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Free energies of CO2/H-2 capture by p-tert-butylcalix[4]arene. A molecular dynamics study

Journal Article · · Journal of Chemical Physics, 127(10):Art. No. 104702
DOI:https://doi.org/10.1063/1.2768961· OSTI ID:920514
The interactions of CO2/H2 with p-tert-butylcalix[4]arene (TBC4) were studied using potential of mean force (PMF) and free energy perturbation approaches. The computed PMFs for the interaction of CO2/H2 with a single TBC4 molecule establish that the interaction of CO2 with the open end of the cage structure is attractive while interaction with H2 is not. Free energy perturbation calculations were performed for the same two guest molecules with a pair of facing TBC4 molecules used as a representative model as found in the TBC4 molecular solid. At low temperature both CO2/H2 have favorable interactions with the TBC4 pair with the CO2 interaction considerably larger. These results are in agreement with recent experimental data showing considerable CO2 uptake by TBC4 at moderate pressures. This work was performed at the Pacific Northwest National Laboratory (PNNL) and was supported by the Division of Chemical Sciences, Office of Basic Energy Sciences, U.S. Department of Energy (DOE). PNNL is operated by Battelle for the DOE.
Research Organization:
Pacific Northwest National Laboratory (PNNL), Richland, WA (US)
Sponsoring Organization:
USDOE
DOE Contract Number:
AC05-76RL01830
OSTI ID:
920514
Report Number(s):
PNNL-SA-55095; KC0301020
Journal Information:
Journal of Chemical Physics, 127(10):Art. No. 104702, Journal Name: Journal of Chemical Physics, 127(10):Art. No. 104702 Journal Issue: 10 Vol. 127; ISSN JCPSA6; ISSN 0021-9606
Country of Publication:
United States
Language:
English

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