非均相类Fenton体系催化氧化脱除模拟汽油中噻吩

石油炼制与化工 ›› 2015, Vol. 46 ›› Issue (4): 16-21.

非均相类Fenton体系催化氧化脱除模拟汽油中噻吩

田亚杰,姚月,支岩辉,吕树祥

天津科技大学材料科学与化学工程学院

收稿日期:2014-10-09 修回日期:2014-12-01 出版日期:2015-04-12 发布日期:2015-03-20
通讯作者: 吕树祥 E-mail:lshx@tust.edu.cn
基金资助:
天津市应用基础与前沿技术研究计划重点项目;大学生创新创业训练计划

NOVEL APPROACH FOR OXIDATIVE DESULFURIZATION OF THIOPHENE IN MODEL GASOLINE WITH HETEROGENOUS FENTON SYSTEM

Received:2014-10-09 Revised:2014-12-01 Online:2015-04-12 Published:2015-03-20

摘要/Abstract

摘要： 以Fe元素作为主要金属组分，γ-Al2O3为载体，制备负载不同第二金属组分的XO-Fe2O3/γ-Al2O3双金属催化剂(X为La，Ce，Co，Cu) ，采用XRD、SEM、氮气吸附-脱附等手段对催化剂进行表征；以H2O2为氧化剂，噻吩为模型硫化物，将含噻吩的正辛烷作为模拟汽油，研究非均相类Fenton试剂催化氧化脱硫过程，考察催化剂中金属元素种类、n(H2O2)/n(S)、催化剂用量等对氧化脱除噻吩效果的影响。结果表明：Fe2O3/γ-Al2O3具有一定的催化H2O2氧化脱硫活性，非均相类Fenton试剂可以催化H2O2产生?OH；在Fe2O3/γ-Al2O3中掺杂少量其它金属可以改变其催化活性，其中以加入Cu后的催化剂活性最高，Cu起到了催化剂助剂的作用，催化剂呈现明显的介孔性质；对于30mL噻吩质量分数为526 μg/g的模拟汽油，以CuO-Fe2O3/γ-Al2O3为催化剂，在反应温度333 K、催化剂加入量0.2 g、n(H2O2)/n(S)=7.40、反应时间120 min的条件下，噻吩脱除率达到95.3%以上，有效硫质量分数降至9.4 μg/g，达到超深度脱硫效果。

Abstract: The XO-Fe2O3/γ-Al2O3 (X: La, Ce, Co and Cu) catalysts in Fenton system (catalyst + oxidant H2O2) were prepared and characterized by XRD, SEM and BET techniques. The oxidation removal of thiophene in model gasoline (n-octane solution) with heterogeneous Fenton system was tested to investigate the effect of kind of metals, n(H2O2)/n(S) and catalyst dosage. The characterized results demonstrate that the catalysts have meso-pore structures. The desulfurization tests indicate that the catalyst Fe2O3/γ-Al2O3 promotes the production of ?OH radical from H2O2 to oxidize the thiophene, thus improves the removal of thiophene. The addition of second metal can improve the catalytic activity of Fe2O3/γ-Al2O3. Among of them, Cu is the best one. Under the conditions of temperature 333K, catalyst dosage 0.2g, n(H2O2)/n(S)=7.40 and reaction time 120 min, 95.3% of thiophene can be removed. The S content in product is reduced to 9.4μg/g, which meet the ultra-deep desulfurization object.

田亚杰姚月支岩辉吕树祥. 非均相类Fenton体系催化氧化脱除模拟汽油中噻吩[J]. 石油炼制与化工, 2015, 46(4): 16-21.