以有序的中孔炭材料CMK-3为模板,以硝酸铈为前体,利用纳米铸型法合成了具有规则结构的中孔氧化铈,考察了模板脱除温度对中孔氧化铈微结构的影响.热重、元素分析、X射线衍射、透射电镜和氮气物理吸附结果表明,炭模板的脱除温度可低至350℃,所得氧化铈具有二维六方规则结构,比表面积高达167 m~2/g,孔径分布集中在3～5nm.采用胶体沉积法将2-5nm的金溶胶粒子沉积到所得氧化铈表面制得了Au/CeO_2催化剂,考察了Au/CeO_2在CO氧化反应中的活性.结果表明,该催化剂的活性较常规氧化铈制备的金催化利有明显提高,这可能与载体的规则结构有关.
Ordered mesoporous ceria oxides (CeO_2) were synthesized by nanocasting using ordered mesoporous carbon (CMK-3) as the template and cerium nitrate as the CeO_2 precursor. The as-prepared materials were characterized by thermogravimetry, elemental analysis, powder X-ray diffraction, transmission electron microscopy, and N_2 adsorption. The obtained ceria exhibits a 2-D hexagonal ordered structure with a high surface area of up to 167 m~2/g and pore size in the range of 3-5 nm. The carbon template can be completely removed at a temperature as low as 350 ℃. Such ceria was then employed as the support for the preparation of gold catalysts by the colloid deposition method. The catalytic activity of the Au/CeO_2 catalyst was evaluated in CO oxidation. An enhanced catalytic activity was observed over such a catalyst possibly due to the nano-sized particle and narrow pore size of the ordered mesoporous ceria.
参考文献
| [1] | Koichi E .[J].Journal of Alloys and Compounds,1997,250:486. |
| [2] | Park B E;Sakai I;Tokumitsu E;Ishiwara H .[J].Applied Surface Science,1997,117-118:423. |
| [3] | 赵波,王秋艳,葛昌华,李光凤,周仁贤.Ce0.67Zr0.33O2材料的制备和表征及其负载单Pd三效催化剂的性能[J].催化学报,2009(05):407-413. |
| [4] | Zhen Y D;Tok A I Y;Jiang S P;Boey FYC .[J].Journal of Power Sources,2008,178:69. |
| [5] | Jasinski P.;Suzuki T.;Anderson HU. .Nanocrystalline undoped ceria oxygen sensor[J].Sensors and Actuators, B. Chemical,2003(1/3):73-77. |
| [6] | 邵建军,张平,唐幸福,张保才,宋巍,徐奕德,申文杰.制备方法及焙烧温度对Co3O4/CeO2催化剂上CO低温氧化反应的影响[J].催化学报,2007(02):163-169. |
| [7] | 郑修成,张晓丽,王淑荣,于丽华,王向宇,吴世华.不同CuO/CeO2催化剂上CO低温氧化反应[J].催化学报,2005(11):971-976. |
| [8] | Shen W H;Dong X P;Zhu Y F;Chen H G Shi J L .[J].Mi-croporous Mesoporous Mater,2005,85:157. |
| [9] | 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. |
| [10] | Yuan Z Y;Idakiev V;Vantomme A;Tabakova T Ren T Z Su B L .[J].Catalysis Today,2008,131:203. |
| [11] | Scire S;Minico S;Crisafulli C;Satriano C Pistone A .[J].Applied Catalysis B:Environmental,2003,40:43. |
| [12] | Wang X Y;Wang S P;Wang S R;Zhao Y Q Huang J Zhang S M Huang W P Wu S H .[J].Catalysis Letters,2006,112:115. |
| [13] | Carrettin S;Concepcion P;Corma A;Nieto J M L,Puntes V F .[J].Angewandte Chemie International Edition,2004,43:2538. |
| [14] | Corma A;Domine ME .Gold supported on a mesoporous CeO2 matrix as an efficient catalyst in the selective aerobic oxidation of aldehydes in the liquid phase[J].Chemical communications,2005(32):4042-4044. |
| [15] | Yin L X;Wang Y Q;Pang G S;Koltypin Y Gedanken A .[J].Journal of Colloid and Interface Science,2002,246:78. |
| [16] | Xie X W;Li Y;Liu Z Q;Haruta M Shen W J .[J].Nature,2009,458:746. |
| [17] | Brezesinski T;Erpen C;Iimura K;Smarsly B .[J].Chemistry of Materials,2005,17:1683. |
| [18] | Lyons D M;McGrath J P;Morris M A .[J].Journal of Physical Chemistry B,2003,107:4607. |
| [19] | Lundberg M;Skarman B;Cesar F;Wallenberg L R .[J].Mi-croporous Mesoporous Mater,2002,54:97. |
| [20] | Terribile D;Trovarelli A;de Leitenburg C;Dolcetti G Llorca J .[J].Chemistry of Materials,1997,9:2676. |
| [21] | Lu A H;Schüth F .[J].Advanced Materials,2006,18:1793. |
| [22] | Rossinyol E;Arbiol J;Peir;o F Cornet A Morante J R Tian B Bo T Zhao D .[J].Sensors and Actuators B:Chemical,2005,109:57. |
| [23] | Laha S C;Ryoo R.[J].Chemical Communications,2003:2138. |
| [24] | Roggenbuck J;Schafer H;Tsoncheva T;Minchev C;Hanss J;Tiemann M .Mesoporous CeO2: Synthesis by nanocasting, characterisation and catalytic properties[J].Microporous and mesoporous materials: The offical journal of the International Zeolite Association,2007(3):335-341. |
| [25] | Lu AH;Li WC;Schmidt W;Kiefer W;Schuth F .Easy synthesis of an ordered mesoporous carbon with a hexagonally packed tubular structure[J].Carbon: An International Journal Sponsored by the American Carbon Society,2004(14):2939-2948. |
| [26] | Comotti M;Li WC;Spliethoff B;Schuth F .Support effect in high activity gold catalysts for CO oxidation[J].Journal of the American Chemical Society,2006(3):917-924. |
| [27] | Lu A H;Schmidt W;Taguchi A;Spliethoff B,Tesche B,Schuth F .[J].Angewandte Chemie International Edition,2002,41:3489. |
| [28] | Sun CW;Li H;Chen LQ .Study of flowerlike CeO2 microspheres used as catalyst supports for CO oxidation reaction[J].The journal of physics and chemistry of solids,2007(9):1785-1790. |
| [29] | Kozlow A I;Kozlova A P;Liu H C;Iwasawa Y .[J].Applied Catalysis A:General,1999,182:9. |
| [30] | Si R;Flytzani-Stephanopoulos M .[J].Angewandte Chemie International Edition,2008,47:2884. |
| [31] | Chen Z;Gao Q .[J].Applied Catalysis B:Environmental,2008,84:790. |
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