New Model for Predicting Adsorption of Polar Molecules in Metal–Organic Frameworks with Unsaturated Metal Sites

Christopher Campbell, José R. B. Gomes, Michael Fischer, Miguel Jorge
  • The Journal of Physical Chemistry Letters, June 2018, American Chemical Society (ACS)
  • DOI: 10.1021/acs.jpclett.8b00967

New Model for Adsorption of Polar Molecules in MOFs with Unsaturated Metal Sites

What is it about?

Conventional molecular models used in grand canonical Monte Carlo simulations fail to correctly describe interactions of adsorbates with coordinatively unsaturated sites present in a large number of metal–organic frameworks. We propose a new approach that combines quantum mechanical density functional theory with Monte Carlo simulations to rigorously account for specific interactions at the CUS, which leads to substantial improvement in adsorption isotherm predictions, and correctly captures the coordination binding mechanism.

Why is it important?

This study represents a major stepping stone in the development of a robust, transferable and generally applicable approach to describe the complex interactions between gas molecules and coordinatively unsaturated sites, with great potential for use in large-scale screening studies.


José Gomes

In summary, we have shown that existing models are unsuitable for capturing the orbital behavior of coordinatively unsaturated sites-containing MOFs, and consequently agree poorly with experimental adsorption isotherms. This work shows the model to be transferable across different adsorbates and adsorbents (metal organic frameworks with the copper paddlewheel).

Read Publication

The following have contributed to this page: José Gomes