Reaction pathway of oxygen evolution on Pt(111) revealed through constant Fermi level molecular dynamics

被引：27

作者：

Bouzid, Assil ^{[1
]}

Gono, Patrick ^{[1
]}

Pasquarello, Alfredo ^{[1
]}

机构：

[1] Ecole Polytech Fed Lausanne, CSEA, CH-1015 Lausanne, Switzerland

来源：

JOURNAL OF CATALYSIS | 2019年 / 375卷

关键词：

OER mechanism; Molecular dynamics; Constant Fermi level molecular dynamics; REDUCTION REACTION; SIMULATION; EMISSIONS; SURFACES; CATALYST;

D O I：

10.1016/j.jcat.2019.05.025

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 pathway of the oxygen evolution reaction at the Pt(1 1 1)/water interface is disclosed through constant Fermi level molecular dynamics. Upon the application of a positive bias potential H2Oads and OHads adsorbates are found to arrange in a hexagonal lattice with an irregular alternation. Increasing further the electrode potential then induces the oxygen evolution reaction, which is found to proceed through a hydrogen peroxide intermediate. Calculation of the associated overpotential shows a reduction of 0.2 eV compared to the associative mechanism. This result highlights the forcefullness of the applied scheme in exploring catalytic reactions in an unbiased way. (C) 2019 Elsevier Inc. All rights reserved.

引用

页码：135 / 139

页数：5

共 45 条

[31] The oxygen reduction reaction on a Pt/carbon fuel cell catalyst in the presence of chloride anions [J].

Schmidt, TJ ;

Paulus, UA ;

Gasteiger, HA ;

Behm, RJ .

JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 2001, 508 (1-2) :41-47

[32] Transport effects in the oxygen reduction reaction on nanostructured, planar glassy carbon supported Pt/GC model electrodes [J].

Schneider, A. ;

Colmenares, L. ;

Seidel, Y. E. ;

Jusys, Z. ;

Wickman, B. ;

Kasemo, B. ;

Behm, R. J. .

PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2008, 10 (14) :1931-1943

[33] Mesoscopic mass transport effects in electrocatalytic processes [J].

Seidel, Y. E. ;

Schneider, A. ;

Jusys, Z. ;

Wickman, B. ;

Kasemo, B. ;

Behm, R. J. .

FARADAY DISCUSSIONS, 2008, 140 :167-184

[34] Density functional theory calculations for the hydrogen evolution reaction in an electrochemical double layer on the Pt(111) electrode [J].

Skulason, Egill ;

Karlberg, Gustav S. ;

Rossmeisl, Jan ;

Bligaard, Thomas ;

Greeley, Jeff ;

Jonsson, Hannes ;

Norskov, Jens K. .

PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2007, 9 (25) :3241-3250

[35] Structure-relationships in electrocatalysis: oxygen reduction and hydrogen oxidation reactions on Pt(111) and Pt(100) in solutions containing chloride ions [J].

Stamenkovic, V ;

Markovic, NM ;

Ross, PN .

JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 2001, 500 (1-2) :44-51

[36] First principles reaction modeling of the electrochemical interface: Consideration and calculation of a tunable surface potential from atomic and electronic structure [J].

Taylor, CD ;

Wasileski, SA ;

Filhol, JS ;

Neurock, M .

PHYSICAL REVIEW B, 2006, 73 (16)

[37] Standard hydrogen electrode and potential of zero charge in density functional calculations [J].

Tripkovic, Vladimir ;

Bjorketun, Marten E. ;

Skulason, Egill ;

Rossmeisl, Jan .

PHYSICAL REVIEW B, 2011, 84 (11)

[38] The oxygen reduction reaction mechanism on Pt(111) from density functional theory calculations [J].

Tripkovic, Vladimir ;

Skulason, Egill ;

Siahrostami, Samira ;

Norskov, Jens K. ;

Rossmeisl, Jan .

ELECTROCHIMICA ACTA, 2010, 55 (27) :7975-7981

[39] EFFICIENT PSEUDOPOTENTIALS FOR PLANE-WAVE CALCULATIONS [J].

TROULLIER, N ;

MARTINS, JL .

PHYSICAL REVIEW B, 1991, 43 (03) :1993-2006

[40] QUICKSTEP: Fast and accurate density functional calculations using a mixed Gaussian and plane waves approach [J].

VandeVondele, J ;

Krack, M ;

Mohamed, F ;

Parrinello, M ;

Chassaing, T ;

Hutter, J .

COMPUTER PHYSICS COMMUNICATIONS, 2005, 167 (02) :103-128

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