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DC Versus AC Electrokinetic-Driven Strategy Coupled with a Miniaturized Electrochemical-SERS Hydrogel Chip toward Dynamic Monitoring of Microplastics
Summary
DC versus AC electrokinetic strategies coupled with microfluidic devices were compared for separating and concentrating microplastics from water samples. The study advances electrokinetic methods as efficient tools for microplastic extraction and preconcentration ahead of analysis.
Electrokinetic-driven surface-enhanced Raman scattering (ED-SERS) integrates the ultrasensitive fingerprint spectral identification capability of SERS with flexible electric field-driven molecular interfacial control, enabling it an emerging advanced analytical technique. However, previous studies of ED-SERS primarily relied on direct current (DC) operation, limiting the mechanistic understanding of the strategy. In this study, we introduce a miniaturized electrochemical-SERS sensing chip functionalized with poly(vinyl alcohol oxide)-gold nanoparticle hydrogel (PVA-AuNPs/SPE) for dynamic SERS monitoring of typical charged microplastics under both DC and alternating current (AC) modulation. We confirm that PVA-AuNPs/SPE achieves charge-selective molecular attraction/exclusion and nanoconfined capture under electric field control. Density functional theory (DFT) simulations are performed to investigate the potential molecular mechanism underlying ED-SERS. Furthermore, in situ dynamic ED-SERS monitoring of microplastics is realized through DC/AC voltage application in both simulated and river water samples. Our results show that the DC mode is particularly suitable for trace-level contaminant detection, while AC modulation can provide in-depth insights into the dynamics of molecular migration and the adsorption process. This research seeks to establish a novel AC-modulated ED-SERS strategy as a versatile platform for both high-performance monitoring of emerging contaminants and new perspectives for decoding electrokinetically driven molecular interactions with interfacial environments.
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