摘要
在500℃下对类煤模型化合物1-萘甲醇与同位素示踪剂的共热解进行了机理研究。利用Py-GC/MS进行快速产物检测,同时联合自由基捕获剂来推断自由基的反应过程。结果表明,在500℃和0.2 min的条件下,1-萘甲醇的热解产物相对单一,但是自由基反应的引发、交换和湮灭极其快速,现有检测方法是对某一时间节点的平衡反应结果的分析。通过D_(2)O和H_(2)^(18)O同位素示踪,成功捕获到了自由基交换后的D取代产物和^(18)O取代产物。揭示了1-萘甲醇经过1-萘甲基自由基转化为1-萘甲醛的转化过程,发现萘环上的取代基在1-萘甲醇的热解过程中起着重要作用。同时对自由基及产物进行了定性和半定量分析,发现在加入自由基捕获剂后产物的丰度较之前降低了一个数量级,说明了自由基捕获剂抑制了产物的生成。
In this study,the mechanism of co-pyrolysis of the coal-like model compound 1-naphthyl methanol and isotope tracer was studied at 500℃.The pyrolysis process is carried out by using a thermal cracker,and then mass spectrometry is used to detect the product to infer the reaction and change behavior of free radicals.The results show that the free radical reaction dominates the pyrolysis process at 500℃,and this behavior is more pronounced.Through the isotope labeling method and spin trapping technology,the hydrogen radicals were successfully captured.The transformation process of the conversion of 1-naphthyl methanol to 1-naphthaldehyde is revealed,and it is found that the substituents on the benzene ring play an important role in the thermal process of 1-naphthyl methanol.At the same time,qualitative and semi-quantitative analysis of free radicals and products was carried out,and it was found that the abundance of products after the addition of free radical traps was an order of magnitude lower than before,indicating that the free radical traps inhibited the formation of products.
作者
罗紫藤
周秋成
王雨露
席引尚
周安宁
陈福欣
LUO Ziteng;ZHOU Qiucheng;WANG Yulu;XI Yinshang;ZHOU Anning;CHEN Fuxin(Department of Chemistry and Chemical Engineering,Xi’an University of Science&Technology,Xi’an 710054,Shaanxi,China;Shaanxi Jintai Chlor-alkali Shenmu Chemical Co.,Ltd.,Yulin 719300,Shaanxi,China)
出处
《化工学报》
EI
CAS
CSCD
北大核心
2022年第2期914-922,共9页
CIESC Journal
基金
国家自然科学基金项目(31760016)
陕西省重点研发项目(2019GY-138,2020GY-236)
自然资源部煤炭资源勘查与综合利用重点实验室开放课题(KF2020-9)。
