First-Principles Investigation of the Structure and Properties of Au Nanoparticles Supported on ZnO

[Image: see text] We present a first-principles investigation of the structure, stability, and reactivity of Au nanoparticles (NPs) supported on ZnO. The morphologies of supported Au NPs are predicted using the formation energy of Au surfaces and the adhesion energy between Au and the dominant ZnO surfaces exposed on ZnO tetrapods. We show how Zn interstitials (a stable intrinsic defect in ZnO) are attracted toward the Au/ZnO interface and in the presence of oxygen can lead to the encapsulation of Au by ZnO, an effect that is observed experimentally. We find that O(2) molecules absorb preferentially at the perimeter of the NP in contact with the ZnO support. These results provide atomistic insight into the structure of ZnO-supported Au NPs with relevance to CO oxidation.