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Published on: February 10, 2014
Interface-regulated MOF/g-C3N4 heterostructure for electrode passivation elimination: Ultrasensitive
Xue Dong1, Qingze Zeng2, Jiangle Yi2
1Key Laboratory of Interfacial Reaction & Sensing Analysis in Universities of Shandong, School of Chemistry and Chemical Engineering, Collaborative Innovation Center for Green Chemical Manufacturing and Accurate Detection, University of Jinan, Jinan, 250022, PR China; Institute for Smart Materials & Engineering, University of Jinan, Jinan, 250022, PR China.
Abstract:
The development of stable and efficient luminophores remains a critical challenge in electrochemiluminescence (ECL) sensing. Graphitic carbon nitride (g-C3N4) has emerged as a promising luminophore due to its high stability and low toxicity, yet its practical application is constrained by limited surface area, poor conductivity, and severe electrode passivation. Herein, a metal-organic framework (MOF)/g-C3N4 (NH2-UiO-66/g-C3N4, NUCN) heterostructure luminophore was constructed via interface engineering. The integration of NH2-UiO-66 (NU) remarkably enhanced electrical conductivity, surface area and ECL efficiency of g-C3N4. Mechanistically, the low LUMO level of NU enabled efficient electron capture from the conduction band of g-C3N4, which eradicated electrode passivation and directly contributed to the 4.6 % enhancement in ECL efficiency. Concurrently, the NUCN heterostructure featured increased Brunauer-Emmett-Teller (BET) surface area and abundant amino groups, collectively enhancing its antibody loading capacity for biomolecular recognition. This dual improvement-electron transfer optimization for ECL performance and structural modification for biomolecule immobilization-collectively enabled the ultrasensitive sensing capability of the NUCN-based platform. In addition, the absorption spectrum of PANI-sCuO quencher exhibited strong overlap with the ECL emission of NUCN at 452 nm, enabling ECL resonance energy transfer (ECL-RET)-mediated signal quenching. This allowed target-induced quenching to generate pronounced ECL intensity variation, thereby achieving ultrasensitive detection via signal amplification. Leveraging the NUCN/PANI-sCuO system, a sandwich-type immunosensor was developed for carbohydrate antigen 15-3 (CA15-3), featuring a linear range of 0.05-600 U/mL and a detection limit of 0.02 U/mL, demonstrating its potential for clinical biomarker analysis.
