摘要
对沥青质进行羧基化、磺化和甲基化反应,从加强与钝化氢键作用两个方面对比研究了不同化学处理对沥青质结构、热稳定性以及沥青质聚集的影响。研究发现:羧基、磺酸基等基团引入沥青质分子后,提高了沥青质分子的极性,增强了分子间的氢键作用,显著促进了沥青质的聚集,并且引入的基团极性越强,促进聚集效果越明显;相反,沥青质中含活泼氢官能团被甲基化后,甲基的引入屏蔽了形成氢键作用的基团,降低了沥青质聚集体形成过程中的氢键数量,从而削弱了沥青质的聚集。实验结果直观地证明了氢键作用对沥青质聚集体形成的影响,揭示了甲基化、羧基化及磺化反应影响沥青质聚集的机理。
The asphaltenes are prone to aggregate and precipitate due to the fused aromatic ring structures with heteroatom functional groups,which leads to a series of problems in the processing and utilization of the heavy oil.However,there is no clear understanding on the intermolecular interaction forces during the asphaltene aggregation process,especially,the role of active hydrogen.For this vein,the carboxylation,methylation and sulfonation reactions were firstly conducted,and the effects of strengthening and weakening hydrogen bonding interactions on asphaltene structure,aggregation and thermal stability were compared.The results show that the introduction of carboxyl and sulfonic group enhances the polarity of asphaltene molecule and strengthens the intermolecular hydrogen bonding interactions,which promotes the asphaltene aggregation.Particularly,the stronger the polarity of the functional groups,the more obvious effects of promoting aggregation.In contrast,after the functional groups containing active hydrogen are methylated,the introduction of methyl group shielded the functional groups forming hydrogen bonding interactions,weakening the hydrogen bonds between the asphaltene molecules,thereby inhibiting the aggregation of asphaltene.The experimental results clearly demonstrate that the impact of hydrogen bonding interactions on the forming of asphaltene supramolecular aggregation and reveal the mechanism of methylation,carboxylation and sulfonation affecting asphaltene aggregation.
作者
韦胜超
姚志林
卞贺
阚爱婷
高智健
朱丽君
夏道宏
WEI Shengchao;YAO Zhilin;BIAN He;KAN Aiting;GAO Zhijian;ZHU Lijun;XIA Daohong(College of Chemical Engineering,State Key Laboratory of Heavy Oil Processing,China University of Petroleum,Qingdao 266580,China)
出处
《石油学报(石油加工)》
EI
CAS
CSCD
北大核心
2021年第3期556-565,共10页
Acta Petrolei Sinica(Petroleum Processing Section)
基金
国家自然科学基金项目(U1662115)资助。
关键词
沥青质
氢键
聚集
甲基化
羧基化
磺化
asphaltene
hydrogen bonding
aggregation
methylation
carboxylation
sulfonation