Effect of the Dendrimer Generation Used in the Synthesis of Pt-Ru Nanoparticles Supported on Carbon Nanofibers on the Catalytic Activity towards Methanol Oxidation

被引:11
作者
Carlos Calderon, Juan [1 ]
Calvillo, Laura [2 ]
Jesus Lazaro, Maria [2 ]
Luis Rodriguez, Jose [1 ]
Pastor, Elena [1 ]
机构
[1] Univ La Laguna, Inst Mat & Nanotecnol, Dept Quim, Ave Astrofis Francisco Sanchez S-N, San Cristobal Laguna 38206, Spain
[2] CSIC, Inst Carboquim, Miguel Luesma Castan 4, Zaragoza 50018, Spain
关键词
Pt-Ru catalysts; carbon nanofibers; methanol electrochemical oxidation; dendrimers; fuel cells; MESOPOROUS CARBON; ELECTROCHEMICAL OXIDATION; METAL NANOPARTICLES; HYDROGEN-PRODUCTION; ENCAPSULATED PD; PLATINUM; ELECTROOXIDATION; CO; TEMPERATURE; ELECTROCATALYST;
D O I
10.3390/en10020159
中图分类号
TE [石油、天然气工业]; TK [能源与动力工程];
学科分类号
0807 ; 0820 ;
摘要
Pt-Ru nanoparticles supported on carbon nanofibers (CNF) were synthesized by the sodium borohydride reduction method, using different generation dendrimers (zero, one, two and three generations). After the synthesis process, these materials were submitted to a heat treatment at 350 degrees C, in order to clean the nanoparticle surface of organic residues. TEM characterization showed that the Pt-Ru nanoparticles size ranged between 1.9 and 5.5 nm. The use of dendrimers did not totally avoid the formation of aggregates, although monodisperse sizes were observed. The heat treatment produces the desired surface cleaning, although promoted the formation of agglomerates and crystalline Ru oxides. The study of the electrochemical activity towards the methanol oxidation displayed some clues about the influence of both the dendrimer generation and the presence of Ru oxides. Moreover, the apparent activation energy E-ap for this reaction was determined. The results showed a beneficial effect of the heat treatment on the methanol oxidation current densities for the materials synthesized with the biggest dendrimers, being the methanol deprotonation and COad diffusion the predominant rate determining steps (rds).
引用
收藏
页数:19
相关论文
共 78 条
[1]   Platinum Ruthenium Catalysts Supported on Carbon Xerogel for Methanol Electro-Oxidation: Influence of the Catalyst Synthesis Method [J].
Alegre, Cinthia ;
Elena Galvez, Maria ;
Moliner, Rafael ;
Baglio, Vincenzo ;
Stassi, Alessandro ;
Arico, Antonino Salvatore ;
Jesus Lazaro, Maria .
CHEMCATCHEM, 2013, 5 (12) :3770-3780
[2]   Oxygen-Functionalized Highly Mesoporous Carbon Xerogel Based Catalysts for Direct Methanol Fuel Cell Anodes [J].
Alegre, Cinthia ;
Elena Galvez, M. ;
Baquedano, Estela ;
Moliner, Rafael ;
Pastor, Elena ;
Jesus Lazaro, M. .
JOURNAL OF PHYSICAL CHEMISTRY C, 2013, 117 (25) :13045-13058
[3]  
ARDOIN N, 1995, B SOC CHIM FR, V132, P875
[4]   Nanocomposite catalysts: Dendrimer encapsulated nanoparticles immobilized in sol-gel silica [J].
Beakley, LW ;
Yost, SE ;
Cheng, R ;
Chandler, BD .
APPLIED CATALYSIS A-GENERAL, 2005, 292 :124-129
[5]   Synthesis of noble metal nanoparticles and their non-ordered superstructures [J].
Bigall, Nadja C. ;
Eychmueller, Alexander .
PHILOSOPHICAL TRANSACTIONS OF THE ROYAL SOCIETY A-MATHEMATICAL PHYSICAL AND ENGINEERING SCIENCES, 2010, 368 (1915) :1385-1404
[6]   About dendrimers: Structure, physical properties, and applications [J].
Bosman, AW ;
Janssen, HM ;
Meijer, EW .
CHEMICAL REVIEWS, 1999, 99 (07) :1665-1688
[7]   Carbon monoxide and methanol oxidations on carbon nanofibers supported Pt-Ru electrodes at different temperatures [J].
Calderon, C. ;
Garcia, G. ;
Querejeta, A. ;
Alcaide, F. ;
Calvillo, L. ;
Lazaro, M. J. ;
Rodriguez, J. L. ;
Pastor, E. .
ELECTROCHIMICA ACTA, 2015, 186 :359-368
[8]   Use of Dendrimers during the Synthesis of Pt-Ru Electrocatalysts for PEM Fuel Cells: Effects on the Physical and Electrochemical Properties [J].
Calderon, J. C. ;
Calvillo, L. ;
Lazaro, M. J. ;
Pastor, E. .
INTERNATIONAL JOURNAL OF ELECTROCHEMISTRY, 2011, 2011
[9]  
Calderon J. C., 2012, TECNOL MAT, V24, p[176, 179]
[10]   Electrochemical oxidation of CO and methanol on Pt-Ru catalysts supported on carbon nanofibers: the influence of synthesis method [J].
Calderona, J. C. ;
Garcia, G. ;
Calvillo, L. ;
Rodriguez, J. L. ;
Lazaro, M. J. ;
Pastor, E. .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2015, 165 :676-686