Zr-oxide secondary building units construct metal–organic
framework (MOF) materials with excellent gas adsorption properties
and high mechanical, thermal, and chemical stability. These attributes
have led Zr-oxide MOFs to be well-recognized for a wide range of applications,
including gas storage and separation, catalysis, as well as healthcare
domain. Here, we report structure search methods within the Cambridge
Structural Database (CSD) to create a curated subset of 102 Zr-oxide
MOFs synthesized to date, bringing a unique record for all researchers
working in this area. For the identified structures, we manually corrected
the proton topology of hydroxyl and water molecules on the Zr-oxide
nodes and characterized their textural properties, Brunauer–Emmett–Teller
(BET) area, and topology. Importantly, we performed systematic periodic
density functional theory (DFT) calculations comparing 25 different
combinations of basis sets and functionals to calculate framework
partial atomic charges for use in gas adsorption simulations. Through
experimental verification of CO2 adsorption in selected
Zr-oxide MOFs, we demonstrate the sensitivity of CO2 adsorption
predictions at the Henry’s regime to the choice of the DFT
method for partial charge calculations. We characterized Zr-MOFs for
their CO2 adsorption performance via high-throughput grand
canonical Monte Carlo (GCMC) simulations and revealed how the chemistry
of the Zr-oxide node could have a significant impact on CO2 uptake predictions. We found that the maximum CO2 uptake
is obtained for structures with the heat of adsorption values >25
kJ/mol and the largest cavity diameters of ca. 6–7 Å.
Finally, we introduced augmented reality (AR) visualizations as a
means to bring adsorption phenomena alive in porous adsorbents and
to dynamically explore gas adsorption sites in MOFs.