A Methanol-Tolerant Carbon-Supported Pt-Au Alloy Cathode Catalyst for Direct Methanol Fuel Cells and Its Evaluation by DFT

被引:136
作者
Selvarani, G. [1 ]
Selvaganesh, S. Vinod [1 ]
Krishnamurthy, S. [1 ]
Kiruthika, G. V. M. [1 ]
Sridhar, P. [1 ]
Pitchumani, S. [1 ]
Shukla, A. K. [1 ,2 ]
机构
[1] Cent Electrochem Res Inst, Karaikkudi 630006, Tamil Nadu, India
[2] Indian Inst Sci, Solid State & Struct Chem Unit, Bangalore 560012, Karnataka, India
关键词
OXYGEN REDUCTION REACTION; DENSITY-FUNCTIONAL THEORY; AUGMENTED-WAVE METHOD; GOLD NANOPARTICLES; ULTRASOFT PSEUDOPOTENTIALS; ELECTROCATALYTIC REDUCTION; NI ALLOYS; ELECTRODES; POLYMER; DMFCS;
D O I
10.1021/jp810970d
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
A Pt-Au alloy catalyst of varying compositions is prepared by codeposition of Pt and An nanoparticles onto a carbon support to evaluate its electrocatalytic activity toward an oxygen reduction reaction (ORR) with methanol tolerance in direct methanol fuel cells. The optimum atomic weight ratio of Pt to Au in the carbon-supported Pt-Au alloy (Pt-Au/C) as established by cell polarization, linear-sweep voltammetry (LSV), and cyclic voltammetry (CV) studies is determined to be 2: 1. A direct methanol fuel cell (DMFC) comprising a carbon-supported Pt-Au (2: 1) alloy as the cathode catalyst delivers a peak power density of 120 mW/cm(2) at 70 degrees C in contrast to the peak power density value of 80 mW/cm(2) delivered by the DMFC with carbon-supported Pt catalyst operating under identical conditions. Density functional theory (DFT) calculations on a small model cluster reflect electron transfer from Pt to Au within the alloy to be responsible for the synergistic promotion of the oxygen-reduction reaction on a Pt-Au electrode.
引用
收藏
页码:7461 / 7468
页数:8
相关论文
共 59 条
[1]   Dynamics of Surface Exchange Reactions Between Au and Pt for HER and HOR [J].
Abrams, Billie L. ;
Vesborg, Peter C. K. ;
Bonde, Jacob L. ;
Jaramillo, Thomas F. ;
Chorkendorff, Ib .
JOURNAL OF THE ELECTROCHEMICAL SOCIETY, 2009, 156 (02) :B273-B282
[2]   Carbon supported Pt75M25 (M = Co, Ni) alloys as anode and cathode electrocatalysts for direct methanol fuel cells [J].
Antolini, E ;
Salgado, JRC ;
Gonzalez, ER .
JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 2005, 580 (01) :145-154
[3]   Carbon-supported Pt-Ni alloys prepared by the borohydride method as electrocatalysts for DMFCs [J].
Antolini, E ;
Salgado, JRC ;
dos Santos, AM ;
Gonzalez, ER .
ELECTROCHEMICAL AND SOLID STATE LETTERS, 2005, 8 (04) :A226-A230
[4]  
Aricò AS, 2001, FUEL CELLS, V1, P133
[5]   PROJECTOR AUGMENTED-WAVE METHOD [J].
BLOCHL, PE .
PHYSICAL REVIEW B, 1994, 50 (24) :17953-17979
[6]   INFLUENCE OF THE PH ON THE CATALYTIC REDUCTION OF OXYGEN TO HYDROGEN-PEROXIDE AT CARBON ELECTRODES MODIFIED BY AN ADSORBED ANTHRAQUINONE POLYMER [J].
DEGRAND, C .
JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 1984, 169 (1-2) :259-268
[7]   An extraordinary electrocatalytic reduction of oxygen on gold nanoparticles-electrodeposited gold electrodes [J].
El-Deab, MS ;
Ohsaka, T .
ELECTROCHEMISTRY COMMUNICATIONS, 2002, 4 (04) :288-292
[8]   Electrocatalysis by nanoparticles: oxygen reduction on gold nanoparticles-electrodeposited platinum electrodes [J].
El-Deab, MS ;
Ohsaka, T .
JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 2003, 553 :107-115
[9]   Fe-modified, Pt-based cathodic electrocatalysts for oxygen reduction reaction with enhanced methanol tolerance [J].
Gong, Yanming ;
Yeboah, Yaw D. ;
Lvov, Serguei N. ;
Balashov, Victor ;
Wang, Zhicheng .
JOURNAL OF THE ELECTROCHEMICAL SOCIETY, 2007, 154 (06) :B560-B565
[10]   Intraalloy Electron Transfer and Catalyst Performance: A Spectroscopic and Electrochemical Study [J].
Goodenough, John B. ;
Manoharan, R. ;
Shukla, A. K. ;
Ramesh, K., V .
CHEMISTRY OF MATERIALS, 1989, 1 (04) :391-398