通过浸渍还原法制备了不同比例的Pt-Mo/SiO2催化剂，采用X射线衍射、透射电镜、X射线近边吸收谱和X射线光电子能谱表征了Pt-Mo/SiO2催化剂的组成、结构及价态。研究结果表明，少量MoOx修饰Pt-Mo/SiO2催化剂在低温水汽变换反应中表现出比Pt/SiO2催化剂更高的催化活性，过量MoOx包覆的Pt-Mo/SiO2催化剂活性较低。低温水汽变换反应活性来自于Pt与表面MoOx的界面协同作用，限域在Pt纳米颗粒表面的MoOx表现出较低价态，高分散MoOx纳米岛修饰的Pt纳米颗粒是低温水汽变换反应的活性结构。
Pt-Mo/SiO2 catalysts were prepared using impregnation-reduction methods. Mo-promoted Pt cata-lysts exhibit much higher water gas shift reaction activity at low temperatures than Pt/SiO2 cata-lysts. Various characterization methods including inductive coupled plasma atomic emission spec-trometry, X-ray diffraction, transmission electron microscopy, X-ray absorption near edge spec-trum, and X-ray photoelectron spectroscopy were applied to investigate the composition, structure and chemical state of the Pt-Mo/SiO2 catalysts. Our results indicate that the added Mo species effec-tively improves the dispersion of Pt nanoparticles and the synergistic effect between the Pt nano-particles and surface MoOxspecies enhances the catalytic performance for the water gas shift reac-tion. Pt nanoparticles decorated with highly dispersed MoOx patches are found to be the active ar-chitecture.
参考文献
| [1] | Guo P J;Chen L F;Yang Q Y;Qiao M H Li H Li H X Xu H L Fan K N .[J].International Journal of Hydrogen Energy,2009,34:2361. |
| [2] | Sagata K;Imazu N;Yahiro H .[J].Catalysis Today,2013,201:145. |
| [3] | Iida H;Ogawa D;Kumasaki T;Iida K Igarashi A .[J].Journal of Chemical Engineering of Japan,2012,45:46. |
| [4] | Andreeva D;Idakiev V;Tabakova T;Andreev A Giovanoli R .[J].Journal of Catalysis,1996,158:354. |
| [5] | Tibiletti D;Amieiro-Fonseca A;Burch R;Chen Y Fisher J M Goguet A Hardacre C Hu P Thompsett A .[J].Journal of Physical Chemistry B,2005,109:22553. |
| [6] | Kim C H;Thompson L T .[J].Journal of Catalysis,2005,230:66. |
| [7] | Panagiotopoulou P;Kondarides D I .[J].Journal of Catalysis,2004,225:327. |
| [8] | Gonzalez I D;Navarro R M;Alvarez-Galvan M C;Rosa F Fierro J L G .[J].CATALYSIS COMMUNICATIONS,2008,9:1759. |
| [9] | Panagiotopoulou P;Kondarides D I .[J].Catalysis Today,2006,112:49. |
| [10] | Ratnasamy C;Wagner J P .[J].CATALYSIS REVIEWS-SCIENCE AND ENGINEERING,2009,51:325. |
| [11] | Rodriguez J A;Ma S;Liu P;Hrbek J Evans J Perez M .[J].SCIENCE,2007,318:1757. |
| [12] | Fu Q;Li W X;Yao Y X;Liu H Y Su H Y Ma D Gu X K Chen L M Wang Z Zhang H Wang B Bao X H .[J].SCIENCE,2010,328:1141. |
| [13] | Liu Z F;Hu J E;Wang Q;Gaskell K Frenkel A I Jackson G S Eich-horn B .[J].Journal of the American Chemical Society,2009,131:6924. |
| [14] | Grgur B N;Markovic N M;Ross P N .[J].Journal of Physical Chemistry B,1998,102:2494. |
| [15] | Mukerjee S;Urian R C;Lee S J;Ticianelli E A McBreen J .[J].J Electro-chem Soc,2004,151:A1094. |
| [16] | Santiago E I;Camara G A;Ticianelli E A .[J].Electrochimica Acta,2003,48:3527. |
| [17] | Dorazio L;Ruettinger W;Castaldi M J;Farrauto R .[J].Topics in Catalysis,2008,51:68. |
| [18] | Ruettinger W;Liu X S;Xu X M;Farrauto R J .[J].Topics in Catalysis,2008,51:60. |
| [19] | Williams W D;Bollmann L;Miller J T;Delgass W N Ribeiro F H .[J].Applied Catalysis B:Environmental,2012,125:206. |
| [20] | Wang J G;Hammer B .[J].Journal of Catalysis,2006,243:192. |
| [21] | Bazin D;Sayers D;Rehr J J;Mottet C .[J].Journal of Physical Chemistry B,1997,101:5332. |
| [22] | Ichikuni N;Iwasawa Y .[J].Catalysis Letters,1993,20:87. |
| [23] | Behafarid F;Ono L K;Mostafa S;Croy J R Shafai G Hong S Rahman T S Bare S R Cuenya B R .[J].Physical Chemistry Chemical Physics,2012,14:11766. |
| [24] | Choi SH.;Lee JS. .XAFS CHARACTERIZATION OF PT-MO BIMETALLIC CATALYSTS FOR CO HYDROGENATION[J].Journal of Catalysis,1997(2):364-371. |
| [25] | Ma L;Zhao X;Si F Z;Liu C P Liao J H Liang L Xing W .[J].Electrochimica Acta,2010,55:9105. |
| [26] | Park J H;Kim Y T;Park E D;Lee H C Kim J Lee D .[J].ChemCatChem,2013,5:806. |
| [27] | Paal Z;Tetenyi P;Muhler M;Wild U Manoli J M Potvin C .[J].JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS,1998,94:459. |
| [28] | Deng, X;Quek, SY;Biener, MM;Biener, J;Kang, DH;Schalek, R;Kaxiras, E;Friend, CM .Selective thermal reduction of single-layer MoO3 nanostructures on Au(111)[J].Surface Science,2008(6):1166-1174. |
| [29] | Xu H;Fu Q;Guo X G;Bao X H .[J].ChemCatChem,2012,4:1645. |
| [30] | Zheng, F.;Alayoglu, S.;Guo, J.;Pushkarev, V.;Li, Y.;Glans, P.-A.;Chen, J.-L.;Somorjai, G. .In-situ X-ray Absorption Study of Evolution of Oxidation States and Structure of Cobalt in Co and CoPt Bimetallic Nanoparticles (4 nm) under Reducing (H_2) and Oxidizing (O_2) Environments[J].Nano letters,2011(2):847-853. |
| [31] | Sun D P;Gu X K;Ouyang R H;Su H Y Fu Q Bao X H Li W X .[J].J Phys Chem C,2012,116:7491. |
| [32] | Sakamoto T;Morishima H;Yoshida A;Naito S .[J].Catalysis Letters,2009,131:419. |
| [33] | Dietrich P J;Lobo-Lapidus R J;Wu T P;Sumer A Akatay M C Fingland B R Guo N Dumesic J A Marshall C L Stach E Jellinek J Delgass W N Ribeiro F H Miller J T .[J].Topics in Catalysis,2012,55:53. |
| [34] | Zafeiratos S;Papakonstantinou G;Jacksic MM;Neophytides SG .The effect of Mo oxides and TiO2 support on the chemisorption features of linearly adsorbed CO on Pt crystallites: an infrared and photoelectron spectroscopy study[J].Journal of Catalysis,2005(1):127-136. |
| [35] | Rodriguez JA;Liu R;Hrbek J;Perez M;Evans J .Water-gas shift activity of Au and Cu nanoparticles supported on molybdenum oxides[J].Journal of molecular catalysis, A. Chemical,2008(1/2):59-65. |
| [36] | Gao D F;Cai F;Xu Q Q;Wang G X Pan X L Bao X H .[J].J Energ Chem,2014,23:694. |
| [37] | Sakamoto T;Kikuchi H;Miyao T;Yoshida A Naito S .[J].Applied Catalysis A:General,2010,375:156. |
| [38] | Elezovic N R;Babic B M;Radmilovic V R;Gojkovic S L Krstajic N V Vracar L M .[J].Journal of Power Sources,2008,175:250. |
| [39] | Cui, Z.M.;Jiang, S.P.;Li, C.M. .Highly dispersed MoO_x on carbon nanotube as support for high performance Pt catalyst towards methanol oxidation[J].Chemical communications,2011(29):8418-8420. |
| [40] | Vellacheri R;Unni S M;Nahire S;Kharul U K Kurungot S .[J].Electro-chim Acta,2010,55:2878. |
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%