中文关键词:沥青质,密度泛函理论,Mulliken重叠布居,分子间相互作用,溶剂化效应 英文关键词:asphaltene, density functional theory, Mulliken overlap, intermolecular interaction, solvation effects 基金项目:陕西省教育厅自然科学研究计划

作者	单位	E-mail
赵理达	西安医学院药学院	15102988708@163.com
颜欢	宜宾天原集团海丰和锐有限公司
李冰	西安医学院药学院
闫平	西安医学院药学院
管玉雷	西北大学化工学院	guanyl@nwu.edu.cn

摘要点击次数:1297 全文下载次数:0 中文摘要: 重质油中沥青质组分易发生聚沉形成团簇，严重影响重质油的加工和利用效率，但目前对于沥青质聚沉的研究较少，其机理尚不明确。本文采用理论计算对沥青质杂环模型分子间相互作用和溶剂化效应进行研究，以此为重质油沥青质聚沉现象的研究及聚沉抑制剂的研发提供一定的数据和理论支持。（1）在M062X/6-31G(d)水平上，计算得到了11种由沥青质杂环分子片段组成的二元体系的全优化稳定构型，讨论分析了构型的几何结构、NBO电荷、Mulliken重叠布居、相互作用能和分子轨道能，得到了最稳定的两种构型。（2）在B3LYP/6-31G(d)水平上，运用SMD模型对沥青质大分子在13种溶剂中进行溶剂化效应的建模和理论计算，通过对静电溶剂化自由能（ΔGelec）、非静电溶剂化自由能（ΔGnonelec）、总溶剂化自由能（ΔGsolv）的分析可知，沥青质溶解性大小的关键在于溶剂对它的远程静电作用的大小。 英文摘要: Asphaltene components in heavy oil are prone to coalesce to form clusters, which seriously affect the processing and utilization efficiency of heavy oil. However, there are few studies on the coagulation of asphaltene, and its mechanism is not clear. In this paper, theoretical calculations are used to study the intermolecular interaction and solvation effects of asphaltene heterocycle models. It provides some data and theoretical support for the study of the coagulation of heavy oil and the development of coagulation inhibitors. (1)By using the density functional theory (DFT), in the M062X / 6-31G (d) level, we can get 11 kinds of stable configurations of binary mixture systems composed of the fragments of asphaltene - heterocyclic molecules (dibenzofuran, acridine and carbazole), The geometries of stable configurations, NBO (natural bonding orbital) charges, Mulliken overlap, interaction energies and molecular orbital energies are analyzed, and the most stable two configurations are obtained. (2)The modeling and theoretical calculation of the solvation effect of asphaltene macromolecules in 13 solvents were carried out in the B3LYP/6-31G (d) level with the SMD model. Through the analysis of the electrostatic solvation free energy(ΔGelec), non-electrostatic solvation free energy(ΔGnonelec) and solvation free energy(ΔGsolv), We can conclude that the key to the solubility of asphaltene lies in the size of the long-range electrostatic effect. 查看全文查看/发表评论下载PDF阅读器 相关附件：版权转让声明书 -->