Abstract
We report a theoretical study of the electronic, thermal, and structural properties of a
series of graphene oxide frameworks (GOFs) using first-principles calculations based on density
functional theory. The molecular structure of GOFs is systematically studied by varying the nature and
concentration of linear boronic acid pillars, and the thermal stability is assessed using ab initio molecular
dynamics. The results demonstrate that GOFs are thermally stable up to 550 K and that electronic
properties, such as their band gap, can be modified controllably by an appropriate choice of pillaring unit
and pillar concentration. The tunability of the electronic structure using nonchemical means, e.g.,
mechanical strain, is also quantified. Overall, this class of materials is predicted to offer highly tunable
materials electronic properties ranging from metallic to semiconducting.
