Ligand-protected gold nanoclusters
(Au NCs) are promising electrochemiluminescence
(ECL) emitters because of their striking optical properties and excellent
biocompatibility, but free vibration and rotation of their ligand
result in low ECL efficiency, dramatically limiting their applications.
Herein, using the ligand of Au NCs as one of the building units, a
Au NC-based metal–organic framework (Au NC-based MOF) was constructed
by the coordination-assisted self-assembly strategy, which not only
impedes the ligand rotation-induced energy dissipation but also diminishes
the self-quenching effect due to the spatial distribution of Au NCs.
As a proof of concept, the prepared GSH-Au NCs@ZIF-8 gives rise to
a 10-fold enhanced anodic ECL efficiency compared to that of densely
aggregated GSH-Au NCs with triethylamine as the coreactant. Based
on high ECL efficiency of GSH-Au NCs@ZIF-8, a “signal off”
sensing platform was proposed with rutin as a model analyte, achieving
a low detection limit of 10 nM. Therefore, the strategy paves an effective
and alternative methodology to enhance ECL efficiency of metal NCs,
considerably broadening their potential applications in sensing analysis,
clinical diagnosis, and light-emitting devices.
Metal nanoclusters (NCs) have attracted extensive interest in electrochemiluminescence (ECL) field, but it is still a significant challenge to prepare high ECL efficiency NCs, which tremendously precludes their application in sensing and imaging. Herein, we report poly(3,4-ethylenedioxythiophene) (PEDOT) as a functional ligand for NCs with a "kill three birds with one stone" role, acting as a stabilizer like existing templates, excitingly, excellent electrical conductivity to accelerate the injection of interfacial electrons, and outstanding electrocatalytic activity toward coreactants (S 2 O 8 2− ), which breaks the convention that traditional ligands act as a double-edged sword in ECL field. As an illustration, PEDOT-hosted Ag NCs were prepared with an unprecedented ECL intensity with S 2 O 8 2− as a cathodic coreactant, which indicates that this novel ligand strategy will bring exciting opportunities, not only in opening up new horizons for rational development of high ECL efficiency metal NCs but also in advancing their potential applications in light-emitting devices and clinical biosensing. As a proof of concept, the PEDOT-hosted Ag NCs were applied as neoteric ECL emitters to achieve sensitive detection of dopamine (DA), which showcased a wide linear response from 1 nM to 10 mM and a low detection limit of 0.17 nM.
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