以四丙基溴化铵为模板剂,以乙二胺(EDA)为碱源,采用干胶法制备了TS-1,并在此基础上引入介孔/大孔模板剂蔗糖而制备出多级孔道TS-1.采用X射线衍射、紫外-可见光谱及N2物理吸附-脱附等手段对所得样品进行了表征,并考察了它们催化噻吩(Th)及苯并噻吩(BT)氧化反应的性能.结果表明,随着釜底部n(EDA)/n(H2O)比的降低,TS-1结晶度、骨架Ti含量及其在Th氧化反应中的催化活性均升高.而当以乙胺和正丁胺为碱源时,TS-1难以晶化.所制备的多级孔道TS-1样品具有介孔/大孔孔道,在Th氧化反应中的催化活性高于TS-1;对于BT的氧化,当n(sucrose)/n(SiO2)为0.35时,制备的多级孔道TS-1样品的催化活性最高,BT脱除率可达100％,而TS-1则无催化活性.
参考文献
| [1] | Taramasso M;Perego G;Notari B .[P].US 4 410 501,1983. |
| [2] | Hulea V.;Bousquet J.;Fajula F. .Mild oxidation with H2O2 over Ti-containing molecular sieves - A very efficient method for removing aromatic sulfur compounds from fuels[J].Journal of Catalysis,2001(2):179-186. |
| [3] | Kong L Y;Li G;Wang X S;Wu B .[J].Energy and Fuels,2006,20:896. |
| [4] | 王晓星,李钢,刘丽萍,刘海鸥.以阳离子聚合物为介孔模板合成多级孔 TS-1[J].催化学报,2011(10):1656-1661. |
| [5] | Li S S;Zhang A F;Liu M;Guo X W .[J].Chinese Chemical Letters,2011,22:303. |
| [6] | 刘民,董毅,郭新闻,王祥生.固定床反应器上TS-1催化丙烯环氧化[J].石油学报（石油加工）,2010(05):677-683. |
| [7] | Sooknoi T;Chitranuwatkul V .[J].Journal of Molecular Catalysis A:Chemical,2005,236:220. |
| [8] | Saxena S;Basak J;Hardin N;Dixit R Bhadauria S Dwivedi R Prasad R Soni A Okram G S Gupta A .[J].Chemical Engineering Journal,2007,132:61. |
| [9] | 杨俊霞,姚明恺,赵松,刘月明,吴鹏,何鸣元.钛硅分子筛/H_2O_2体系催化合成丁酮肟的反应行为[J].催化学报,2010(01):95-99. |
| [10] | Thangaraj A;Kumar R;Ratnasamy P .[J].Applied Catalysis,1990,57:L1. |
| [11] | 王丽琴,王祥生,郭新闻,李钢,修景海,刘松.合成TS-1分子筛的结晶动力学及催化性能研究[J].催化学报,2003(02):132-136. |
| [12] | Fan WB;Duan RG;Yokoi T;Wu P;Kubota Y;Tatsumi T .Synthesis, crystallization mechanism, and catalytic properties of titanium-rich TS-1 free of extraframework titanium species[J].Journal of the American Chemical Society,2008(31):10150-10164. |
| [13] | Xu W Y;Dong J X;Li J P;Li J Q,Wu F.[J].Journal of the Chemical Society,Chemical Communications,1990:755. |
| [14] | 张海娇,刘月明,焦正,阮孟财,吴鹏,何鸣元.晶种对TS-1分子筛干胶合成及其催化性能的影响[J].硅酸盐学报,2009(03):453-457. |
| [15] | 柯学斌,徐莉,曾昌凤,张利雄,徐南平.蒸气促进干胶法合成硅胶负载的TS-1纳米晶[J].高等学校化学学报,2007(08):1411-1415. |
| [16] | Ke X B;Xu L;Zeng Ch F;Zhang L X Xu N P .[J].Microporous and Mesoporous Materials,2007,106:68. |
| [17] | Zhou, J.;Hua, Z.;Cui, X.;Ye, Z.;Cui, F.;Shi, J. .Hierarchical mesoporous TS-1 zeolite: A highly active and extraordinarily stable catalyst for the selective oxidation of 2,3,6-trimethylphenol[J].Chemical communications,2010(27):4994-4996. |
| [18] | Naik S P;Chiang A S T;Thompson R W .[J].Journal of Physical Chemistry B,2003,107:7006. |
| [19] | Zhou J;Hua Z;Zhao J;Gao Z Zeng S Shi J .[J].Journal of Materials Chemistry,2010,20:6764. |
| [20] | Kong L Y;Li G;Wang X S .[J].Catalysis Today,2004,93-95:341. |
| [21] | 李钢 .[D].大连:大连理工大学,2000. |
| [22] | Wang X X;Li G;Wang W H;Jin C Z Chcn Y Y .[J].Microporous and Mesoporous Materials,2011,142:494. |
| [23] | Wang W H;Li G;Li W G;Liu L P.[J].Chemical Communications,2011:3529. |
上一张
下一张
上一张
下一张
计量
- 下载量()
- 访问量()
文章评分
- 您的评分：
-
10%
-
20%
-
30%
-
40%
-
50%