以4-硝基苯甲醇与氯金酸的络合物为模板,利用聚合物空腔内胺基捕获NaBH4还原的纳米粒子,设计和制备了一种具有底物识别性能的分子印迹聚合物负载纳米Au催化剂(Au/MIP).运用红外光谱、紫外-可见光谱和扫描电镜等方法对催化剂进行了表征.同时以水为溶剂,过氧化氢为氧化剂,考察了催化剂在取代苯甲醇氧化反应中的催化性能.结果表明,以Au/MIP为催化剂时,4-硝基苯甲醇转化率为75.6%,而以非印迹聚合物负载的纳米Au (Au/NIP)为催化剂时,4-硝基苯甲醇转化率仅为41.5%.以其它取代苯甲醇为底物时,Au/MIP与Au/NIP的催化活性差别不大.这说明Au/MIP催化剂活性与反应底物结构有关,脱除模板剂后它具有与4-硝基苯甲醇相匹配的空腔结构和识别位点,对反应底物表现出专一的识别性,因而提高了催化剂活性.
参考文献
[1] | Pauling L .[J].Journal of the American Chemical Society,1940,62:2643. |
[2] | Wulff G;Gross T;Schonfeld R .[J].Angewandte Chemie International Edition,1997,36:1962. |
[3] | Locatelli F.;Lemaire M.;Gamez P. .Molecular imprinting of polymerised catalytic complexes in asymmetric catalysis[J].Journal of molecular catalysis, A. Chemical,1998(1):89-98. |
[4] | Strikovsky AG.;Grun M.;Green BS.;Hradil J.;Wulff G.;Kasper D. .Catalytic molecularly imprinted polymers using conventional bulk polymerization or suspension polymerization: Selective hydrolysis of diphenyl carbonate and diphenyl carbamate[J].Journal of the American Chemical Society,2000(26):6295-6296. |
[5] | Liu J Q;WulffG .[J].Journal of the American Chemical Society,2004,126:7452. |
[6] | Visnjevski A E;Yilmaz E;Brüggemann O .[J].Applied Catalysis A:General,2004,260:169. |
[7] | Burri E;Ohm M;Daguenet C;Severin K .Site-isolated porphyrin catalysts in imprinted polymers[J].Chemistry: A European journal,2005(17):5055-5061. |
[8] | Li S J;Ge Y;Tiwar A;Wang S Q Turner A P F Piletsky S A .[J].Journal of Catalysis,2011,278:173. |
[9] | Zhang H;Piacham T;Drew M;Patek M Mosbach K Ye L .[J].Journal of the American Chemical Society,2006,128:4178. |
[10] | Brunkan NM.;Gagne MR. .Effect of chiral cavities associated with molecularly imprinted platinum centers on the selectivity of ligand-exchange reactions at platinum[J].Journal of the American Chemical Society,2000(26):6217-6225. |
[11] | Li YZ.;Fan YN.;Yang HP.;Xu BL.;Feng LY.;Yang MF.;Chen Y. .Strong metal-support interaction and catalytic properties of anatase and rutile supported palladium catalyst Pd/TiO2[J].Chemical Physics Letters,2003(1/2):160-165. |
[12] | Tang Z C;Li Q Y;Lu G X .[J].CARBO,2007,45:41. |
[13] | Li S J;Gong S Q .[J].Advanced Functional Materials,2009,19:2601. |
[14] | Viton F;White P S;Gagne M R.[J].Chemical Communications,2003:3040. |
[15] | Hashm A S K .[J].Chemical Reviews,2007,107:3180. |
[16] | Yadav G D;Mistry C K .[J].Journal of Molecular Catalysis A:Chemical,2001,172:135. |
[17] | Liu C;Tan R;Yu N Y;Yin D H .[J].Microporous and Mesoporous Materials,2010,131:162. |
[18] | Li SJ;Liao C;Li W;Chen YF;Hao X .Rationally designing molecularly imprinted polymer towards predetermined high selectivity by using metal as assembled pivot[J].Macromolecular bioscience,2007(9/10):1112-1120. |
[19] | Zhang D L;Li S J;Li W K;Chen Y F .[J].Catalysis Letters,2007,115:169. |
[20] | Park J E;Momma T;Osaka T .[J].Electrochimica Acta,2007,52:5914. |
[21] | Liu X H;Hong Y;Li S J;Li W K .[J].Journal of Inorganic and Organometallic Polymers,2009,19:335. |
[22] | Itoh H;Naka K;Chujo Y .[J].Journal of the American Chemical Society,2004,126:3026. |
[23] | Luo L R;Yu N Y;Tan R;Jin Y Yin D L Yin D H .[J].Catalysis Letters,2009,130:489. |
[24] | 庄大英,金勇,喻宁亚,秦亮生,刘建福,银董红,杨翠清.有机官能化介孔硅基材料负载纳米金催化剂的制备及其催化性能[J].催化学报,2009(09):896-900. |
[25] | Hoshino Y;Koide H;Urakami T;Kanazawa H,Kodama T,Oku N,Shea K J .[J].Journal of the American Chemical Society,2010,132:6644. |
[26] | Wu X Y;Goswami K;Shimizu K D .[J].Journal of Molecular Recognition,2008,21:410. |
[27] | Zayats M;Kanwar M;Ostermeier M;Searson P C .[J].Macromolecules,2011,44:3966. |
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%