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主管单位 中华人民共和国
工业和信息化部
主办单位 中国材料研究学会
哈尔滨工业大学
主编 苑世剑 国际刊号ISSN 1005-0299 国内刊号CN 23-1345/TB

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引用本文:唐冉帆,栗嘉琪,刘丹,雷家珩.胶晶模板法制备有序大孔HPW/TiO2催化剂及其脱硫性能[J].材料科学与工艺,2024,32(6):35-40.DOI:10.11951/j.issn.1005-0299.20230067.
TANG Ranfan,LI Jiaqi,LIU Dan,LEI Jiaheng.Preparation of ordered macroporous HPW/TiO2 catalyst by colloidal crystal template method and its desulfurization performance[J].Materials Science and Technology,2024,32(6):35-40.DOI:10.11951/j.issn.1005-0299.20230067.
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胶晶模板法制备有序大孔HPW/TiO2催化剂及其脱硫性能
唐冉帆,栗嘉琪,刘丹,雷家珩
(武汉理工大学 化学化工与生命科学学院,武汉 430070)
摘要:
为了有效解决燃油氧化脱硫技术中磷钨酸(HPW)的负载与回收问题,以PS胶晶为模板,通过溶胶-凝胶和干胶450 ℃脱模板方法制备得到一系列负载型有序大孔HPW/TiO2催化剂,并筛选出性能优异的HPW/TiO2-20(HPW负载量为20wt.%),采用扫描电子显微镜(SEM)、X射线粉末衍射仪(XRD)、红外光谱仪(FT-IR)、氮吸附-脱附等现代测试技术对其结构和性能进行表征。结果表明,该催化剂大孔孔径约为250 nm,比表面积约为92.3 m2/g,且大孔排列规整有序,并存在纳米颗粒烧结而形成的介孔,孔径分布约20~45 nm。HPW/TiO2-20的催化氧化实验表明,在反应温度50 ℃、O/S比为4、加入量为0.5 g时,2 h对模拟燃油中二苯并噻吩(DBT)的催化氧化脱硫率为100%,重复使用9次仅下降2.1%。在上述条件下,该催化剂对燃油中BT和4,6-DMDBT的催化氧化脱硫率分别达到94%和92.5%。HPW/TiO2-20中HPW的负载量既保留了催化剂大孔的有序结构,又保留了HPW良好的催化氧化活性,且催化剂回收后的重复次数也明显提高。
关键词:  胶晶模板法  有序大孔材料  催化剂  氧化脱硫  HPW
DOI:10.11951/j.issn.1005-0299.20230067
分类号:TQ426.95
文献标识码:A
基金项目:国家自然科学基金资助项目(21476177).
Preparation of ordered macroporous HPW/TiO2 catalyst by colloidal crystal template method and its desulfurization performance
TANG Ranfan,LI Jiaqi, LIU Dan,LEI Jiaheng
(School of Chemical, Chemical Engineering and Life Sciences,Wuhan University of Technology, Wuhan 430070,China)
Abstract:
In order to effectively address the issue of loading and recovery of phosphotungstic acid (HPW) in fuel oxidation desulfurization technology, a series of loaded ordered macroporous HPW/TiO2 catalysts were prepared by using PS colloidal crystal as template and by the method of sol-gel and dry glue stripping at 450 ℃, HPW/TiO2-20 (HPW load of 20wt.%) with excellent performance was screened out. The structure and performance of catalysts were characterized by SEM, XRD, FT-IR and nitrogen adsorption-desorption. The results show that the catalyst has a macropore size of approximately 250 nm, a specific surface area of approximately 92.3 m2/g, and a well-organized and ordered arrangement of macropopres. The catalyst also exhibits mesopores formed by sintering nanoparticles, and the pore size distribution is about 20 to 45 nm. The catalytic oxidation experiment shows that when the reaction temperature of HPW/TiO2-20 is 50 ℃, the O/S ratio is 4, and the dosage is 0.5 g, the catalytic oxidation desulfurization rate of Dibenzothiophene (DBT) in simulated fuel is 100% in 2 h, and it only decreases by 2.1% after being reused for 9 times. Under the same conditions, the catalytic oxidation desulfurization rates of BT and 4,6-DMDBT in fuel oil reaches 94% and 92.5% respectively. The loading of HPW in HPW/TiO2-20 not only preserves the ordered structure of catalyst macropores, but also maintains the good catalytic oxidation activity of HPW, and the number of repetitions after catalyst recovery is also obviously improved.
Key words:  colloidal template method  ordered macroporous material  catalyst  oxidative desulfurization  HPW

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