RESUMEN
Efficient and robust electrochemiluminescence (ECL) emitters are crucial for enhancing the ECL immunosensor sensitivity. This study introduces a novel ECL emitter, CoBIM/Cys, featuring a hierarchical core-shell structure. The core of the structure is created through the swift coordination between the sulfhydryl and carboxyl groups of l-cysteine (l-Cys) and cobalt ions (Co2+), while the shell is constructed by sequentially coordinating benzimidazole (BIM) with Co2+. This design yields a greater specific surface area and a more intricate porous structure compared to CoBIM, markedly enhancing mass transfer and luminophore accessibility. Moreover, the l-Cys and Co2+ core introduces Co-S and Co-O catalytic sites, which improve the catalytic decomposition of H2O2, leading to an increased production of hydroperoxyl radicals (OOHâ¢). This mechanism substantially amplifies the ECL performance. Leveraging the competitive interaction between isoluminol and BIM for OOH⢠during ECL emission, we developed a ratiometric immunosensor for cardiac troponin I (cTnI) detection. This immunosensor demonstrates a remarkably broad detection range (1 pg mL-1 to 10 ng mL-1), a low detection limit (0.4 pg mL-1), and exceptional reproducibility and specificity.
Asunto(s)
Bencimidazoles , Cisteína , Técnicas Electroquímicas , Mediciones Luminiscentes , Troponina I , Bencimidazoles/química , Cisteína/análisis , Cisteína/química , Mediciones Luminiscentes/métodos , Técnicas Electroquímicas/métodos , Inmunoensayo/métodos , Troponina I/análisis , Troponina I/sangre , Humanos , Límite de Detección , Técnicas Biosensibles/métodos , Cobalto/química , Peróxido de Hidrógeno/químicaRESUMEN
Precise tuning the structure of catalytic center is of great importance for the construction of enhanced electrochemiluminescence (ECL) emitters and the development of ECL amplification strategies, which is a key factor in improving the sensitivity of biosensors. In this work, we report the enhanced ECL emitters based on the porphyrin-based paddlewheel framework (PPF) with axial coordinated imidazole-like ligands (PPF/X, X = 2-methylimidazole (MeIm), imidazole (Im), benzimidazole (BIM)). In this system, the electron-donating ability of the axial ligands is positively correlated to its coordination ability to the paddlewheel units and the catalytic ability of the axially coordinated paddlewheel units. In addition, the electrochemical and ECL behavior of PPF/X (X = MeIm, Im, BIM) with different axial coordinated ligands are explored.
RESUMEN
Selective and sensitive detection of nitrite has important medical and biological implications. In the present work, to obtain an enhanced electrochemiluminescence (ECL) determination of nitrite, a novel nano-ECL emitter CoBIM/cetyltrimethylammonium bromide (CTAB) was prepared via a micelle-assisted, energy-saving, and ecofriendly method based on benzimidazole (BIM) and CTAB. Unlike conventional micelle assistance, the deprotonated BIM (BIM-) preferential placement was in the palisade layer of cationic CTAB-based micelles. Enriching the original CTAB micelle with BIM- disrupted its stability and resulted in the formation of considerably smaller BIM/CTAB-based micelles, providing a confined coordination environment for BIM- and Co2+. As a result, the growth of CoBIM/CTAB was also limited. Owing to the unusual nitration reaction between BIM and nitrite, the prepared CoBIM/CTAB was successfully applied as a novel ECL probe for the detection of nitrite with a wide linear range of 1-1500 µM and a low detection limit of 0.67 µM. This work also provides a promising ECL platform for ultrasensitive monitoring of nitrite and it was applied with sausages and pickled vegetables.
Asunto(s)
Compuestos de Cetrimonio , Nitritos , Cetrimonio , Micelas , BencimidazolesRESUMEN
Exploring the depolymerization strategy of liposoluble luminophores in the aqueous phase is vital for the development of electrochemiluminescence (ECL). In this work, tetraoctylammonium bromide (TOAB) with four long hydrophobic chains and short hydrophilic ends is used as a template to limit the aggregation of benzimidazole (BIM). By adjusting the loading of BIM on the hydrophobic chains of TOAB, a two-dimensional lamellar BIM/TOAB is formed, the ECL intensity of which is 6.4 times higher than that of the aggregated BIM (H2O2 as the coreactant). In terms of ECL spectroscopies, cyclic voltammetry , ECL transients, and the adjustment of the scanning potential range, the ECL mechanism is thoroughly studied. This work provides a new way to depolymerize organic luminophores and reveals a possible pathway in the annihilation ECL mechanism.
RESUMEN
Metal-organic frameworks (MOFs) act as versatile coordinators for the subsequent synthesis of high-performance catalysts by providing dispersed metal-ion distribution, initial coordination condition, dopant atom ratios, and so on. In this work, a crystalline MOF trans-[Cu(NO3)2(Him)4] was synthesized as the novel precursor of a redox-alternating CuxO electrochemical catalyst. Through simple temperature modulation, the gradual transformation toward a highly active nanocomposite was characterized to ascertain the signal enhancing mechanism in H2O2 reduction. Owing to the proprietary structure of the transducer material and its ensuing high activity, a proof-of-principle sensor was able to provide an amplified sensitivity of 2330 µA mM-1 cm-2. The facile one-pot preparation and intrinsic nonenzymatic nature also suggests its wide potentials in medical settings.
Asunto(s)
Estructuras Metalorgánicas , Nanocompuestos , Catálisis , Peróxido de Hidrógeno , TransductoresRESUMEN
The Atlantic sea nettle ( Chrysaora quinquecirrha) has an important evolutionary position due to its high ecological value. However, due to limited sequencing technologies and complex jellyfish genomic sequences, the current C. quinquecirrha genome assembly is highly fragmented. Here, we used the most advanced high-throughput chromosome conformation capture (Hi-C) technology to obtain high-coverage sequencing data of the C. quinquecirrha genome. We then anchored these data to the previously published contig-level assembly to improve the genome. Finally, a high-continuity genome sequence of C. quinquecirrha was successfully assembled, which contained 1 882 scaffolds with a N50 length of 3.83 Mb. The N50 length of the genome assembly was 5.23 times longer than the previously released one, and additional analysis revealed that it had a high degree of genomic continuity and accuracy. Acquisition of the high-continuity genome sequence of C. quinquecirrha not only provides a basis for the study of jellyfish evolution through comparative genomics but also provides an important resource for studies on jellyfish growth and development.
Asunto(s)
Genoma , Escifozoos/genética , Animales , Evolución Biológica , Análisis de Secuencia de ADN/métodosRESUMEN
A series of new hybrids of dehydroandrographolide (TAD), a biologically active natural product, bearing nitric oxide (NO)-releasing moieties were synthesized and designated as NO-donor dehydroandrographolide. The biological activities of target compounds were studied in human erythroleukemia K562 cells and breast cancer MCF-7 cells. Biological evaluation indicated that the most active compound I-5 produced high levels of NO and inhibited the proliferation of K562 (IC50 1.55 µmol·L-1) and MCF-7 (IC50 2.91 µmol·L-1) cells, which were more potent than the lead compound TAD and attenuated by an NO scavenger. In conclusion, I-5 is a novel hybrid with potent antitumor activity and may become a promising candidate for future intensive study.