Abstract
The effect of an excess of surfactant on the thermophoresis of a sterically stabilized ferrofluid is investigated experimentally by forced Rayleigh scattering (FRS). The experiments are performed with a stable magnetic fluid sample to which controlled amounts of surfactant are added. A decrease in the thermally induced transport of magnetic nanoparticles is observed while increasing the temperature T. The positive Soret coefficient \(S_{\mathrm{T}}\) decreases by adding 2 vol% of surfactant at room temperature. As shown by FRS relaxation, this decreasing is mainly associated with a reduction of the interaction between the carrier fluid and individual nanoparticles. No significant effect of extra surfactant on the sign of \(S_{\mathrm{T}}\) is observed at higher T’s (up to \(\sim \,85\,^{\circ }\)C). Dynamic light scattering at room temperature reveals the presence of a small amount of clusters/aggregates in the samples, which are hardly detectable by FRS relaxation. The presence of these small clusters/aggregates is confirmed by a rheological probing of the fluid properties. Whatever T, a small amount of added surfactant first causes a decrease of the ferrofluid viscosity, associated with a 10% decreasing of the flow activation energy. Further on, viscosity and activation energy both recover at higher excess surfactant concentrations. These results are analyzed in terms of saturation of the surfactant layer, concentration of free surfactant chains and heat of transport of the nanoparticles.
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Notes
We neglect here the term \(\frac{1}{n_{_{\mathrm{NP}}}kT} \frac{\partial \Pi }{\partial T}\) in front of \(\frac{{\hat{S}} _{{\mathrm{NP}}}}{kT}\), as it is here always smaller than 9.\(10^{-3}\) \(\hbox {K}^{-1}\).
Fluid carrier = tetradecane + dissolved free OA chains
We suppose here that \(\chi \) is associated with the entropic effect of excluded volume of the hard spheres, leading to an effective interparticle interaction with a second virial coefficient \(A_{2}=4\). We implicitly suppose that the hard sphere volume is here, at the first order, independent of the concentration of added surfactant. This point is discussed in Sects. 6 and 2 of E.S.I., where the value of \(\zeta \chi \) is also discussed.
Note that due to the adsorption process, the concentration of free OA at equilibrium in solution, which is small, is, however, not strictly zero.
A compatible value 1.38–1.43 for the OA-layer is found in the rheological study of ferrofluids in transformer oil [53].
The bi-exponential fit is as well not really convincing at \(T=85\,^{\circ }\)C for both 0 vol\(\%\) and 2 vol\(\%\) of added OA.
This is clear in Fig. 12 of [72]. Under low applied field and large Mason number, the relative viscosity of the dispersions at \(\Phi =1.5\%\) increases by a factor 10 for pH increasing from 2 to 3.5. It is stated in this text that in these conditions the system behavior is close to the zero-field one and in this range of pHs at the limit between a Sol of clusters and Gel is observed.
An analysis in terms of clusters of 3 (resp. 4) NPs would lead to a mean hydrodynamic diameter of clusters of 32.2 nm (resp. 35.4 nm), which are slightly larger (but almost compatible) with the short-time DLS determination.
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Acknowledgements
We thank Ansis Mezulis for consultations on experimental work, Guillaume Mériguet and Mikhail S. Krakov for useful discussions and Amandine Anfry, Michail M. Maiorov and Frédéric Gélébart for technical support in the experiments.
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Latvian State Research Program IMIS2 PHC OSMOSE 2018 contract \(\hbox {n}^{\circ }\)40033S between France and Latvia
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Viesturs Sints was involved in the conceptualization, investigation, and writing—original draft. Mitradeep Sarkar contributed to the methodology and investigation. Jesse Riedl was involved in the methodology. Gilles Demouchy contributed to the methodology and investigation. Emmanuelle Dubois was involved in the methodology and investigation. Régine Perzynski was involved in the conceptualization, writing—original draft and supervision. Dmitry Zablotsky contributed to the investigation. Gunars Kronkalns contributed to the methodology and resources. Elmars Blums was involved in the conceptualization and supervision.
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Sints, V., Sarkar, M., Riedl, J. et al. Effect of an excess of surfactant on thermophoresis, mass diffusion and viscosity in an oily surfactant-stabilized ferrofluid. Eur. Phys. J. E 45, 43 (2022). https://doi.org/10.1140/epje/s10189-022-00200-7
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DOI: https://doi.org/10.1140/epje/s10189-022-00200-7