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CO Oxidation Facilitated by Robust Surface States on Au-Covered Topological Insulators

Surface states refer to electronic states emerging as a solid material terminates at a surface, and can be present in many systems. Despite their spatial proximity to material surfaces, surface states have been largely overlooked in fundamental understanding of surface catalysis and potential real-world applications, because of their vulnerability to local impurities or defects. In contrast, the recently discovered three-dimensional topological insulators (3DTI) have exceptionally robust metallic surface states that are topologically protected against surface contamination and imperfection. The robust topological surface state(s) (TSS) provides a perfect platform for exploiting novel physical phenomena and potential applications of surface states in less stringent environments. Here we employ first-principles density functional theory to demonstrate that the TSS can play a vital and elegant role in facilitating surface reactions by serving as an effective electron bath. We use CO oxidation on gold-covered Bi2Se3 as a prototype example, and first show that the TSS is preserved when a stable ultrathin Au film is deposited onto a Bi-terminated Bi2Se3 substrate. Furthermore, the TSS can significantly enhance the adsorption energy of both CO and O2 molecules, by promoting different directions of electron transfer. For CO, the TSS accepts electrons from the CO-Au system, thereby decreasing the undesirable occupation of the CO antibonding states. For O2, the TSS donates the needed electrons to promote the molecule towards dissociative adsorption. The present study adds a new arena to the technological potentials of 3DTI, and the central concept of TSS as an electron bath as revealed here may lead to new design principles beyond the conventional d-band theory of heterogeneous catalysis.