ScholarWorks@성균관대학교

초록

In this research, a creative strategy utilizing electrochemiluminescence resonance energy transfer (ECL-RET) has been presented, which is enabled by a newly introduced donor-acceptor pair. The donor of self-enhanced Cu:Zn-MOF@Ru was proposed through modifying the Ru(bpy)32+ on Cu2+-incorporated Zn-based metal-organic framework (Cu:Zn-MOF). The acceptor of Pd/Ni-CoNCs was the Ni-Co nanocages (NCs) derived from Prussian blue analogs that could accommodate substantial amounts of Pd nanoparticles (NPs). An ultrasensitive detection of neuron-specific enolase (NSE) has been obtained via the construction of this quenched ECL immunosensor. Cu:Zn-MOF, a distinctive three-dimensional (3D) bulk construction framework, has distinguished the strategy of confining electrochemically active Cu nanoparticles within the channels of Zn-MOF, which could not only effectively maintain metal atom discreteness and promote electron density, but also weaken the chemisorption energy of specific intermediates, thereby, accelerating the generation of activated species and facilitating the catalytic behavior. Furthermore, the Cu:Zn-MOF has been simultaneously applied as an excellent encapsulation agent and effective coreactant accelerator, which facilitates the modification of Ru(bpy)32+ and production of radicals. Therefore, a self-enhanced Cu:Zn-MOF@Ru emitter was subsequently constructed to shorten the distance between reactive participants and minimize energy loss, and thus achieving a significantly higher ECL efficiency. More significantly, the partial overlap between ultraviolet-visible (UV–vis) absorption of Pd/Ni-CoNCs and the ECL spectrum of Cu:Zn-MOF@Ru has facilitated efficient ECL-RET interaction. Consequently, a “signal-off”-type ECL immunosensor was developed for the analysis of NSE, achieving a broad linear range from 1 fg/mL to 20 ng/mL and an exceptionally low detection limit of 0.33 fg/mL.

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