Abstract
Hydrophobic magnetic nanoparticles (NPs) consisting of undecanoate-cappedmagnetite (Fe3O4, average diameter ca. 5 nm) are used to control quantized electron transferto surface-confined redox units and metal NPs. A two-phase system consisting of anaqueous electrolyte solution and a toluene phase that includes the suspended undecanoate-capped magnetic NPs is used to control the interfacial properties of the electrode surface.The attracted magnetic NPs form a hydrophobic layer on the electrode surface resulting inthe change of the mechanisms of the surface-confined electrochemical processes. Aquinone-monolayer modified Au electrode demonstrates an aqueous-type of theelectrochemical process (2e- 2H+ redox mechanism) for the quinone units in the absence ofthe hydrophobic magnetic NPs, while the attraction of the magnetic NPs to the surfaceresults in the stepwise single-electron transfer mechanism characteristic of a dry non-aqueous medium. Also, the attraction of the hydrophobic magnetic NPs to the Au electrodesurface modified with Au NPs (ca. 1.4 nm) yields a microenvironment with a low dielectricconstant that results in the single-electron quantum charging of the Au NPs.
Highlights
Functionalized nanoparticles (NPs) can be associated with modified electrode surfaces and used to enhance electrochemical, photoelectrochemical or bioelectrochemical processes [1,2]
In the present study we report on the effect of hydrophobic magnetic NPs attracted to the electrode, by means of an external magnet, on the mechanisms of electrochemical processes at monolayerfunctionalized electrodes, namely on the quantized electron transfer to surface-confined quinone units and Au NPs
The present study has described a new method to control the mechanism of electrochemical reactions on modified electrode surfaces, namely to achieve quantized single-electron charging processes for molecular redox species and metal NPs
Summary
Functionalized nanoparticles (NPs) can be associated with modified electrode surfaces and used to enhance electrochemical, photoelectrochemical or bioelectrochemical processes [1,2]. In the present study we report on the effect of hydrophobic magnetic NPs attracted to the electrode, by means of an external magnet, on the mechanisms of electrochemical processes at monolayerfunctionalized electrodes, namely on the quantized electron transfer to surface-confined quinone units and Au NPs. Chemicals and materials
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