Most known chemiluminescence (CL) reactions exhibit flash-type light emission. Great efforts have been devoted to the development of CL systems that emit light with high intensity and long-lasting time. However, a long-lasting CL system that can last for hundreds of hours is yet-to-be-demonstrated. Here we show firefly-mimicking intensive and long-lasting CL hydrogels consisting of chitosan, CL reagent N-(4-aminobutyl)-N-ethylisoluminol (ABEI) and catalyst Co2+. The light emission is even visible to naked eyes and lasts for over 150 h when the hydrogels are mixed with H2O2. This is attributed to slow-diffusion-controlled heterogeneous catalysis. Co2+ located at the skeleton of the hydrogels as an active site catalyzes the decomposition of slowly diffusing H2O2, followed by the reaction with ABEI to generate intensive and long-lasting CL. This mimics firefly bioluminescence system in terms of intensity, duration time and catalytic characteristic, which is of potential applications in cold light sources, bioassays, biosensors and biological imaging.
Despite much progress in functionalized gold nanomaterial (GNMs), chemiluminescent (CL) functionalized GNMs with high CL efficiency are far from fully developed. In this work, we report a general strategy for the synthesis of gold nanoparticles (GNPs) bifunctionalized by CL reagent and catalyst metal complexes (BF-GNPs) by taking N-(aminobutyl)-N-(ethylisoluminol) (ABEI) as a model of CL reagents. The complexes of 2-[bis[2-[carboxymethyl-[2-oxo-2-(2-sulfanylethylamino)ethyl]amino]ethyl]amino]acetic acid (DTDTPA) with various metal ions, including Co(2+), Cu(2+), Pb(2+), Ni(2+), Hg(2+), Cr(3+), Eu(3+), La(3+), Gd(3+), Sm(3+), Er(3+), Dy(3+), Ce(4+), and Ce(3+), were grafted on the surface of ABEI functionalized GNPs (ABEI-GNPs) to form a series of BF-GNPs. These BF-GNPs exhibited excellent CL activity. In particular, the CL intensity of DTDTPA/Co(2+)-ABEI-GNPs was over 3 orders of magnitude higher than ABEI-GNPs. This work demonstrates for the first time that metal complexes grafted on the surface of GNPs have unique catalytic activity on the CL reaction, superior to that in the liquid phase. Such BF-GNPs may find future applications in bioassays, microchips, and molecular/cellular imaging.
In this work, the eletrochemiluminescence (ECL) behavior of Cu/cysteine complexes and N-(aminobutyl)- N-(ethylisoluminol) (ABEI) functionalized gold nanoparticles combined with chitosan (Cu-Cys-ABEI-GNPs-CS) were studied by cyclic voltammetry and a double-step potential, which exhibited excellent ECL properties without any coreactant. It was found that the ECL intensity of Cu-Cys-ABEI-GNPs-CS could increase at least 1 order of magnitude compared with that of Cu-Cys-ABEI-GNPs. Furthermore, a coreactant-free and label-free ECL immunosensor has been established for the determination of early acute myocardial infarction biomarker copeptin based on luminescent immuno-gold nanoassemblys consisting of Cu-Cys-ABEI-GNPs-CS and immuno-gold nanoparticles prepared by connecting copeptin antibody with trisodium citrate stabilized gold nanoparticles. In the presence of copeptin, an obvious decrease in ECL intensity was observed due to the formation of antibody-antigen immunocomplex, which could be used for the determination of copeptin in the range of 2.0 × 10-1.0 × 10 mol/L with a detection limit of 5.18 × 10 mol/L. The detection limit of the ECL immunosensor is at least 2 orders of magnitude lower than that of sandwich immunoassays based on labeling technology. Also, the ECL immunosensor does not need any coreactant and avoids complicated labeling and purification procedure. It is ultrasensitive, simple, specific, and low-cost. This work reveals that the proposed luminescent immuno-gold nanoassemblies are ideal nanointerfaces for the construction of immunosensors. The proposed strategy may be used for the determination of other antigens if corresponding antibodies are available.
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