Title :

Ab Initio Molecular Dynamics calculations on NO oxidation over oxygen functionalized Highly Oriented Pyrolytic Graphite

Author(s) :

Angulo, Gilberto A. Alou [Auteur]
Physico-Chimie Moléculaire Théorique [PCMT]
Rivero Santamaria, Alejandro [Auteur correspondant]
Physico-Chimie Moléculaire Théorique [PCMT]
Toubin, Céline [Auteur]
Physico-Chimie Moléculaire Théorique [PCMT]
Monnerville, Maurice [Auteur]
Physico-Chimie Moléculaire Théorique [PCMT]

Publication date :

2024-06-24

HAL domain(s) :

Chimie/Chimie théorique et/ou physique
Physique [physics]/Physique [physics]/Chimie-Physique [physics.chem-ph]

English abstract : [en]

The oxidation of NO molecules on epoxy-functionalized highly oriented pyrolytic graphite, thermalized at 300 K, was studied by means of ab initio molecular dynamics (AIMD) calculations. Four collision energies and two ...
Show more >The oxidation of NO molecules on epoxy-functionalized highly oriented pyrolytic graphite, thermalized at 300 K, was studied by means of ab initio molecular dynamics (AIMD) calculations. Four collision energies and two different orientations were analyzed where the reaction, adsorption, and scattering probabilities were computed. Our results reveal that NO₂ formation can occur even at the lowest collision energy investigated (0.025 eV), approximately equivalent to room temperature (300 K), which agrees qualitatively with the experimental results. This underscores the influence of dynamics on the NO oxidation process, since this oxidation barrier was previously theoretically estimated to be about 0.1 eV at 0 K, which is four times higher than our lowest collision energy. Additionally, we obtained angular and energy distributions of the products under selected simulation conditions. Scattered NO molecules show low specular reflection, lose half of their initial translational energy, and remain vibrationally cold with minimal rotational excitation. Furthermore, a statistical analysis of all reactive trajectories, focusing on configurations at specific reaction moments, elucidated the structural requirements for the reaction to occur under dynamic conditions. Finally, this study demonstrates the potential of oxygen-doped carbon surfaces for the conversion of NO to NO₂.Show less >

Language :

Anglais

ANR Project :

Physiques et Chimie de l'Environnement Atmosphérique

Collections :

• Laboratoire de Physique des Lasers, Atomes et Molécules (PhLAM) - UMR 8523

Source :

Harvested from HAL

Submission date :

2024-06-30T02:07:59Z