Potential
applications of pillared graphene oxide frameworks (GOF)
with phenyldiboronic acid linkers in gas storage and separation have
been systematically explored using a combination of density functional
theory calculations and Grand Canonical Monte Carlo simulations. A
systematic computational screening of the efficiency of such frameworks
in the capture and separation of a wide variety of potent greenhouse
gases, as well as gases with significant applications in the energy
sector, such as hydrogen and natural gas constituents, has been performed.
A classical interaction potential model was employed for the pillared
GOF, using the intramolecular geometry and atomic charges obtained
by the quantum mechanical calculations. Well-established Lennard-Jones
parameters for the nanoporous material and intermolecular potential
models for the gases under investigation were also adopted. A high
uptake of pure SF6, SO2, H2S, and
CO2 has been observed at ambient pressures and temperatures.
The CF4 and N2O uptake values at ambient pressure
are also among the highest values reported in the literature. The
pure H2 uptake reaches the United States Department of
Energy targets at low temperatures (77 K) and pressures P > 5 bar, while the total volumetric uptake for CH4 at
50 bar and ambient temperature compares well with the most efficient
adsorbents for methane storage. The simulations also revealed that
the investigated type of materials is efficient for the separation
of SF6–N2, CO2–H2, and H2S-CH4 fluid mixtures. In general,
the present work indicates that this particular class of porous frameworks
can have applications in industrial-scale gas storage and separation
and greenhouse-gas capture to prevent global warming and climate change.