以1,2-环氧环己烷水解为主要探针反应研究了钛硅分子筛HTS-1的表面酸催化性能.结果表明,HTS-1表面酸中心具有较高的催化活性,它的扩散性能和溶剂极性对反应活性的影响很大.还采用吸附吡啶的红外光谱和紫外光谱对HTS-1催化剂表面酸性进行了定性和定量分析.这些结果不仅拓展了HTS-1在精细有机合成中的应用,而且为有效提高HTS-1的催化氧化性能提供了依据.
Hydrolysis of 1,2-epoxycyclohexane as a probe reaction was employed to investigate the surface acid properties of tita-nium-silicate zeolite (HTS-1) catalyst under various conditions. The results indicated that the hydrolysis reaction was mainly affected by solvent polarity and diffusion limitation, and HTS-! showed outstanding catalytic performance for this reaction. Quantitative and qualitative analysis of acidity and acid sites by means of pyridine adsorption was performed using UV-Vis and FT-IR spectroscopy, respectively, which can distinguish Breasted acidic sites and Lewis acidic sites and to calculate precisely the surface acid amount of HTS-1. These results not only expand the applications of HTS- 1 in fine chemical synthesis but also provide a basis for effectively improving the catalytic performance of HTS- 1 in oxidation.
参考文献
[1] | 张义华,王祥生,郭新闻,刘松.钛硅分子筛TS-1的合成、表征及催化性能[J].催化学报,2001(01):92-94. |
[2] | Wang X Sh;Guo X W;Wang L .[J].Studies in surface science and catalysis,2004,154:2589. |
[3] | Borin M F;Da Silva T;Felisbino R F;Cardoso D .[J].Journal of Physical Chemistry B,2006,110:15080. |
[4] | 张海娇,姚明恺,谢伟,刘月明,吴鹏.TS-1分子筛的无机法合成及其催化苯酚羟基化性能[J].催化学报,2007(10):895-899. |
[5] | Park S Y;Cho K M;Youn M H;Seo J G Baeck S H Kim T J Chung Y M Oh S H Song I K .[J].Catalysis Letters,2008,122:349. |
[6] | Bordiga S;Damin A;Bonino F;Ricchiardi G,Lamberti C,Zecchina A .[J].Angewandte Chemie International Edition,2002,41:4734. |
[7] | 李钢,王祥生,闫海生,刘民,刘毅慧,陈永英.钛硅分子筛中铝杂质对其性能的影响[J].催化学报,2001(05):465-468. |
[8] | Zhuang J Q;Ma D;Yan Zh M;Liu X M Han X W Bao X H Zhang Y H Guo X W Wang X Sh .[J].Applied Catalysis A:General,2004,258:1. |
[9] | Srinivas D;Srivastava R;Ratnasamy P .[J].Catalysis Today,2004,96:127. |
[10] | Sasidharan M;Kumar R .[J].Journal of Catalysis,2003,220:326. |
[11] | Zecchina A;Spoto G;Bordiga S;Padovan M Leofanti G Petrini G .[J].Studies in Surface Science and Catalysis,1991,65:671. |
[12] | Janchen J;Vorbeck G;Stach H;Parlitz B van HooffJ H C .[J].Studies in Surface Science and Catalysis,1995,94:108. |
[13] | 王伊蕾,邢双英,曹亮,王善鹏,周丹红.TS-1分子筛Lewis酸性的理论研究[J].催化学报,2009(01):24-30. |
[14] | Damin A;Bonino F;Ricchiardi G;Bordiga S Zecchina A Lamberti C .[J].Journal of Physical Chemistry B,2002,106:7524. |
[15] | Sastre G;Corma A .[J].Chemical Physics Letters,1999,302:447. |
[16] | Zhuang J Q;Ma D;Yan Zh M;Deng F Liu X M Hart X W Bao X H Liu X W Guo X W Wang X Sh .[J].Journal of Catalysis,2004,221:670. |
[17] | Yang, G;Zhuang, JQ;Ma, D;Lan, XJ;Zhou, LJ;Liu, XC;Han, XW;Bao, XH .A joint experimental-theoretical study on trimethylphosphine adsorption on the Lewis acidic sites present in TS-1 zeolite[J].Journal of Molecular Structure,2008(1/3):24-29. |
[18] | Yang G;Lan X J;Zhuang J Q;Ma D Zhou L J Liu X Ch Han X W Bao X H .[J].Applied Catalysis A:General,2008,337:58. |
[19] | Hu Sh W;Willey R J;Notari B .[J].Journal of Catalysis,2003,220:240. |
[20] | 林民;舒兴田;汪燮卿;朱斌 .[P].CN 99126289,2001. |
[21] | 郭建平,尹笃林,郭军.溶液中固体催化剂表面酸量的紫外光谱分析收稿日期:2001-03-15[J].湘潭师范学院学报(自然科学版),2001(03):65-68. |
[22] | Scarano D;Zecchina A;Bordiga S;Geobaldo F,Spoto G,Petrini G,Leofanti G,Padovan M,Tozzola G .[J].Journal of the Chemical Society,Faraday Transactions,1993,89:4123. |
[23] | Ricchiardi G;Damin A;Bordiga S;Lamberti C Spano G Rivetti F Zecchina A .[J].Journal of the American Chemical Society,2001,123:11409. |
[24] | Bonino F.;Damin A.;Bordiga S.;Lamberti C.;Zecchina A. .Interaction of CD3CN and pyridine with the Ti(IV) centers of TS-1 catalysts: a spectroscopic and computational study[J].Langmuir: The ACS Journal of Surfaces and Colloids,2003(6):2155-2161. |
[25] | Post M F M .[J].Studies in Surface Science and Catalysis,1991,58:391. |
[26] | Ramachandran C E;Zhao Q;Zikanova A;Kocirik M Broadbelt L J Snurr R Q .[J].Catalysis Communications,2006,7:936. |
[27] | 甄开吉;王国甲;毕颖丽;李荣生,阚秋斌.催化作用基础[M].北京:科学出版社,2005:86. |
[28] | Thiele G F;Roland E .[J].Journal of Molecular Catalysis A:Chemical,1997,117:351. |
[29] | Hutter R;Mallat T;Baiker A .[J].Studies in surface science and catalysis,1997,108:329. |
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