Some observations on the behaviour of the thermodynamic interaction parameter in dilute polymer solutions

Dijk, Marc A. van; Wakker, A.

doi:10.1016/0032-3861(93)90295-l

Cited by 9 publications

(14 citation statements)

References 9 publications

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“…Opalescence and phase separation in solution have been thoroughly studied in binary liquid systems and in polymer (colloidal) solutions, ,− and the knowledge gained has been of immense help in understanding the physical instabilities in protein solutions. In this section, the thermodynamics and the kinetic mechanism resulting in phase separation for protein solutions (in accordance with the colloidal theory) are briefly discussed followed by a discussion on the theoretical concepts of opalescence or light scattering in solution.…”

Section: Theoretical Aspects Of Opalescence and Liquid–liquid Phase S...mentioning

confidence: 99%

“…This section briefly discusses thermodynamically stable–unstable system as represented by a generic phase diagram followed by a discussion on fluctuations of thermodynamic quantities and change in enthalpy/entropy associated with it. Please note that the thermodynamic equations/terms are simplified in this section to fit the scope of the current manuscript, and readers can refer to thermodynamic books/references for further detail equations/derivations. − …”

Section: Theoretical Aspects Of Opalescence and Liquid–liquid Phase S...mentioning

confidence: 99%

“…Phase separation in pure liquids and binary systems are commonly described by a pressure–volume and temperature–concentration phase diagram, respectively. ,,,− Phase diagram for a binary system (Figure ) has a liquidus or solubility line, corresponding to the solid–liquid phase transition in one-component system, and a liquid–liquid coexistence line (binodal curve/miscibility curve), corresponding to the vapor/gas–liquid phase transition in one-component system. Protein being nonvolatile exhibits liquid–liquid equilibrium, while the binary system constituting volatile component may also exhibit vapor–liquid equilibrium.…”

Section: Theoretical Aspects Of Opalescence and Liquid–liquid Phase S...mentioning

confidence: 99%

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Pharmaceutical Perspective on Opalescence and Liquid–Liquid Phase Separation in Protein Solutions

Raut

Kalonia

2016

Mol. Pharmaceutics

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Opalescence in protein solutions reduces aesthetic appeal of a formulation and can be an indicator of the presence of aggregates or precursor to phase separation in solution signifying reduced product stability. Liquid-liquid phase separation of a protein solution into a protein-rich and a protein-poor phase has been well-documented for globular proteins and recently observed for monoclonal antibody solutions, resulting in physical instability of the formulation. The present review discusses opalescence and liquid-liquid phase separation (LLPS) for therapeutic protein formulations. A brief discussion on theoretical concepts based on thermodynamics, kinetics, and light scattering is presented. This review also discusses theoretical concepts behind intense light scattering in the vicinity of the critical point termed as "critical opalescence". Both opalescence and LLPS are affected by the formulation factors including pH, ionic strength, protein concentration, temperature, and excipients. Literature reports for the effect of these formulation factors on attractive protein-protein interactions in solution as assessed by the second virial coefficient (B2) and the cloud-point temperature (Tcloud) measurements are also presented. The review also highlights pharmaceutical implications of LLPS in protein solutions.

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Section: Theoretical Aspects Of Opalescence and Liquid–liquid Phase S...mentioning

confidence: 99%

Section: Theoretical Aspects Of Opalescence and Liquid–liquid Phase S...mentioning

confidence: 99%

Section: Theoretical Aspects Of Opalescence and Liquid–liquid Phase S...mentioning

confidence: 99%

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Pharmaceutical Perspective on Opalescence and Liquid–Liquid Phase Separation in Protein Solutions

Raut

Kalonia

2016

Mol. Pharmaceutics

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“…Thus, the χ parameter characterizes the overall interaction of a polymer segment with solvent molecules. Presently, it is common practice to express χ as the sum of an enthalpic and an entropic contribution: χ h and χ s are considered constants that depend on the polymer and solvent but are independent of the fluid temperature, T , and polymer molecular weight, M. Recent findings have shown that χ s is correlated with χ h and the polymer–solvent theta temperature θ3: Thus, the dependence of χ on the temperature can be expressed as the sum of enthalpic, χ h / T , and entropic, χ s = ½ − (χ h /θ), contributions: Use of this expression for χ in eq. (1) gives K θ and χ h are constants for a given polymer and solvent.…”

Section: Introductionmentioning

confidence: 99%

Intrinsic viscosity dependence on polymer molecular weight and fluid temperature

Rushing

Hester

2003

J of Applied Polymer Sci

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Experimental solution intrinsic viscosity responses to temperature and polymer molecular weight variations were used to test the modeling capability of a simplified intrinsic viscosity equation. The multiple linear equation contains three parameters that are related to the thermodynamic properties of a polymer solution. Simple linear regression was used to produce an intrinsic viscosity equation containing unique fitted parameters for each of three solutions. These parameters describe the polymer coil size at unperturbed conditions and the polymer coil expansion capabilities of the solvent as a function of fluid temperature and molecular weight.

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“…χ h and χ s are considered as constants that depend on the polymer and solvent but are independent of the fluid temperature, T , and polymer average molecular weight, M . Recent findings have shown that χ s is correlated with χ h and the polymer–solvent theta temperature, θ 27 …”

Section: Resultsmentioning

confidence: 99%

Solution thermodynamics of poly(ethylene glycol)/water systems

Özdemir

Güner

2006

J of Applied Polymer Sci

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ABSTRACT:The unperturbed molecular dimensions of poly(ethylene glycol) (PEG) samples (of different molecular weights) have been evaluated in aqueous solutions from viscosity measurements at 25, 30, 35, and 40°C. The unperturbed dimension, K , has been determined from extrapolation methods, i.e., Kurata-Stockmayer-Fixman (KSF), Inagaki-Suzuki-Kurata (ISK), and Berry equations. The hydrodynamic expansion factor, ␣ , as well as the unperturbed root-mean-square end-to-end distance, ͗r, found for the system indicated that the polymer coils contract as the temperature is raised from 25 to 40°C. The long-range interaction (excluded volume) parameter, B, was also evaluated and a significant decrease was found for the PEG/water system between 25 and 40°C. The theta temperatures, , were obtained from the temperature dependence of (1/2 Ϫ ) and the second virial coefficient was detected in the temperature interval of 25-40°C for the system and quite a good agreement with the calculated values evaluated via extrapolation and interpolation methods was observed. The thermodynamic interaction parameter was evaluated through the sum of the individual values of enthalpy and entropy dilution parameters, H and S , for PEG samples. All the unperturbed molecular dimensions of PEG/water system were calculated and compared according to M w and M n values of PEG samples. Calculated values were interpreted mainly on the basis of hydrogen-bond formation between polymer segments and PEG-water molecules in solution.

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Some observations on the behaviour of the thermodynamic interaction parameter in dilute polymer solutions

Cited by 9 publications

References 9 publications

Pharmaceutical Perspective on Opalescence and Liquid–Liquid Phase Separation in Protein Solutions

Pharmaceutical Perspective on Opalescence and Liquid–Liquid Phase Separation in Protein Solutions

Intrinsic viscosity dependence on polymer molecular weight and fluid temperature

Solution thermodynamics of poly(ethylene glycol)/water systems

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