Elucidating the activity of stepped Pt single crystals for oxygen reduction

被引:96
作者
Bandarenka, Aliaksandr S. [1 ]
Hansen, Heine A. [2 ]
Rossmeisl, Jan [3 ]
Stephens, Ifan E. L. [4 ]
机构
[1] Ctr Electrochem Sci CES, D-44780 Bochum, Germany
[2] Tech Univ Denmark, Dept Energy Convers & Storage, DK-4000 Roskilde, Denmark
[3] Tech Univ Denmark, Dept Phys, Ctr Atom Scale Mat Design, DK-2800 Lyngby, Denmark
[4] Tech Univ Denmark, Dept Phys, Ctr Individual Nanoparticle Funct, DK-2800 Lyngby, Denmark
基金
新加坡国家研究基金会;
关键词
FUEL-CELL CATHODE; PLATINUM SURFACES; ACIDIC MEDIA; N(111)-(100) SERIES; METAL-SURFACES; ELECTROCATALYSIS; WATER; SIZE; NANOPARTICLES; ELECTRODES;
D O I
10.1039/c4cp00260a
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 unexpectedly high measured activity of Pt[n(111) x (111)] and Pt[n(111) x (100)] stepped single crystal surfaces towards the oxygen reduction reaction (ORR) is explained utilizing the hydroxyl binding energy as the activity descriptor. Using this descriptor (estimated using experimental data obtained by different groups), a well-defined Sabatier-type volcano is observed for the activities measured for the Pt[n(111) x (111)] and Pt[n(111) x (100)] stepped single crystals, in remarkable agreement with earlier theoretical studies. We propose that the observed destabilisation of *OH species at these surfaces is due to the decreased solvation of the adsorbed hydroxyl intermediates on adjacent terrace sites.
引用
收藏
页码:13625 / 13629
页数:5
相关论文
共 46 条
[1]   Scaling properties of adsorption energies for hydrogen-containing molecules on transition-metal surfaces [J].
Abild-Pedersen, F. ;
Greeley, J. ;
Studt, F. ;
Rossmeisl, J. ;
Munter, T. R. ;
Moses, P. G. ;
Skulason, E. ;
Bligaard, T. ;
Norskov, J. K. .
PHYSICAL REVIEW LETTERS, 2007, 99 (01)
[2]   Probing adsorption phenomena on a single crystal Pt-alloy surface under oxygen reduction reaction conditions [J].
Bondarenko, Alexander S. ;
Stephens, Ifan E. L. ;
Bech, Lone ;
Chorkendorff, Ib .
ELECTROCHIMICA ACTA, 2012, 82 :517-523
[3]   The Pt(111)/Electrolyte Interface under Oxygen Reduction Reaction Conditions: An Electrochemical Impedance Spectroscopy Study [J].
Bondarenko, Alexander S. ;
Stephens, Ifan E. L. ;
Hansen, Heine A. ;
Perez-Alonso, Francisco J. ;
Tripkovic, Vladimir ;
Johansson, Tobias P. ;
Rossmeisl, Jan ;
Norskov, Jens K. ;
Chorkendorff, Ib .
LANGMUIR, 2011, 27 (05) :2058-2066
[4]   Tailoring the catalytic activity of electrodes with monolayer amounts of foreign metals [J].
Calle-Vallejo, Federico ;
Koper, Marc T. M. ;
Bandarenka, Aliaksandr S. .
CHEMICAL SOCIETY REVIEWS, 2013, 42 (12) :5210-5230
[5]   Direct observation of the oxygenated species during oxygen reduction on a platinum fuel cell cathode [J].
Casalongue, Hernan Sanchez ;
Kaya, Sarp ;
Viswanathan, Venkatasubramanian ;
Miller, Daniel J. ;
Friebel, Daniel ;
Hansen, Heine A. ;
Norskov, Jens K. ;
Nilsson, Anders ;
Ogasawara, Hirohito .
NATURE COMMUNICATIONS, 2013, 4
[6]   Specific reactivity of step sites towards CO adsorption and oxidation on platinum single crystals vicinal to Pt(111) [J].
Chen, Qing-Song ;
Berna, Antonio ;
Climent, Victor ;
Sun, Shi-Gang ;
Feliu, Juan M. .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2010, 12 (37) :11407-11416
[7]   Platinum-Alloy Cathode Catalyst Degradation in Proton Exchange Membrane Fuel Cells: Nanometer-Scale Compositional and Morphological Changes [J].
Chen, Shuo ;
Gasteiger, Hubert A. ;
Hayakawa, Katsuichiro ;
Tada, Tomoyuki ;
Shao-Horn, Yang .
JOURNAL OF THE ELECTROCHEMICAL SOCIETY, 2010, 157 (01) :A82-A97
[8]   ELECTROCHEMISTRY AT PLATINUM SINGLE-CRYSTAL SURFACES IN ACIDIC MEDIA - HYDROGEN AND OXYGEN-ADSORPTION [J].
CLAVILIER, J ;
RODES, A ;
ELACHI, K ;
ZAMAKHCHARI, MA .
JOURNAL DE CHIMIE PHYSIQUE ET DE PHYSICO-CHIMIE BIOLOGIQUE, 1991, 88 (7-8) :1291-1337
[9]   Nanoscale compositional changes and modification of the surface reactivity of Pt3Co/C nanoparticles during proton-exchange membrane fuel cell operation [J].
Dubau, L. ;
Maillard, F. ;
Chatenet, M. ;
Andre, J. ;
Rossinot, E. .
ELECTROCHIMICA ACTA, 2010, 56 (02) :776-783
[10]   Activity benchmarks and requirements for Pt, Pt-alloy, and non-Pt oxygen reduction catalysts for PEMFCs [J].
Gasteiger, HA ;
Kocha, SS ;
Sompalli, B ;
Wagner, FT .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2005, 56 (1-2) :9-35