Le, TTB;
Striolo, A;
Cole, DR;
(2018)
Structural and dynamical properties predicted by reactive force fields simulations for four common pure fluids at liquid and gaseous non-reactive conditions.
Molecular Simulation
, 44
(10)
pp. 826-839.
10.1080/08927022.2018.1455005.
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Abstract
Four common pure fluids were chosen to elucidate the reliability of reactive force fields in estimating bulk properties of selected molecular systems: CH 4 , H 2 O, CO 2 and H 2 . The pure fluids are not expected to undergo chemical reactions at the conditions chosen for these simulations. The ‘combustion’ ReaxFF was chosen as reactive force field. In the case of water, we also considered the ‘aqueous’ ReaxFF model. The results were compared to data obtained implementing popular classic force fields. In the gas phase, it was found that simulations conducted using the ‘combustion’ ReaxFF formalism yield structural properties in reasonable good agreement with classic simulations for CO 2 and H 2 , but not for CH 4 and H 2 O. In the liquid phase, ‘combustion’ ReaxFF simulations reproduce reasonably well the structure obtained from classic simulations for CH 4 , degrade for CO 2 and H 2 , and are rather poor for H 2 O. In the gas phase, the simulation results are compared to experimental second virial coefficient data. The ‘combustion’ ReaxFF simulations yield second virial coefficients that are not sufficiently negative for CH 4 and CO 2 , and slightly too negative for H 2 . The ‘combustion’ ReaxFF parameterisation induces too strong an effective attraction between water molecules, while the ‘aqueous’ ReaxFF yields a second virial coefficient that is in reasonable agreement with experiments. The ‘combustion’ ReaxFF parameterisation yields acceptable self-diffusion coefficients for gas-phase properties of CH 4 , CO 2 and H 2 . In the liquid phase, the results are good for CO 2 , while the self-diffusion coefficient predicted for liquid CH 4 is slower, and that predicted for liquid H 2 is about nine times faster than those expected based on classic simulations. The ‘aqueous’ ReaxFF parameterisation yields good results for both the structure and the diffusion of both liquid and vapour water.
| Type: | Article |
|---|---|
| Title: | Structural and dynamical properties predicted by reactive force fields simulations for four common pure fluids at liquid and gaseous non-reactive conditions |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1080/08927022.2018.1455005 |
| Publisher version: | https://doi.org/10.1080/08927022.2018.1455005 |
| Language: | English |
| Additional information: | This version is the author accepted manuscript. For information on re-use, please refer to the publisher’s terms and conditions. |
| Keywords: | Self-diffusion coefficient, radial distribution function, bulk fluids |
| UCL classification: | UCL UCL > Provost and Vice Provost Offices > UCL BEAMS UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science > Dept of Chemical Engineering |
| URI: | https://discovery.ucl.ac.uk/id/eprint/10048230 |
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