic resonance and molecular dynamics calculations.The results show that the macromolecular structures of SFC,SFV and SFI can be expressed as C_(128)H_(106)N_2O_(11),C_(133)H_(114)N_2O_(12)and C_(137)H_(110)N_2O_(11),respectively.For SFI,the degree of aromaticity and unsaturation is high,the degree of condensation of aromatic rings is high,and nitrogen mainly exists in pyrrole;SFV has more carboxyl functional groups,and nitrogen mainly exists in pyridine.In the process of simulating and constructing the aggregated state structure,the macromolecular structures are continuously adjusted and optimized,and the non-bonding energy is significantly reduced.The simulated density of SFV is 1.25 g/cm^(3),it has high surface area and abundant pore,and its non-bonding energy is-105.59 kJ/mol;The simulated density of SFI is 1.35g/cm^(3),its aggregated state structure has a high degree of overlap with the surrounding periodic units,and its non-bonding energy is 2231.39 kJ/mol,the structure is stable,and the intermolecular interaction force is strong;The simulated density of SFC is 1.30 g/cm^(3)and its non-bonding energy is 1567.96 kJ/mol,all between SFV and SFI.

关 键 词：显微组分 分子模型 结构优化 动力学模拟 聚集态结构 

分 类 号：TQ530[化学工程—煤化学工程]