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Silica-detoxified perovskite ECL: Cas13a-triggered signal-on sensing with CsPbBr₃@SiO₂@Au
Kangqi Xie1, Haozhen Ren2, Dingpeng Ban1
1Guangxi Key Laboratory for Preclinical and Translational Research on Bone and Joint Degenerative Diseases, Affiliated Hospital of Youjiang Medical University for Nationalities, Baise, Guangxi 533000, China.
Abstract:
Perovskite nanocrystals are attractive ECL emitters but suffer from poor water stability and potential toxicity. Here we report a signal-on electrochemiluminescent biosensor that integrates CsPbBr₃@SiO₂@Au nanocomposites with a CRISPR/Cas13a-Nb.BbvCI amplification cascade for ultrasensitive microRNA detection. The CsPbBr₃ core provides bright emission, a conformal SiO₂ shell enhances water compatibility and suppresses ion leakage, and surface Au nanoparticles offer abundant sites for thiolated ferrocene-hairpin (Fc-HP) immobilization. In the resting state, proximal Fc efficiently quenches the CsPbBr₃ ECL. Target miRNA activates Cas13a to cleave a dumbbell probe and release an intermediate strand that hybridizes with Fc-HP; subsequent Nb.BbvCI nicking removes Fc from the electrode and is recycled, producing robust signal restoration. Morphology (TEM), composition (EDS/XPS), and stepwise electrochemistry (CV/EIS) verify a core-shell-Au architecture and a reliably assembled interface that follows the expected quench→restore behavior. Under optimized conditions (0.5 mg mL-1 CsPbBr₃@SiO₂@Au, 2.0 μM Fc-HP, 40 min target incubation, 100 mM TPrA, 120 s pre-reaction), the assay affords a 1 aM-1.0 × 109 aM linear range with an estimated limit of detection (LOD) of 1.86 aM. The sensor shows high specificity against homologous sequences and achieves 95.22%-104.61% recoveries with RSD < 5% in spiked serum. Pilot measurements distinguish patient serum samples from healthy controls, underscoring clinical potential. This modular platform couples stable perovskite ECL emission with programmable CRISPR chemistry, offering a sensitive, selective, and water-compatible route for microRNA analysis and readily extensible nucleic-acid diagnostics.
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