he interaction of CO with graphene was studied at differenttheoretical levels. Qua ntum-mechanical calculations on finitegraphene models with the use of coronene for coupled clustercalculations and circumcoronene for B97D calculations showedthat there was no preferential site for adsorption and that themost important factor was the orientation of CO relative tographene. The parallel orientation was preferred, with bindingenergies around 9 kJmol1at the CCSD(T) and B97D levels,which was in good agreement with experimental findings.From a large number of CO–circumcoronene and CO–CO inter-actions, computed at different distances and randomly gener-ated orientations, parameters were fit to the improved Len-nard–Jones potential. Such potentials, together with others de-scribing the intramolecular dynamics of graphene, were subse-quently employed in classical molecular-dynamics simulationsof the adsorption of CO on graphene by using the canonicalensemble. The obtained results showed that the introductionof flexibility in graphene, which simulated the effects associat-ed to curvature of the surface, diminished the adsorption leveland that, as expected, adsorption also diminished with temper-ature.
Modeling the Interaction of Carbon Monoxide with Flexible Graphene: From Coupled Cluster Calculations to Molecular-Dynamics Simulations
Faginas-Lago, Noelia
Membro del Collaboration Group
;Vekeman, JelleMembro del Collaboration Group
;
2018
Abstract
he interaction of CO with graphene was studied at differenttheoretical levels. Qua ntum-mechanical calculations on finitegraphene models with the use of coronene for coupled clustercalculations and circumcoronene for B97D calculations showedthat there was no preferential site for adsorption and that themost important factor was the orientation of CO relative tographene. The parallel orientation was preferred, with bindingenergies around 9 kJmol1at the CCSD(T) and B97D levels,which was in good agreement with experimental findings.From a large number of CO–circumcoronene and CO–CO inter-actions, computed at different distances and randomly gener-ated orientations, parameters were fit to the improved Len-nard–Jones potential. Such potentials, together with others de-scribing the intramolecular dynamics of graphene, were subse-quently employed in classical molecular-dynamics simulationsof the adsorption of CO on graphene by using the canonicalensemble. The obtained results showed that the introductionof flexibility in graphene, which simulated the effects associat-ed to curvature of the surface, diminished the adsorption leveland that, as expected, adsorption also diminished with temper-ature.I documenti in IRIS sono protetti da copyright e tutti i diritti sono riservati, salvo diversa indicazione.
