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

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