Hydrogen bond network restructuring in water: Dielectric spectroscopy insights from dissolved gas studies

This study investigates the relationship between dissolved gases, particularly nitrogen, and the complex permittivity of liquids under test (LUTs). Measurements were conducted using an open-ended coaxial probe positioned inside a pressure vessel containing the LUT. Pressures ranged from 1 to 16 bar absolute, with frequency measurements between 0.5 to 10 GHz. A significant increase in the real relative permittivity ( ε ′ ) was observed in aqueous solutions, while the loss factor ( ε " ′ ) exhibited less significant changes. Conversely, non-aqueous liquids with inherently low permittivity, such as olive oil and propan-2-ol, displayed negligible changes, remaining within the measurement uncertainty. Although an increase in ε ′ was consistently observed, its magnitude varied across repeated experiments. At 5 bar in pressurised deionised water or saline solutions, approximately 60 % of experiments showed around a 4 % increase in ε ′ , while the remainder exhibited a lower increase of around 2 %. Similarly, aeration of deionised water at atmospheric pressure produced an approximate 3 % increase in ε ′ across the entire frequency range. The increase in complex permittivity was proportional to aeration time, stabilising after 30–60 min. Temperature fluctuations remained insignificant throughout all experiments, and the compressive effects of pressurisation on the LUT’s complex permittivity were confirmed to be negligible. The observed permittivity changes were attributed to the restructuring of water’s hydrogen-bond network around small hydrophobic solutes. • Gases were dissolved either via pressurisation or aeration at atmospheric pressure. • A significant increase in ε ′ of water was observed upon dissolution of gases. • A less significant increase was observed in ε " ′ . • A slim form open-ended coaxial probe was used for measurements. • The changes in complex permittivity were attributed to hydrophobic hydration.

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Publication Details

Journal
Journal of Molecular Liquids
Published
2025-10-27
DOI
https://doi.org/10.1016/j.molliq.2025.128775
Citations
1
Primary Topic
Spectroscopy and Quantum Chemical Studies
Type
article
Field-Weighted Citation Impact
1.25
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article

Hydrogen bond network restructuring in water: Dielectric spectroscopy insights from dissolved gas studies

Julian Bonello, Charles V. Sammut, Josette Caruana, Iman Farhat et al.
1 citations
Journal of Molecular Liquids
Spectroscopy and Quantum Chemical Studies
1.25
article

Hydrogen bond network restructuring in water: Dielectric spectroscopy insights from dissolved gas studies

Julian Bonello, Charles V. Sammut, Josette Caruana, Iman Farhat, Jonathan Farrugia
article en
1 citations

Abstract

This study investigates the relationship between dissolved gases, particularly nitrogen, and the complex permittivity of liquids under test (LUTs). Measurements were conducted using an open-ended coaxial probe positioned inside a pressure vessel containing the LUT. Pressures ranged from 1 to 16 bar absolute, with frequency measurements between 0.5 to 10 GHz. A significant increase in the real relative permittivity ( ε ′ ) was observed in aqueous solutions, while the loss factor ( ε " ′ ) exhibited less significant changes. Conversely, non-aqueous liquids with inherently low permittivity, such as olive oil and propan-2-ol, displayed negligible changes, remaining within the measurement uncertainty. Although an increase in ε ′ was consistently observed, its magnitude varied across repeated experiments. At 5 bar in pressurised deionised water or saline solutions, approximately 60 % of experiments showed around a 4 % increase in ε ′ , while the remainder exhibited a lower increase of around 2 %. Similarly, aeration of deionised water at atmospheric pressure produced an approximate 3 % increase in ε ′ across the entire frequency range. The increase in complex permittivity was proportional to aeration time, stabilising after 30–60 min. Temperature fluctuations remained insignificant throughout all experiments, and the compressive effects of pressurisation on the LUT’s complex permittivity were confirmed to be negligible. The observed permittivity changes were attributed to the restructuring of water’s hydrogen-bond network around small hydrophobic solutes. • Gases were dissolved either via pressurisation or aeration at atmospheric pressure. • A significant increase in ε ′ of water was observed upon dissolution of gases. • A less significant increase was observed in ε " ′ . • A slim form open-ended coaxial probe was used for measurements. • The changes in complex permittivity were attributed to hydrophobic hydration.

Journal of Molecular LiquidsVol. 439
University of Malta (MT)
Openalex Percentile: Top 16%
Spectroscopy and Quantum Chemical Studies
1.25
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