CO2 Hydration Shell Structure and Transformation
| Autor: | Pavlin D. Mitev, Dor Ben-Amotz, Samual R. Zukowski, Kersti Hermansson |
|---|---|
| Rok vydání: | 2017 |
| Předmět: |
010304 chemical physics
Chemistry Hydrogen bond 010402 general chemistry 01 natural sciences 0104 chemical sciences symbols.namesake Crystallography Transformation (function) Solvation shell 0103 physical sciences Tetrahedron Theoretical chemistry symbols Molecule General Materials Science Physics::Chemical Physics Physical and Theoretical Chemistry Spectroscopy Raman spectroscopy Physics::Atmospheric and Oceanic Physics |
| Zdroj: | The Journal of Physical Chemistry Letters. 8:2971-2975 |
| ISSN: | 1948-7185 |
| DOI: | 10.1021/acs.jpclett.7b00971 |
| Popis: | The hydration-shell of CO2 is characterized using Raman multivariate curve resolution (Raman-MCR) spectroscopy combined with ab initio molecular dynamics (AIMD) vibrational density of states simulations, to validate our assignment of the experimentally observed high-frequency OH band to a weak hydrogen bond between water and CO2. Our results reveal that while the hydration-shell of CO2 is highly tetrahedral, it is also occasionally disrupted by the presence of entropically stabilized defects associated with the CO2-water hydrogen bond. Moreover, we find that the hydration-shell of CO2 undergoes a temperature-dependent structural transformation to a highly disordered (less tetrahedral) structure, reminiscent of the transformation that takes place at higher temperatures around much larger oily molecules. The biological significance of the CO2 hydration shell structural transformation is suggested by the fact that it takes place near physiological temperatures. |
| Databáze: | OpenAIRE |
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