双亲型Ti/ZSM-5分子筛催化剂的制备及氧化脱硫性能
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摘要
通过使用二苯基硅烷和氨丙基三乙氧基硅烷对Ti/ZSM-5分子筛进行非对称修饰,获得了外侧亲油、内侧亲水的双亲型催化剂材料am-Ti/ZSM-5.修饰过程及后处理过程并未破坏分子筛的骨架结构.样品在不添加萃取剂的情况下,在以H_2O_2为氧化剂的二苯并噻吩(DBT)氧化脱硫(ODS)反应中表现出高催化活性,在35 min内可以实现模拟油中DBT的完全脱除.实验结果表明,分子筛催化剂的双亲型结构使其在极性-非极性混合体系中具有优异的催化性能.
Amphiphilic Ti/ZSM-5 zeolite( am-Ti/ZSM-5) was successfully prepared by asymmetric modification of Ti/ZSM-5 zeolite with diphenylsilane and aminopropyltriethoxysilane. The modification and post-treatment process did not destroy the framework structure of zeolite. The sample showed high catalytic activity in the oxidative desulfurization( ODS) of dibenzothiophene( DBT) using H_2O_2 as the oxidant and without adding the extractant. The complete removal of DBT from the simulated oil can be achieved within 35 min. These results indicate that the unique amphiphilic structure of am-Ti/ZSM-5 makes it have excellent catalytic performance in polar-nonpolar mixtures.
Amphiphilic Ti/ZSM-5 zeolite( am-Ti/ZSM-5) was successfully prepared by asymmetric modification of Ti/ZSM-5 zeolite with diphenylsilane and aminopropyltriethoxysilane. The modification and post-treatment process did not destroy the framework structure of zeolite. The sample showed high catalytic activity in the oxidative desulfurization( ODS) of dibenzothiophene( DBT) using H_2O_2 as the oxidant and without adding the extractant. The complete removal of DBT from the simulated oil can be achieved within 35 min. These results indicate that the unique amphiphilic structure of am-Ti/ZSM-5 makes it have excellent catalytic performance in polar-nonpolar mixtures.
引文
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[2]Dehghan R.,Anbia M.,Fuel Processing Technology,2017,167,99-116
[3]Li S.W.,Li J.R.,Gao Y.,Liang L.L.,Zhang R.L.,Zhao J.S.,Fuel,2017,197,551-561
[4]Palomeque-Santiago J.F.,Lopez-Medina R.,Oviedo-Roa R.,Navarrete-Bolanos J.,Mora-Vallejo R.,Montoya-de L.F.,Martinez-Magadan J.M.J.,Appl.Catal.B:Environ.,2018,236,326-337
[5]Fu J.W.,Guo Y.,Ma W.W.,Ma W.W.,Fu C.,Li L.,Wang H.Y.,Zhang H.,Journal of Materials Science,2018,53(22),15418-15429
[6]Xue F.,Ma R.,Sun Y.D.,Abdukadera A.,Zhang Y.H.,Liu C.J.,Chem.J.Chinese Universities,2015,36(7),1298-1303(薛飞,麻荣,孙亚栋,阿布力米提·阿布都卡德,张永红,刘晨江.高等学校化学学报,2015,36(7),1298-1303)
[7]Du Q.,Guo Y.P.,Wu P.,Microporous and Mesoporous Materials,2018,264,272-280
[8]Zhang T.J.,Chen X.X.,Chen G.R.,Chen M.Y.,Bai R.S.,Jia M.J.,Yu J.H.,Journal of Materials Chemistry A,2018,6(20),9473-9479
[9]Bai R.S.,Sun Q.M.,Song Y.,Wang N.,Zhang T.J.,Wang F.,Zou Y.C.,Feng Z.C.,Miao S.,Yu J.H.,Journal of Materials Chemistry A,2018,6(18),8757-8762
[10]Leng K.Y.,Li X.L.,Ye G.,Du Y.C.,Sun Y.Y.,Xu W.,Catalysis Science&Technology,2016,6(20),7615-7622
[11]Kim T.K.,Yang S.T.,Park D.R.,Song I.K.,Jung K.E.,Ahn W.S.,Top Catal.,2010,53(7-10),470-478
[12]Leng K.Y.,Sun Y.Y.,Zhang X.,Yu M.,Xu W.,Fuel,2016,174,9-16
[13]Chen H.Y.,Yang M.F.,Shang W.J.,Tong Y.,Liu B.Y.,Han X.L.,Zhang J.B.,Hao Q.Q.,Sun M.,Ma X.X.,Industrial&Engineering Chemistry Research,2018,57(32),10956-10966
[14]Li D.Z.,Zhao B.,Long Y.,Yang G.Q.,Tung C.H.,Song K.,RSC Adv.,2015,5(91),74362-74365
[15]Leng Y.,Zhao J.W.,Jiang P.P.,Wang J.,ACS Applied Materials&Interfaces,2014,6(8),5947-5954
[16]Leng Y.,Wu J.H.,Jiang P.P.,Wang J.,Catalysis Science&Technology,2014,4(5),1293-1300
[17]Jing L.,Shi J.,Zhang F.M.,Zhong Y.J.,Zhu W.D.,Industrial&Engineering Chemistry Research,2013,52(30),10095-10104
[18]Hu D.L.,Zhang D.Y.,Zhang C.L.,Ding S.J.,Yang Z.Z.,Chem.J.Chinese Universities,2012,33(10),2345-2350(胡大林,张东阳,张成亮,丁书江,杨振忠.高等学校化学学报,2012,33(10),2345-2350)
[19]Nisar A.,Zhuang J.,Wang X.,Advanced Materials,2011,23(9),1130-1135
[20]Ding S.J.,Liu B.,Zhang C.L.,Wu Y.,Xu H.F.,Qu X.Z.,Liu J.G.,Yang Z.Z.,Journal of Materials Chemistry,2009,19(21),3443-3448
[21]Nakao R.,Rhee H.,Uozumi Y.,Org.Lett.,2005,7,163-165
[22]Hamasaka G.,Muto T.,Uozumi Y.,Angew.Chem.Int.Ed.,2011,50,4876-4878
[23]Zou H.B.,Wang R.W.,Dai J.Y.,Wang Y.,Wang X.,Zhang Z.T.,Qiu S.L.,Chemical Communications,2015,51,14601-14604
[24]Li J.,Wu H.S.,Yang L.N.,Ma B.,China Petroleum Processing&Petrochemical Technology,2016,18(2),33-42
[25]Peng B.L.,Zhang Z.T.,Wang P.M.,Wang R.W.,Ding B.,Luo J.H.,He L.P.,Wang Y.,Geng X.F.,Preparation of Amphiphilic Zeolite with Lipophilic Groups on the Outer Surface and Hydrophilic Groups on the Inner Surface,CN108298557A,2018-07-20(彭宝亮,张宗弢,王平美,王润伟,丁彬,罗健辉,贺丽鹏,王影,耿向飞.外侧含有亲油基团内侧含有亲水基团的双亲分子筛及其制备方法,CN108298557A,2018-07-20)
[26]Groen J.C.,Bach T.,Ziese U.,Donk A.M.P.,Jong K.P.,Moulijn J.A.,Perez-Ramirez J.,Journal of the American Chemical Society,2005,127(31),10792-10793
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[28]Sun C.Y.,Wang Y.,Wang R.W.,Qiu S.L.,Zhang Z.T.,Chem.J.Chinese Universities,2017,38(8),1431-1435(孙传胤,王影,王润伟,裘式纶,张宗弢.高等学校化学学报,2017,38(8),1431-1435)
[29]Lv Q.,Li G.,Sun H.,Fuel,2014,130,70-75
[30]Serrano D.P.,Sanz R.,Pizarro P.,Moreno I.,Medina S.,Applied Catalysis A:General,2012,435,32-42
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