4.7 Article

Surface motifs regulated aggregation induced emission in AuAg nanoclusters combined with Ce(III)/Ce(IV) catalytic cyclic amplification strategy for sensitive bioanalysis

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SENSORS AND ACTUATORS B-CHEMICAL
卷 400, 期 -, 页码 -

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ELSEVIER SCIENCE SA
DOI: 10.1016/j.snb.2023.134911

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AuAg NCs; Mixed valence Ce-MOF; Electrochemiluminescence; Biosensor; Aggregation induced emission

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By regulating the surface motifs of metal nano-clusters (MNCs) based on aggregation-induced emission (AIE) strategy, a highly efficient luminescent probe AuAg NCs was designed. The introduction of Ag(I) resulted in denser surface patterns, reducing the non-radiative energy dissipation. Additionally, the spontaneous catalytic cycle amplification strategy improved the electrochemiluminescence (ECL) efficiency of AuAg NCs. The biosensor showed a wide linear relationship range and low detection limit using cardiac troponin I as a model.
Achieving high luminescence intensity in electrochemiluminescence biosensors is a challenge for metal nano-clusters (MNCs) due to their non-radiative relaxation-mediated self-quenching tendency. Here, the surface motifs [M(I)-SR] of MNCs were regulated based on aggregation-induced emission (AIE) strategy was proposed to mitigate non-radiative relaxation vibrations, and an efficient luminescent AuAg NCs was designed via host-guest assembly as a signal probe. The Au(I)-SR of AuAg NCs used glutathione (GSH) as a template and reducing agent, and the introduction of Ag(I) made the Au(I)-SR of AuAg NCs cross-linked and interlocked, resulting in AuAg NCs with denser surface patterns. The aggregation of surface motifs limited the ligand movement to reduce the non-radiative energy dissipation. Furthermore, the spontaneous catalytic cycle amplification strategy of Ce(III)/Ce (IV) redox pairs in the matrix material of Ce-MOF promoted the reaction of more co-reactants triethylamine (TEA), obtaining potent reducing radicals TEA* for further improving the ECL efficiency of AuAg NCs. Using cardiac troponin I (cTnI) as the analytical model, the biosensor exhibited a wide linear relationship range (50 fg & sdot;mL-1 -500 ng & sdot;mL-1) and a low detection limit (4.77 fg & sdot;mL-1). The breakthrough in surface motifs regulation of MNCs guides a new way to design high luminiferous MNCs, and further expands the application potential of MNCs.

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