摘要
通过离子交换法制备以天冬氨酸(Asp)、组氨酸(His)、甘氨酸(Gly)、色氨酸(Try)为阴离子的氨基酸咪唑离子液体,与H_(2)O_(2)协同深度去除模拟汽油中的二苯并噻吩(DBT)。对合成的氨基酸咪唑离子液体进行了FT-IR、^(1)H NMR表征,并优化氧化脱硫工艺条件。结果表明,与以组氨酸、甘氨酸和色氨酸作为离子液体的阴离子相比,天冬氨酸作为阴离子时,离子液体与H_(2)O_(2)体系的催化萃取脱硫效果最好。通过对反应温度、H_(2)O_(2)/模拟油体积比和反应时间的工艺优化,探讨了[C_(8)mim]Asp和H_(2)O_(2)催化萃取脱硫的效果,最优工艺条件下,脱硫率可达96.5%。[C_(8)mim]Asp离子液体再生循环7次后脱硫率仍能保持在93.7%。对[C_(8)mim]Asp和H_(2)O_(2)协同催化脱硫机理的研究发现,[C_(8)mim]Asp的羧基与双氧水反应成过氧化羧基,将二苯并噻吩氧化成为二苯并噻吩砜,从而达到脱硫的目的。
Amino acid-based imidazole ionic liquid was prepared with aspartic acid(Asp),histidine(His),glycine(Gly)and tryptophan(Try)as anions by ion-exchange method.Dibenzothiophene(DBT)in simulated gasoline was advanced treated by synergistic ionic liquid and H_(2)O_(2).The synthesized amino acid imidazole ionic liquid was characterized by FT-IR and ^(1)H NMR,and the oxidative desulfurization process conditions were optimized.The results showed that,compared with histidine,glycine and tryptophan as the anion of the ionic liquid,when aspartic acid was used as the anion,the catalytic extraction desulfurization effect of the ionic liquid and H_(2)O_(2) system was the best.Through the process optimization of reaction temperature,H_(2)O_(2)/simulated oil volume ratio and reaction time,the extraction desulfurization effect of[C_(8)mim]Asp and H_(2)O_(2) catalytic was discussed.Under the optimal process conditions,the desulfurization rate could reach 96.5%.The desulfurization rate of[C_(8)mim]Asp ionic liquid could remain at 93.7%after 7 regeneration cycles.Through the study of[C_(8)mim]Asp and H_(2)O_(2) synergistic catalytic desulfurization mechanism,it was found that the carboxyl group of[C_(8)mim]Asp reacted with hydrogen peroxide to form carboxyl peroxide,which oxidized dibenzothiophene to dibenzothiophene sulfone,thereby achieving the purpose of desulfurization.
作者
姚培
张怿涵
李恩田
甘银雪
YAO Pei;ZHANG Yi-han;LI En-tian;GAN Yin-xue(School of Chemical and Pharmaceutical Engineering,Changzhou Vocational Institute of Engineering,Changzhou 213164,China;School of Petroleum Engineering,Changzhou University,Changzhou 213000,China)
出处
《化学研究与应用》
CAS
CSCD
北大核心
2021年第10期1956-1963,共8页
Chemical Research and Application
基金
国家自然科学基金项目(21375117)资助
2020年江苏“青蓝工程”教学团队项目资助
江苏省高职院校教师专业带头人高端研修项目资助
江苏省工业和信息化厅项目(苏财工贸(2018)419号)资助
常州工程职业技术学院院级科技创新团队项目(2020)资助
常州市科技支撑计划(社会发展)项目(CE20195007)资助。
关键词
汽油
二苯并噻吩
氨基酸基咪唑离子液体
脱硫
gasoline
dibenzothiophene
amino acid-based imidazole ionic liquids
desulfurization
