Dynamics Studies of O₂ Collision on Pt(111) Using a Global Potential Energy Surface

Abstract

The dynamics of O2 collision on Pt(111) has been studied by molecular dynamics simulations using a global potential energy surface (PES), which was developed by fitting ∼4800 plane-wave density functional theory points using the permutation invariant polynomial-neural network method. The simulations were performed for the normal and off-normal incidences at a wide range of incident energies and surface temperatures. A generalized Langevin oscillator model was used to incorporate the molecule–surface coupling that plays an important role in this collision process. The trapping probability, final energy distribution, scattering angle distributions of scattered molecules, and the energy transfer to surface distribution were determined and analyzed. The PES shows an activated path to the chemisorption states, as the trapping probability directly increases with incident energy (larger than 0.1 eV) to reach a maximum and then decreases at high incident energy. The trapping probability obviously reduces by raising surface temperature at low incident energy because the initial kinetic energy of molecule is more likely to be dissipated into surface motions than molecular internal ro-vibrational modes. Additional parallel momentum of off-normal incidence leads to a strong suppression of the trapping probability, caused by the energetic corrugation of the lateral barrier heights. The scattering angular distributions are found to be quasispecular and the final translational energy slightly increases with scattering angle deviating significantly from the hard-cube model, indicating the nonconservation of parallel momentum during the collision on the corrugate PES.

Computational approaches to dissociative chemisorption on metals: towards chemical accuracy

“…sticking of H 2 to Pd surfaces, 475 vibrational excitation of H 2 scattering from Cu(111), 168 sticking of N 2 to W surfaces, 86,132 sticking of O 2 to Pd(100) 522 and Cu/Ru(0001), 130 and scattering of O 2 from Ag(111) 94 and Pt (111). 523 A more sophisticated treatment than the GLO is due to Jackson and co-workers, 524,525 and has been called various names, including e.g. the lattice reconstruction sudden (LRS) model (the term we will use) and the lattice sudden model.…”

Quantum Effects in the Dissociative Chemisorption of N2 on Fe(111): Full-Dimensional Quantum Dynamics and Quasi-Classical Trajectory Study

“…The interaction between gas-phase molecules and the transition-metal surface plays an important role in heterogeneous catalysis, − for example, the famous industrial catalytic reactionthe synthesis of ammonia from N 2 and H 2 over an iron-based catalysis. In this ammonia synthesis process, the dissociative chemisorption (DC) of the N 2 molecule is the rate-limiting step. , Iron is a well-known and efficient catalyst for ammonia synthesis, mainly because of its low price and high reactivity.…”

Homogeneous Fluorine Distribution in Graphene through Thermal Dissociation of Molecular F2: Implications for Thermal Conduction and Electrical Insulation

“…When the bond length of F 2 is 1.5 times that of the ground state, it has the largest Δ G . It is generally believed that the chemical bond is broken when the bond length is extended to two times that of the ground state . As a result, when the bond length is extended to 1.5 times that of the ground state, it can be considered that molecular F 2 has the enough energy for rapid dissociation.…”