  Covalent-organic frameworks (COFs) are intriguing platforms for designing
functional molecular materials. Here, we present a computational study based on
van der Waals dispersion-corrected hybrid density functional theory (DFT-D) to
design boroxine-linked and triazine-linked COFs intercalated with Fe. Keeping
the original $P-6m2$ symmetry of the pristine COF (COF-Fe-0), we have
computationally designed seven new COFs by intercalating Fe atoms between two
organic layers. The equilibrium structures and electronic properties of both
the pristine and Fe-intercalated COF materials are investigated here. We
predict that the electronic properties of COFs can be fine tuned by adding Fe
atoms between two organic layers in their structures. Our calculations show
that these new intercalated-COFs are promising semiconductors. The effect of Fe
atoms on the electronic band structures and density of states (DOSs) has also
been investigated using the aforementioned DFT-D method. The contribution of
the $d$-subshell electron density of the Fe atoms plays an important role in
improving the semiconductor properties of these new materials. These
intercalated-COFs provide a new strategy to create semi-conducting materials
within a rigid porous network in a highly controlled and predictable manner.
