Effect of redox state of PtRu electrocatalysts on methanol oxidation activity

被引:70
作者
Sirk, AHC
Hill, JM
Kung, SKY
Birss, VI
机构
[1] Univ Calgary, Dept Chem, Calgary, AB T2N 1N4, Canada
[2] Univ Calgary, Dept Chem & Petr Engn, Calgary, AB T2N 1N4, Canada
关键词
D O I
10.1021/jp036602x
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
PtRu is a promising catalyst for methanol oxidation in direct methanol fuel cells. However, the most active Pt:Ru ratio and oxidation state of the Ru component are still under investigation. PtRu black was obtained from Johnson Matthey, and the as-received catalyst was treated with either hydrogen or oxygen at elevated temperatures to alter the oxidation state. The samples were characterized by cyclic voltarnmetry (CV), thermogravimetric analysis (TGA), transmission electron microscopy (TEM), and X-ray diffraction (XRD) to confirm their redox states and for correlation with their methanol oxidation activity. All of the characterization techniques support successful oxidation and reduction of the PtRu catalyst. The methanol oxidation activity was measured, and the sequence at 25 degreesC was found to be reduced > as-received > oxidized much greater than strongly oxidized. The effect of the drying regime and the dispersing agent for the catalysts was also investigated, and it was found that samples supported using acetic acid were more active than those supported by Nafion, but were less stable and more susceptible to change in catalyst state from heat gun drying.
引用
收藏
页码:689 / 695
页数:7
相关论文
共 24 条
[1]   Platinum-macrocycle co-catalysts for the electrochemical oxidation of methanol [J].
Bett, JS ;
Kunz, HR ;
Aldykiewicz, AJ ;
Fenton, JM ;
Bailey, WF ;
McGrath, DV .
ELECTROCHIMICA ACTA, 1998, 43 (24) :3645-3655
[2]   ELECTRON-MICROSCOPY STUDY OF FORMATION OF THICK OXIDE-FILMS ON IR AND RU ELECTRODES [J].
BIRSS, V ;
MYERS, R ;
ANGERSTEINKOZLOWSKA, H ;
CONWAY, BE .
JOURNAL OF THE ELECTROCHEMICAL SOCIETY, 1984, 131 (07) :1502-1510
[3]   The electro-oxidation of carbon monoxide on ruthenium modified Pt(111) [J].
Davies, JC ;
Hayden, BE ;
Pegg, DJ ;
Rendall, ME .
SURFACE SCIENCE, 2002, 496 (1-2) :110-120
[4]   Improvement of the high energy ball-milling preparation procedure of CO tolerant Pt and Ru containing catalysts for polymer electrolyte fuel cells [J].
Denis, MC ;
Gouérec, P ;
Guay, D ;
Dodelet, JP ;
Lalande, G ;
Schulz, R .
JOURNAL OF APPLIED ELECTROCHEMISTRY, 2000, 30 (11) :1243-1253
[5]   Electrocatalysis in direct methanol fuel cells: in-situ probing of PtRu anode catalyst surfaces [J].
Dinh, HN ;
Ren, XM ;
Garzon, FH ;
Zelenay, P ;
Gottesfeld, S .
JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 2000, 491 (1-2) :222-233
[6]   TEMPERATURE-DEPENDENT METHANOL ELECTROOXIDATION ON WELL-CHARACTERIZED PT-RU ALLOYS [J].
GASTEIGER, HA ;
MARKOVIC, N ;
ROSS, PN ;
CAIRNS, EJ .
JOURNAL OF THE ELECTROCHEMICAL SOCIETY, 1994, 141 (07) :1795-1803
[7]   Binary and ternary anode catalyst formulations including the elements W, Sn and Mo for PEMFCs operated on methanol or reformate gas [J].
Gotz, M ;
Wendt, H .
ELECTROCHIMICA ACTA, 1998, 43 (24) :3637-3644
[8]   Electrooxidation of H2, CO and H2/CO mixtures on a well-characterized Pt-Re bulk alloy electrode and comparison with other Pt binary alloys [J].
Grgur, BN ;
Markovic, NM ;
Ross, PN .
ELECTROCHIMICA ACTA, 1998, 43 (24) :3631-3635
[9]   Methanol oxidation on PtRu electrodes. Influence of surface structure and Pt-Ru atom distribution [J].
Iwasita, T ;
Hoster, H ;
John-Anacker, A ;
Lin, WF ;
Vielstich, W .
LANGMUIR, 2000, 16 (02) :522-529
[10]  
Lamy C, 1996, ELEC SOC S, V96, P356