离子液体负载的金属框架Py/MOF-199的制备及其吸附脱硫性能  

Preparation of ionic liquid supported metal-organic framework Py/MOF-199 and its adsorption desulfurization performance

作　　者：巩明月 李晓娟[1] 张梅[1,2] 宋华[1,2] 赫英明[3] GONG Ming-yue;LI Xiao-juan;ZHANG Mei;SONG Hua;HE Ying-ming(College of Chemistry&Chemical Engineering,Northeast Petroleum University,Daqing 163318,China;Provincial Key Laboratory of Oil&Gas Chemical Technology,Northeast Petroleum University,Daqing 163318,China;Research Institute of Exploration and Development of Daqing Oilfield Company Ltd,Daqing 163000,China)

机构地区：[1]东北石油大学化学化工学院,黑龙江大庆163318 [2]东北石油大学石油与天然气化工省重点实验室,黑龙江大庆163318 [3]大庆油田有限责任公司勘探开发研究院,黑龙江大庆163000

出　　处：《燃料化学学报》2018年第10期1175-1183,共9页Journal of Fuel Chemistry and Technology

基　　金：国家自然科学基金(21276048);黑龙江省自然科学基金(ZD201201);黑龙江省教育厅面上项目(12541060)资助~~

摘　　要：制备了金属框架MOF-199(Cu-BTC),并将[Hnmp][H2PO4]离子液体负载到MOF-199上合成了离子液体负载的金属框架Py/MOF-199。对吸附剂进行了X射线衍射、红外光谱、扫描电镜、比表面积表征。考察了MOF-199预处理条件、离子液体负载方式、负载量、负载温度、负载时间对噻吩吸附脱除性能的影响,通过正交实验优化了吸附剂的制备条件和吸附脱硫条件。结果表明,离子液体改性得到的Py/MOF-199保持了MOF-199的规则的八面体结构。Py/MOF-199的适宜制备条件为:采用二氯甲烷索氏提取并真空干燥法进行预处理MOF-199后,再用溶剂热法负载[Hnmp][H_2PO_4],负载温度为50℃,负载时间为8 h,负载量为7%。各因素对吸附剂脱硫性能影响大小顺序为:负载温度>负载时间>离子液体负载量。适宜Py/M OF-199吸附脱硫条件为:模拟油为10 mL,吸附剂用量0.2 g,吸附温度70℃,吸附时间1 h。在此条件下,噻吩脱除率可达到96.7%。MOF-199(Cu-BTC)was prepared and the ionic liquid supported MOF-199 adsorbents(Py/MOF-199)were successfully obtained via fixing ionic liquid[Hnmp][H 2 PO 4]onto the MOF-199.Adsorbents were characterized via XRD,FT-IR,SEM,and BET methods.The effects of pretreatment conditions of MOF-199,ionic liquid loading method,ionic liquid content,loading temperature and time on adsorptive removal performance of thiophene were studied.The preparation conditions of Py/MOF-199 adsorbent were optimized via orthogonal experiment,and the desulfurization conditions were also optimized.The results show that after the introduction of[Hnmp][H 2 PO 4]the regular octahedron structure of MOF-199 of Py/MOF-199 was maintained unchanged and the average pore diameter was increased.The optimal preparation conditions of Py/MOF-199 adsorbent are pretreating MOF-199 with Soxhlet extraction and drying in vacuum,then loading[Hnmp][H 2 PO 4]using solvothermal method,loading temperature of 50℃,loading time of 8 h,ionic liquid content of 7%.The influence of preparation factors on the desulfurization performance of adsorbent is in order:loading temperature>loading time>ionic liquid content.The optimal desulfurization conditions are model oil of 10 mL,Py/MOF-199 dosage of 0.2 g,adsorption under 70℃for 1 h.Under these conditions,the thiophene desulfurization rate over Py/MOF-199 reached 96.7%.

关 键 词：吸附脱硫 离子液体 Py/MOF-199 噻吩(TP) 

分 类 号：O643.361[理学—物理化学]