摘要
采用气相色谱-质谱法(GC/MS)、傅立叶变换红外光谱法(FTIR)和热裂解气质联用仪(Py-GC/MS)等先进表征仪器,探究了不同溶剂(CS_(2)、丙酮和等体积丙酮/CS_(2)混合溶剂)萃取焦油渣(coal tar residue,CTR)后,萃取物的组成特征及萃余物(分别记为RCTR1、RCTR2和RCTR3)的热解产物分布规律。进一步结合热重分析(TG-DTG)与Coats-Redfern动力学模型,探究CTR萃余物热解过程中的潜在反应路径。结果表明:相比于CTR,三种萃余物中苯环类官能团含量减少且具有较好的热稳定性。萃取物中可检测的化合物以芳烃为主,相对含量分别为37.06%、32.86%和33.61%。表明以上三种溶剂可选择性破坏芳环间的π—π作用、强氢键作用和氢键/π—π复合作用,从而削弱分子量较小的多环芳烃(1~5环)与CTR中较大分子(如稠环芳烃,≥6环)间的作用力,使得分子量较小的芳烃类化合物更易被提取。此外,三种萃余物在460°C下的热解产物以烷烃为主,其中RCTR1和RCTR3热解产物中主要是C_(21)~C_(30)的正构烷烃,而RCTR2热解产物中的烷烃以C11~C20为主。最后,动力学模型随温度升高呈现从D1型向F2型的渐进转变,表明萃余物热解过程中存在物理扩散与化学键断裂的协同作用机制。
The compositional characteristics of the extracts and the distribution of pyrolysis products of the extracted residues after the extraction of coal tar residue(CTR)by different solvents(CS_(2),acetone,and equal volume acetone/CS_(2)mixed solvents,be respectively denoted as RCTR1,RCTR2,RCTR3),were investigated using advanced characterization instruments such as gas chromatography-mass spectrometry(GC/MS),Fourier transform infrared spectrometry(FTIR),and pyrolysis gas chromatography/mass spectrometry(Py-GC/MS).By further combining thermogravi-metric analysis(TG-DTG)with the Coats-Redfern kinetic model,the potential reaction pathways during the pyrolysis process of CTR residue were explored.The results show that compared to CTR,the content of benzene ring functional groups in the three extracted decreases(FTIR)and exhibites better thermal stability(TG-DTG).The detectable compounds in the extract are mainly aromatic hydrocarbons(GC/MS),with relative contents of 37.06%,32.86%,and 33.61%,respectively.This indicates that the above three solvents can selectively disrupt theπ—πstacking interactions,strong hydrogen bonding,and hydrogen bonding/π—πrecombination between aromatic rings,thereby weakening the interaction between smaller polycyclic aromatic hydrocarbons(1-5 rings)and larger molecules(such as polycyclic aromatic hydrocarbons,≥6 rings)in CTR,making smaller aromatic compounds easier to extract.In addition,the pyrolysis products of the three residues at 460℃are mainly alkanes(Py-GC/MS),among which the pyrolysis products of RCTR1 and RCTR3 are mainly normal alkanes of C_(21)-C_(30),while the alkanes in the pyrolysis products of RCTR2 are mainly C11-C20.Finally,the kinetic model shows a gradual transition from D1 type to F2 type with increasing tempera-ture,indicating the synergistic mechanism of physical diffusion and chemical bond breaking during the pyrolysis process of the extracted residues.
作者
庞宇翔
王乾月
马亚亚
阚辉
杨伟强
莫文龙
樊星
魏贤勇
丁峰军
袁杰
胡兵
PANG Yuxiang;WANG Qianyue;MA Yaya;KAN Hui;YANG Weiqiang;MO Wenlong;FAN Xing;WEI Xianyong;DING Fengjun;YUAN Jie;HU Bing(State Key Laboratory of Chemistry and Utilization of Carbon Based Energy Resources and Key Laboratory of Coal Clean Conversion and Chemical Engineering Process(Xinjiang Uyghur Autonomous Region),School of Chemical Engineering and Technology,Xinjiang University,830017 Urumqi,China;Xinjiang Career Technical College,833200 Kuitun,China;College of Chemical and Biological Engineering,Shandong University of Science and Technology,266590 Qingdao,China;Yili Xindi New Materials Company Limited,835213 Kekdala,China;Hami Jinyun Energy Technology Company Limited,839000 Hami,China)
出处
《煤炭转化》
北大核心
2026年第1期1-20,共20页
Coal Conversion
基金
新疆维吾尔自治区“天山英才”项目(2024TSYCCX0006)
哈密市科学研究与技术开发计划项目(hmkjjh202307)
兵团第四师科技计划项目(2025GG015)
伊犁州科技计划项目(YYD2023A15)。
关键词
焦油渣
萃取分离
萃余物
多环芳烃
热裂解
tar residue
solvent extraction
residue
polycyclic aromatic hydrocarbons
ther-mol cracking behavior
