利用硝基甲烷还原法制备了一系列不同粒径的纳米Au颗粒,用浸渍法担载于ZSM-5分子筛上制得Au/ZSM-5催化剂,并考察了其对分子氧氧化β-紫罗兰酮的催化性能. 结果发现,该催化剂可以有效地催化分子氧氧化β-紫罗兰酮生成 5,6-环氧-β-紫罗兰酮、4-氧代-β-紫罗兰酮、4-羟基-β-紫罗兰酮以及少量的二氢猕猴桃内酯,这些产物均是优质的香料及其前体. 与传统的铬盐催化剂相比,本文制备的催化剂可选择性地将β-紫罗兰酮氧化为环氧化合物,并且反应后催化剂容易分离. 详细探讨了不同载体、氧化剂、溶剂、反应温度和反应时间对β-紫罗兰酮氧化反应的影响. 结果表明,催化剂的催化性能与担载金的颗粒大小密切相关,同时溶剂的性质也对反应有明显影响. 以氯仿为溶剂时催化剂催化性能最好. 催化剂循环使用五次仍具有较高的催化活性.
参考文献
| [1] | Sakamaki H;Itoh K;Chai W;Hayashida Y Kitanaka S Horiuchi C A .[J].Journal of Molecular Catalysis B:Enzymatic,2004,27(4-6):177. |
| [2] | Janitschke L;Hoffmann W .[P].US 4517382,1985. |
| [3] | Chidambaram N;Chandrasekaran S .[J].Journal of Organic Chemistry,1987,52(22):5048. |
| [4] | Hirao T;Mikami S;Mori M;Ohshiro Y .[J].Tetrahedron Letters,1991,32(14):1741. |
| [5] | Jaedicke H;Paust J .[P].US 4209450,1980. |
| [6] | Henbest H B .[J].Journal of The Chemical Society,1951,73(03):1074. |
| [7] | Haruta M;Yamada N;Kobayashi T;Iijima S .[J].Journal of Catalysis,1989,115(02):301. |
| [8] | Hutchings G J .[J].Journal of Catalysis,1985,96(02):292. |
| [9] | Nkosi B;Coville N J;Hutchings G J;Adams M D Friedl J Wagner F E .[J].Journal of Catalysis,1991,128(02):366. |
| [10] | Haruta M;Tsubota S;Kobayashi T;Kageyama H Genet M J Delmon B .[J].Journal of Catalysis,1993,144(01):175. |
| [11] | Berndt H.;Pitsch I.;Evert S.;Struve K.;Pohl MM.;Radnik J.;Martin A. .Oxygen adsorption on Au/Al2O3 catalysts and relation to the catalytic oxidation of ethylene glycol to glycolic acid[J].Applied Catalysis, A. General: An International Journal Devoted to Catalytic Science and Its Applications,2003(1):169-179. |
| [12] | Hayashi T.;Haruta M.;Tanaka K. .Selective vapor-phase epoxidation of propylene over Au/TiO2 catalysts in the presence of oxygen and hydrogen[J].Journal of Catalysis,1998(2):566-575. |
| [13] | Stangland E E;Stavens K B;Andres R P;Delgass W N .[J].Studies in surface science and catalysis,2000,130:827. |
| [14] | Patil N S;Uphade B S;Jana P;Bharagava S K Choudhary V R .[J].Journal of Catalysis,2004,223(01):236. |
| [15] | Patil NS;Jha R;Uphade BS;Bhargava SK;Choudhary VR .Epoxidation of styrene by anhydrous t-butyl hydroperoxide over gold supported on Al2O3, Ga2O3, In2O3 and Tl2O3[J].Applied Catalysis, A. General: An International Journal Devoted to Catalytic Science and Its Applications,2004(1/2):87-93. |
| [16] | Salama T M;Ohnishi R;Ichikawa M.[J].Chemistry Communications,1997(01):105. |
| [17] | Biella S;Rossi M.[J].Chemistry Communications,2003(03):378. |
| [18] | Hughes M D;Xu Y J;Jenkins P;McMorn P Landon P Enache D I Carley A F Attard G A Hutchings G J King F Stitt E H Johnston P Griffin K Kiely C J .[J].NATURE,2005,437(7062):1132. |
| [19] | Enache DI;Edwards JK;Landon P;Solsona-Espriu B;Carley AF;Herzing AA;Watanabe M;Kiely CJ;Knight DW;Hutchings GJ .Solvent-free oxidation of primary alcohols to aldehydes using Au-Pd/TiO2 catalysts[J].Science,2006(5759):362-365. |
| [20] | Brust M;Walker M;Bethell D;Schiffrin D J Whyman R.[J].Chemistry Communications,1994(07):801. |
| [21] | Zhou Y;Wang C;Zhu Y;Chen Z .[J].CHEMISTRY OF MATERIALS,1999,11(09):2310. |
| [22] | Henglein A.;Meisel D. .Radiolytic control of the size of colloidal gold nanoparticles[J].Langmuir: The ACS Journal of Surfaces and Colloids,1998(26):7392-7396. |
| [23] | Mizukoshi Y;Okitsu K;Maeda Y;Yamamoto T A Oshima R Nagata Y .[J].Journal of Physical Chemistry B,1997,101(36):7033. |
| [24] | Nakamoto M;Yamamoto M;Fukusumi M.[J].Chemistry Communications,2002(15):1622. |
| [25] | Shimizu T;Teranishi T;Hasegawa S;Miyake M .[J].Journal of Physical Chemistry B,2003,107(12):2719. |
| [26] | San T K;Pal A;Pal T .[J].Journal of Physical Chemistry B,2001,105(38):9266. |
| [27] | Kozlov A I;Kozlova A P;Liu H;Iwasawa Y .[J].Applied Catalysis A:General,1999,182(01):9. |
| [28] | Mulvaney P .[J].Langmuir,1996,12(03):788. |
| [29] | Deki S;Aoi Y;Yanagimoto H;Ishii K Akamatsu K Mizuhata M Kajinami A .[J].Journal of Materials Chemistry,1996,6(12):1879. |
| [30] | Gugumus, F .Physico-chemical aspects of polyethylene processing in an open mixer. Part 23: Mechanisms and kinetics of trans-vinylene group consumption[J].Polymer Degradation and Stability,2006(9):2079-2092. |
| [31] | Mukherjee S;Samanta S;Bhaumik A;Ray B C .[J].Applied Catalysis B:Environmental,2006,68(01):12. |
| [32] | Groves J T;Stern M K .[J].Journal of the American Chemical Society,1988,110(26):8628. |
| [33] | Castellino A J;Bruice T C .[J].Journal of the American Chemical Society,1988,110(22):7512. |
| [34] | Traylor T G;Mikzstal A R .[J].Journal of the American Chemical Society,1987,109(09):2770. |
| [35] | Liu H;Kozlov A I;Kozlova A P;Shido T Asakura K Iwasawa Y .[J].Journal of Catalysis,1999,185(02):252. |
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