In this paper, we
report a novel redox-responsive water-in-oil
Pickering emulsion stabilized by negatively charged silica nanoparticles
in combination with a trace amount of redox switchable fluorescent
molecule ferrocene azine (FcA), in which ferrocene serves as a redox-sensitive
group and anthryl unit serves as a fluorescence emission center. By
alternately adding oxidants and reducing agents at a moderate condition,
the amphiphilicity of silica nanoparticles changes because of the
adsorption of Fc+A and the desorption of FcA on the silica
surface. On the one hand, the stability of emulsions can be transformed
between stable and unstable at ambient temperature via redox trigger
and the regulation process can be cycled at least three times. On
the other hand, the fluorescent intensity of the FcA molecule can
be regulated by redox stimuli; thus, the change in fluorescent behavior
of the emulsion droplets is observed upon redox cycles, which makes
it useful in the fluorescent label of stimuli-responsive Pickering
emulsions. This work provides a deep understanding of the regulation
mechanism of Pickering emulsions upon redox stimuli and opens the
new way for in situ fluorescent label of stimulus-responsive Pickering
emulsions without introducing additional fluorescent molecules.
In this paper, electrical impedance spectroscopy (EIS) was applied to investigate the stability of oil-in-water (O/W) Pickering emulsions prepared with negatively charged silica nanoparticles in combination with a trace amount of redox switchable fluorescent molecules, ferrocene azine (FcA). Electrical impedance values of emulsions obtained at different emulsification speeds were estimated according to the frequency response data with frequencies ranging from 1 MHz to 1 Hz. The equivalent circuit model of toluene-in-water emulsion was established by the resistor (RO/W) and capacitor (CO/W) in parallel connection. Nyquist diagrams for the emulsions prepared by toluene and water were characterized by the formation of one semi-circle. The droplet size distribution is one of the important factors that affect the stability of the emulsion, except for the volume fraction of water and oil, the size of stabilizing particles, etc. The average particle size of the emulsion droplets decreased as the emulsification speed increased, indicating the higher stability of the emulsion. It was found that the fitted impedance value RO/W of the emulsion decreased with decreasing particle size prepared at different emulsification speeds and storage time by performing real-time EIS detection techniques. The results suggested that EIS could be used to characterize the stability of a toluene-in-water emulsion stabilized by FcA modified silica nanoparticles. Moreover, based on the good electrochemical activity of the FcA molecule, the stability of the Pickering emulsion can be modulated by adding oxidant and reductant and detected by EIS in real-time.
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