以有机金属二氯二茂钛作为Ti源,以HMS作为载体,采用嫁接法合成了一系列不同载Ti量的Ti-HMS.HMS的模板剂通过600 ℃焙烧或乙醇萃取紧随400 ℃焙烧脱除.合成Ti-HMS用热重-差热分析、 X射线粉末衍射、 N2吸附-脱附等温线、漫反射紫外可见光谱和傅里叶变换红外光谱进行了表征,并在温和反应条件下考察了Ti-HMS对过氧化氢液相氧化对叔丁基甲苯的催化性能. 结果表明,对载体采取乙醇萃取和低温焙烧的方法脱除模板剂有利于保护嫁接反应所需要的羟基; 随着载Ti量增加,骨架Ti逐渐减少,四配位的骨架Ti在对叔丁基甲苯氧化反应中具有催化活性; 非骨架Ti导致催化活性降低.在实验条件下,对叔丁基甲苯的转化率可达9.3%, 对叔丁基苯甲醛的选择性为100%.
参考文献
| [1] | Arends I W C E;Sheldon R A .[J].Applied Catalysis A:General,2001,212(1-2):175. |
| [2] | Blasco T.;Navarro MT.;Pariente JP.;Corma A. .SYNTHESIS, CHARACTERIZATION, AND CATALYTIC ACTIVITY OF TI-MCM-41 STRUCTURES[J].Journal of Catalysis,1995(1):65-74. |
| [3] | Rios LA;Weckes P;Schuster H;Hoelderich WF .Mesoporous and amorphous Ti-silicas on the epoxidation of vegetable oils[J].Journal of Catalysis,2005(1):19-26. |
| [4] | Eimer GA;Casuscelli SG;Ghione GE;Crivello ME;Herrero ER .Synthesis, characterization and selective oxidation properties of Ti-containing mesoporous catalysts[J].Applied Catalysis, A. General: An International Journal Devoted to Catalytic Science and Its Applications,2006(0):232-242. |
| [5] | Tanev P T;Chibwe M;Pinnavaia T J .[J].Nature,1994,368(6469):321. |
| [6] | Lapisardi G;Chiker F;Launay F;Nogier J P, Bonardet J L .[J].Catalysis Communications,2004,5(06):277. |
| [7] | 吕爱霞,伏再辉,尹笃林,徐友志,明杜鹃,阳清,银董红.HMS和NaY固载酒石酸钛配合物的研究[J].物理化学学报,2004(07):749-754. |
| [8] | 伏再辉,尹笃林,赵伟,毛丽秋,张鲁西,银董红,张友玉.中孔载体上组装Ti催化活性中心的研究Ⅰ-钛配合物在中孔HMS载体上的组装[J].无机化学学报,2000(04):624-630. |
| [9] | Aronson B J;Blanford C F;Stein A .[J].Chemistry of Materials,1997,9(12):2842. |
| [10] | Maschmeyer T;Rey F;Sankar G;Thomas J M .[J].Nature,1995,378(6553):159. |
| [11] | Calleja G;van Grieken R;García R;Melero J A, Iglesias J .[J].Journal of Molecular Catalysis A:Chemical,2002,182/183:215. |
| [12] | Ahn W S;Lee D H;Kim T J;Kim J H, Seo G, Ryoo R .[J].Applied Catalysis A:General,1999,181(01):39. |
| [13] | Marchese L;Gianotti E;Dellarocca V;Maschmeyer T, Rey F, Coluccia S, Thomas J M .[J].Chemical Physics and Physical Chemistry,1999,1(04):585. |
| [14] | Sensarma S;Bouh A O;Scott S L;Alper H .[J].Journal of Molecular Catalysis A:Chemical,2003,203(1-2):145. |
| [15] | Wang S;Yang Q;Wu Z;Li M, Lu J, Tan Z, Li C .[J].Journal of Molecular Catalysis A:Chemical,2001,172(1-2):219. |
| [16] | Brutchey RL;Ruddy DA;Andersen LK;Tilley TD .Influence of surface modification of Ti-SBA15 catalysts on the epoxidation mechanism for cyclohexene with aqueous hydrogen peroxide[J].Langmuir: The ACS Journal of Surfaces and Colloids,2005(21):9576-9583. |
| [17] | Zhang W Zh;Pauly T R;Pinnavaia T J .[J].Chemistry of Materials,1997,9(11):2491. |
| [18] | Pauly TR.;Pinnavaia TJ. .Pore size modification of mesoporous HMS molecular sieve silicas with wormhole framework structures[J].Chemistry of Materials,2001(3):987-993. |
| [19] | Liu Y;Kim S S;Pinnavaia T J .[J].Journal of Catalysis,2004,225(02):381. |
| [20] | Tanev P T;Pinnavaia T J .[J].Chemistry of Materials,1996,8(08):2068. |
| [21] | Oldroyd R D;Sankar G;Thomas J M;Oezkaya D .[J].Journal of Physical Chemistry B,1998,102(11):1849. |
| [22] | Pauly T R;Liu Y;Pinnavaia T J;Billinge S J L, Rieker T P .[J].Journal of the American Chemical Society,1999,121(38):8835. |
| [23] | Gregg S J;Sing K S W.Adsorption,Surface Area and Porosity[M].New York:Academic Press,Inc,1982:286. |
| [24] | 李钢,王祥生,金长子,李桂民.Ti-HMS分子筛的合成与表征[J].催化学报,2004(04):315-318. |
| [25] | 于健强,李灿,许磊,李美俊,辛勤,刘中民.以硅溶胶和三氯化钛为原料合成Ti-MCM-41分子筛Ⅰ.Ti-MCM-41分子筛的合成[J].催化学报,2001(03):267-270. |
| [26] | Zhang W Zh;Froba M;Wang J L;Tanev P T, Wong J, Pinnavaia T J .[J].Journal of the American Chemical Society,1996,118(38):9164. |
| [27] | Damyanova S;Dimitrov L;Mariscal R;Fierro J L G, Petrov L, Sobrados I .[J].Applied Catalysis A:General,2003,256(1-2):183. |
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%