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Quantifying non-specific interactions via liquid chromatography

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Abstract

Determinations of solute–cosolute interactions from chromatography have often resulted in problems, such as the “antibinding” (or a negative binding constant) between the solute and micelle in micellar liquid chromatography (MLC) or indeterminacy of salt–ligand binding strength in high-performance affinity chromatography (HPAC). This shows that the stoichiometric binding models adopted in many chromatographic analyses cannot capture the non-specific nature of solvation interactions. In contrast, an approach using statistical thermodynamics handles these complexities without such problems and directly links chromatographic data to, for example, solubility data via a universal framework based on Kirkwood–Buff integrals (KBI) of the radial distribution functions. The chromatographic measurements can now be interpreted within this universal theoretical framework that has been used to rationalize small solute solubility, biomolecular stability, binding, aggregation and gelation. In particular, KBI analysis identifies key solute–cosolute interactions, including excluded volume effects. We present (i) how KBI can be obtained directly from the cosolute concentration dependence of the distribution coefficient, (ii) how the classical binding model, when used solely as a fitting model, can yield the KBIs directly from the literature data, and (iii) how chromatography and solubility measurements can be compared in the unified theoretical framework provided via KBIs without any arbitrary assumptions about the stationary phase. To perform our own analyses on multiple datasets we have used an “app”. To aid readers’ understanding and to allow analyses of their own datasets, the app is provided with many datasets and is freely available on-line as an open-source resource.

Graphical abstract: Quantifying non-specific interactions via liquid chromatography

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Publication details

The article was received on 20 Nov 2018, accepted on 24 Dec 2018 and first published on 15 Jan 2019


Article type: Paper
DOI: 10.1039/C8AN02244E
Citation: Analyst, 2019, Advance Article

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    Quantifying non-specific interactions via liquid chromatography

    S. Shimizu, S. Abbott, K. Adamska and A. Voelkel, Analyst, 2019, Advance Article , DOI: 10.1039/C8AN02244E

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