采用固相研磨法制备了有序介孔树脂FDU-14孔道限阈分散的Al2O3复合材料Al2O3@FDU-14.以其为载体,采用浸渍法制备了4.0％ Pt/Al2O3@FDU- 14催化剂,并利用X射线衍射、透射电子显微镜和N2吸附等手段对催化剂进行了表征.结果表明,Pt/Al2O3@FDU- 14催化剂保持了FDU-14的介孔结构特征.经手性分子辛可尼定修饰后,考察了该催化剂在丙酮酸乙酯不对称氧化反应中的催化性能.当复合材料载体中Al2O3含量为5％～15％时,Al2O3主要以无定形态均匀分布于FDU-14孔道内.随着催化剂中Al2O3含量增加,丙酮酸乙酯不对称氢化反应的活性和产物的光学选择性都有所提高,其中后者最高可达80％ee.Al2O3的引入可降低FDU-14介孔树脂材料表面的电子密度,有利于辛可尼定在催化剂表面的吸附,因此,Pt/Al2O3@FDU-14催化剂手性诱导能力比Pt/FDU-14强.
参考文献
| [1] | Mallat T;Orglmeister E;Baiker A .[J].Chemical Reviews,2007,107:4863. |
| [2] | Wehrli J T;Baiker A;Monti D M;Blaser H U .[J].Journal of Molecular Catalysis,1990,61:207. |
| [3] | Blaser H U;Jalett H P;Müller M;Studer M .[J].Catalysis Today,1997,37:441. |
| [4] | Zuo X B;Liu H F;Yue Ch .[J].Journal of Molecular Catalysis A:Chemical,1999,147:63. |
| [5] | T(o)r(o)k B;Felf(o)ldi K;Baláizsik K;Bartók M.[J].Chemical Communications,1999:1725. |
| [6] | Bhaduri S.;Munshi P.;Mukesh D.;Lahiri GK. .Asymmetric hydrogenation of methyl pyruvate using platinum carbonyl cluster supported on an anion exchanger as the catalyst[J].Catalysis Letters,2000(1/3):61-66. |
| [7] | Studer M;Blaser H U;Exner C .[J].Advanced Synthesis and Catalysis,2003,345:45. |
| [8] | Bürgi T;Baiker A .[J].Accounts of Chemical Research,2004,37:909. |
| [9] | Balázsik K;Bartok M .[J].Journal of Molecular Catalysis A:Chemical,2004,219:383. |
| [10] | 姜鹏,李晓红,关业军,应品良,李灿.亲水性高分子稳定的纳米铂催化丙酮酸乙酯不对称氢化[J].分子催化,2004(05):381-384. |
| [11] | Bartok M .Heterogeneous catalytic enantioselective hydrogenation of activated ketones[J].Current organic chemistry,2006(13):1533-1567. |
| [12] | Balázsik K;Sz(o)ri K;Felf(o)ldi K;T(o)r(o)k B,Bartók M.[J].Chemical Communications,2000:555. |
| [13] | 韩涤非,杨启华,李灿.表面上和纳米孔道内以及乳液中的手性催化[J].催化学报,2008(09):789-816. |
| [14] | Balázsik, K.;Szri, K.;Szllsi, G.;Bartók, M. .The first case of competitive heterogeneously catalyzed enantioselective hydrogenation of ketones[J].Chemical communications,2011(5):1551-1552. |
| [15] | Tálas, E.;Margitfalvi, J.L.;Egyed, O. .Additional data to the origin of rate enhancement in the enantioselective hydrogenation of activated ketones over cinchonidine modified platinum catalyst[J].Journal of Catalysis,2009(2):191-198. |
| [16] | T(o)r(o)k B;Sz(o)ll(o)si G;Balázsik K;Felf(o)ldi K Kun I Bartók M .[J].Ultrasonics Sonochemistry,1999,6:97. |
| [17] | Griffiths SP.;Wells PB.;Johnston P. .Enantioselective hydrogenation: chemistry of the modification of platinum by cinchonidine[J].Applied Catalysis, A. General: An International Journal Devoted to Catalytic Science and Its Applications,2000(1/2):193-204. |
| [18] | 陈志坚,李晓红,李灿.介孔载体负载Pt催化剂上α-酮酸酯的不对称氢化[J].催化学报,2011(01):155-161. |
| [19] | Wang H N;Li X H;Wang Y M;Wu P .[J].ChemCatChem,2010,2:1303. |
| [20] | Li X H;Shen Y L;Xing R;Liu Y M Wu H H He M Y Wu P .[J].Catalysis Letters,2008,122:325. |
| [21] | 沈亚丽,李晓红,宋丽英,王红娜,吴鹏.手性修饰的介孔树脂材料负载铂催化剂上丙酮酸乙酯的不对称氢化反应[J].高等学校化学学报,2009(07):1375-1379. |
| [22] | Chen Z J;Guan Z H;Li M R;Yang Q H,Li C .[J].Angewandte Chemie International Edition,2011,50:4913. |
| [23] | Xing L;Du F;Liang JJ;Chen YS;Zhou QL .Preparation of Pt/SWNTs for heterogeneous asymmetric hydrogenation of ethyl pyruvate[J].Journal of molecular catalysis, A. Chemical,2007(1/2):191-196. |
| [24] | Li B;Li X H;Wang H N;Wu P .[J].Journal of Molecular Catalysis A:Chemical,2011,345:81. |
| [25] | 陶国忠,卢冠忠,郭耘,王艳芹,郭杨龙,张志刚,刘晓晖,王筠松.丙酮酸乙酯多相不对称催化加氢反应的初始过渡期研究[J].催化学报,2009(05):391-395. |
| [26] | 彭宗海,马梦林,付海燕,陈华,李贤钧.对烷氧基取代MeO-BIPHEP型手性双膦钌配合物催化β-酮酸酯不对称加氢反应[J].催化学报,2010(02):191-194. |
| [27] | Zhang F Q;Meng Y;Gu D;Yan Y Yu Ch Zh Tu B Zhao D Y .[J].Journal of the American Chemical Society,2005,127:13508. |
| [28] | Zhang FQ;Meng Y;Gu D;Yan Y;Chen ZX;Tu B;Zhao DY .An aqueous cooperative assembly route to synthesize ordered mesoporous carbons with controlled structures and morphology[J].Chemistry of Materials: A Publication of the American Chemistry Society,2006(22):5279-5288. |
| [29] | Wang Y M;Wu Zh Y;Shi L Y;Zhu J H .[J].Advanced Materials,2005,17:323. |
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