“先核后壳”和“先壳后核”的简便途径制备M@SiO2(M=Ag,Au,Pt)纳米核壳结构及其催化活性

催化学报 , 2013, 34(11): 2098-2109. doi: 10.1016/S1872-2067(12)60716-5

“先核后壳”和“先壳后核”的简便途径制备M@SiO2(M=Ag,Au,Pt)纳米核壳结构及其催化活性

何圣超 ^1, , 费兆阳 ^2, , 李雷 ^3, , 孙博 ^4, , 冯新振 ^5, , 季伟捷 ^6,

1.南京大学化学化工学院介观化学教育部重点实验室,江苏南京210093

2.南京大学化学化工学院介观化学教育部重点实验室,江苏南京210093

3.南京大学化学化工学院介观化学教育部重点实验室,江苏南京210093

4.南京大学化学化工学院介观化学教育部重点实验室,江苏南京210093

5.南京大学化学化工学院介观化学教育部重点实验室,江苏南京210093

6.南京大学化学化工学院介观化学教育部重点实验室,江苏南京210093

基金项目: the Specialized Reaearch Fund for the Doctoral Program of High Education(20110091110023) 江苏省自然科学基金(BK2011439) 国家高技术研究发展计划(863计划,2013AA031703).This work was supported by the National Natural Science Foundation of China(21173118) 国家自然科学基金(21173118) the Natural Science Foundation of Jiangsu Province(BK2011439) the National High Technology Research and Development Program of China(863 Program,2013AA031703) 高等学校博士学科点专项科研基金(20110091110023)

关键词：核壳结构 , 银 , 金 , 铂 , 纳米粒子 , 二氧化硅 , 一氧化碳氧化 , 对硝基酚还原

Synthesis and catalytic activity of M@SiO2 (M =Ag, Au, and Pt) nanostructures via "core to shell" and "shell then core" approaches

Shengchao He ^1, , Zhaoyang Fei ^2, , Lei Li ^3, , Bo Sun ^4, , Xinzhen Feng ^5, , Weijie Ji ^6,

1.南京大学化学化工学院介观化学教育部重点实验室,江苏南京210093

2.南京大学化学化工学院介观化学教育部重点实验室,江苏南京210093

3.南京大学化学化工学院介观化学教育部重点实验室,江苏南京210093

4.南京大学化学化工学院介观化学教育部重点实验室,江苏南京210093

5.南京大学化学化工学院介观化学教育部重点实验室,江苏南京210093

6.南京大学化学化工学院介观化学教育部重点实验室,江苏南京210093

Keywords： Core-shell structure , Silver , Gold , Platinum , Nanoparticle , Silica , CO oxidation , 4-Nitrophenol reduction

采用简便的“先核后壳”和“先壳后核”途径制备了M@SiO2 (M=Ag,Au,Pt)核壳结构.采用“先核后壳”途径时,金属内核可以控制在6-9 nm,粒径分布均匀,SiO2壳层织构可调.该途径制备过程简便,无需高速离心分离,可有效节约制备成本.由该途径制得的Au@mSiO2中纳米Au的热稳定性高,经550℃空气焙烧后仍能保持高的CO氧化性能(T100=235℃).由“先壳后核”途径制得的核壳结构内核金属粒子也可以控制在＜ 10nm,粒径分布均匀,且SiO2壳层孔隙率可以预调,即使在液相中也可有效消除对硝基苯酚反应物分子的扩散限制,并于室温下将其还原为对氨基苯酚.两种途径所得的核壳结构均呈高单分散态.使用含有不同有机官能团的硅源可对介孔SiO2壳层进行进一步改性,拓展应用领域,因而具有很好的潜在应用前景.

参考文献

[1]	Reiss P;Protiere M;Li L .[J].Small,2009,5:154.
[2]	Guerrero-Martínez A;Pérez-Juste J;Liz-Marzán L M .[J].Advanced Materials,2010,22:1182.
[3]	Burns A;Ow H;Wiesner U .Fluorescent core-shell silica nanoparticles: towards "Lab on a Particle'' architectures for nanobiotechnology[J].Chemical Society Reviews,2006(11):1028-1042.
[4]	Chi F L;Guo Y N;Liu J;Liu Y L Huo Q S .[J].The Journal of Physical Chemistry C,2010,114:2519.
[5]	Jun Y W;Choi J S;Cheon J.[J].Chemical Communications,2007:1203.
[6]	Zhou S H;Varughese B;Eichhorn B;Jackson G.McIlwrath K .[J].Angewandte Chemie International Edition,2005,44:4539.
[7]	Chen YM;Yang F;Dai Y;Wang WQ;Chen SL .Ni@Pt core-shell nanoparticles: Synthesis, structural and electrochemical properties[J].The journal of physical chemistry, C. Nanomaterials and interfaces,2008(5):1645-1649.
[8]	Deng Y H;Qi D W;Deng C H;Zhang X M Zhao D Y .[J].Journal of the American Chemical Society,2008,130:28.
[9]	Lu J L;Fu B S;Kung M C;Xiao G Elam J W Kung H H Stair P C .[J].Science,2012,335:1205.
[10]	Song C;Du J P;Zhao J H;Feng S A Du G X Zhu Z P .[J].Chemistry of Materials,2009,21:1524.
[11]	Yu G B;Sun B;Pei Y;Xie S H Yan S R Qiao M H Pan K N Zhang X X Zong B N .[J].Journal of the American Chemical Society,2010,132:935.
[12]	Yang P;Zhang W;Du Y K;Wang X M .[J].Journal of Molecular Catalysis A:Chemical,2006,260:4.
[13]	Huang W Y;Kuhn J N;Tsung C K;Zhang Y W Habas S E Yang P D Somorjai G A .[J].Nano Letters,2008,8:2027.
[14]	Miyamoto M;Kamei T;Nishiyama N;Egashira Y Ueyama K .[J].Advanced Materials,2005,17:1985.
[15]	Li X G;He J J;Meng M;Yoneyama Y Tsubaki N .[J].Journal of Catalysis,2009,265:26.
[16]	Sun B;Yu G B;Lin J;Xu K Pei Y Yan S R Qiao M H Fan K N Zhang X X Zong B N .[J].Catalysis Science & Technology,2012,2:1625.
[17]	李雷;李彦兴;姚瑶;姚良宏季伟捷区泽棠 .[J].化学进展,2013,25:71.
[18]	Joo S H;Park J Y;Tsung C K;Yamada Y Yang P D Somorjai G A .[J].Nature Materials,2009,8:126.
[19]	Chen, Y.;Chen, H.;Zeng, D.;Tian, Y.;Chen, F.;Feng, J.;Shi, J. .Core/shell structured hollow mesoporous nanocapsules: A potential platform for simultaneous cell imaging and anticancer drug delivery[J].ACS nano,2010(10):6001-6013.
[20]	Liu J;Qiao S Z;Hartono S B;Lu G Q .[J].Angewandte Chemie International Edition,2010,49:4981.
[21]	Huang, XQ;Guo, CY;Zuo, LQ;Zheng, NF;Stucky, GD .An Assembly Route to Inorganic Catalytic Nanoreactors Containing Sub-10-nm Gold Nanoparticles with Anti-Aggregation Properties[J].Small,2009(3):361-365.
[22]	Chen H M;Deng C H;Zhang X M .[J].Angewandte Chemie International Edition,2010,49:607.
[23]	Ohmori M;Matijevic E .[J].Journal of Colloid and Interface Science,1992,150:594.
[24]	Ryan J N;Elimelech M;Baeseman J L;Magelky R D .[J].Environmental Science and Technology,2000,34:2000.
[25]	Graf C.;Vossen DLJ.;Imhof A.;van Blaaderen A. .A general method to coat colloidal particles with silica[J].Langmuir: The ACS Journal of Surfaces and Colloids,2003(17):6693-6700.
[26]	Gorelikov I;Matsuura N .Single-step coating of mesoporous silica on cetyltrimethyl ammonium bromide-capped nanoparticles[J].Nano letters,2008(1):369-373.
[27]	Park J C;Lee H J;Jung H S;Kim M Kim H J Park K H Song H .[J].ChemCatChem,2011,3:755.
[28]	Hah H J;Kim J S;Jeon B J;Koo S M,Lee Y E.[J].Chemical Communications,2003:1712.
[29]	Hah H J;Um J I;Han S H;Koo S M .[J].Chemical Communications,2004,8:1012.
[30]	Chen D;Li L L;Tang F Q;Qi S .[J].Advanced Materials,2009,21:3804.
[31]	Tan L F;Chen D;Liu H Y;Tang F Q .[J].Advanced Materials,2010,22:4885.
[32]	Li L;Yao Y;Sun B;Fei Z Y,Xia H,Zhao J,Ji W J,Au C T.[J].ChemCatChem,2013
[33]	Li, L.;He, S.;Song, Y.;Zhao, J.;Ji, W.;Au, C.-T..Fine-tunable Ni@porous silica core-shell nanocatalysts: Synthesis, characterization, and catalytic properties in partial oxidation of methane to syngas[J].Journal of Catalysis,2012:54-64.
[34]	Li L;Lu P;Yao Y;Ji W J .[J].Catalysis Communications,2012,26:72.
[35]	Yao L H;Shi T B;Li Y X;Zhao J Ji W J Au C T .[J].Catalysis Today,2011,164:112.
[36]	Li Y X;Yao L H;Song Y Y;Liu S Q Zhao J Ji W J Au C T .[J].Chemical Communications,2010,46:5298.
[37]	Chen H M;Hu T;Zhang X M;Huo K F Chu P K He J H .[J].Langmuir,2010,26:13556.
[38]	Haruta M;Tsubota S;Kobayashi T;Kageyama H Genet M J Delmon B .[J].Journal of Catalysis,1993,144:175.
[39]	Hartua M .[J].GoMBull,2004,37:27.
[40]	Tsubota S;Cunningham D A H;Bando Y;Haruta M .[J].Studies in Surface Science and Catalysis,1995,91:227.
[41]	Cunningham DAH.;Kageyama H.;Tsubota S.;Haruta M.;Vogel W. .The relationship between the structure and activity of nanometer size gold when supported on Mg(OH)(2)[J].Journal of Catalysis,1998(1):1-10.
[42]	Wolf A;Schüth F .[J].Applied Catalysis A:General,2002,226:1.
[43]	Li, L.;Wang, A.;Qiao, B.;Lin, J.;Huang, Y.;Wang, X.;Zhang, T..Origin of the high activity of Au/FeO_x for low-temperature CO oxidation: Direct evidence for a redox mechanism[J].Journal of Catalysis,2013:90-100.
[44]	Costello C K;Yang J H;Law H Y;Wang Y Lin J N Marks L D Kung M C Kung H H .[J].Applied Catalysis A:General,2003,243:15.
[45]	Akita T.;Ichikawa S.;Tanaka K.;Haruta M.;Lu P. .Analytical TEM study on the dispersion of Au nanoparticles in Au/TiO2 catalyst prepared under various temperatures[J].Surface and Interface Analysis: SIA: An International Journal Devoted to the Development and Application of Techniques for the Analysis of Surfaces, Interfaces and Thin Films,2001(2):73-78.
[46]	Daté M;Ichihashi Y;Yamashita T;Chiorino A Boccuzzi F Haruta M .[J].Catalysis Today,2002,72:89.
[47]	Schumacher B;Plzak V;Kinne M;Behrn R J .[J].Catalysis Letters,2003,89:109.
[48]	Zanella R;Louis C .[J].Catalysis Today,2005,107-108:768.
[49]	Vogel W;Cunningham D A H;Tanaka K;Haruta M .[J].Catalysis Letters,1996,40:175.
[50]	Schubert M M;PIzak V;Garche J;Behm R J .[J].Catalysis Letters,76:143.
[51]	Konova P;Naydenov A;Venkov Cv;Mehandjiev D Andreeva D Tabakova T .[J].Journal of Molecular Catalysis A:Chemical,2004,213:235.
[52]	Moreau F;Bond GC .Gold on titania catalysts, influence of some physicochemical parameters on the activity and stability for the oxidation of carbon monoxide[J].Applied Catalysis, A. General: An International Journal Devoted to Catalytic Science and Its Applications,2006(1):110-117.

上一张下一张

计量

下载量()
访问量()

作者相关

文章评分

您的评分：
1

0%
2

0%
3

0%
4

0%
5

0%

材料期刊网