化工进展2026，Vol.45Issue(8)：4562-4573,12.DOI:10.16085/j.issn.1000-6613.2025-1451
传统溶剂分离含氮化合物的分子识别与萃取剂优选
Molecular recognition and extractant optimization for traditional solvent separation of nitrogen-containing compounds
摘要
Abstract
Nitrogen-containing compounds,which are ubiquitous in coal tar and diesel streams,represent species with both environmental concerns and high-value potential.Conventional hydrodenitrogenation is limited by high energy consumption and the degradation of valuable heterocyclic structures.To address these limitations,this study focused on economically viable and scalable traditional solvent systems for nitrogen removal.Using the COSMO-RS simulation,we conducted systematic solvent pre-screening and mechanistic analysis.Infinite dilution activity coefficients were employed to quantify solubility,selectivity,and a comprehensive performance index,thereby allowing the separation behaviors and driving forces to be elucidated.The results revealed that hydrogen-bonding interactions governed the separation efficiency.Among amide solvents,N,N-dimethylformamide(DMF)showed the best performance for basic nitrogen compounds,whereas N-methyl-2-pyrrolidone(NMP)performed optimally for non-basic species.In acidic media,sulfuric acid(H2SO4)outperformed hydrochloric acid(HCl)for both substrate types.Molecular surface charge distribution analysis indicateed that the key mechanisms involveed directed N-H…O=C hydrogen bonding and an enhanced mass-transfer process facilitated by a protonation-coupled hydrogen-bond network.Based on these insights,practical solvent-selection guidelines were proposed:Solvents with well-defined donor-acceptor sites,strong interaction capability,and the ability to form stable hydrogen-bonding networks should be prioritized.This study provided a quantitative basis for rapid solvent screening and formulation in nitrogen-containing systems and offered a practical pathway toward molecular-structure-preserving separation and valorization of heterocyclic nitrogen compounds.关键词
传统溶剂/含氮化合物/氢键/溶剂筛选/分离Key words
traditional solvent/nitrogen-containing compounds/hydrogen bond/solvent screening/separation分类
化学化工引用本文复制引用
齐宇宁,贝鹏志,姚辉,高晓露,邓莉莉,刘红晶,徐兴堂..传统溶剂分离含氮化合物的分子识别与萃取剂优选[J].化工进展,2026,45(8):4562-4573,12.基金项目
辽宁省科技计划联合计划(2024-BSLH-201,2024JH2/102600215) （2024-BSLH-201,2024JH2/102600215）
省部共建煤基能源清洁高效利用国家重点实验室开放基金(MJNYSKL202509) （MJNYSKL202509）
辽宁省教育厅基本科研项目(LJ212510142013) （LJ212510142013）
国家自然科学基金青年基金(22308241) （22308241）
山西省基础研究计划(自由探索类)青年项目(202303021212037). （自由探索类）
