Molecular diffusion in ternary poly(vinyl alcohol) solutions

doi:10.1007/s11705-021-2121-3

Front. Chem. Sci. Eng.

2022, Vol. 16

Issue (6) : 1003-1016 https://doi.org/10.1007/s11705-021-2121-3

RESEARCH ARTICLE

Molecular diffusion in ternary poly(vinyl alcohol) solutions

Katarzyna Majerczak¹, Ophelie Squillace¹, Zhiwei Shi², Zhanping Zhang², Zhenyu J. Zhang¹(

)

¹. School of Chemical Engineering, University of Birmingham, Birmingham B15 2TT, UK
². The Procter and Gamble Company, Cincinnati, OH 45040, USA

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Abstract

The diffusion kinetics of a molecular probe—rhodamine B—in ternary aqueous solutions containing poly(vinyl alcohol), glycerol, and surfactants was investigated using fluorescence correlation spectroscopy and dynamic light scattering. We show that the diffusion characteristics of rhodamine B in such complex systems is determined by a synergistic effect of molecular crowding and intermolecular interactions between chemical species. The presence of glycerol has no noticeable impact on rhodamine B diffusion at low concentration, but significantly slows down the diffusion of rhodamine B above 3.9% (w/v) due to a dominating steric inhibition effect. Furthermore, introducing surfactants (cationic/nonionic/anionic) to the system results in a decreased diffusion coefficient of the molecular probe. In solutions containing nonionic surfactant, this can be explained by an increased crowding effect. For ternary poly(vinyl alcohol) solutions containing cationic or anionic surfactant, surfactant–polymer and surfactant–rhodamine B interactions alongside the crowding effect of the molecules slow down the overall diffusivity of rhodamine B. The results advance our insight of molecular migration in a broad range of industrial complex formulations that incorporate multiple compounds, and highlight the importance of selecting the appropriate additives and surfactants in formulated products.

Keywords fluorescence correlation spectroscopy poly(vinyl alcohol) anomalous diffusion crowding effects dynamic light scattering binding effects rhodamine B

Corresponding Author(s): Zhenyu J. Zhang

Online First Date: 27 December 2021 Issue Date: 28 June 2022

Cite this article:

Katarzyna Majerczak,Ophelie Squillace,Zhiwei Shi, et al. Molecular diffusion in ternary poly(vinyl alcohol) solutions[J]. Front. Chem. Sci. Eng., 2022, 16(6): 1003-1016.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-021-2121-3
https://academic.hep.com.cn/fcse/EN/Y2022/V16/I6/1003

Fig.1 Chemical structures of the compounds used.

Scheme 1 Preparation method for test solutions of various compositions: (a) PVA solutions of various concentrations, (b) PVA/glycerol solutions of various ratio of components (with changes in PVA concentration), (c) PVA/glycerol solutions of various ratio of components (with almost constant PVA concentration), (d) PVA/surfactant solutions, (e) PVA/glycerol/surfactant solutions, and (f) concentrated PVA/glycerol/surfactant solutions.

Tab.1 Compositions used to investigate the dependence of RhB diffusion coefficient on PVA concentration ^a)

Fig.2 Normalized diffusion coefficient of RhB as a function of PVA concentration without (samples 2–6) and with glycerol (samples 1a–5a). Solid lines represent fitting based on Eq. (6), with diffusion coefficient calculated using Eq. (1). Closed symbols correspond to PVA solution diluted with water, while open symbols are for PVA solution diluted with glycerol solution. Color code for each PVA concentration corresponds to DLS data (Fig. 3). Standard errors are based on 10 measurements.

Fig.3 Distribution of hydrodynamic diameter for solutions of various PVA concentration with the addition of (a) water, (b) glycerol stock solution, and (c) pure glycerol. The percentage of polymer in the graph is given in %(w/v).

Tab.2 Composition of PVA-based solutions with the addition of glycerol ^a)

Fig.4 Diffusion coefficient of RhB in PVA solution with the addition of pure glycerol. Error bars are one standard error around the mean, number of measurements equal to 10.

Tab.3 Viscosity and average hydrodynamic diameter of PVA solutions with the addition of glycerol and surfactant of various head group chemistry

Fig.5 Average diffusion coefficient of RhB in PVA solutions with the addition of surfactant and water (samples 4c–4e) or glycerol solution (samples 4f–4h), compared against control samples with no surfactants (4, 4a). Error bars are standard error based on 10 repeats.

Fig.6 Possible interactions between (a) RhB and both cationic and anionic surfactants; (b) PVA–surfactant tail group interactions, using SDS molecule as an example.

Fig.7 Particle size distribution for (a) PVA/water/surfactant (compositions 4c–4e), (b) PVA/glycerol/surfactant solutions (compositions 4f–4h), and (c) PVA/pure glycerol/pure surfactant solutions (compositions 4i–4k). The percentages of polymer and glycerol in the graphs are given in %(w/v).

Fig.8 Average diffusion coefficients of RhB in PVA solutions with the addition of pure glycerol and surfactant (samples 4i–4k, blue columns), compared against equivalent samples with the addition of glycerol and surfactant solutions (4f–4h, green columns) and corresponding control solutions containing no surfactant (4b and 4a). Error bars are standard error based on 10 repeats.

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