Single Gold Atoms in Heterogeneous Catalysis: Selective 1,3‐Butadiene Hydrogenation over Au/ZrO2

The origin of the species: The first principles method reveals the origin and activity of a heterogeneous Au monomer in the catalysis of a selective 1,3-butadiene hydrogenation. The active Au species is an AuI complex, produced from AuIII in situ by reduction, stabilized by ZrO2 defects. The high catalytic activity and selectivity comes from the stable, but flexible, structure of the AuI catalytic center, which dissociates H2 heterolytically.