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  Ion association in hydrothermal aqueous NaCl solutions: implications for the microscopic structure of supercritical water

Elbers, M., Schmidt, C., Sternemann, C., Sahle, C. J., Jahn, S., Albers, C., et al. (2021). Ion association in hydrothermal aqueous NaCl solutions: implications for the microscopic structure of supercritical water. Physical Chemistry Chemical Physics, 23, 14845-14856. doi:10.1039/D1CP01490K.

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 Creators:
Elbers, Mirko1, Author
Schmidt, Christian1, Author
Sternemann, Christian1, Author
Sahle, Christoph J.1, Author
Jahn, Sandro1, Author
Albers, Christian1, Author
Sakrowski, Robin1, Author
Gretarsson, Hlynur2, Author           
Sundermann, Martin2, Author           
Tolan, Metin1, Author
Wilke, Max1, Author
Affiliations:
1External Organizations, ou_persistent22              
2Physics of Correlated Matter, Max Planck Institute for Chemical Physics of Solids, Max Planck Society, ou_1863445              

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Free keywords: Alkali halides, Hydrogen bonds, Molecular structure, Oxygen, Sodium chloride, Sodium hydroxide, Aqueous NaCl solutions, Hydrogen bond networks, Microscopic structures, Pressure and temperature, Simulated trajectories, Structural information, Supercritical condition, Temperature-dependent changes, Ions
 Abstract: Knowledge of the microscopic structure of fluids and changes thereof with pressure and temperature is important for the understanding of chemistry and geochemical processes. In this work we investigate the influence of sodium chloride on the hydrogen-bond network in aqueous solution up to supercritical conditions. A combination ofin situX-ray Raman scattering andab initiomolecular dynamics simulations is used to probe the oxygen K-edge of the alkali halide aqueous solution in order to obtain unique information about the oxygen's local coordination around the ions,e.g.solvation-shell structure and the influence of ion pairing. The measured spectra exhibit systematic temperature dependent changes, which are entirely reproduced by calculations on the basis of structural snapshots obtainedvia ab initiomolecular dynamics simulations. Analysis of the simulated trajectories allowed us to extract detailed structural information. This combined analysis reveals a net destabilizing effect of the dissolved ions which is reduced with rising temperature. The observed increased formation of contact ion pairs and occurrence of larger polyatomic clusters at higher temperatures can be identified as a driving force behind the increasing structural similarity between the salt solution and pure water at elevated temperatures and pressures with drawback on the role of hydrogen bonding in the hot fluid. We discuss our findings in view of recent results on hot NaOH and HCl aqueous fluids and emphasize the importance of ion pairing in the interpretation of the microscopic structure of water. © the Owner Societies 2021.

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Language(s): eng - English
 Dates: 2021-06-222021-06-22
 Publication Status: Published in print
 Pages: -
 Publishing info: -
 Table of Contents: -
 Rev. Type: -
 Identifiers: DOI: 10.1039/D1CP01490K
 Degree: -

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Title: Physical Chemistry Chemical Physics
  Abbreviation : Phys. Chem. Chem. Phys.
Source Genre: Journal
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Publ. Info: Cambridge, England : Royal Society of Chemistry
Pages: - Volume / Issue: 23 Sequence Number: - Start / End Page: 14845 - 14856 Identifier: ISSN: 1463-9076
CoNE: https://pure.mpg.de/cone/journals/resource/954925272413_1