TY - JOUR

T1 - Modeling ammonia oxidation over a Pt (533) surface

AU - Rafti, Matías

AU - Vicente, José Luis

AU - Albesa, Alberto

AU - Scheibe, Axel

AU - Imbihl, Ronald

N1 - Funding Information: This work was supported by the DFG under the priority program No. 1091 “Bridging the gap between ideal and real systems in heterogeneous catalysis”. M.R., J.L.V., and A.A. gratefully acknowledge financial support from the UNLP (Universidad Nacional de La Plata) , CICPBA (Comisión de Investigaciones Científicas de la Prov. de Buenos Aires — Argentina) , CONICET (Consejo de Investigaciones Científicas y Tecnológicas) , and DAAD (Deutscher Akademischer Austauch Dienst) . One of the authors (R.I.) is greatly indebted to W. Offermans for many fruitful discussions. (This work was partially carried while one of the authors (M.R.) was visiting Prof. Imbihl group at Liebniz Hannover University, the kind hospitality and stimulating discussions are gratefully acknowledged).

PY - 2012/1

Y1 - 2012/1

N2 - We present a new reaction model for ammonia oxidation on a Pt (533) surface and perform numerical simulations using mean field equations. Kinetic parameters were taken from experiments and Density Functional Theory (DFT) calculations. The model is based on an oxygen-activated ammonia decomposition and includes NHx (x = 0, 1, 2) intermediates. Reaction rates and coverages obtained from calculations show semiquantitative agreement with values from kinetic and in-situ XPS measurements up to 0.1 mbar pressures. Pathways for ammonia oxidation were analyzed by varying kinetic parameters in the model, which provides new insights into the relative importance of different reaction steps.

AB - We present a new reaction model for ammonia oxidation on a Pt (533) surface and perform numerical simulations using mean field equations. Kinetic parameters were taken from experiments and Density Functional Theory (DFT) calculations. The model is based on an oxygen-activated ammonia decomposition and includes NHx (x = 0, 1, 2) intermediates. Reaction rates and coverages obtained from calculations show semiquantitative agreement with values from kinetic and in-situ XPS measurements up to 0.1 mbar pressures. Pathways for ammonia oxidation were analyzed by varying kinetic parameters in the model, which provides new insights into the relative importance of different reaction steps.

KW - Adsorption kinetics

KW - Ammonia

KW - Catalysis

KW - Computer simulations

KW - Models of surface kinetics

KW - Platinum

KW - Single crystal surfaces

KW - Surface chemical reaction

UR - http://www.scopus.com/inward/record.url?scp=80255123898&partnerID=8YFLogxK

U2 - 10.1016/j.susc.2011.08.014

DO - 10.1016/j.susc.2011.08.014

M3 - Article

AN - SCOPUS:80255123898

VL - 606

SP - 12

EP - 20

JO - Surface science

JF - Surface science

SN - 0039-6028

IS - 1-2

ER -