Elucidation and Design of NO Reduction Reaction Process by First-Principles Multiscale Simulation

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We studied the co-adsorption of NO-H2O on Cu(111) using the van der Waals density functional theory method. We first studied the adsorption of NO and H2O clusters on Cu(111). The energetics, adsorption geometries, and vibrational properties of several NO-H2O complexes are estimated, and the relative stabilities of those complexes are compared with respective NO and H2O clusters on Cu(111). We find that the mixed complexes between NO and H2O on Cu(111) are more stable than the separated clusters of NO and water, which arises from the hydrogen bonding between NO and H2O and NO - NO interaction. Electronic structure analysis indicates that attractive NO-H2O interaction arises from the hydrogen bonding with the enhancements of back-donation to valence orbitals of NO, while the NO - NO interaction arises from the hybridization among valance orbitals. The vibrational analysis also confirms the formation of the mixed NO-H2O complexes and N-O stretching modes are red-shifted due to hydrogen bonding with water. Our result provides an insightful interpretation of experimental observation.We also have studied the metal-support interaction (MSI) of the platinum metal group (PGM) supported on some metal oxide materials under three-way catalyst (TWC) operating conditions using machine-learning enhanced global optimization and thermodynamics.