Development of computation‐ready metal–organic framework databases (MOF DBs) has accelerated high‐throughput computational screening (HTCS) of materials to identify the best candidates for gas storage and separation. These DBs were constructed using structural curations to make MOFs directly usable for molecular simulations, which caused the same MOF to be reported with different structural features in different DBs. We examined thousands of common materials of the two recently updated, very widely used MOF DBs to reveal how structural discrepancies affect simulated CH4, H2, CO2 uptakes and CH4/H2 separation performances of MOFs. Results showed that DB selection has a significant effect on the calculated gas uptakes and ideal selectivities of materials at low pressure. A detailed analysis on the curated structures was provided to isolate the critical elements of MOFs determining the gas uptakes. Identification of the top‐performing materials for gas separation was shown to strongly depend on the DB used in simulations.
Covalent organic
frameworks (COFs) have high potential in gas separation
technologies because of their porous structures, large surface areas,
and good stabilities. The number of synthesized COFs already reached
several hundreds, but only a handful of materials were tested as adsorbents
and/or membranes. We used a high-throughput computational screening
approach to uncover adsorption-based and membrane-based CO
2
/H
2
separation potentials of 288 COFs, representing the
highest number of experimentally synthesized COFs studied to date
for precombustion CO
2
capture. Grand canonical Monte Carlo
(GCMC) simulations were performed to assess CO
2
/H
2
mixture separation performances of COFs for five different cyclic
adsorption processes: pressure swing adsorption, vacuum swing adsorption,
temperature swing adsorption (TSA), pressure−temperature swing
adsorption (PTSA), and vacuum−temperature swing adsorption
(VTSA). The results showed that many COFs outperform traditional zeolites
in terms of CO
2
selectivities and working capacities and
PTSA is the best process leading to the highest adsorbent performance
scores. Combining GCMC and molecular dynamics (MD) simulations, CO
2
and H
2
permeabilities and selectivities of COF
membranes were calculated. The majority of COF membranes surpass Robeson’s
upper bound because of their higher H
2
permeabilities compared
to polymers, indicating that the usage of COFs has enormous potential
to replace current materials in membrane-based H
2
/CO
2
separation processes. Performance analysis based on the structural
properties showed that COFs with narrow pores [the largest cavity
diameter (LCD) < 15 Å] and low porosities (ϕ < 0.75)
are the top adsorbents for selective separation of CO
2
from
H
2
, whereas materials with large pores (LCD > 20 Å)
and high porosities (ϕ > 0.85) are generally the best COF
membranes
for selective separation of H
2
from CO
2
. These
results will help to speed up the engineering of new COFs with desired
structural properties to achieve high-performance CO
2
/H
2
separations.
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