以TiCl4和SiCl4为原料,采用水解和非水水解溶胶-凝胶两种方法制备了一系列不同Ti含量的Ti-Si复氧化物载体,继而用沉积-沉淀法制得载金催化剂.采用X射线衍射、紫外-可见漫反射光谱、N2吸附和高分辨透射电镜对催化剂进行了表征,并考察了催化剂在氢气和氧气存在下的丙烯气相环氧化催化性能研究表明,钛含量在6%～14%范围内时,两种方法制得的Ti-Si复氧化物均为无定形结构,但采用非水水解溶胶-凝胶法制得的载体比表面积较高.以非水水解溶胶-凝胶法制备的钛含量10%的Ti-Si复氧化物为载体得到的载金催化剂表现出较高的活性和选择性,反应60 min时,丙烯转化率为5.7%,240 min后降为3.3%,环氧丙烷的选择性稳定于95%左右.还考察了非水水解溶胶-凝胶的陈化时间和金沉积-沉淀溶液的pH值等对反应结果的影响.
参考文献
| [1] | Cleric M G;Bellussi G;Romano U .[J].Journal of Catalysis,1991,129(01):159. |
| [2] | Xi Z W;Zhou N;Sun Y;Li K L .[J].Science,2001,292(5519):1139. |
| [3] | Geenen P V;Boss H J;Pott G T .[J].Journal of Catalysis,1982,77(02):499. |
| [4] | Nijhuis T.A. .The direct epoxidation of propene by molten salts[J].Applied Catalysis, A. General: An International Journal Devoted to Catalytic Science and Its Applications,2000(2):217-224. |
| [5] | Yoshida H;Tanaka T;Yamamoto M;Funabiki T Yoshida S.[J].Chemistry Communications,1996(18):2125. |
| [6] | Nijhuis TA;Makkee M;Moulijn JA;Weckhuysen BM .The production of propene oxide: Catalytic processes and recent developments[J].Industrial & Engineering Chemistry Research,2006(10):3447-3459. |
| [7] | Haruta M .[J].Catalysis Today,1997,36(01):153. |
| [8] | Uphade BS.;Hayashi T.;Haruta M.;Tsubota S. .Selective oxidation of propylene to propylene oxide or propionaldehyde over Au supported on titanosilicates in the presence of H-2 and O-2[J].Chemistry Letters,1998(12):1277-1278. |
| [9] | Kalvachev Y A;Hayashi T;Tsubota S;Haruta M .[J].Journal of Catalysis,1999,186(01):228. |
| [10] | Uphade BS.;Tsubota S.;Haruta M.;Okumura M. .Effect of physical mixing of CsCl with Au/Ti-MCM-41 on the gas-phase epoxidation of propene using H-2 and O-2: Drastic depression of H-2 consumption[J].Applied Catalysis, A. General: An International Journal Devoted to Catalytic Science and Its Applications,2000(1/2):43-50. |
| [11] | Uphade B S;Yamada Y;Nakamura T;Haruta M .[J].Applied Catalysis A:General,2001,215(1-2):137. |
| [12] | Uphade B S;Akita T;Nakamura T;Haruta M .[J].Journal of Catalysis,2002,209(02):331. |
| [13] | Sinha A K;Seelan S;Tsubota S;Haruta M .[J].Angewandte Chemie International Edition,2004,43(12):1546. |
| [14] | Cumaranatunge L;Delgass WN .Enhancement of Au capture efficiency and activity of Au/TS-1 catalysts for propylene epoxidation[J].Journal of Catalysis,2005(1):38-42. |
| [15] | Chowdhury B;Bravo-Suárez J J;Daté M;Tsubota S,Haruta M .[J].Angewandte Chemie-international Edition In English,2006,45(03):412. |
| [16] | 孙菲菲,钟顺和.丙烯环氧化反应用Au/TiO2系列催化剂的制备与表征[J].催化学报,2003(08):600-604. |
| [17] | 原宇航,祁炜,周兴贵,袁渭康.丙烯气相直接环氧化Au/TiO2催化剂的研究[J].分子催化,2004(03):185-189. |
| [18] | 刘文明,李凤仪,刘芬,罗来涛.在Au/TS-1上原位再生H2O2用于丙烯环氧化反应研究[J].分子催化,2001(06):487-489. |
| [19] | Vioux A .[J].Chemistry of Materials,1997,9(11):2292. |
| [20] | Andrianainarivelo M;Corriu R;Leclercq D;Mutin P H Vioux A .[J].Journal of Materials Chemistry,1996,6(10):1665. |
| [21] | Lafond V;Mutin P H;Vioux A .[J].CHEMISTRY OF MATERIALS,2004,16(25):5380. |
| [22] | Hay JN.;Raval HM. .Solvent-free synthesis of binary inorganic oxides[J].Journal of Materials Chemistry: An Interdisciplinary Journal dealing with Synthesis, Structures, Properties and Applications of Materials, Particulary Those Associated with Advanced Technology,1998(5):1233-1239. |
| [23] | Lafond V;Mutin P H;Vioux A .[J].Journal of Molecular Catalysis A:chemical,2002,81(01):182. |
| [24] | Dai M H;Tang D L;Lin Zh J;Yang H W Yuan Y Zh .[J].Chemistry Letters,2006,35(08):878. |
| [25] | Gu J L;Xiong L M;Shi J L;Hua Z L Zhang L X Li L .[J].Journal of Solid State Chemistry,2006,179(04):1060. |
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%