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Narrow-WindowCathodic Electrochemiluminescence fromLaser-Engineered Graphitic Carbon Nitride: A Next-Generation Emitterfor Microplastics Biosensing
Summary
Scientists developed a new way to detect tiny plastic particles (microplastics) in seawater that is more accurate than current methods. The technique can find extremely small amounts of plastic pollution - as little as 0.2 billionths of a gram per milliliter of water. This matters because microplastics in our oceans can enter the food chain and potentially harm human health, so better detection helps us monitor and address this pollution problem.
The accuracy of anode electrochemiluminescence (ECL)-based microplastic detection in seawater is undermined by ubiquitous reducing agents. These substances quench the signal by both competing for electrons with the emitter and coreactant to limit critical intermediate generation and directly deactivating the excited species via electron transfer, which induces nonradiative decay. In contrast, the cathode ECL system is free from such interference but is susceptible to the hydrogen evolution reaction and subsequent passivation inactivation of the emitter under a broad potential window. In this work, a surface-state-mediated band gap emission cathodic ECL emitter is introduced for the first time, synthesized via a laser irradiation to fabricate nitrogen vacancy-enriched graphitic carbon nitride (g-C3N4). A unique ECL emission mechanism is exhibited within a narrow potential window, where electron-filled holes react with sulfate radicals to release sufficient energy for triggering intrinsic electron transition. A poly(vinyl chloride) (PVC) microplastics sensor using as-purposed g-C3N4 as emitter was developed, achieving accurate quantification within a concentration range of 0.20 ng/mL to 0.20 μg/mL. Satisfactory sensitivity was enabled via rolling circle amplification strategy assisted by the trans-cleavage activity of CRISPR/Cas12a. The study addresses a critical gap in current microplastic detection technologies and offers an original strategy for rationally designing and constructing novel ECL luminophors.