Predicting the activation energy of catalytic dissociation of the heteroatomic AB bond

TY - JOUR

T1 - Predicting the activation energy of catalytic dissociation of the heteroatomic AB bond

AU - German, Ernst D.

AU - Kuznetsov, Alexander M.

AU - Sheintuch, Moshe

N1 - Funding Information: This work was supported by the Israel Science Foundation. A.M.K. thanks the Russian Foundation for Basic Research, Grant No. 03-03-32935 for partial financial support.

PY - 2006/5/9

Y1 - 2006/5/9

N2 - Two analytical formalisms, adiabatic and diabatic ones, were developed for the description of catalytic dissociation of heteroatomic bond AB interacting with a metal surface in the adsorption processes. In the adiabatic formalism, the transition state was localized on a four-dimensional potential energy surface in classical approximation. This approach generalizes the previous three-dimensional model for dissociative adsorption of homonuclear molecules X2 on metals surfaces, and it was used for studying the effect of non-parallel orientation to a surface of O2 molecules in the adsorption precursor state. The second formalism takes into account a possible quantum character of vibrations along the chemical bond AB. The calculation of the activation energy in this approach is performed by the density matrix method. This approach is applied for studying catalytic dissociation of CO molecule on a Ni(1 1 1) surface. The calculated apparent activation energy for this reaction is compared with published data for this system.

AB - Two analytical formalisms, adiabatic and diabatic ones, were developed for the description of catalytic dissociation of heteroatomic bond AB interacting with a metal surface in the adsorption processes. In the adiabatic formalism, the transition state was localized on a four-dimensional potential energy surface in classical approximation. This approach generalizes the previous three-dimensional model for dissociative adsorption of homonuclear molecules X2 on metals surfaces, and it was used for studying the effect of non-parallel orientation to a surface of O2 molecules in the adsorption precursor state. The second formalism takes into account a possible quantum character of vibrations along the chemical bond AB. The calculation of the activation energy in this approach is performed by the density matrix method. This approach is applied for studying catalytic dissociation of CO molecule on a Ni(1 1 1) surface. The calculated apparent activation energy for this reaction is compared with published data for this system.

KW - Activation energy

KW - Co

KW - Kinetic of dissociative adsorption

KW - Ni(1 1 1)

UR - http://www.scopus.com/inward/record.url?scp=33646263348&partnerID=8YFLogxK

U2 - 10.1016/j.chemphys.2005.10.010

DO - 10.1016/j.chemphys.2005.10.010

M3 - 文章

AN - SCOPUS:33646263348

SN - 0301-0104

VL - 324

SP - 129

EP - 139

JO - Chemical Physics

JF - Chemical Physics

IS - 1 SPEC. ISS.

ER -