High throughput experimental and theoretical predictive screening of materials - A comparative study of search strategies for new fuel cell anode catalysts

被引:209
作者
Strasser, P
Fan, Q
Devenney, M
Weinberg, WH
Liu, P
Norskov, JK
机构
[1] Symyx Technol Inc, Santa Clara, CA 95051 USA
[2] Tech Univ Denmark, Dept Phys, Ctr Atom Scale Mat Phys, DK-2800 Lyngby, Denmark
关键词
D O I
10.1021/jp030508z
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 comparative study of experimental and theoretical combinatorial and high-throughput screening methods for the development of novel materials is presented. Both methods were applied to the development of new anode fuel cell alloy catalysts with improved CO tolerance. Combinatorial experimental electrocatalysis was performed on a 64-element electrode array. Sputter-deposited ternary thin-film electrocatalysts of composition PtRuM (NI = Co,Ni,W) were screened in parallel for their methanol oxidation activity, and their individual geometric and specific chronoamperometric current density were monitored and evaluated against standard PtRu catalysts. Density functional theory calculations of a variety of model ternary PtRuM alloy catalysts yielded detailed adsorption energies and activation barriers. Feeding these thermodynamic and kinetic data into a simple micro kinetic model for the CO electro oxidation reaction, the relative activities of a number of PtRuM ternary alloys were calculated. The experimental and theoretical computational results reveal very similar trends in electrocatalytic activity as a function of alloy composition; they also point at similar ternary PtRuM alloys as candidates for improved anode catalysts for low-temperature fuel cells.
引用
收藏
页码:11013 / 11021
页数:9
相关论文
共 41 条
  • [1] Design of a surface alloy catalyst for steam reforming
    Besenbacher, F
    Chorkendorff, I
    Clausen, BS
    Hammer, B
    Molenbroek, AM
    Norskov, JK
    Stensgaard, I
    [J]. SCIENCE, 1998, 279 (5358) : 1913 - 1915
  • [2] Formate, an active intermediate for direct oxidation of methanol on Pt electrode
    Chen, YX
    Miki, A
    Ye, S
    Sakai, H
    Osawa, M
    [J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2003, 125 (13) : 3680 - 3681
  • [3] INTERACTION OF HYDROGEN WITH SOLID-SURFACES
    CHRISTMANN, K
    [J]. SURFACE SCIENCE REPORTS, 1988, 9 (1-3) : 1 - 163
  • [4] Anode materials for low-temperature fuel cells: A density functional theory study
    Christoffersen, E
    Liu, P
    Ruban, A
    Skriver, HL
    Norskov, JK
    [J]. JOURNAL OF CATALYSIS, 2001, 199 (01) : 123 - 131
  • [5] The CO/Pt(111) puzzle
    Feibelman, PJ
    Hammer, B
    Norskov, JK
    Wagner, F
    Scheffler, M
    Stumpf, R
    Watwe, R
    Dumesic, J
    [J]. JOURNAL OF PHYSICAL CHEMISTRY B, 2001, 105 (18) : 4018 - 4025
  • [6] METHANOL ELECTROOXIDATION ON WELL-CHARACTERIZED PT-RN ALLOYS
    GASTEIGER, HA
    MARKOVIC, N
    ROSS, PN
    CAIRNS, EJ
    [J]. JOURNAL OF PHYSICAL CHEMISTRY, 1993, 97 (46) : 12020 - 12029
  • [7] Structural and electrochemical characterization of binary, ternary, and quaternary platinum alloy catalysts for methanol electro-oxidation
    Gurau, B
    Viswanathan, R
    Liu, RX
    Lafrenz, TJ
    Ley, KL
    Smotkin, ES
    Reddington, E
    Sapienza, A
    Chan, BC
    Mallouk, TE
    Sarangapani, S
    [J]. JOURNAL OF PHYSICAL CHEMISTRY B, 1998, 102 (49): : 9997 - 10003
  • [8] Hammer B., 1997, CHEMISORPTION REACTI
  • [9] Jandeleit B, 1999, ANGEW CHEM INT EDIT, V38, P2495
  • [10] Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
    Kresse, G
    Furthmuller, J
    [J]. COMPUTATIONAL MATERIALS SCIENCE, 1996, 6 (01) : 15 - 50