通过乙二醇还原,在Vulcan XC-72 炭黑上负载了三种具有不同平均粒径(1.7 nm,3.0 nm和5.0 nm)的Pt催化剂.利用透射电子显微镜,研究了载体炭黑表面的微孔与Pt催化剂之间的几何相互作用.结果表明:尺寸较小的Pt颗粒(平均粒径为1.7 nm)通常被包含在载体表面的微孔中,表现为被一薄碳层所覆盖并嵌入炭黑基体.而尺寸较大的Pt颗粒(平均粒径为3.0 nm和5.0 nm)则不存在这种现象,往往显示出裸露的清洁表面.这种与载体表面微孔的不同相互作用引起了Pt颗粒在电化学活性比表面上的反常尺寸效应,进而影响了其催化甲醇氧化的质量比活性.
Pt catalysts with different average particle sizes (1.7,3.0,and 5.0 nm) were supported on Vulcan XC-72 carbon black through ethylene glycol reduction of H_2PtCl_6.Using transmission electron microscopy,we found a geometric interaction between the micropores on the surface of carbon black support and the supported Pt catalysts.Small Pt nanoparticles (with an average particle size of 1.7 nm) were found to be frequently incorporated into the micropores,and thus appeared to be covered by a thin carbon layer and embedded in the carbon matrix.However,such a phenomenon was absent for Pt particles with larger average particle sizes (3.0 and 5.0 nm),which generally showed an exposed clean surface.The different interaction with the micropores therefore induced an abnormal particle size effect of the supported Pt catalysts on their electrochemically active surface area,and had an influence on their mass electrocatalytic activity towards methanol oxidation.
参考文献
| [1] | J. Guo;G. San;Q. Wang .Carbon nanofibers supported Pt-Ru electrocatalysts for direct methanol fuel cells[J].Carbon: An International Journal Sponsored by the American Carbon Society,2006(1):152-157. |
| [2] | U. A. Paulus;A. Wokaun;G. G. Scherer;T. J. Schmidt;V. Stamenkovic;V. Radmilovic;N. M. Markovic;P. N. Ross .Oxygen Reduction on Carbon-Supported Pt-Ni and Pt-Co Alloy Catalysts[J].The journal of physical chemistry, B. Condensed matter, materials, surfaces, interfaces & biophysical,2002(16):4181-4191. |
| [3] | Wenzhen Li;Changhai Liang;Weijiang Zhou;Jieshan Qiu;Zhenhua Zhou;Gongquan Sun;Qin Xin .Preparation and Characterization of Multiwalled Carbon Nanotube-Supported Platinum for Cathode Catalysts of Direct Methanol Fuel Cells[J].The journal of physical chemistry, B. Condensed matter, materials, surfaces, interfaces & biophysical,2003(26):6292-6299. |
| [4] | 杜鸿达,李宝华,干林,吴鹏,康飞宇,曾毓群.炭气凝胶负载PtRu纳米颗粒用作甲醇氧化催化剂[J].新型炭材料,2008(01):58-62. |
| [5] | 黄宇晴,邱新平,朱文涛.PREPARATION OF SUPPORTED Pt FROM INTERCALATION COMPOUNDS[J].新型炭材料,2001(01):10-14. |
| [6] | Kleber Bergamaski;Alexei L.N.Pinheiro;Erico Teixeira-Neto .Nanoparticle Size Effects on Methanol Electrochemical Oxidation on Carbon Supported Platinum Catalysts[J].The journal of physical chemistry, B. Condensed matter, materials, surfaces, interfaces & biophysical,2006(39):19271-19279. |
| [7] | Xiang Li;Wei-Xiang Chen;Jie Zhao .Microwave polyol synthesis of Pt/CNTs catalysts: Effects of pH pH particle size and electrocatalytic activity for methanol electrooxidization[J].Carbon: An International Journal Sponsored by the American Carbon Society,2005(10):2168-2174. |
| [8] | Frelink T.;Vanveen JAR.;Visscher W. .PARTICLE SIZE EFFECT OF CARBON-SUPPORTED PLATINUM CATALYSTS FOR THE ELECTROOXIDATION OF METHANOL[J].Journal of Electroanalytical Chemistry: An International Journal Devoted to All Aspects of Electrode Kinetics, Interfacial Structure, Properties of Electrolytes, Colloid and Biological Electrochemistry,1995(1/2):65-72. |
| [9] | Mukerjee S;McBreen J .Effect of particle size on the electrocatalysis by carbon-supported Pt electrocatalysts:an in situ XAS investigation[J].Journal of Electroanalytical Chemistry,1999,448(02):163-171. |
| [10] | Joelma Perez;E. R. Gonzalez;E. A. Ticianelli .Oxygen electrocatalysis on thin porous coating rotating platinum electrodes[J].Electrochimica Acta,1998(8/9):1329-1339. |
| [11] | Bernal S;Calvino JJ;Cauqui MA et al.Some contributions of electron microscopy to the characterization of the strong metal-support interaction effect[J].Catalysis Today,2003,77(04):385-406. |
| [12] | In-Su Park;Kyung-Won Park;Jong-Ho Choi .Electrocatalytic enhancement of methanol oxidation by graphite nanofibers with a high loading of PtRu alloy nanoparticles[J].Carbon: An International Journal Sponsored by the American Carbon Society,2007(1):28-33. |
| [13] | Christina Bock;Chantal Paquet;Martin Couillard;Gianluigi A.Botton;Barry R.MacDougall .Size-Selected Synthesis of PtRu Nano-Catalysts:Reaction and Size Control Mechanism[J].Journal of the American Chemical Society,2004(25):8028-8037. |
| [14] | Zerda T W;Qian J;Pantea C et al.Structure of carbon blacks[J].Materials Research Society Symposium Proceedings,2001,661:KK6.4.1-KK6.6.8. |
| [15] | F.Stoeckli;A.Guillot;A.M.Slasli;D.Hugi-Cleary .Microporosity in carbon blacks[J].Carbon: An International Journal Sponsored by the American Carbon Society,2002(2):211-215. |
| [16] | Daley MA.;Economy J.;Hippo EJ.;Tandon D. .ELUCIDATING THE POROUS STRUCTURE OF ACTIVATED CARBON FIBERS USING DIRECT AND INDIRECT METHODS[J].Carbon: An International Journal Sponsored by the American Carbon Society,1996(10):1191-1200. |
| [17] | Liu J .Advanced electron microscopy characterizaiton of nanostructured heterogenous catalysts[J].Microscopy and Microanalysis,2003,10:55-76. |
| [18] | Yangchuan Xing .Synthesis and Electrochemical Characterization of Uniformly-Dispersed High Loading Pt Nanoparticles on Sonochemically-Treated Carbon Nanotubes[J].The journal of physical chemistry, B. Condensed matter, materials, surfaces, interfaces & biophysical,2004(50):19255-19259. |
| [19] | Ruizhi Yang;Zhaoxiang Wang;Xuejie Huang;Liquan Chen;Xinping Qiu;Huairuo Zhnag .Monodispersed hard carbon spherules as a catalyst support for the electrooxidation of methanol[J].Carbon: An International Journal Sponsored by the American Carbon Society,2005(1):11-16. |
| [20] | Gottesfeld S;Raistrick I D;Srinivasan S .Oxygen reduction kinetics on a platinum RDE coated with a recast Nafion film[J].Journal of the Electrochemical Society,1987,134(06):1455-1462. |
- 下载量()
- 访问量()
- 您的评分：
-
10%
-
20%
-
30%
-
40%
-
50%