ORCID Profile
0000-0001-8900-4240
Current Organisation
University of Zurich
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Publisher: American Chemical Society (ACS)
Date: 05-04-2021
DOI: 10.26434/CHEMRXIV.14363024.V1
Abstract: Metal-organic frameworks offer a convenient means for capturing, transporting, and releasing small molecules. Rational design of such systems requires an in-depth understanding of the underlying non-covalent interactions, and the ability to easily and rapidly pre-screen candidate architectures in silico. In this work, we devised a recipe for computing the strength and analysing the nature of the host-guest interactions in MOFs. Using experimentally characterised complexes of calcium-adipate framework with 4,4’-bipyridine and 1,2-bis(4-pyridyl)ethane guests as test systems, we have assessed a range of density functional theory methods, energy decomposition schemes, and non-covalent interactions indicators across realistic periodic and finite supramolecular cluster scales. We find that appropriately constructed clusters readily reproduce the key interactions occurring in periodic models at a fraction of the computational cost and with an added benefit of erse density partitioning schemes. Host-guest interaction energies can be reliably computed with dispersion- corrected density functional theory methods however, decoding their precise nature demands insights from energy decomposition schemes and quantum-chemical tools beyond local bonding indices (e.g., the quantum theory of atoms in molecules), such as the non-covalent interactions index and the density overlap regions indicator.
Publisher: Wiley
Date: 24-02-2022
Abstract: Metal‐organic frameworks (MOFs) offer a convenient means for capturing, transporting, and releasing small molecules. Their rational design requires an in‐depth understanding of the underlying non‐covalent host‐guest interactions, and the ability to easily and rapidly pre‐screen candidate architectures in silico . In this work, we devised a recipe for computing the strength and analysing the nature of the host‐guest interactions in MOFs. By assessing a range of density functional theory methods across periodic and finite supramolecular cluster scale we find that appropriately constructed clusters readily reproduce the key interactions occurring in periodic models at a fraction of the computational cost. Host‐guest interaction energies can be reliably computed with dispersion‐corrected density functional theory methods however, decoding their precise nature demands insights from energy decomposition schemes and quantum‐chemical tools for bonding analysis such as the quantum theory of atoms in molecules, the non‐covalent interactions index or the density overlap regions indicator.
Publisher: Wiley
Date: 08-04-2019
Abstract: We report the high-pressure structural characterization of an organic polyiodide salt in which a progressive addition of iodine to triiodide groups occurs. Compression leads to the initial formation of discrete heptaiodide units, followed by polymerization to a 3D anionic network. Although the structural changes appear to be continuous, the insulating salt becomes a semiconducting polymer above 10 GPa. The features of the pre-reactive state and the polymerized state are revealed by analysis of the computed electron and energy densities. The unusually high electrical conductivity can be explained with the formation of new bonds.
Publisher: Wiley
Date: 26-05-2023
Abstract: Metal‐organic frameworks (MOF) and covalent organic frameworks (COFs) are promising nanocarriers for targeted drug delivery. Noncovalent interactions between frameworks and drugs play a fundamental role in the therapeutic uptake and release of the latter. However, the scope of framework functionalizations and deliverable drugs remains underexplored. Using a multilevel approach combining molecular docking and density functional theory, we show for a range of drugs and frameworks that experimentally reported release metrics are in good agreement with the in silico computed host–guest interaction energies. Functional groups within the framework significantly impact the strength of these host–guest interactions, while a given framework can serve as an efficient delivery agent for drugs beyond the prototypical few. Our findings identify the interaction energy as a reliable and relatively easy to compute descriptor of organic framework materials for drug delivery, able to facilitate their high‐throughput screening and targeted design towards extended‐release times.
Publisher: American Chemical Society (ACS)
Date: 20-07-2022
DOI: 10.26434/CHEMRXIV-2022-93PST
Abstract: Molecular docking has traditionally mostly been employed in the field of protein-ligand binding. Here, we extend this method, in combination with DFT-level geometry optimizations, to locate guest molecules inside the pores of metal-organic frameworks. The position and nature of the guest molecules tune the physicochemical properties of the host-guest systems. Therefore, it is essential to be able to reliably locate them to rationally enhance the performance of the known metal-organic frameworks and facilitate new material discovery. The results obtained with this novel method are compared to experimental structures. We show that the presented method can, in general, accurately locate adsorption sites and structures of the guests. We therefore propose our approach as a computational alternative when no experimental structures of guest-loaded MOFs are available. Additional information on the adsorption strength in the studied host-guest systems emerges from the computed interaction energies. Our findings provide the basis for other computational studies on MOF-guest systems and contribute to a better understanding of the structure-interaction-property interplay associated with them.
Publisher: AIP Publishing
Date: 20-10-2023
DOI: 10.1063/5.0144827
No related grants have been discovered for Michelle Ernst.