A DFT Investigation on the Electronic Structures and Au Adatom Assisted Hydrogenation of Graphene Nanoflake Array

Abstract

Graphene nanoribbons with zigzag edges(ZGNRs) have attracted much attention for their spin-polarized edge states predicted more than 15 years ago. Since the ZGNRs are fabricated on metal substrates using molecular precursors, due to their strong coupling with metal substrates, experimental detection of the spin-polarized edge states is still difficult. Here, we design a partially hydrogenated graphene(PHGr), in which periodic hexagonal graphene nanoflakes(GNFs) with zigzag boundaries are embedded in a hydrogenated graphene layer. Using density functional theory(DFT) based first-principles calculations, we find that the hexagonal GNFs exhibit spin-polarized boundary states at their opposite zigzag boundaries, which is similar with the bow-tie-shaped GNFs and ZGNRs. DFT calculations demonstrate that the PHGr is a semiconductor with an antiferromagnetic ground state. Moreover, the antiferromagnetic boundary states and semiconducting properties keep unchanged when the size of GNF varies from 1.4 nm to 2.3 nm. The robustness of the spin-polarized boundary states enables this PHGr as a robust material for detecting spin-polarized boundary states coming from zigzag boundaries. In addition, we find that single Au atoms selectively adsorbed on boundaries catalyze H2 dissociation and therefore lower the barrier of graphene hydrogenation. Therefore, the PHGr can be used not only in carbon-based spintronic devices but also as a platform for single atom catalyst.