Thesis
Analysis of the effects of forcefields on adsorption simulation in MOFs
- Creator
- Rights statement
- Awarding institution
- University of Strathclyde
- Date of award
- 2022
- Thesis identifier
- T16414
- Person Identifier (Local)
- 201789169
- Qualification Level
- Qualification Name
- Department, School or Faculty
- Abstract
- Metal-organic frameworks (MOFs) are crystalline and porous materials consisting ofcoordination bonds between transition-metal cations and organic ligands. Theimmense number of existing MOFs poses great challenges for experimentalscreening. Computational methods like Grand-Canonical Monte Carlo offer a viablealternative for screening, but they rely strongly on the accuracy of the underlyingmolecular model, or force field. In particular, the assignment of atomic point chargesto each atom of the framework is required for modelling Coulombic interactionsbetween the MOF and the adsorbate(s), which are crucial in adsorption of polarcompounds. This thesis reports a systematic analysis of the effect of point charges onadsorption predictions by molecular modelling, with the results showing that the useof charges developed by periodic DFT methods produce the most accurate andconsistent results.Furthermore, conventional molecular models for adsorption in MOFs neglectimportant physics of the process, and thus can lead to inaccurate predictions. This isparticularly the case for MOFs that possess open metal sites (OMS) – the complexinteraction of these sites with particular adsorbate molecules is not captured bystandard force fields. The impact of neglecting these interactions can be huge,particularly considering that MOFs that contain OMS are among the most promisingmaterials for gas storage and separation applications, precisely due to these strongand selective binding sites. In this work, experimental adsorption measurements ofethane and ethylene on CuBTC (a widely studied MOF that contains OMS) werecarried out and compared to simulations implementing a bespoke model previouslydeveloped by our group to account for OMS interactions. This thesis validated themodel and demonstrated its robustness even at low temperatures.In summary, the results of this work offer a more consistent way to assess thesuitability of molecular models to provide more accurate adsorption predictions.
- Advisor / supervisor
- Jorge, Miguel
- Resource Type
- DOI
Las relaciones
Elementos
| Miniatura | Título | Fecha de subida | Visibilidad | Acciones |
|---|---|---|---|---|
|
|
PDF of thesis T16414 | 2023-03-17 | Público | Descargar |