Explicit treatment of hydrogen bonds in the universal force field: validation and application for metal-organic frameworks, hydrates, and host-guest complexes
| Autor: | Damien E. Coupry, Matthew Addicoat, Thomas Heine |
|---|---|
| Jazyk: | angličtina |
| Rok vydání: | 2017 |
| Předmět: |
Condensed Matter - Materials Science
Materials science Hydrogen Hydrogen bond Coordination number Materials Science (cond-mat.mtrl-sci) FOS: Physical sciences General Physics and Astronomy chemistry.chemical_element 02 engineering and technology Electronic structure 010402 general chemistry 021001 nanoscience & nanotechnology 01 natural sciences Bond order Force field (chemistry) 0104 chemical sciences Molecular dynamics chemistry hydrogen bonds universal force field metal-organic frameworks hydrates host-guest complexes Chemical physics Metal-organic framework ddc:541 Physical and Theoretical Chemistry 0210 nano-technology |
| ISSN: | 0021-9606 |
| Popis: | A straightforward means to include explicit hydrogen bonds within the Universal Force Field (UFF) is presented. Instead of treating hydrogen bonds as non-bonded interaction subjected to electrostatic and Lennard-Jones potentials, we introduce an explicit bond with a negligible bond order, thus maintaining the structural integrity of the H-bonded complexes and avoiding the necessity to assign arbitrary charges to the system. The explicit hydrogen bond changes the coordination number of the acceptor site and the approach is thus most suitable for systems with under-coordinated atoms, such as many metal-organic frameworks; however, it also shows an excellent performance for other systems involving a hydrogen-bonded framework. In particular, it is an excellent means for creating starting structures for molecular dynamics and for investigations employing more sophisticated methods. The approach is validated for the hydrogen bonded complexes in the S22 dataset and then employed for a set of metal-organic frameworks from the Computation-Ready Experimental database and several hydrogen bonded crystals including water ice and clathrates. We show that the direct inclusion of hydrogen bonds reduces the maximum error in predicted cell parameters from 66% to only 14%, and the mean unsigned error is similarly reduced from 14% to only 4%. We posit that with the inclusion of hydrogen bonding, the solvent-mediated breathing of frameworks such as MIL-53 is now accessible to rapid UFF calculations, which will further the aim of rapid computational scanning of metal-organic frameworks while providing better starting points for electronic structure calculations. |
| Databáze: | OpenAIRE |
| Externí odkaz: |
|