Combinatorial discovery of bifunctional oxygen reduction — water oxidation electrocatalysts for regenerative fuel cells

Abstract Electrode arrays containing 715 unique combinations of five elements (Pt, Ru, Os, Ir, and Rh) were prepared by borohydride reaction of aqueous metal salts, and were screened for activity as oxygen reduction and water oxidation catalysts. Using a consensus map, catalysts that showed high activity for both reactions and good resistance to anodic corrosion were identified in the Pt–Ru rich region of the Pt–Ru–Ir ternary. The ternary catalyst Pt4.5Ru4Ir0.5 (subscripts indicate atomic ratios) is significantly more active than the previously described Pt1Ir1 bifunctional catalyst for both reactions. While the best ternary catalyst is close to Pt1Ru1 in composition, the latter is unstable with respect to anodic corrosion. A detailed kinetic comparison of anodically stable catalysts Pt4.5Ru4Ir0.5 and Pt1Ir1 showed that the addition of the oxophilic element Ru increases the reaction rate by stabilizing S–O bonds ( S ≡ surface atom ) and accelerating the oxidative deprotonation of S–OH groups.

[1]  Gustaf Arrhenius,et al.  X-ray diffraction procedures for polycrystalline and amorphous materials , 1955 .

[2]  Anghaie Proceedings of the 33. intersociety energy conversion engineering conference , 1998 .

[3]  Fred Mitlitsky,et al.  Integrated Modular Propulsion and Regenerative Electro-energy Storage System (IMPRESS) for small satellites , 1996 .

[4]  H. Scheffé Experiments with Mixtures , 1958 .

[5]  Remo Guidieri Res , 1995, RES: Anthropology and Aesthetics.

[6]  Andrew G. Glen,et al.  APPL , 2001 .

[7]  M. Agha,et al.  Experiments with Mixtures , 1992 .

[8]  P. A. Barnes,et al.  A new approach to the statistical optimisation of catalyst preparation , 1992 .

[9]  B. Brinkworth Solar energy , 1974, Nature.

[10]  Leonardo A. B. Tôrres,et al.  Simulation of a solar-hydrogen-fuel cell system : Results for different locations in Mexico , 1998 .

[11]  J. Morken,et al.  Thermographic selection of effective catalysts from an encoded polymer-bound library , 1998, Science.

[12]  G. G. Stokes "J." , 1890, The New Yale Book of Quotations.

[13]  Alan Cooper,et al.  REACTIVE DYES AS A METHOD FOR RAPID SCREENING OF HOMOGENEOUS CATALYSTS , 1998 .

[14]  E. Cairns,et al.  Direct Anodic Oxidation of Methanol on Supported Platinum/Ruthenium Catalyst in Aqueous Cesium Carbonate , 1995 .

[15]  Shimshon Gottesfeld,et al.  Thin-film catalyst layers for polymer electrolyte fuel cell electrodes , 1992 .

[16]  B. Yi,et al.  Bifunctional electrodes with a thin catalyst layer for `unitized' proton exchange membrane regenerative fuel cell , 1999 .

[17]  W. H. Weinberg,et al.  High-Throughput Synthesis and Screening of Combinatorial Heterogeneous Catalyst Libraries. , 1999, Angewandte Chemie.

[18]  J. Bockris Kinetics of Activation Controlled Consecutive Electrochemical Reactions: Anodic Evolution of Oxygen , 1956 .

[19]  Jandeleit,et al.  Combinatorial Materials Science and Catalysis. , 1999, Angewandte Chemie.

[20]  M. Barak,et al.  Power Sources 4 , 1974 .

[21]  S. Golunski,et al.  Synthesis of higher alcohols over copper/cobalt catalysts , 1989 .

[22]  Dan Luss,et al.  Infrared Thermographic Screening of Combinatorial Libraries of Heterogeneous Catalysts , 1996 .

[23]  C. Iwakura,et al.  Anodic evolution of oxygen on ruthenium in acidic solutions , 1977 .

[24]  Márcio Nele,et al.  Composition effects on the activity of Cu–ZnO–Al2O3 based catalysts for the water gas shift reaction: A statistical approach , 1998 .

[25]  Anthony B. LaConti,et al.  Proton-exchange membrane regenerative fuel cells , 1994 .

[26]  N. Ibl Kalte Verbrennung; fuel cells : E. W. Justi and A. W. Winsel, 397 pages, DM 64 = ca. 16 $, F. Steiner Verlag, Wiesbaden (Germany). , 1963 .

[27]  Manfred T Reetz,et al.  Time-Resolved IR-Thermographic Detection and Screening of Enantioselectivity in Catalytic Reactions. , 1998, Angewandte Chemie.

[28]  Reddington,et al.  Combinatorial electrochemistry: A highly parallel, optical screening method for discovery of better electrocatalysts , 1998, Science.

[29]  C. Hill,et al.  The first combinatorially prepared and evaluated inorganic catalysts. Polyoxometalates for the aerobic oxidation of the mustard analog tetrahydrothiophene (THT) , 1996 .

[30]  Ralph E. White,et al.  Comprehensive Treatise of Electrochemistry , 1981 .

[31]  G. Tamizhmani,et al.  A rapid half-cell technique for the pre-screening of polymer fuel cell catalysts , 1998 .

[32]  S. Trasatti,et al.  Electrocatalytic properties of ternary oxide mixtures of composition Ru0.3Ti(0.7−x)CexO2: oxygen evolution from acidic solution , 1996 .

[33]  H. Dhar,et al.  A unitized approach to regenerative solid polymer electrolyte fuel cells , 1993 .

[34]  Selim M. Senkan,et al.  High-throughput screening of solid-state catalyst libraries , 1998, Nature.

[35]  A. Damjanović,et al.  Kinetics of oxygen evolution and dissolution on platinum electrodes , 1966 .

[36]  P. Lehman,et al.  Operating experience with a photovoltaic-hydrogen energy system , 1997 .

[37]  Brian E. Conway,et al.  Modern Aspects of Electrochemistry , 1974 .

[38]  Ø. Ulleberg,et al.  TRNSYS simulation models for solar-hydrogen systems , 1997 .

[39]  Hinderling,et al.  Rapid Screening of Olefin Polymerization Catalyst Libraries by Electrospray Ionization Tandem Mass Spectrometry. , 1999, Angewandte Chemie.