铁基磁性离子液体萃取耦合催化氧化燃油深度脱硫  

Deep desulfurization study of fuel oil by Fe-based magnetic ionic liquid extraction coupling catalytic oxidation

作　　者：余文卉 王涛 李谭香凝 王雨婷 栗静文 胡兵 Yu Wenhui;Wang Tao;Li-Tan Xiangning;Wang Yuting;Li Jingwen;Hu Bing(School of Materials and Chemical Engineering,Hubei University of Technology,Wuhan,Hubei 430068)

机构地区：[1]湖北工业大学材料与化学工程学院,湖北省武汉市430068

出　　处：《炼油技术与工程》2022年第1期16-21,共6页Petroleum Refinery Engineering

基　　金：湖北省自然科学基金项目(2013CKB032);湖北工业大学博士基金项目(0701);湖北省高校创新创业教育改革专项(019-12030);大学生创新创业训练项目(201810500025)。

摘　　要：以1,8-二氮杂二环[5.4.0]壬-7-烯(DBU)为阳离子,利用两步合成法制备了铁基的磁性离子液体(MIL)[C_(4)DBU]Cl/2FeCl_(3),将其作为一种高效的催化剂和萃取剂用于萃取-催化氧化脱硫,氧化剂选用H_(2)O_(2),实现了对噻吩类硫化物的深度脱除。使用红外光谱仪、紫外-可见吸收光谱仪和振动样品磁强计对[C_(4)DBU]Cl/2FeCl_(3)进行表征,采用高效液相色谱法对脱硫产率进行检测。考察了不同参数下该MIL对模拟油中硫化物的脱除效果,优化了反应条件,提出了可能的脱硫机理。结果表明,在反应温度为60℃、反应时间为100 min,[C_(4)DBU]Cl/2FeCl_(3)用量为1.0 g、氧硫比(摩尔比)为5的条件下,[C_(4)DBU]Cl/2FeCl_(3)对二苯并噻吩脱除率最高,达到了98.38%。各种硫化物的脱除效果为二苯并噻吩>4,6-二甲基二苯并噻吩>苯并噻吩>噻吩。在附加磁场的辅助下,可实现[C_(4)DBU]Cl/2FeCl_(3)与油相的高效分离;[C_(4)DBU]Cl/2FeCl_(3)循环使用6次后,其脱硫性能未明显降低。A novel Fe-based magnetic ionic liquid(MIL)[C_(4)DBU]Cl/2FeCl_(3)is synthesized by two-step method.As an efficient catalyst and extractant,MIL is used in the extractive coupled catalytic oxidative desulfurization(ECODS)system with H_(2)O_(2)as oxidant to achieve the deep remove of thiophene sulfide.The[C_(4)DBU]Cl/2FeCl_(3)is characterized by FT-IR,UV-Vis and VSM,and the desulfurization yield is detected by high-performance liquid chromatography.The removal performance of MIL for sulfide in simulated oil under different parameters is investigated,the reaction conditions are optimized,and the possible desulfurization mechanism is proposed.The results show that under the conditions:reaction temperature is 60℃,reaction time is 100 min,[C_(4)DBU]Cl/2FeCl_(3)dosage is 1.0 g and oxygen sulfur molar ratio is 5,the removal rate of DBT is the highest,reaches 98.38%.The order of selectivity for different sulfides is DBT>4,6-dimethyldibenzothiophene(4,6-DMDBT)>benzothiophene(BT)>thiophene(TH).The separation of[C_(4)DBU]Cl/2FeCl_(3)from oil phase can be realized under the action of external magnetic field,and the desulfurization activity of[C_(4)DBU]Cl/2FeCl_(3)has no obvious decrease after being recycled for 6 times.

关 键 词：铁基 磁性离子液体 萃取 催化氧化 燃油 深度脱硫 

分 类 号：TE624.55[石油与天然气工程—油气加工工程]