摘要
以N-甲基咪唑、溴代正丁烷、磷钨酸为原料制备了1-丁基-3-甲基咪唑磷钨酸离子液体[BMIM]3PW12O40,将其通过超声浸渍法负载于氨基化Fe3O4(Fe3O4—NH2),得到枣糕型结构的[BMIM]3PW12O40/Fe3O4—NH2磁性复合材料,通过FTIR、XRD、XPS、TEM、振动样品磁强计(VSM)、SEM等对其组成、形貌等进行表征。以[BMIM]3PW12O40/Fe3O4—NH2磁性复合材料为催化剂,以H2O2为氧化剂,催化氧化以二苯并噻吩为硫源的正辛烷模拟油样,通过单因素法分别考察了超声时间、H2O2用量、反应温度和催化剂用量等因素对脱硫效果的影响,并初步探讨了[BMIM]3PW12O40/Fe3O4—NH2磁性复合材料催化脱硫机制。结果表明:0.5 g/L[BMIM]3PW12O40/Fe3O4—NH2磁性复合材料超声辅助催化氧化浓度为500 mg/g模拟油样,在323 K下H2O2与二苯并噻吩的摩尔比n(O)∶n(S)为8∶1经超声10 min时,催化脱硫率达到最佳,为88.13%;重复使用5次后,[BMIM]3PW12O40/Fe3O4—NH2磁性复合材料对模拟油样的催化降解率仅下降了2.51%。说明该材料具有良好的催化脱硫性能,并可重复使用。催化机制初步研究表明,活性中心可能为杂多酸阴离子、Fe3O4—NH2和离子液体分别起到载体和协同增容作用。
The 1-butyl-3-methylimidazolium phosphotungstic acid ionic liquid([BMIM]3PW12O40),was prepared from N-methylimidazole,bromo-n-butane and phosphotungstic acid.It was loaded on amino-functionalized Fe3O4(Fe3O4—NH2)by ultrasonic impregnation method.A jujube-like structure[BMIM]3PW12O40/Fe3O4—NH2 magnetic composite was obtained.The[BMIM]3PW12O40/Fe3O4—NH2 magnetic composite was characterized by FTIR,XRD,XPS,TEM,vibrating sample magnetometer(VSM)and SEM.The[BMIM]3PW12O40/Fe3O4—NH2 magnetic composite was used as catalyst for the oxidation of n-octane simulated oil samples with dibenzothiophene(DBT)as sulfur source,via hydrogen peroxide as oxidant.The effects of ultrasonic time,H2O2 usage amount,reactive temperature and catalyst dosage on desulfurization were investigated.The catalytic desulfurization mechanism was discussed.The results showed that the optimized catalytic degradation rate reached 88.13%with the H2O2 to DBT n(O)∶n(S)molar ratio of 8∶1 at 323 K when 0.5 g/L[BMIM]3PW12O40/Fe3O4—NH2 was used for the desulfurization of simulated oil sample with the concentration of dibenzothiophene at 500 mg/g for 10 mins.After reused for 5 times,the catalytic degradation rate decreased only 2.51%,which indicated that the[BMIM]3PW12O40/Fe3O4—NH2 magnetic composite was of good catalytic desulfurization performance and can be reused.The primary desulfurization mechanism study shows that the catalytic active center might be the heteropoly acid anion of the[BMIM]3PW12O40/Fe3O4—NH2 magnetic composite,with the Fe3O4—NH2 serving as a supporter and the ionic liquid as a cooperative compatibilizer,respectively.
作者
胡亚一
陈嘉磊
刘琦
吴冠雄
周贞妊
周靖松
沈昊宇
胡美琴
HU Yayi;CHEN Jialei;LIU Qi;WU Guanxiong;ZHOU Zhenren;ZHOU Jingsong;SHEN Haoyu;HU Meiqin(Ningbo Institute of Technology,Zhejiang University,Ningbo 315100,China)
出处
《复合材料学报》
EI
CAS
CSCD
北大核心
2020年第3期650-661,共12页
Acta Materiae Compositae Sinica
基金
国家自然科学基金(51608479
81502421)
宁波市自然科学基金(2018A610206)
国家级大学生创新创业训练计划项目(201813022009)
宁波市新苗计划项目(甬教基2018-242)
关键词
杂多酸离子液体
磁性复合材料
氧化脱硫
模拟油样
催化性能
heteropoly acid ionic liquids
magnetic composite
oxidative desulfurization
simulated oil
catalytic property