Nanochannel confined graphene quantum dots/platinum nanoparticles boosts electrochemiluminescence of luminal-O(2) system for sensitive immunoassay.

Sensitive detection of tumor biomarkers is of great significance for early cancer diagnosis, treatment evaluation, and recurrence monitoring. Development of convenient electrochemiluminescence (ECL) immunosensor using dissolved oxygen (O2) as an endogenous co-reactant of luminol combined with efficient nanocatalysts to boost ECL signal in neutral media is highly desirable. Herein, sensitive detection of tumor biomarker using ECL of luminal-O2 enhanced by confinement of nitrogen-doped graphene quantum dots (N-GQDs) and platinum nanoparticles (PtNPs) on nanochannel array was demonstrated. A high-density nanochannel array-modified electrode was achieved by rapidly growing an amino-functionalized. Vertically-ordered mesoporous silica film (NH2-VMSF) on the inexpensive and readily available indium tin oxide (ITO) electrode. Through simple electrodeposition, N-GQDs were confined and PtNPs were in-situ synthesized in nanochannels of NH2-VMSF. These confined nanocomposites catalyzed the electroreduction of O2 at negative potentials to generate a large amount of reactive oxygen species (ROS) and facilitated luminol oxidation, enhancing the ECL signal of luminol by 25 times. Two immunosensors were fabricated after covalent immobilization of the recognition antibody of carbohydrate antigen 199 (CA199) or carbohydrate antigen 125 (CA125) on the outer surface of the NH2-VMSF and blocking of non-specific sites. When tumor biomarkers bind to the corresponding antibodies on the recognition interface, the formed immunocomplex hindered the diffusion of luminol to the underlying electrode, resulting in a decrease in the ECL signal and sensitive detection of tumor biomarker. The constructed CA199 immunosensor exhibited a linear detection range for CA199 from 0.5 mU mL-1 to 50 U mL-1, with a detection limit (DL) of 0.03 mU mL-1. For CA125 detection, linear detection ranged from 0.5 mU mL-1 to 500 U mL-1, with a DL of 0.005 mU mL-1. The fabricated immunosensors demonstrated good selectivity and high reproducibility. This study provides great potential for the development of efficient luminol ECL systems in neutral media and expands the biological application in sensitive detection of tumor biomarker.

Zhou Y ，Zhang C ，Liu J ，Mou Y ... -  《-》

Sensitive Detection of Biomarker in Gingival Crevicular Fluid Based on Enhanced Electrochemiluminescence by Nanochannel-Confined Co(3)O(4) Nanocatalyst.

Zhu C ，Zhao Y ，Liu J 《Biosensors-Basel》

Enhanced Electrochemiluminescence of Luminol and-Dissolved Oxygen by Nanochannel-Confined Au Nanomaterials for Sensitive Immunoassay of Carcinoembryonic Antigen.

Li W ，Yu R ，Xi F 《MOLECULES》

RuSiNPs@N,S-GQDs as self-enhanced anodic electrochemiluminescent immunobeacons for the highly sensitive quantitation of okadaic acid in shellfish.

A competitive electrochemiluminescence (ECL) immunosensor is proposed to accurately and rapidly assess okadaic acid (OA) levels in shellfish using a novel self-reinforced solid-state ECL marker, which is essential for ensuring seafood safety. Graphene quantum dots doped with nitrogen and sulfur (N,S-GQDs) were synthesized, for the first time, through the electrolysis of graphite in 3-(N-morpholine) propane sulfonic acid solution. Intriguingly, these N,S-GQDs exhibited exceptional co-reactant properties, significantly enhancing the anodic ECL performance of Ru(bpy)32+ in a phosphate-buffered saline solution. Following the functionalization of Ru(bpy)32+-doped silica nanoparticles (RuSiNPs) with poly(diallyldimethylammonium) chloride, we achieved a well-dispersed assembly of N,S-GQDs on the exterior of the RuSiNPs through electrostatic interactions. Importantly, the core-shell structure of RuSiNPs@N,S-GQDs efficiently encapsulated both the luminophore and co-reactant, thus improving the transfer rates of electrons, shorting interaction distances, and reducing energy loss during light emission. Leveraging this "bright" ECL beacon, the ECL immunosensor demonstrated remarkable analytical performance, yielding a low half maximal inhibitory concentration (IC50) of 0.14 ng mL-1, an extensive linear range spanning 0.003-40 ng mL-1, and impressively low limit of detection of 0.001 ng mL-1 for OA determination.

Li S ，Peng J ，Lin X ，Chen J ，Wu Y ，Chen Q ，Chen X ... -  《-》

Point-of-Care Detection of Carcinoembryonic Antigen (CEA) Using a Smartphone-Based, Label-Free Electrochemical Immunosensor with Multilayer CuONPs/CNTs/GO on a Disposable Screen-Printed Electrode.

Khonyoung S ，Mangkronkaew P ，Klayprasert P ，Puangpila C ，Palanisami M ，Arivazhagan M ，Jakmunee J ... -  《Biosensors-Basel》