Energetic origin of proton affinity to the air/water interface.
作者： Hideaki Takahashi , Kunihiro Maruyama , Yasuhito Karino , Akihiro Morita , Masayoshi Nakano
DOI: 10.1021/JP2015676
关键词: Ion 、 Hydrogen 、 Solvation 、 Chemical physics 、 Molecule 、 Chemistry 、 Solvent 、 Proton affinity 、 Gibbs free energy 、 Crystallography 、 Polarization (electrochemistry)
摘要: Recent experimental and theoretical studies showed the preference of hydronium ion for vapor/water interface. To investigate mechanism responsible surface propensity this ion, we performed a series novel quantum chemical simulations combined with theory solutions. The solvation free energy H(3)O(+) solute placed at interface was obtained as -97.9 kcal/mol, being more stable by 3.6 kcal/mol than that embedded in bulk. Further, decomposed energies into contributions from water molecules residing oxygen hydrogen sides to clarify origin preference. When displaced bulk interface, it shown contribution side is destabilized ∼10 because reduction number surrounding solvent molecules. It observed, however, due unexpectedly stabilizing surpasses destabilization opposite side. We found stabilization originates solute-solvent interaction medium range beyond nearest neighbor. also revealed solute's electronic polarization amounts about half total change associated displacement
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