Regulating Reactive Oxygen Species over M–N–C Single-Atom Catalysts for Potential-Resolved Electrochemiluminescence

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(17), С. 12197 - 12205

Опубликована: Апрель 17, 2024

The development of potential-resolved electrochemiluminescence (ECL) systems with dual emitting signals holds great promise for accurate and reliable determination in complex samples. However, the practical application such is hindered by inevitable mutual interaction mismatch between different luminophores or coreactants. In this work, first time, precisely tuning oxygen reduction performance M–N–C single-atom catalysts (SACs), we present a luminol ECL system employing endogenous dissolved O2 as coreactant. Using advanced situ monitoring theoretical calculations, elucidate intricate mechanism involving selective efficient activation through central metal species modulation. This modulation leads to controlled generation hydroxyl radical (·OH) superoxide (O2·–), which subsequently trigger cathodic anodic emission, respectively. well-designed Cu–N–C SACs, their moderate oxophilicity, enable simultaneous ·OH O2·–, thereby facilitating ECL. As proof concept, employed principal component analysis statistical method differentiate antibiotics based on output dual-potential signals. work establishes new avenue constructing platform single luminophore coreactant precise regulation active intermediates.

Язык: Английский

---

Multi‐Mode/Signal Biosensors: Electrochemical Integrated Sensing Techniques

Advanced Functional Materials, Год журнала: 2024, Номер unknown

Опубликована: Май 14, 2024

Abstract Electrochemical (EC) analysis has emerged as a high‐sensitivity, reliable, cost‐effective, and rapidly evolving technique that garnered significant attention across diverse domains. Furthermore, EC‐based techniques hold great potential for miniaturization integration. The integration of EC with mode/signal (such light, magnetic, thermal signals, etc.) provides unique opportunities biosensors to acquire more information through single sensing platform. By coupling multiple signals or processing them logically, the detection accuracy can be further improved, probability false positives negatives minimized. In this review, thorough multi‐ sensors in field is conducted, along their various (e.g., fluorescence, photothermal, colorimetry, microfluidic, etc.). aim delve into latest advances, applications, well challenges multi‐mode/signal biosensors, where utilization modalities helps enhance accuracy, sensitivity, selectivity. This review new insight synergistic effects integrating other techniques, aiming shed light on near‐future developments EC‐integrated biosensors.

Язык: Английский

---

Timescale correlation of shallow trap states increases electrochemiluminescence efficiency in carbon nitrides

Nature Communications, Год журнала: 2024, Номер 15(1)

Опубликована: Апрель 27, 2024

Abstract Highly efficient interconversion of different types energy plays a crucial role in both science and technology. Among them, electrochemiluminescence, an emission light excited by electrochemical reactions, has drawn attention as powerful tool for bioassays. Nonetheless, the large differences timescale among diverse charge-transfer pathways from picoseconds to seconds significantly limit electrochemiluminescence efficiency hamper their broad applications. Here, we report coordination strategy improve carbon nitrides engineering shallow electron trap states via Au-N bond functionalization. Quantitative kinetics measurements theoretic calculations jointly disclose that bonds endow states, which coordinate fast transfer bulk emitter slow redox reaction co-reagent at diffusion layers. The ultimately accelerate rate emissive electron-hole recombination, setting new cathodic record nitrides, empowering visual sensor nitrite ion, typical environmental contaminant, with superior detection range limit.

Язык: Английский

---

Electrochemiluminescence Microscopy

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(29)

Опубликована: Май 14, 2024

Electrochemiluminescence (ECL) is rapidly evolving from an analytical method into optical microscopy. The orthogonality of the electrochemical trigger and readout distinguishes it classic microscopy techniques, owing to its near-zero background, remarkable sensitivity, absence photobleaching phototoxicity. In this minireview, we summarize recent advances in ECL imaging technology, emphasizing original configurations which enable biological entities improvement properties by increasing complexity multiplexing bioassays. Additionally, mapping (electro)chemical reactivity space provides valuable information on nanomaterials facilitates deciphering mechanisms for improving their performances diagnostics (electro)catalysis. Finally, highlight achievements at ultimate limits single molecules, photons or chemical reactions, current challenges translate other fields such as material science, catalysis biology.

Язык: Английский

---

Bimodal Oxidation Electrochemiluminescence Mechanism of Coreactant‐Embedded Covalent Organic Frameworks via Postsynthetic Modification

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(17)

Опубликована: Март 5, 2024

Abstract Electrochemiluminescence (ECL) efficiency is determined by charge transfer between coreactants and emitters in coreactant systems, which are usually limited their slow intermolecular transfer. In this study, a covalent organic framework (COF) with aldehyde residue was synthesized, then were covalently integrated into the skeleton through postsynthetic modification strategy, resulting crystalline coreactant‐embedded COF nanoemitter (C–COF). Compared to pristine an equivalent external coreactant, C–COF exhibited extraordinary 1008‐fold enhancement of ECL intensity due rapid intrareticular Significantly, pH increase, shows protonation‐induced for first peaked at +1.1 V opposite trend second +1.4 V, attributed antedating oxidation self‐oxidation, respectively. The bimodal mechanism rationalized spectral characterization density functional theory calculations. nanoemitters present innovative universal avenues advancing systems.

Язык: Английский

---

Logic Signal Amplification System for Sensitive Electrochemiluminescence Detection and Subtype Identification of Cancer Cells

Analytical Chemistry, Год журнала: 2024, Номер 96(18), С. 7172 - 7178

Опубликована: Апрель 22, 2024

Achieving sensitive detection and accurate identification of cancer cells is vital for diagnosing treating the disease. Here, we developed a logic signal amplification system using DNA tetrahedron-mediated three-dimensional (3D) nanonetworks electrochemiluminescence (ECL) subtype cells. Specially designed hairpins were integrated into tetrahedral nanostructures (DTNs) to perform catalytic hairpin assembly (CHA) reaction in presence target microRNA, forming hyperbranched 3D nanonetworks. Benefiting from "spatial confinement effect," (DTCHA) displayed significantly faster kinetics greater cycle conversion efficiency than traditional CHA. The resulting could load large amount Ru(phen)

Язык: Английский

---

Controllable and Low-Loss Electrochemiluminescence Waveguide Supported by a Micropipette Electrode

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(8), С. 5423 - 5432

Опубликована: Фев. 14, 2024

One-dimensional molecular crystal waveguide (MCW) can transmit self-generated electrochemiluminescence (ECL), but heavy optical loss occurs because of the small difference in refractive index between and its surroundings. Herein, we report a micropipette electrode-supported MCW (MPE/MCW) for precisely controlling far-field transmission ECL air with low loss. is generated from one terminal positioned inside MPE, which transmitted along to other air. In comparison conventional waveguides on solid substrates or solutions, MPE/MCW propitious total internal reflection light at MCW/air interface, thus confining efficiently improving performance an extremely low-loss coefficient 4.49 × 10–3 dB μm–1. Moreover, by regulation gas atmosphere, active passive be resolved simultaneously MPE This offers unique advantage spatially separating signal readout generation, holding great promise biosensing without less electrical/chemical disturbance.

Язык: Английский

---

A spatial-potential resolved bipolar electrode electrochemiluminescence biosensor based on polarity conversion for dual-mode detection of miRNA-122 and CEA

Biosensors and Bioelectronics, Год журнала: 2024, Номер 255, С. 116258 - 116258

Опубликована: Март 28, 2024

Язык: Английский

---

Ligand-controlled electrochemiluminescence generation from CdSe/CdS/ZnS core/shell/shell quantum dots

Nano Research, Год журнала: 2024, Номер 17(8), С. 7776 - 7785

Опубликована: Июнь 4, 2024

Язык: Английский

---

Enhanced Electrochemiluminescence at the Gas/Liquid Interface of Bubbles Propelled into Solution

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(32), С. 22724 - 22735

Опубликована: Авг. 2, 2024

Electrochemiluminescence (ECL) is typically confined to a micrometric region from the electrode surface. This study demonstrates that ECL emission can extend up several millimeters away employing electrogenerated chlorine bubbles. The mechanism behind this bubble-enhanced was investigated using an Au microelectrode in chloride-containing and chloride-free electrolyte solutions. We discovered at gas/solution interface driven by two parallel effects. First, bubble corona effect facilitates generation of hydroxyl radicals capable oxidizing luminol while attached Second, hypochlorite generated sustains for over 200 s extends range 5 mm into solution, following detachment. new approach increase intensity luminol-based assays 5-fold compared conventional method. demonstrated through glucose bioassay, midrange mobile phone camera detection. These findings significantly expand potential applications extending its effective time space.

Язык: Английский

---