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机构地区:[1]天津科技大学化工与材料学院,天津300457
出 处:《石油学报(石油加工)》2017年第1期71-78,共8页Acta Petrolei Sinica(Petroleum Processing Section)
基 金:天津市应用基础与前沿技术研究计划重点项目(14JCZDJC40600);大学生创新创业训练计划项目(201410057043)资助
摘 要:以碳纳米管为载体(CNTs),采用浸渍法制备了新型催化剂H_5PMo_(10)V_2O_(40)/CNTs,并对所制备催化剂进行TEM、XRD、FT-IR和TG表征;以二苯并噻吩的正十二烷溶液为模拟油,氧气为氧化剂,评价H_5PMo_(10)V_2O_(40)/CNTs的催化氧化脱硫活性;考察了反应温度、反应时间、氧气分压和催化剂用量对该氧化脱硫反应的影响。结果表明,负载的H_5PMo_(10)V_2O_(40)依然保持了原有的Keggin结构,且H_5PMo_(10)V_2O_(40)/CNTs具有较高催化模拟油氧化脱硫活性;在反应温度125℃、反应时间4h、氧气分压0.3 MPa、模拟油15mL、催化剂用量0.02g时,二苯并噻吩的脱除率达到99.3%,催化剂重复使用5次,催化剂活性没有明显的下降。讨论了氧气为氧化剂H_5PMo_(10)V_2O_(40)/CNTs催化氧化脱硫的可能反应机理。A new oxidation catalyst H_5PMo_(10)V_2O_(40)/CNTs was prepared by impregnation method,and characterized by TEM,XRD,FT-IR and TG.The performance of the catalyst for the oxidative desulfurization of model oil composed of dibenzothiophene(DBT)and n-dodecane was investigated by O_2 as oxidant.The effects of reaction temperature,time,oxygen partial pressure and catalyst dosage on the removal of DBT were studied.The results indicated that the Keggin structure of H_5PMo_(10)V_2O_(40) was remained after supported on CNTs and the H5PMo10 V2O_40/CNTs catalyst showed high activity on oxidative desulfurization with O_2.The desulfurization rate of 99.3% was obtained at reaction temperature 125℃,reaction time 4h,0.3 MPa O_2 partial pressure,15 mL model oil and 0.02 g H_5PMo_(10)V_2O_(40)/CNTs.There was no obvious decrease on catalytic activity after five times recycle of the catalyst.Meanwhile,the possible reaction mechanism on oxidation desulfurization with O_2 was discussed.
关 键 词:氧气 碳纳米管(CNTs) 磷钼钒杂多酸 氧化脱硫
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