A combined computational and experimental study of high pressure and supercritical CO2 adsorption on Basolite MOFs

•High pressure CO2 capture with Basolite® MOFs for pressures up to 225 bar.•Uprecedented rise in CO2 capture for MOFs beyond 25 bars.•DFT predictions for high pressure CO2 capture performance and matching comparison with the experimental data.•In-situ IR measurements with CO2 up 30 3000 mbars for characterizing preferential adsorption sites.•Monte Carlo molecular simulations for inferring the nanoscopic information of the adsorption mechanism.

Metal organic frameworks (such as commercial Basolite®) display significant promise for CO2 capture and storage. Here, in order to monitor CO2 capture of Basolite®, we combined high pressure CO2 adsorption with high-pressure FTIR and Monte Carlo simulations. We found that Basolite® C300 show an unprecedented rise in capture capacity above 25 bars, as predicted by the DFT calculations. Adsorption isotherms were measured up to 200 bar using a state-of-the-art magnetic suspension balance, and in-situ FTIR studies as a function of pressure allowed characterizing the preferential adsorption sites, and their occupancy with increasing pressure. Monte Carlo molecular simulations were used to infer nanoscopic information of the adsorption mechanism, showing the sorbent–CO2 interactions from structural and energetic viewpoints.

Graphical abstractUnit cells for studied Basolite® MOFs and absolute CO2 absorbed amounts (n).Figure optionsDownload full-size imageDownload as PowerPoint slide