以无定形高比表面积水合钛酸(H2Ti2O5·xH2O)为载体,采用等体积浸渍法制备了新型晶须状介孔SO42-/TiO2固体酸催化剂,利用X射线衍射、N2吸附-脱附、扫描电镜、红外光谱、热重和氨程序升温脱附等技术考察了催化剂的结构特征和表面酸性及其对乙酸与正丁醇液相酯化反应的催化活性.结果表明,SO42-/TiO2同体酸催化剂不仅具有纳米级晶粒、晶须状形貌、高比表面积和介孔结构,还保持了完善的锐钛矿晶型、较强的酸性和较高的热稳定性;当焙烧温度高于500℃时,催化剂表面结合的SO42-逐渐流失,酸中心数逐渐减少.在m(催化剂)=0.2 g、n(正丁醇)/n(乙酸)=1.5和反应时间3 h条件下,500℃焙烧的催化剂活性最高,正丁醇转化率达94%,乙酸正丁酯选择性为100%,且催化性能和分离沉降性能均优于SO42-/P25催化剂.
参考文献
| [1] | Luo Z Y;Wang S;Liao Y F;Zhou J S Gu Y L Cen K F .[J].Biomass and Bioenergy,2004,26(05):455. |
| [2] | Yadav G D;Pathre G S .[J].Microporous and Mesoporous Materials,2006,89(1-3):16. |
| [3] | 郑仲,杨祝红,刘畅,冯新,陆小华.氧化钛基固体酸催化剂的研究进展[J].化学通报,2003(08):574-574. |
| [4] | 杜迎春,吴彩金.固体酸催化剂上酯化反应研究进展[J].工业催化,2003(05):30-33. |
| [5] | 赵玉宝,曾燕伟,陶克毅.SO2-4/ZrO2的相结构和超强酸性及其对丁烷异构化反应的催化活性[J].催化学报,2002(02):168-172. |
| [6] | 张琦,常杰,王铁军,徐莹.固体酸催化剂SO2-4/SiO2-TiO2的制备及其催化酯化性能[J].催化学报,2006(11):1033-1038. |
| [7] | Yin H L;Tan Z Y;Liao Y T;Feng Y J .[J].Journal of Environmental Radioactivity,2006,87(02):227. |
| [8] | Wang J;Yang P P;Fan M Q;Yu W Jing X Y Zhang M L Duan X .[J].Materials Letters,2007,61(11-12):2235. |
| [9] | Jiang Y X;Chen X M;Mo Y F;Tong Z E .[J].Journal of Molecular Catalysis A:Chemical,2004,213(02):231. |
| [10] | Hagfeldt A;Gratzel M .[J].Chemical Reviews,1995,95(01):49. |
| [11] | Rolison D R .[J].Science,2003,299(5613):1698. |
| [12] | He M;Lu XH;Feng X;Yu L;Yang ZH .A simple approach to mesoporous fibrous titania from potassium dititanate[J].Chemical communications,2004(19):2202-2203. |
| [13] | 孟庆浩,李啸风,杜志强,殷学锋.高长径比钛酸钾晶须的合成及其结构研究[J].化学通报,2002(07):482-484. |
| [14] | 杨祝红,暴宁钟,刘畅,冯新,谢敬伟,吉晓燕,陆小华.TiO2纤维的制备及其光催化活性研究[J].高等学校化学学报,2002(07):1371-1374. |
| [15] | 朱银华,周亚新,杨祝红,陆小华,冯新.新型Mo/TiO2的噻吩加氢脱硫性能[J].石油学报（石油加工）,2007(04):76-81. |
| [16] | Samantaray S K;Mohapatra P;Parida K .[J].Journal of Molecular Catalysis A:Chemical,2003,198(1-2):277. |
| [17] | Samantaray S K;Parida K .[J].Reaction Kinetics and Catalysis Letters,2003,78(02):381. |
| [18] | Jung S M;Grange E .[J].Catalysis Today,2000,59(3-4):305. |
| [19] | Wang XC;Yu JC;Liu P;Wang XX;Su WY;Fu XZ .Probing of photocatalytic surface sites on SO4 (2-)/TiO2 solid acids by in situ FT-IR spectroscopy and pyridine adsorption[J].Journal of Photochemistry and Photobiology, A. Chemistry,2006(3):339-347. |
| [20] | Yang H.;Lu R.;Zhao JZ.;Yang XW.;Shen LC.;Wang ZC. .Sulfated binary oxide solid superacids[J].Materials Chemistry and Physics,2003(1):68-72. |
| [21] | Lopez D E;Goodwin Jr J G;Bruce D A;Furuta S .[J].Applied Catalysis A:General,2008,339(01):76. |
| [22] | 季山,廖世军,王乐夫,Vladimir Linkov,Leslie Petrik.SO42-/Zr-ZSM-5 超强酸催化剂的制备和表征[J].分子催化,2002(05):379-383. |
| [23] | Li, XB;Nagaoka, K;Simon, LJ;Olindo, R;Lercher, JA .Influence of calcination procedure on the catalytic property of sulfated zirconia[J].Catalysis Letters,2007(1/2):34-40. |
| [24] | Jermy B R;Pandurangan A .[J].J Mol CatalA,2005,237(1-2):146. |
| [25] | Juan, JC;Zhang, JC;Jiang, YJ;Cao, WL;Yarmo, MA .Zirconium sulfate supported on activated carbon as catalyst for esterification of oleic acid by n-butanol under solvent-free conditions[J].Catalysis Letters,2007(3/4):153-158. |
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%