The catalytic activity and methanol tolerance of transition metal modified-ruthenium-selenium catalysts

被引:23
作者
Cheng, H. [1 ]
Yuan, W.
Scott, K.
Browning, D. J.
Lakeman, J. B.
机构
[1] Univ Newcastle Upon Tyne, Sch Chem Engn & Adv Mat, Newcastle Upon Tyne NE1 7RU, Tyne & Wear, England
[2] Def Sci & Technol Lab, Dept Phys Sci, Salisbury SP4 0QR, Wilts, England
基金
英国工程与自然科学研究理事会;
关键词
direct methanol fuel cells; oxygen reduction; methanol tolerant cathode catalysts; ruthenium-selenium-tungsten; ruthenium-selenium-molybdenum; ruthenium-selenium-rhodium;
D O I
10.1016/j.apcatb.2007.04.016
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
The activity of ruthenium-based catalysts towards oxygen reduction was enhanced by addition of tungsten, molybdenum and rhodium. The catalysts were produced by decarbonylation of the ruthenium and transition metal carbonyls in the presence of selenium (sulphur) and carbon powders. The produced materials were characterised by scanning electron microscopy and energy dispersive spectroscopy as well as by electrochemical evaluations in both half cells and direct methanol fuel cells. All transition metal-modified catalysts exhibited better performance than those of ruthenium-selenium (sulphur) alone, but the tungsten modification seemed the best approach. The RuSe0.20W0.29 catalyst delivered the maximum power density of up to 40 mW cm(-2). The improvement is a consequence of the enhanced activity towards oxygen reduction with a minor loss in methanol tolerance as well as a stabilising effect of tungsten on catalysts. The new catalysts were compared to Pt and to sulphur-containing catalysts. (c) 2007 Elsevier B.V. All rights reserved.
引用
收藏
页码:221 / 228
页数:8
相关论文
共 40 条
[11]   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
[12]  
GUSTAVO L, 2006, ELECTROCHIM ACTA, V51, P4061
[13]  
Hilgendorff M, 2002, J NEW MAT ELECTR SYS, V5, P71
[14]   Tungsten oxide as active matrix for dispersed carbon-supported RuSex nanoparticles:: Enhancement of the electrocatalytic oxygen reduction [J].
Kulesza, Pawel J. ;
Miecznikowski, Krzysztof ;
Baranowska, Beata ;
Skunik, Magdalena ;
Fiechter, Sebastian ;
Bogdanoff, Peter ;
Dorbandt, Iris .
ELECTROCHEMISTRY COMMUNICATIONS, 2006, 8 (05) :904-908
[15]   Tungsten oxides as active supports for highly dispersed platinum microcenters: Electrocatalytic reactivity toward reduction of hydrogen peroxide and oxygen [J].
Kulesza, PJ ;
Grzybowska, B ;
Malik, MA ;
Galkowski, MT .
JOURNAL OF THE ELECTROCHEMICAL SOCIETY, 1997, 144 (06) :1911-1917
[16]  
Laramie J, 2003, FUEL CELL SYSTEMS EX
[17]   Stability and electrocatalytic activity for oxygen reduction in WC plus Ta catalyst [J].
Lee, KC ;
Ishihara, A ;
Mitsushima, S ;
Kamiya, N ;
Ota, KI .
ELECTROCHIMICA ACTA, 2004, 49 (21) :3479-3485
[18]   METHANOL OXIDATION CHARACTERISTICS OF RARE-EARTH TUNGSTEN BRONZE ELECTRODES DOPED WITH PLATINUM [J].
MACHIDA, K ;
ENYO, M ;
ADACHI, G ;
SHIOKAWA, J .
JOURNAL OF THE ELECTROCHEMICAL SOCIETY, 1988, 135 (08) :1955-1961
[19]   Sol-gel derived WOx and WOx/Pt films for direct methanol fuel cell catalyst applications [J].
McLeod, EJ ;
Birss, VI .
ELECTROCHIMICA ACTA, 2005, 51 (04) :684-693
[20]   Novel Pt-free catalyst for oxygen electroreduction [J].
Meng, H ;
Shen, PK .
ELECTROCHEMISTRY COMMUNICATIONS, 2006, 8 (04) :588-594