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In recent years, microplastics have been found in seawater, soil, food, and even human blood and tissues. The ubiquity of microplastics is alarming, but the health and environmental impacts of microplastics are just beginning to be understood. Accordingly, sampling, separating, and quantifying exposure to microplastics to devise a total risk assessment is the focus of ongoing research. Unfortunately, traditional separation methods ( i.e. , size- and density-based methods) unintentionally exclude the smallest microplastics (<10 μm). Limited data about the smallest microplastics is problematic because they are likely the most pervasive and have distinct properties from their larger plastic counterparts. To that end, in this Perspective, we discuss using electrokinetic methods for separating the smallest microplastics. Specifically, we describe three methods for forming electric field gradients, discuss key results within the field for continuously separating microplastics, and lastly discuss research avenues which we deem critical for advancing electrokinetic separation platforms for targeting the smallest microplastics., Competing Interests: The authors state that there are no conflicts of interest., (This journal is © The Royal Society of Chemistry.)

A key goal of nanoparticle-based catalysis research is to correlate the structure of nanoparticles (NPs) to their catalytic function. The most common approach for achieving this goal is to synthesize ensembles of NPs, characterize the ensemble, and then evaluate its catalytic properties. This approach is effective, but it excludes the certainty of structural heterogeneity in the NP ensemble. One means of addressing this shortcoming is to carry out analyses on individual NPs. This approach makes it possible to establish direct correlations between structures of single NPs and, in the case reported here, their electrocatalytic properties. Accordingly, we report on enhanced electrocatalytic formic acid oxidation (FAO) activity using individual Cu-modified, high-indexed Pt NPs. The results show that the Cu-modified Pt NPs exhibit significantly higher currents for FAO than the Pt-only analogs. The increased activity is enabled by the Cu submonolayer on the highly stepped Pt surface, which enhances the direct FAO pathway but not the indirect pathway which proceeds via surface-absorbed CO*., Competing Interests: The authors declare no competing interests., (This journal is © The Royal Society of Chemistry.)

Here we use experiments and finite element simulations to investigate the electrokinetics within straight microchannels that contain a bipolar electrode and an unbuffered electrolyte solution. Our findings indicate that in the presence of a sufficiently high electric field, water electrolysis proceeds at the bipolar electrode and leads to variations in both solution conductivity and ionic current density along the length of the microchannel. The significance of this finding is twofold. First, the results indicate that both solution conductivity and ionic current density variations significantly contribute to yield sharp electric field gradients near the bipolar electrode poles. The key point is that ionic current density variations constitute a fundamentally new mechanism for forming electric field gradients in solution. Second, we show that the electric field gradients that form near the bipolar electrode poles in unbuffered solution are useful for continuously separating microplastics from water in a bifurcated microchannel. This result expands the potential scope of membrane-free separations using bipolar electrodes., Competing Interests: The authors declare no conflict of interest., (This journal is © The Royal Society of Chemistry.)

In this article, we report continuous sorting of two microplastics in a trifurcated microfluidic channel using a new method called serial faradaic ion concentration polarization (fICP). fICP is an electrochemical method for forming ion depletion zones and their corresponding locally elevated electric fields in microchannels. By tuning the interplay between the forces of electromigration and convection during a fICP experiment, it is possible to control the flow of charged objects in microfluidic channels. The key findings of this report are threefold. First, fICP at two bipolar electrodes, configured in series and operated with a single power supply, yields two electric field gradients within a single microfluidic channel ( i.e. , serial fICP). Second, complex flow variations that adversely impact separations during fICP can be mitigated by minimizing convection by electroosmotic flow in favor of pressure-driven flow. Finally, serial fICP within a trifurcated microchannel is able to continuously and quantitatively focus, sort, and separate microplastics. These findings demonstrate that multiple local electric field gradients can be generated within a single microfluidic channel by simply placing metal wires at strategic locations. This approach opens a vast range of new possibilities for implementing membrane-free separations., (This journal is © The Royal Society of Chemistry 2020.)

We report a new and general approach that will be useful for adapting the method of electrocatalytic amplification (ECA) to biosensing applications. In ECA, individual collisions of catalytic nanoparticles with a noncatalytic electrode surface lead to bursts of current. In the work described here, the current arises from catalytic electrooxidation of N 2 H 4 at the surface of platinum nanoparticles (PtNPs). The problem with using ECA for biosensing applications heretofore, is that it is necessary to immobilize a receptor, such as DNA (as in the case here) or an antibody on the PtNP surface. This inactivates the colliding NP, however, and leads to very small collision signatures. In the present article, we show that single-stranded DNA (ssDNA) present on the PtNP surface can be detected by selectively removing a fraction of the ssDNA using the enzyme Exonuclease I (Exo I). About half of the current associated with collisions of naked PtNPs can be recovered from fully passivated PtNPs after exposure to Exo I. Experiments carried out using both Au and Hg ultramicroelectrodes reveal some mechanistic aspects of the collision process before and after treatment of the ssDNA-modified PtNPs with Exo I.

Here, we report on the electrochemical detection of individual collisions between a conjugate consisting of silver nanoparticles (AgNPs) linked to conductive magnetic microbeads (cMμBs) via DNA hybridization and a magnetized electrode. The important result is that the presence of the magnetic field increases the flux of the conjugate to the electrode surface, and this in turn increases the collision frequency and improves the limit of detection (20 aM). In addition, the magnitude of the charge associated with the collisions is greatly enhanced in the presence of the magnetic field. The integration of DNA into the detection protocol potentially provides a means for using electrochemical collisions for applications in biological and chemical sensing.