Comment on “Determination of the quaternary phase diagram of the water–ethylene glycol–sucrose–NaCl system and a comparison between two theoretical methods for synthetic phase diagrams” Cryobiology 61 (2010) 52–57

Zielinski, Michal W.; McGann, Locksley E.; Nychka, John A.; Elliott, Janet A.W.

doi:10.1016/j.cryobiol.2015.03.006

Cited by 5 publications

(11 citation statements)

References 13 publications

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“…However, we point out in Zielinski et al that because the osmotic virial equation mass balance has one more degree of freedom than the gaseous virial equation (due to the presence of a solvent), the reasons that make these combining rules inappropriate for the gaseous virial equation do not apply to the osmotic virial equation. The multisolute osmotic virial equation, eq , is extremely useful because this single equation can make accurate predictions for combinations of many types of solutes such as organic solvents, ,,, alcohols, ,,, sugars, , starches, proteins, , electrolytes, ,, and ionic and nonionic micelle-forming surfactants, whereas most thermodynamic solution theories are only applicable to a small class of molecules and cannot be used for mixtures of molecules from different classes. Three examples are shown in Figure .…”

Section: Gibbsian Composite-system Thermodynamics Methodsmentioning

confidence: 99%

“…Several of the thermodynamic models developed by our group (including equations of state, Gibbsian thermodynamics, and nonequilibrium thermodynamics) have been motivated by cryobiology, the study of the response of living cells and tissues to extremely low temperature such as the temperature of liquid nitrogen (−196 °C) used for long-term storage ubiquitously in cell and tissue banking for transplant medicine, in the commercial supply of cells for research, and in managing the supply of cells within research laboratories. ,− ,− ,,− In cryobiology applications, the two fluid phases in equilibrium might be the inside and outside of a cell separated by the plasma membrane, or pure water ice and the unfrozen fraction more concentrated in solutes than before freezing.…”

Section: Applications Of Gibbsian Composite-system Thermodynamicsmentioning

confidence: 99%

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Gibbsian Surface Thermodynamics

Elliott

2020

J. Phys. Chem. B

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Gibbsian composite-system thermodynamics is the framework governing the equilibrium of composite systems, including systems that at equilibrium have more than one value of pressure because of the action of surface tension, semipermeable membranes, or fields, and thus cannot be treated as simple systems. J. W. Gibbs’s paper that lays out composite-system thermodynamics, “On the Equilibrium of Heterogeneous Substances”, communicated in two parts in 1876 and 1878, is widely regarded as one of the most important pieces of scientific literature of its century. Many scientists adopted and stressed the importance of Gibbsian thermodynamics. In 1960, H. B. Callen wrote a textbook that made Gibbsian composite-system thermodynamics more accessible to thermodynamicists. However, Callen’s book left out Gibbs’s work on curved fluid interfaces and did not treat the complicated nonideal systems of interest to today’s thermodynamicists. In this Feature Article, I have attempted to convey in a comprehensive manner the framework of Gibbsian composite-system thermodynamics including in detail the treatment of systems with interface effects and with nonideal, multicomponent phases. This work lays out the relationships between important equilibrium equations including the following: the Gibbs–Duhem equation, the Gibbs adsorption equation, the Young–Laplace equation, the Young equation, the Cassie–Baxter equation, the Wenzel equation, the Kelvin equation, the Gibbs–Thompson equation, and the Ostwald–Freundlich equation, including nonideal and multicomponent forms. Equations of state that are often useful for Gibbsian composite-system thermodynamics are reviewed including adsorption isotherms and our own work on two semiempirical equations of state: the Elliott et al. form of the osmotic virial equation and the Shardt–Elliott–Connors–Wright equation for the temperature and composition dependence of surface tension. I summarize the work of our group developing Gibbisan composite-system thermodynamics including new equations for such things as the curvature-induced depression of the eutectic temperature or the removal of azeotropes by nanoscale fluid interface curvature. Gibbsian composite-system thermodynamics has broad applications in biotechnology, nanostructured materials, surface textures and coatings, microfluidics, nanoscience, atmospheric and environmental physics, among others.

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Section: Gibbsian Composite-system Thermodynamics Methodsmentioning

confidence: 99%

Section: Applications Of Gibbsian Composite-system Thermodynamicsmentioning

confidence: 99%

Gibbsian Surface Thermodynamics

Elliott

2020

J. Phys. Chem. B

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“…The virial coefficients are functions of temperature and weak functions of pressure . However, when the osmotic virial equation is fit to phase equilibrium data that is a function of temperature, good fits are empirically obtained with constant osmotic virial coefficients. − The polynomial is usually truncated to second order or third order for highly nonideal solutions (such as those with nondilute macromolecules).…”

Section: Theorymentioning

confidence: 99%

“…However, the problem is in developing appropriate mixing rules . Different types of equations of state have been used to model activity coefficients based on type of mixtures, such as the Soave–Redlich–Kwong equation and the Peng–Robinson equation for vapor–liquid equilibrium of petrochemical mixtures and the osmotic virial equations of state for aqueous mixtures. − …”

Section: Introductionmentioning

confidence: 99%

“…The osmotic virial equation fits are then compared with fits with the one- or two-parameter Margules model for five water/solute systems: water/glycerol, water/acetic acid, water/propanoic acid, water/mono-ethylene glycol, and water/sulfolane. A main advantage of the osmotic virial equation is that mixing rules have been derived from statistical first principles and have been successfully used to predict the phase behavior of aqueous multisolute systems with a wide range of solutes including solvents, , electrolytes, − alcohols, − sugars, − starches, proteins, , and even ionic or nonionic micelle-forming surfactants. With the similarity of the Margules model to the osmotic virial equation developed in this work, it is possible that similar mixing rules can be used for applying the Margules model to multisolute mixtures.…”

Section: Introductionmentioning

confidence: 99%

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Comparison of the Osmotic Virial Equation with the Margules Activity Model for Solid–Liquid Equilibrium

Zargarzadeh

Elliott

2019

J. Phys. Chem. B

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The main goal of this paper is to compare the general polynomial forms of the osmotic virial equation and the Margules model for the liquid activity coefficients in binary systems. The coefficients/parameters in each model can be calculated based on best fits to experimental phase equilibrium data. Here, the activity coefficient models were combined with the equation of solid−liquid equilibrium. We obtain the coefficients/parameters for the osmotic virial equation and the one-and two-parameter Margules models and compare the accuracy of each model for fitting the experimental data for five water/solute systems: water/glycerol, water/acetic acid, water/propanoic acid, water/mono-ethylene glycol, and water/sulfolane. In obtaining the osmotic virial coefficients, we present a method to fit the equation to the entire range of data including both the ice-formation region and the solute-precipitation region. In expression of the concentration effect of the solute, we showed that the integration constant that arises from the Gibbs−Duhem equation is dependent on the osmotic virial coefficients. The osmotic virial equation is of great interest for its ability to empirically model a very wide range of aqueous solutions and as such is one of the most widely used solution models in biology.

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Nonideal Solute Chemical Potential Equation and the Validity of the Grouped Solute Approach for Intracellular Solution Thermodynamics

et al. 2017

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The prediction of nonideal chemical potentials in aqueous solutions is important in fields such as cryobiology, where models of water and solute transport-that is, osmotic transport-are used to help develop cryopreservation protocols and where solutions contain many varied solutes and are generally highly concentrated and thus thermodynamically nonideal. In this work, we further the development of a nonideal multisolute solution theory that has found application across a broad range of aqueous systems. This theory is based on the osmotic virial equation and does not depend on multisolute data. Specifically, we derive herein a novel solute chemical potential equation that is thermodynamically consistent with the existing model, and we establish the validity of a grouped solute model for the intracellular space. With this updated solution theory, it is now possible to model cellular osmotic behavior in nonideal solutions containing multiple permeating solutes, such as those commonly encountered by cells during cryopreservation. In addition, because we show here that for the osmotic virial equation the grouped solute approach is mathematically equivalent to treating each solute separately, multisolute solutions in other applications with fixed solute mass ratios can now be treated rigorously with such a model, even when all of the solutes cannot be enumerated.

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Comment on “Determination of the quaternary phase diagram of the water–ethylene glycol–sucrose–NaCl system and a comparison between two theoretical methods for synthetic phase diagrams” Cryobiology 61 (2010) 52–57

Cited by 5 publications

References 13 publications

Gibbsian Surface Thermodynamics

Gibbsian Surface Thermodynamics

Comparison of the Osmotic Virial Equation with the Margules Activity Model for Solid–Liquid Equilibrium

Nonideal Solute Chemical Potential Equation and the Validity of the Grouped Solute Approach for Intracellular Solution Thermodynamics

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