Lambert, H;
Castillo Bonillo, A;
Zhu, Q;
Zhang, YW;
Lee, TC;
(2022)
Supramolecular gating of guest release from cucurbit[7]uril using de novo design.
npj Computational Materials
, 8
(1)
, Article 21. 10.1038/s41524-022-00702-0.
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Abstract
Herein we computationally explore the modulation of the release kinetics of an encapsulated guest molecule from the cucurbit[7]uril (CB7) cavity by ligands binding to the host portal. We uncovered a correlation between the ligand-binding affinity with CB7 and the guest residence time, allowing us to rapidly predict the release kinetics through straightforward energy minimization calculations. These high-throughput predictions in turn enable a Monte-Carlo Tree Search (MCTS) to de novo design a series of cap-shaped ligand molecules with large binding affinities and boosting guest residence times by up to 7 orders of magnitude. Notably, halogenated aromatic compounds emerge as top-ranking ligands. Detailed modeling suggests the presence of halogen-bonding between the ligands and the CB7 portal. Meanwhile, the binding of top-ranked ligands is supported by 1H NMR and 2D DOSY-NMR. Our findings open up possibilities in gating of molecular transport through a nanoscale cavity with potential applications in nanopore technology and controlled drug release.
| Type: | Article |
|---|---|
| Title: | Supramolecular gating of guest release from cucurbit[7]uril using de novo design |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1038/s41524-022-00702-0 |
| Publisher version: | https://doi.org/10.1038/s41524-022-00702-0 |
| Language: | English |
| Additional information: | © 2022 Springer Nature Limited. This article is licensed under a Creative Commons Attribution 4.0 International License (http://creativecommons.org/licenses/by/4.0/). |
| Keywords: | Atomistic models, Molecular self-assembly, Nanopores, Self-assembly |
| UCL classification: | UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > MAPS Faculty Office > Institute for Materials Discovery UCL > Provost and Vice Provost Offices > UCL BEAMS UCL UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > MAPS Faculty Office |
| URI: | https://discovery.ucl.ac.uk/id/eprint/10143787 |
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