铁基磁性离子液体萃取耦合催化氧化燃油深度脱硫

炼油技术与工程 ›› 2022, Vol. 52 ›› Issue (1): 16-21.

铁基磁性离子液体萃取耦合催化氧化燃油深度脱硫

余文卉,王涛,李谭香凝,王雨婷,栗静文,胡兵**

湖北工业大学材料与化学工程学院，湖北省武汉市 430068

收稿日期:2021-09-03 出版日期:2022-01-15 发布日期:2022-01-18
通讯作者: 胡兵,教授，硕士生导师，主要从事离子液体的设计、合成及其催化氧化脱硫的研究。E-mail：hbwh04@163.com。
作者简介:余文卉，在读本科生，师从胡兵教授，主要研究方向为离子液体脱硫。联系电话：15072806631，E-mail：1537454338@qq.com

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

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

Received:2021-09-03 Online:2022-01-15 Published:2022-01-18

摘要/Abstract

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)[C₄DBU]Cl/2FeCl₃，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H₂O₂，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[C₄DBU]Cl/2FeCl₃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°C、反应时间为100 min，[C₄DBU]Cl/2FeCl₃用量为1.0 g、氧硫比（摩尔比）为5的条件下，[C₄DBU]Cl/2FeCl₃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[C₄DBU]Cl/2FeCl₃与油相的高效分离；[C₄DBU]Cl/2FeCl₃循环使用6次后，其脱硫性能未明显降低。

关键词: 铁基, 磁性离子液体, 萃取, 催化氧化, 燃油, 深度脱硫

Abstract: A novel Fe-based magnetic ionic liquid (MIL) [C₄DBU]Cl/2FeCl₃ 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 H₂O₂ as oxidant to achieve the deep remove of thiophene sulfide. The [C₄DBU]Cl/2FeCl₃ 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, [C₄DBU]Cl/2FeCl₃ 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 [C₄DBU]Cl/2FeCl₃ from oil phase can be realized under the action of external magnetic field, and the desulfurization activity of [C₄DBU]Cl/2FeCl₃ has no obvious decrease after being recycled for 6 times.

Key words: iron base, magnetic ionic liquid, extraction, catalytic oxidation, fuel oil, deep desulfurization

余文卉, 王涛, 李谭香凝, 王雨婷, 栗静文, 胡兵. 铁基磁性离子液体萃取耦合催化氧化燃油深度脱硫[J]. 炼油技术与工程, 2022, 52(1): 16-21.

Yu Wenhui, Wang Tao, Li Tan Xiangning, Wang Yuting, Li Jingwen, Hu Bing. Deep desulfurization study of fuel oil by Fe-based magnetic ionic liquid extraction coupling catalytic oxidation[J]. Petroleum Refinery Engineering, 2022, 52(1): 16-21.

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