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Can Jones-Dole's B-Coefficient be a Consistent Structure-Making/Breaking Marker? Rigorous Molecular-Based Analysis
Ariel A Chialvo1, Oscar D Crisalle2
1Retired scientist, Knoxville, Tennessee 37922-3108, United States.
The Journal of Physical Chemistry. B
|October 26, 2021
Summary
The study questions the reliability of Jones-Dole
Area of Science:
- Physical Chemistry
- Solution Thermodynamics
- Solute-Solvent Interactions
Background:
- The Jones-Dole B-coefficient is widely used to infer solute behavior in solutions.
- Its correlation with structure-making/breaking ability is often assumed but lacks rigorous justification.
- Microstructural information embedded within the B-coefficient remains unclear.
Purpose of the Study:
- To rigorously analyze the connection between the Jones-Dole B-coefficient and solute structure-making/breaking ability.
- To determine if the B-coefficient contains microstructural information.
- To evaluate the validity of using the B-coefficient as a marker for solute-induced structural changes.
Main Methods:
- Developed a fundamental statistical mechanical approach linking microscopic solute-induced perturbations to macroscopic solution thermodynamics.
- Derived conditions for the B-coefficient and its temperature derivative to signify structure-making or breaking.
- Utilized a transition-state interpretation of the B-coefficient and tested with aqueous solutes.
Main Results:
- The study found a lack of unique correspondence between the B-coefficient's sign and actual solute-induced structural changes.
- Thermodynamic arguments and molecular-based signatures contradicted the predictive power of B-coefficient markers.
- The B-coefficient and its derivative were shown to be inadequate descriptors of solute-solvent interactions.
Conclusions:
- The widely used Jones-Dole B-coefficient is an unreliable marker for solute structure-making/breaking ability.
- Rigorous thermodynamic and molecular-level analysis is necessary for accurate interpretation of solute behavior.
- A cautionary approach is recommended when using viscosity-based markers in solution studies.
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