Computational Modeling of Reticular Materials: The Past, the Present, and the Future.

Reticular materials rely on a unique building concept where inorganic and organic building units are stitched together giving access to an almost limitless number of structured ordered porous materials. Given the versatility of chemical elements, underlying nets, and topologies, reticular materials provide a unique platform to design materials for timely technological applications. Reticular materials have now found their way in important societal applications, like carbon capture to address climate change, water harvesting to extract atmospheric moisture in arid environments, and clean energy applications.

Water motifs in zirconium metal-organic frameworks induced by nanoconfinement and hydrophilic adsorption sites.

The intricate hydrogen-bonded network of water gives rise to various structures with anomalous properties at different thermodynamic conditions. Nanoconfinement can further modify the water structure and properties, and induce specific water motifs, which are instrumental for technological applications such as atmospheric water harvesting. However, so far, a causal relationship between nanoconfinement and the presence of specific hydrophilic adsorption sites is lacking, hampering the further design of nanostructured materials for water templating.

Reaching Quantum Accuracy in Predicting Adsorption Properties for Ethane/Ethene in Zeolitic Imidazolate Framework-8 at Low Pressure Regime.

Nanoporous materials in the form of metal-organic frameworks such as zeolitic imidazolate framework-8 (ZIF-8) are promising membrane materials for the separation of hydrocarbon mixtures. To compute the adsorption isotherms in such adsorbents, grand canonical Monte Carlo simulations have proven to be very useful. The quality of these isotherms depends on the accuracy of adsorbate-adsorbent interactions, which are mostly described using force fields owing to their low computational cost.

Gas adsorption and framework flexibility of CALF-20 explored via experiments and simulations.

In 2021, Svante, in collaboration with BASF, reported successful scale up of CALF-20 production, a stable MOF with high capacity for post-combustion CO capture which exhibits remarkable stability towards water. CALF-20's success story in the MOF commercialisation space provides new thinking about appropriate structural and adsorptive metrics important for CO capture. Here, we combine atomistic-level simulations with experiments to study adsorptive properties of CALF-20 and shed light on its flexible crystal structure.

DFT-Quality Adsorption Simulations in Metal-Organic Frameworks Enabled by Machine Learning Potentials.

Nanoporous materials such as metal-organic frameworks (MOFs) have been extensively studied for their potential for adsorption and separation applications. In this respect, grand canonical Monte Carlo (GCMC) simulations have become a well-established tool for computational screenings of the adsorption properties of large sets of MOFs. However, their reliance on empirical force field potentials has limited the accuracy with which this tool can be applied to MOFs with challenging chemical environments such as open-metal sites.

Nuclear quantum effects on zeolite proton hopping kinetics explored with machine learning potentials and path integral molecular dynamics.

Proton hopping is a key reactive process within zeolite catalysis. However, the accurate determination of its kinetics poses major challenges both for theoreticians and experimentalists. Nuclear quantum effects (NQEs) are known to influence the structure and dynamics of protons, but their rigorous inclusion through the path integral molecular dynamics (PIMD) formalism was so far beyond reach for zeolite catalyzed processes due to the excessive computational cost of evaluating all forces and energies at the Density Functional Theory (DFT) level.