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Issue 22, 2018
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Solute clustering in undersaturated solutions – systematic dependence on time, temperature and concentration

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Abstract

Molecular clustering and solvent–solute interactions in isopropanol solutions of fenoxycarb have been thoroughly and systematically investigated by dynamic light scattering, small-angle X-ray scattering, and nanoparticle tracking, supported by infrared spectroscopy and molecular dynamics simulations. The existence of molecular aggregates, clusters, ranging in size up to almost a micrometre is clearly recorded at undersaturated as well as supersaturated conditions by all three analysis techniques. The results systematically reveal that the cluster size increases with solute concentration and time at stagnant conditions. For most concentrations the time scale of cluster growth is of the order of days. In undersaturated solutions the size appears to eventually reach a maximum value, higher the higher the concentration. Below a certain concentration threshold clusters are significantly smaller. Clusters are found to be smaller in solutions pre-heated at a higher temperature, which offers a possible explanation for the so-called “history of solution” effect. The cluster distribution is influenced by filtration through membranes with a pore size of 0.1 μm, offering an alternative explanation for the “foreign particle-catalysed nucleation” effect. At moderate concentrations larger clusters appear to be sheared into smaller ones, but the original size distribution is rapidly re-established. At higher concentrations, although still well below solubility, the cluster size as well as solute concentration are strongly affected, suggesting that larger clusters contain at least a core of more organized molecules not able to pass through the filter.

Graphical abstract: Solute clustering in undersaturated solutions – systematic dependence on time, temperature and concentration

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Supplementary files

Article information


Submitted
07 Mar 2018
Accepted
21 May 2018
First published
21 May 2018

This article is Open Access

Phys. Chem. Chem. Phys., 2018,20, 15550-15559
Article type
Paper

Solute clustering in undersaturated solutions – systematic dependence on time, temperature and concentration

M. Svärd, K. Renuka Devi, D. Khamar, D. Mealey, D. Cheuk, J. Zeglinski and Å. C. Rasmuson, Phys. Chem. Chem. Phys., 2018, 20, 15550
DOI: 10.1039/C8CP01509K

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