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- Title
A density functional theory study of reactions of relevance to catalytic hydrocarbon synthesis and combustion.
- Authors
Arya, Mina; Niklasson, Joakim; Mohsenzadeh, Abas; Bolton, Kim
- Abstract
Synthesis and combustion of hydrocarbons on a series of metal surfaces (Ag, Au, Al, Cu, Rh, Pt and Pd) were investigated using density functional theory (DFT). The adsorption energies for all species involved in these reactions, as well as the reaction energies and activation barriers on these surfaces, were calculated using the same models and DFT methods. The results were used to test the validity of the Brønsted-Evans-Polanyi (BEP) and transition state scaling (TSS) relationships for these reactions on these metal surfaces. The BEP relationship appears to be a valid indicator for the synthesis reactions with R2 values of 0.83, 0.88 and 0.94 for CO dissociation, CO hydrogenation and formyl (CHO) dissociation to CH + O, respectively. In addition to CH splitting, which has been studied before, the BEP relationship also appears to be valid for the CH oxidation and CHO dissociation to CO + H combustion reactions with R2 values of 0.94, 0.89 and 0.88, respectively. Also, the TSS relationship is excellent with a R2 value of 1 for all synthesis and combustion reactions. The BEP and TSS relationships were subsequently used to estimate the energetics of the synthesis and combustion reactions on Ni, Co and Fe surfaces. The results reveal that the transition state energies estimated by the TSS relationships are in better agreement with data obtained from DFT calculations than the activation energies estimated by the BEP relationships. Therefore, the TSS relationship is preferred when predicting energetics of these reactions on these surfaces.
- Subjects
DENSITY functional theory; CHEMICAL reactions; HYDROCARBON synthesis; CATALYSIS; SELF-propagating high-temperature synthesis
- Publication
Theoretical Chemistry Accounts: Theory, Computation, & Modeling, 2018, Vol 137, Issue 11, p1
- ISSN
1432-881X
- Publication type
Article
- DOI
10.1007/s00214-018-2339-4