采用具有分等级孔道结构的SiO2(HMS)为载体,通过润湿浸渍引入少量CeO2,经焙烧得到CeO2/HMS复合载体,然后采用沉积沉淀法负载上Au纳米粒子,得到Au/CeO2/HMS三元复合催化剂.通过X射线衍射、程序升温还原和原位红外光谱等手段表征了催化剂的结构.结果表明,CeO2的存在可控制Au颗粒的沉积并稳定载体上的纳米Au颗粒.Au/CeO2/HMS上CO低温氧化反应完全转化温度为60℃.高度分散的Au0可以活化CO,CeO2颗粒则可以提供反应需要的氧.稳定性测试结果显示,反应48h催化剂活性维持不变.
Hierarchical composite nanostructure composed of Au,CeO2,and SiO2 was fabricated by sequentially depositing ceria nanoparticles through impregnation and calcination,and then gold nanoparticles through a deposition-precipitation method on hierarchical monolithic silica (HMS) with multi-length scale pore structure.The Au/CeO2/HMS composite nanostructure was characterized by X-ray diffraction,temperature-programmed reduction,and diffuse reflectance infrared Fourier transform spectroscopy.The results indicate that the presence of ceria had a significant effect on targeted deposition and stabilization of small metallic gold nanoparticles on the support.The temperature for complete conversion of CO to CO2 over Au/CeO2/HMS is ca.60 ℃ at a space velocity of 80000 ml/(g·h).The highly dispersed metallic gold nanoparticles can activate CO and the small ceria nanoparticles supply oxygen in the reaction.The catalytic activity remains considerably stable during 48 h stability testing.The interaction between gold and ceria contributed greatly to CO oxidation and the presence of silica improved the stability of the gold catalyst.
参考文献
[1] | Haruta M;Yamada N;Kobayashi T;(I)ijima S .[J].Journal of Catalysis,1989,115:301. |
[2] | Chen Z;Gao Q M .[J].Applied Catalysis B:Environmental,2008,84:790. |
[3] | Wang G H;Li W C;Jia K M;Spliethoff B Schüth F Lu A H .[J].Applied Catalysis A:General,2009,364:42. |
[4] | Yoon B;H(a)kkinen H;Landman U;W(o)rz A S Antonietti J M Abbet S Judai K Heiz U .[J].Science,2005,307:403. |
[5] | 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. |
[6] | Bailie J E;Hutchings G J.[J].Chemical Communications,1999:2151. |
[7] | Tabakova T;Idakiev V;Andreeva D;Mitov I .[J].Applied Catalysis A:General,2000,202:91. |
[8] | Yan L;Zhang X M;Ren T;Zhang H P,Wang X L,Suo J H.[J].Chemical Communications,2002:860. |
[9] | Costello C K;Kung M C;Oh H S;Wang Y Kung H H .[J].Applied Catalysis A:General,2002,232:159. |
[10] | Guo QL.;Davis KA.;Goodman DW.;Luo K. .Initial growth of Au on oxides[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(1):161-165. |
[11] | Wang G Y;Lian H L;Zhang W X;Jiang D Z Wu T H .[J].Kinetics and Catalysis,2002,43:433. |
[12] | Kim C H;Thompson L T .[J].Journal of Catalysis,2005,230:66. |
[13] | Zhu H G;Ma Z;Clark J C;Pan Z W Overbury S H Dai S .[J].Applied Catalysis A:General,2007,326:89. |
[14] | Wang H P;Liu C J .[J].Applied Catalysis B:Environmental,2011,106:672. |
[15] | Wolf A;Schiith F .[J].Applied Catalysis A:General,2002,226:1. |
[16] | Penkova A;Martínez Blanes J M;Cruz S A;Centeno M A Hadjiivanov K Odriozola J A .[J].Microporous and Mesoporous Materials,2009,117:530. |
[17] | Lee B;Ma Z;Zhang Z T;Park C Dai S .[J].Microporous and Mesoporous Materials,2009,122:160. |
[18] | Zhu H G;Liang C D;Yan W F;Overbury S H Dai S .[J].Journal of Physical Chemistry B,2006,110:10842. |
[19] | Veith GM;Lupini AR;Rashkeev S;Pennycook SJ;Mullins DR;Schwartz V;Bridges CA;Dudney NJ .Thermal stability and catalytic activity of gold nanoparticles supported on silica[J].Journal of Catalysis,2009(1):92-101. |
[20] | Okumura M.;Tsubota S.;Nakamura T.;Azuma M.;Haruta M.;Nakamura S. .Chemical vapor deposition of gold on Al2O3, SiO2, and TiO2 for the oxidation of CO and of H-2[J].Catalysis Letters,1998(1/2):53-58. |
[21] | Hu J C;Chen L F;Zhu K K;Suchopar A Richards R .[J].Catalysis Today,2007,122:277. |
[22] | Magureanu M;Mandache N B;Hu J C;Richards R Florea M Parvulescu V I .[J].Applied Catalysis B:Environmental,2007,76:275. |
[23] | Lu GM;Ji D;Qian G;Qi YX;Wang XL;Suo JS .Gold nanoparticles in mesoporous materials showing catalytic selective oxidation cyclohexane using oxygen[J].Applied Catalysis, A. General: An International Journal Devoted to Catalytic Science and Its Applications,2005(2):175-180. |
[24] | Lee B;Zhu H;Zhang Z;Overbury S H Dai S .[J].Microporous and Mesoporous Materials,2004,70:71. |
[25] | Zhu H;Lee B;Dai S;Overbury S H .[J].Langmuir,2003,19:3974. |
[26] | Apríle C;Abad A;García H;Corma A .[J].Journal of Materials Chemistry,2005,15:4408. |
[27] | Kónya Z;Puntes V F;Kiricsi I;Zhu J Ager Ⅲ J W Ko M K Frei H Alivisatos P Somorjai G A .[J].Chemistry of Materials,2003,15:1242. |
[28] | Zhu J.;Konya Z.;Puntes VF.;Kiricsi I.;Miao CX.;Ager JW.;Alivisatos AP.;Somorjai GA. .Encapsulation of metal (Au, Ag, Pt) nanoparticles into the mesoporous SBA-15 structure[J].Langmuir: The ACS Journal of Surfaces and Colloids,2003(10):4396-4401. |
[29] | Lin H P;Chi Y S;Lin J N;Mou C Y,Wan B Z.[J].Chemistry Letters,2001:1116. |
[30] | 苏继新,张慎平,马丽媛,屈文,张明博.Au/SBA-15的制备及其催化CO氧化反应性能[J].催化学报,2010(07):839-845. |
[31] | Qian K;Huang W X;Jiang Z Q;Sun H X .[J].Journal of Catalysis,2007,248:137. |
[32] | Qian K;Huang W X;Fang J;Lv S S He B Jiang Z Q Wei S Q .[J].Journal of Catalysis,2008,255:269. |
[33] | Qian, K.;Zhang, W.;Sun, H.;Fang, J.;He, B.;Ma, Y.;Jiang, Z.;Wei, S.;Yang, J.;Huang, W. .Hydroxyls-induced oxygen activation on "inert" Au nanoparticles for low-temperature CO oxidation[J].Journal of Catalysis,2011(1):95-103. |
[34] | Zou X H;XuJG;Qi S X;Suo ZH An LD Li F .[J].Journal of Natural Gas Chemistry,2011,20:41. |
[35] | 单文娟,刘畅,郭红娟,杨利华,王晓楠,冯兆池.0,1,3维CeO2的可控制备及CuO/CeO2催化剂上CO氧化反应[J].催化学报,2011(08):1336-1341. |
[36] | Carrettin S;Concepción P;Corma A;López Nieto J M,Puntes V F .[J].Angewandte Chemie International Edition,2004,43:2538. |
[37] | Moreau F;Bond G C;Vander Linden B;Silberova B A A Makkee M .[J].Applied Catalysis A:General,2008,347:208. |
[38] | Qian K;Lva S S;Xiao X Y;Sun H X Lu J Q Luo M F Huang W X .[J].Journal of Molecular Catalysis A:Chemical,2009,306:40. |
[39] | Smatt JH.;Schunk S.;Linden M. .Versatile double-templating synthesis route to silica monoliths exhibiting a multimodal hierarchical porosity[J].Chemistry of Materials,2003(12):2354-2361. |
[40] | Lu AH;Smatt JH;Linden M .Combined surface and volume templating of highly porous nanocast carbon monoliths[J].Advanced functional materials,2005(5):865-871. |
[41] | Somodi F;Borbáth I;Hegedús M;Tompos A Sajó I E Szegedi A Rojas S Fierro J L G Margitfalvi J L .[J].Appl Catal 4,2008,347:216. |
[42] | Zhang R R;Ren L H;Lu A H;Li W C .[J].Catalysis Communications,2011,13:18. |
[43] | Haruta M .[J].Gold Bulletin,2004,37:27. |
[44] | Pillai UR;Deevi S .Highly active gold-ceria catalyst for the room temperature oxidation of carbon monoxide[J].Applied Catalysis, A. General: An International Journal Devoted to Catalytic Science and Its Applications,2006(0):266-273. |
[45] | Hernandez J A;Pawelec S G B;Zepeda T A .[J].Applied Catalysis B:Environmental,2009,89:128. |
[46] | Ying F;Wang S J;Au C T;Lai S Y .[J].Microporous and Mesoporous Materials,2011,142:308. |
[47] | Ousmane M;Liotta L F;Di Carlo G;Pantaleo G Venezia A M Deganello G Retailleau L Boreave A Giroir-Fendler A .[J].Applied Catalysis B:Environmental,2011,101:629. |
[48] | Fu Q;Kudriavtseva S;Saltsburg H;Flytzani-Stephanopoulos M .[J].Chemical Engineering Journal,2003,93:41. |
[49] | Romero-Sarria F;Martínez T L M;Centeno M A;Odriozola J A .[J].Journal of Physical Chemistry C,2007,111:14469. |
[50] | Karpenko, A;Denkwitz, Y;Plzak, V;Cai, J;Leppelt, R;Schumacher, B;Behm, RJ .Low-temperature water-gas shift reaction on Au/CeO2 catalysts - the influence of catalyst pre-treatment on the activity and deactivation in idealized reformate[J].Catalysis Letters,2007(3/4):105-115. |
[51] | Wu Z L;Zhou S H;Zhu H G;Dai S Overbury S H .[J].Journal of Physical Chemistry C,2009,113:3726. |
[52] | Tabakova T;Boccuzzi F;Manzoli M;Andreeva D .[J].Applied Catalysis A:General,2006,252:385. |
[53] | Concepción P;Carrettin S;Corma A .[J].Applied Catalysis A:General,2006,307:42. |
[54] | Park E D;Lee J S .[J].Journal of Catalysis,1999,186:1. |
[55] | Vindigni F;Manzoli M;Chiorino A;Boccuzzi F .[J].Gold Bulletin,2009,42:106. |
[56] | Costello C K;Guzman J;Yang J H;Wang Y M Kung M C Gates B C Kung H H .[J].Journal of Physical Chemistry B,2004,108:12529. |
[57] | Guzman J;Gates B C .[J].Journal of the American Chemical Society,2004,126:2672. |
[58] | Dekkers MAP.;Nieuwenhuys BE.;Lippits MJ. .CO adsorption and oxidation on Au/TiO2[J].Catalysis Letters,1998(4):195-197. |
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