Understanding the Activity of Single-Atom Catalysis from Frontier Orbitals
Zhaoming Fu, Bowen Yang, Ruqian Wu
Abstract
The d-band center and charge states are often used to analyze the catalytic activity of noble or transition metal surfaces and clusters, but their applicability for single-atom catalysts (SACs) is unsure. This work suggests that the spatial structure and orientation of frontier orbitals which are closest to the Fermi level of SACs play a vital role. Taking adsorption of several molecules and CO oxidization on C_{3}N-supported single-atom Au as examples, we demonstrate that adsorption and catalytic activities are well correlated with the characteristics of frontier orbitals. This work provides an effective guidance for understanding the performance of single-atom catalysts.
Topics & Concepts
Atomic orbitalAtom (system on chip)CatalysisFrontierMaterials scienceFermi levelChemical physicsOrientation (vector space)Work (physics)Molecular orbitalAdsorptionAtomic physicsMoleculePhysicsChemistryPhysical chemistryQuantum mechanicsComputer scienceElectronGeometryMathematicsHistoryEmbedded systemArchaeologyBiochemistryCatalytic Processes in Materials ScienceMachine Learning in Materials ScienceElectrocatalysts for Energy Conversion