Surface functionalized AuNCs optical biosensor as an emerging food safety indicator: Fundamental mechanism to future prospects

Electrochemiluminescence nanoemitters for immunoassay of protein biomarkers.

Screening high-performance anodic electrochemiluminescence (ECL) systems with low triggering potential is a promising way to broaden their applications. In addition to electrochemiluminophore, co-reactant also plays an important role in the ECL process, since the oxidation of co-reactants is one of the most important steps in the anodic ECL process. Herein, a novel co-reactant-mediated high-performance low-potential Au nanocluster (AuNC)-based ECL system has been successfully developed. Benefiting from the isopropyl substitution and hydroxyl addition to the triethylamine (TEA), the BSA-AuNC/2-(diisopropylamino)ethanol (DIPEA-OH) ECL system achieved higher energy efficiency at a lower potential of 0.75 V. In addition, compared with the BSA-AuNC/TEA system, the ECL intensity and quantum yield (ΦECL) with DIPEA-OH as a co-reactant increased 22.34-fold and 13-fold (as high as 68.17%), respectively. Based on the low potential, high ΦECL of the AuNC/DIPEA-OH ECL system, a sandwich-type immunosensor has been constructed for a highly selective SARS-CoV-2 N protein assay. In the absence of any complex signal amplification strategies, the ECL immunosensor for the SARS-CoV-2 N protein detection showed a linear range of 0.001-100 ng/mL and a detection limit of 0.35 pg/mL. Moreover, the ECL platform had good reproducibility and stability and exhibited acceptable detection performance in the detection of actual serum samples. This work established a framework for in-depth design and study of anode ECL co-reactants for AuNCs and other luminophores, and expanded the potential application of ECL sensors in the clinical diagnosis of COVID-19.

Co-Reactant-Mediated Low-Potential Anodic Electrochemiluminescence Platform and Its Immunosensing Application.

Electrochemiluminescence (ECL) is a powerful electroanalytical transduction technique in biosensing and clinic immunodiagnostics, however its practical applications for point-of-care testing (POCT) are rather limited because of the requirements of large sized electrochemical workstation for electrical stimulation and photomultiplier tube for light detection. Herein we report a fully integrated and handheld ECL device consisting of a flexible printed circuit board based electrochemical module, a silicon photomultiplier and a Bluetooth enabled smartphone with an Android application interface. The device together with an electrochemical cell and light-tight box has a dimension of 17 cm × 9 cm × 9 cm, thus being suitable for on-site detection and POCT. To demonstrate the performance and efficiency of this device, we implemented the detection of dopamine (DA), using the indium tin oxide glass electrode coated with antifouling silica nanoporous membrane as the working electrode for improving the sensing stability and sensitivity. A fast response to DA with a wide linear range of 5 nM ∼ 20 μM and an ultralow detection limit of 3.5 nM were obtained with the handheld ECL device. These attractive features allow the device to satisfy the basic requirements for POCT of DA in complex bio-samples, including urine and rat brain homogenate. This work provides a novel strategy for ECL based POCT, showing the potential of broad utility in resource-limited settings where there is a lack of medical facilities. 

A fully integrated and handheld electrochemiluminescence device for detection of dopamine in bio-samples

Exploration of a novel and efficient sensing mechanism of Au nanocluster (AuNC)-based electrochemiluminescence (ECL) sensors is still a great challenge and opportunity for further applications. Herein, we proposed that the electron transfer (ET) could be used as a novel sensing regulation factor for the construction of an ECL-sensing platform based on the AuNC probe. As a proof-of-concept, the ECL quenching effect and mechanism of Cu2+ on pre-oxidation-treated l-methionine-capped AuNCs (OM-AuNCs) was investigated in detail. The results revealed that after the electrochemical excitation of the AuNC probe, the electron is transferred from the highest occupied molecular orbital (HOMO) of Met-Cu2+ to that of the OM-AuNCs, along with the ET from lowest-unoccupied molecular orbital (LUMO) of the OM-AuNCs back to the HOMO of Met-Cu2+, leading to the ECL quenching of OM-AuNCs. Since the ECL intensity of OM-AuNCs is sensitively affected by the ET process, a preferable linear dependence was obtained in the concentration range from 1.0 × 10-18 to 1.0 × 10-14 M with high selectivity. More importantly, a record low detection limit (LOD, 2.3 × 10-20 M) at the single copper ion level has been realized without any other amplification technique. Furthermore, the actual sample detection for Cu2+ exhibited satisfactory results. Therefore, this study enriches an ET-mediated ECL application and promotes a more rational design of ECL sensors.

Gold Nanocluster Probe-Based Electron-Transfer-Mediated Electrochemiluminescence Sensing Strategy for an Ultrasensitive Copper Ion Detection.

Biomolecule-functionalized Au nanoclusters (AuNCs) have drawn great interest in the electrochemiluminescence (ECL) field due to their unique optical/electrical properties, biocompatibility, and versatile bioapplication potentials. Herein, we proposed a two-in-one ECL probe of immunoglobulin G-encapsulated AuNCs (IgG-AuNCs) for the development of a high-performance ECL immunoassay (ECLIA) platform. The IgG-AuNCs were not only used as an ECL probe due to their excellent anodic ECL performance with triethylamine (TEA) as a coreactant but also used as the biorecognition element because of their well-retained bioactivity of the IgG. As a proof of concept, a new type of competitive immunosensing platform has been applied to detect IgG representing several merits of facile preparation, rapid detection, sample saving, and good analytical performance. The sensing platform exhibited a linear range of 0.5-50,000 ng/mL with a limit of detection of 0.06 ng/mL for IgG detection with high selectivity. In addition, this convenient ECLIA platform also performed well in real serum sample detection. Notably, our work not only proved the "two-in-one" immuno-AuNC probe-based ECLIA strategy but also developed a rational framework for study of ECL bioassay platforms based on multifunctional AuNCs and other related nanomaterials.

Electrochemiluminescence Immunoassay Platform with Immunoglobulin G-Encapsulated Gold Nanoclusters as a "Two-In-One" Probe.

Monitoring nicotine concentrations in human fluids is extremely crucial owing to the harmful effect of nicotine on human health. Herein, it is shown that nicotine could quench the cathodic electroc...

Mechanistic Insight into a Novel Ultrasensitive Nicotine Assay Base on High-Efficiency Quenching of Gold Nanocluster Cathodic Electrochemiluminescence.

6-Aza-2-thio-thymine-gold nanoclusters: an excellent candidate in the photoelectrochemical field.

Herein, we have developed a method for the facile aqueous synthesis of ligand-free cesium lead halide perovskite nanoplatelets with pure CsPb2Br5. The ligand-free CsPb2Br5 nanoplatelets showed good environmental stability, green...

Photoelectrochemical performance of ligand-free CsPb2Br5 perovskite

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Electrochemiluminescence Immunoassay Platform with Immunoglobulin G-Encapsulated Gold Nanoclusters as a "Two-In-One" Probe.

Mechanistic Insight into a Novel Ultrasensitive Nicotine Assay Base on High-Efficiency Quenching of Gold Nanocluster Cathodic Electrochemiluminescence.

6-Aza-2-thio-thymine-gold nanoclusters: an excellent candidate in the photoelectrochemical field.

Photoelectrochemical performance of ligand-free CsPb2Br5 perovskite