Au/Ce1-xZrxO2催化剂的制备、表征及其在CO氧化和水煤气变换反应中的催化性能

催化学报 , 2008, 29(2): 134-140.

Au/Ce1-xZrxO2催化剂的制备、表征及其在CO氧化和水煤气变换反应中的催化性能

廖卫平 ^1, , 董园园 ^2, , 金明善 ^3, , 何涛 ^4, , 索掌怀 ^5,

1.烟台大学应用催化研究所,山东烟台,264005

2.烟台大学应用催化研究所,山东烟台,264005

3.烟台大学应用催化研究所,山东烟台,264005

4.烟台大学应用催化研究所,山东烟台,264005

5.烟台大学应用催化研究所,山东烟台,264005

基金项目: 山东省自然科学基金(Y2004B07) 国家自然科学基金(20473070)

关键词：氧化铈 , 氧化锆 , 复合氧化物 , 金催化剂 , 一氧化碳氧化 , 水煤气变换

Preparation and Characterization of Au/Ce1-xZrxO2 Catalysts and Their Catalytic Performance for CO Oxidation and Water-Gas Shift Reaction

采用共沉淀法制备了不同锆铈摩尔比的Ce1-xZrxO2(x=0, 0.1, 0 .3, 0.5, 0.7, 0.9和1.0)氧化物,并以改性的浸渍法制备了金担载量为1%(质量分数) 的Au/Ce1-xZrxO2催化剂. 考察了催化剂在低温CO氧化和水煤气变换反应中的催化性能. 应用氮物理吸附、X射线衍射、透射电镜和H2程序升温还原等技术对氧化物载体及其负载金催化剂进行了表征,并与其催化性能进行了关联. 结果表明,与纯CeO 2和ZrO2相比, Ce1-xZrxO2的比表面积增大而孔径减小,孔分布更加集中. Zr的加入使表面Ce4+的还原更加困难,使体相Ce4+的还原更加容易. 活性组分金的加入有利于铈锆氧化物的还原. ZrO2载体较大的孔径使金在载体表面分散均匀而粒子较小,因此与Au/CeO2和Au/Ce1-xZrxO2相比, Au/ZrO2具有更好的低温CO氧化活性和水煤气变换活性,而Au/Ce1-xZrxO2在高温下的水煤气变换反应中表现出更好的催化性能.

参考文献

[1]	Thammachart M;Meeyoo V;Risksomboon T;Osuwan S .[J].Catalysis Today,2001,68(1-3):53.
[2]	Gutiérrez-Ortiz J I;de Rivas B;López-Fonseca R;González-Velasco J R .[J].Applied Catalysis B:Environmental,2006,65(3-4):191.
[3]	叶青,徐柏庆.Ce1-xZrxO2的氧化还原性能及其对CO2重整CH4反应的影响[J].催化学报,2006(02):151-156.
[4]	Ye Q;Gao Q;Zhang X R;Xu B Q .[J].Catalysis Communications,2006,7(08):589.
[5]	Fornasiero P;Kapar J;Graziani M .[J].Journal of Catalysis,1997,167(02):576.
[6]	Hickey N;Fornasiero P;Kapar J;Gatica J M,Bernal S .[J].Journal of Catalysis,2001,200(01):181.
[7]	Fornasiero P.;Kaspar J.;L'Erario F.;Graziani M.;Rao GR. .Reduction of NO by CO over Rh/CeO2-ZrO2 catalysts - Evidence for a support-promoted catalytic activity[J].Journal of Catalysis,1998(2):269-279.
[8]	Ruettinger W;Liu XS;Farrauto RJ .Mechanism of aging for a Pt/CeO2-ZrO2 water gas shift catalyst[J].Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications,2006(1/2):135-141.
[9]	Pengpanich S;Meeyoo V;Rirksomboon T .[J].Catalysis Today,2004,93-95:95.
[10]	Huijun Wan,Xiujin Li,Shengfu Ji,Bingyao Huang,Kai Wang,Chengyue Li.Effect of Ni Loading and CexZr1-xO2 Promoter on Ni-Based SBA-15 Catalysts for Steam Reforming of Methane[J].天然气化学（英文版）,2007(02):139-147.
[11]	Cortie M B;van der Lingen E .[J].Materials Forum,2002,26(01):1.
[12]	Hashmi A S K;Hutchings G J .[J].Angewandte Chemie International Edition,2006,45(47):7896.
[13]	Wang S P;Zhang T Y;Wang X Y;Zhang S M Wang S R Huang W P Wu S H .[J].Journal of Molecular Catalysls A:Chemical,2007,272(1-2):45.
[14]	Tibiletti D;Amieiro-Fonseca A;Burch R;Chen Y Fisher J M Goguet A Hardacre C Hu P Thompsett D .[J].Journal of Physical Chemistry B,2005,109(47):225-253.
[15]	Goguet A;Burch R;Chen Y;Hardacre C Hu P Joyner R W Meunier F C Mu n B S Thompsett D Tibiletti D .[J].Journal of Physical Chemistry C,2007,111(45):16927.
[16]	索掌怀,翁永根,金明善,吕爱花,徐金光,安立敦.金溶液pH值及浸泡处理对Au/Al2O3催化剂上CO氧化反应活性的影响[J].催化学报,2005(11):1022-1026.
[17]	Tsai H Y;Lin Y D;Fu W T;Lin S D .[J].Gold Bulletin,2007,40(03):184.
[18]	Zanella R;Delannoy L;Louis C .Mechanism of deposition of gold precursors onto TiO2 during the preparation by cation adsorption and deposition-precipitation with NaOH and urea[J].Applied Catalysis, A. General: An International Journal Devoted to Catalytic Science and Its Applications,2005(1/2):62-72.
[19]	Letichevsky S;Tellez CA;de Avillez RR;da Silva MIP;Fraga MA;Appel LG .Obtaining CeO2-ZrO2 mixed oxides by coprecipitation: role of preparation conditions[J].Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications,2005(3/4):203-210.
[20]	Si R;Zhang Y W;Li S J;Lin B X Yan C H .[J].Journal of Physical Chemistry B,2004,108(33):12481.
[21]	Chen Y Z;Liaw B J;Chen H C .[J].International Journal of Hydrogen Energy,2006,31(03):427.
[22]	Fu Q;Deng WL;Saltsburg H;Flytzani-Stephanopoulos M .Activity and stability of low-content gold-cerium oxide catalysts for the water-gas shift reaction[J].Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications,2005(1/2):57-68.
[23]	Hutchings G J;Hall M S;Carley A F;Landon P Solsona B E Kiely C J H erzing A Makkee M Moulijn J A Overweg A Fierro-Gonzalez J C Guzman J Gate s B C .[J].Journal of Catalysis,2006,242(01):71.
[24]	Idakiev V;Tabakova T;Naydenov A;Yuan ZY;Su BL .Gold catalysts supported on mesoporous zirconia for low-temperature water-gas shift reaction[J].Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications,2006(3/4):178-186.
[25]	Burch R .[J].Physical Chemistry Chemical Physics,2006,8(47):5483.
[26]	Kim C H;Thompson L T .[J].Journal of Catalysis,2005,230(01):66.

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