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Fumonisin B1 (FB1), a highly toxic secondary metabolite produced by Fusarium fungi, poses a significant threat to global food safety; therefore, sensitive, selective, and reliable analytical methods are urgently needed. In this work, we report a novel molecularly imprinted electrochemiluminescence (ECL) sensor for the quantitative determination of FB1. A Co/Zn bimetallic metal-organic framework@polyoxometalate (Co/Zn-MOF@POMs) nanocomposite was synthesized via a one-pot strategy and used to modify a glassy carbon electrode. The incorporated polyoxometalates (POMs) markedly improved the interfacial electron-transfer kinetics of the Co/Zn-MOF scaffold, resulting in substantial amplification of the ECL signal generated by ZnAgInS quantum dots (QDs). Subsequently, a molecularly imprinted polymer (MIP) layer was electropolymerized on the modified electrode using o-phenylenediamine as the functional monomer and 1,2,3-propanetricarboxylic acid as a structural dummy template designed to mimic key topological and functional features of FB1. Upon FB1 rebinding, the exposed amine groups on the captured FB1 molecules underwent a condensation reaction with carboxyl-functionalized ZnAgInS QDs, enabling site-specific immobilization of the luminophores close to the recognition cavities. Under optimized conditions, the sensor exhibited a linear ECL response to FB1 over a concentration range of 6.0 × 10-14 to 1.0 × 10-10 mol L-1 (R2 = 0.9987), with a detection limit of 3.3 × 10-15 mol L-1 (S/N = 3). This approach offers a robust and reproducible platform for trace-level FB1 monitoring in real-world food and agricultural samples.
Sulfadimethoxine (SDM) is a widely used veterinary antibiotic. Its residues in food and the environment may cause bacterial resistance and threaten human health. In this study, a novel electrochemiluminescence (ECL) biosensor with signal amplification was developed for the sensitive detection of SDM. A g-C3N4@Au composite was modified on the electrode surface, generating a strong ECL signal with K2S2O8 as the coreactant. Hairpin DNA terminated with ferrocene carboxylic acid (FcA) was self-assembled onto g-C3N4@Au via thiol-gold bonds, causing Fc to quench the electrochemiluminescence signal of g-C3N4. Upon SDM addition, it specifically bound to the aptamer strand, releasing the DNA Walker. The DNA walker then continuously hybridized with the activator strand S1 and was cleaved by the nicking endonuclease Nt.BsmAI, generating a large number of S1. S1 further activated the trans-cleavage activity of CRISPR/Cas12a, which cleaves the hairpin DNA on the electrode, releasing Fc and recovering the ECL signal. By monitoring the ECL intensity change during the "signal-off" to "signal-on" transition, quantitative detection of SDM was indirectly realized. The detection range for SDM is 1.0 × 10-14 to 1.0 × 10-7 mol L-1, with a detection limit of 7.15 × 10-15 mol L-1. The sensor was successfully applied to the detection of SDM in food and water samples. Benefiting from the catalytic cascade amplification involving multiple enzymes, the developed method demonstrated high ultrahigh sensitivity.
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