期刊
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES
卷 113, 期 D19, 页码 -出版社
AMER GEOPHYSICAL UNION
DOI: 10.1029/2007JD009148
关键词
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资金
- Swiss Federal Institute of Technology (ETH), Zurich
- Schweizerischer Nationalfonds [200020-113476]
We present results from ab initio calculations for the structures and energetic properties of neutral clusters containing water, carbon dioxide, and nitrous oxide using the complete basis set CBS-Q multilevel procedure. Gas phase hydration energies Delta G(0), enthalpies Delta H-0, and entropies Delta S-0 for the stepwise attachment of water onto clusters according to X center dot(H2O)(n) + H2O <-> X center dot(H2O)(n+1) (X = CO2, N2O, and H2O) are reported for n <= 4. In particular, our results demonstrate that values for the incremental hydration enthalpies and entropies of all three gases CO2, N2O, and H2O asymptotically approach values characteristic of bulk water (i.e., -44.0 kJ mol(-1) for the enthalpy and -118.8 J K-1 mol(-1) for the entropy of condensation) following attachment of around three to four water molecules. Our ab initio calculations indicate that water attachment onto CO2, N2O, and H2O is a thermodynamically favorable process, such that hydrated CO2 center dot(H2O)(n), N2O center dot(H2O)(n), and H2O center dot(H2O)(n) clusters would form a significant atmospheric repository of these species.
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