Simulating Linear Sweep Voltammetry from First-Principles: Application to Electrochemical Oxidation of Water on Pt(111) and Pt3Ni(111)

被引：74

作者：

Viswanathan, Venkatasubramanian ^{[2
]}

Hansen, Heine Anton ^{[1
]}

Rossmeisl, Jan ^{[3
]}

Jaramillo, Thomas Francisco ^{[1
]}

Pitsch, Heinz ^{[2
]}

Norskov, Jens K. ^{[1
,4
]}

机构：

[1] Stanford Univ, Dept Chem Engn, Stanford, CA 94305 USA

[2] Stanford Univ, Dept Mech Engn, Stanford, CA 94305 USA

[3] Tech Univ Denmark, Dept Phys, Ctr Atom Scale Mat Design, DK-2800 Lyngby, Denmark

[4] SLAC Natl Accelerator Lab, SUNCAT, Menlo Pk, CA 94025 USA

来源：

JOURNAL OF PHYSICAL CHEMISTRY C | 2012年 / 116卷 / 07期

关键词：

DENSITY-FUNCTIONAL THEORY; OXYGEN REDUCTION; ANION ADSORPTION; ACID-SOLUTIONS; OH ADSORPTION; SURFACE; ELECTRODES; ELECTROCATALYSTS; INTERMEDIATE; OVERLAYERS;

D O I：

10.1021/jp210802q

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：

Cyclic voltaminetry is a fundamental experimental method for characterizing adsorbates on electrochemical surfaces. We present a model for the electrochemical solid liquid interface, and we simulate the linear sweep voltammogram of the electrochemical oxidation of H2O on Pt(111) and Pt3Ni(111), based on kinetic and thermodynamic parameters computed by Density Functional Theory (DFT) and the dynamics of the system solved through Monte Carlo-based methods. The model predicts onset of OH and O formation in good agreement with voltammetric and ex situ XPS experiments.

引用

页码：4698 / 4704

页数：7

共 37 条

[11] GENERAL METHOD FOR NUMERICALLY SIMULATING STOCHASTIC TIME EVOLUTION OF COUPLED CHEMICAL-REACTIONS [J].

GILLESPIE, DT .

JOURNAL OF COMPUTATIONAL PHYSICS, 1976, 22 (04) :403-434

[12] Improved adsorption energetics within density-functional theory using revised Perdew-Burke-Ernzerhof functionals [J].

Hammer, B ;

Hansen, LB ;

Norskov, JK .

PHYSICAL REVIEW B, 1999, 59 (11) :7413-7421

[13] Water desorption from an oxygen covered Pt(111) surface:: Multichannel desorption [J].

Karlberg, G. S. ;

Wahnstrom, G. ;

Clay, C. ;

Zimbitas, G. ;

Hodgson, A. .

JOURNAL OF CHEMICAL PHYSICS, 2006, 124 (20)

[14] Density-functional based modeling of the intermediate in the water production reaction on Pt(111) -: art. no. 136103 [J].

Karlberg, GS ;

Wahnström, G .

PHYSICAL REVIEW LETTERS, 2004, 92 (13) :136103-1

[15] An interaction model for OH+H2O-mixed and pure H2O overlayers adsorbed on Pt(111) -: art. no. 194705 [J].

Karlberg, GS ;

Wahnström, G .

JOURNAL OF CHEMICAL PHYSICS, 2005, 122 (19)

[16] Modeling the butterfly:: the voltammetry of (√3 x √3)R30° and p(2x2) overlayers on (111) electrodes [J].

Koper, MTM ;

Lukkien, JJ .

JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 2000, 485 (02) :161-165

[17] Efficient Monte Carlo methods for the simulation of catalytic surface reactions [J].

Lukkien, JJ ;

Segers, JPL ;

Hilbers, PAJ ;

Gelten, RJ ;

Jansen, APJ .

PHYSICAL REVIEW E, 1998, 58 (02) :2598-2610

[18] Kinetics of oxygen reduction on Pt(hkl) electrodes: Implications for the crystallite size effect with supported Pt electrocatalysts [J].

Markovic, N ;

Gasteiger, H ;

Ross, PN .

JOURNAL OF THE ELECTROCHEMICAL SOCIETY, 1997, 144 (05) :1591-1597

[19] Dynamical properties and the proton transfer mechanism in the wetting water layer on Pt(111) [J].

Meng, S .

SURFACE SCIENCE, 2005, 575 (03) :300-306

[20] Different surface chemistries of water on Ru{0001}: From monomer adsorption to partially dissociated bilayers [J].

Michaelides, A ;

Alavi, A ;

King, DA .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2003, 125 (09) :2746-2755

← 1 2 3 4 →