期刊
JOURNAL OF CHEMICAL PHYSICS
卷 130, 期 3, 页码 -出版社
AIP Publishing
DOI: 10.1063/1.3059008
关键词
ab initio calculations; carbon compounds; heat of vaporisation; Monte Carlo methods
资金
- University of Nottingham High-Performance Computing facility
- Engineering and Physical Sciences Research Council [EP/E06082X/1]
- EPSRC [EP/E06082X/1] Funding Source: UKRI
- Engineering and Physical Sciences Research Council [EP/E06082X/1] Funding Source: researchfish
We describe quantum-chemical calculations on dimers of CO2 and use the results to develop first-principles models for Gibbs ensemble Monte Carlo simulations of the phase coexistence curve. Isotropic pairwise potentials are insufficient to model the phase behavior and overestimate the binding in liquid CO2 by 4 kJ mol(-1). An anisotropic treatment of the atoms in the pairwise potential reduces the strength of the binding by similar to 0.5 kJ mol(-1). We use ab initio calculations on trimers of CO2 to assess the strength of nonadditive interactions. Including nonadditive dispersion in Gibbs ensemble simulations gives an enthalpy of vaporization within 1.5 kJ mol(-1) of the experimental value over a wide range of temperatures.
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