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

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Polymerized carbon dots with high electrochemiluminescence efficiency and long wavelength ECL emission for ultrasensitive detection of MicroRNA-222

Biosensors and Bioelectronics, Год журнала: 2024, Номер 254, С. 116193 - 116193

Опубликована: Март 5, 2024

Язык: Английский

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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

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Host–Guest Recognition-Mediated Supramolecular Aggregation-Induced Electrochemiluminescence of Iridium(III) Complexes for Nucleic Acid Bioassay

Analytical Chemistry, Год журнала: 2024, Номер 96(16), С. 6218 - 6227

Опубликована: Апрель 10, 2024

Currently reported aggregation-induced electroluminescence (AIECL) is usually based on the electrostatic integration of luminous monomers, and its application still limited by low ECL efficiency poor structural stability integration-based AIECL emitters. Herein, host-guest recognition-mediated supramolecular was creatively developed to overcome defects electrostatic-integration-based AIECL. Cucurbit[8]uril (CB[8]) as host recognized tris (2-phenylpyridine) iridium(III) [Ir(ppy)

Язык: Английский

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Self-Assembled Tetraphenylethene-Based Nanoaggregates with Tunable Electrochemiluminescence for the Ultrasensitive Detection of E. coli

Analytical Chemistry, Год журнала: 2024, Номер 96(12), С. 4809 - 4816

Опубликована: Март 11, 2024

As an effective ECL emitter, tetraphenylethene (TPE)-based molecules have recently been reported with aggregation-induced electrochemiluminescence (AIECL) property, while it is still a big challenge to control its aggregation states and obtain uniform aggregates intense emission. In this study, we develop three TPE derivatives carrying pyridinium group, alkyl chain, quaternary ammonium group via the Menschutkin reaction. The resulting exhibit significantly red-shifted FL enhanced emissions due tunable reduction of energy gap between highest occupied molecular orbitals (HOMOs) lowest unoccupied (LUMOs). More importantly, amphiphilicity as-developed enables their spontaneous self-assembly into well-controlled spherical nanoaggregates, intensity nanoaggregates 3 −CH2– (named as C3) 17.0-fold higher compared that original 4-(4-(1,2,2-triphenylvinyl)phenyl)pyridine (TPP) molecule. These cationic demonstrate high affinity toward bacteria, sensor for profiling Escherichia coli (E. coli) was developed broad linear range good selectivity in presence E. coli-specific aptamer. This study provides way enhance emission through derivatization simple prepare AIECL application.

Язык: Английский

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Solvent Regulation Induced Cathode Aggregation-Induced Electrochemiluminescence of Tetraphenylethylene Nanoaggregates for Ultrasensitive Zearalenone Analysis

Analytical Chemistry, Год журнала: 2024, Номер 96(22), С. 9043 - 9050

Опубликована: Май 22, 2024

Zearalenone (ZEN) is an extremely hazardous chemical widely existing in cereals, and its high-sensitivity detection possesses significant significance to human health. Here, the cathodic aggregation-induced electrochemiluminescence (AIECL) performance of tetraphenylethylene nanoaggregates (TPE NAs) was modulated by solvent regulation, based on which (ECL) aptasensor constructed for sensitive ZEN. The aggregation state AIECL TPE NAs were directly simply controlled adjusting type organic fraction water, solved current shortcomings low strength weak stability cathode ECL signal TPE. Impressively, a tetrahydrofuran–water mixed solution (volume ratio, 6:4), relative efficiency reached 16.03%, 9.2 times that pure water conditions, maximum spectral wavelength obviously red-shifted 617 nm. In addition, "H"-shape DNA structure-mediated dual-catalyzed hairpin self-assembly (H-D-CHA) with higher synergistic effect between two CHA reactions utilized construct ZEN analysis limit 0.362 fg/mL. conclusion, regulation simple efficient method improving materials, proposed had great potential monitoring food safety.

Язык: Английский

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Zero-Background Dual-Mode Closed Bipolar Electrode Electrochemiluminescence Biosensor Based on ZnCoN-C Potential Regulation for Ultrasensitive Detection of Ochratoxin A

Analytical Chemistry, Год журнала: 2024, Номер unknown

Опубликована: Авг. 14, 2024

In this work, the relationship between electrochemiluminescence (ECL) signal and driving voltage was first studied by self-made reduced oxidized closed bipolar electrodes (CBPEs). It found that when large enough, maximum ECL signals for two kinds of CBPEs were same but their required drive voltages different. Zinc cobalt nitrogen doped carbon material (ZnCoN-C) had an outstanding electric double layer (EDL) property conductivity. Therefore, it could significantly reduce CBPE systems, reaching Ru(bpy)32+. Interestingly, ZnCoN-C modified electrode reached signal, bare zero. As a proof-of-concept application, zero-background dual-mode CBPE-ECL biosensor constructed ultrasensitive detection ochratoxin A (OTA) in beer. Considering beer samples contained number reducing substances, system selected to build biosensor. Furthermore, convenient imaging platform using smartphone built OTA. This work used unique EDL regulate time; thus, novel sensor constructed. Further, provided deeper understanding opened new door detection.

Язык: Английский

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Dual-Ligand Ruthenium Coordination Polymer-Derived Self-Enhanced Electrochemiluminescent Emitters for Sensitive Detection of Procalcitonin

Analytical Chemistry, Год журнала: 2024, Номер 96(26), С. 10809 - 10816

Опубликована: Июнь 17, 2024

Ru-based electrochemiluminescence (ECL) coordination polymers are widely employed for bioanalysis and medical diagnosis. However, commonly used face the limitation of low efficiency due to long distance between ECL reagent coreactant dispersed in detecting solution. Herein, we report a dual-ligand self-enhanced polymer, composed tris(4,4′-dicarboxylic acid-2,2′-bipyridyl) ruthenium(II) dichloride (Ru(dcbpy)32+) as reactant ligand ethylenediamine (EDA) corresponding into Zn2+ metal node, termed Zn-Ru-EDA. Zn-Ru-EDA shows excellent performance which is attributed effective intramolecular electron transport two ligands. Furthermore, polymer allows an anodic excitation potential (+1.09 V) luminescence. The shift energy level highest occupied molecular orbital (HOMO) upward after synthesis has resulted reduced potential. biomolecular damage destruction modified electrodes. biosensor been constructed using with high ultrasensitive detection bacterial infection sepsis biomarker, procalcitonin (PCT), range from 1.00 × 10–6 10 ng·mL–1 outstanding selectivity, limit was 0.47 fg·mL–1. Collectively, dual-ligand-based may provide ideal strategy improvement well designing new multiple-ligand-based sensitive early disease diagnostics.

Язык: Английский

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Insight into the charge transfer behavior of an electrochemiluminescence sensor based on porphyrin–coumarin derivatives with a donor–acceptor configuration

Chemical Science, Год журнала: 2024, Номер unknown

Опубликована: Янв. 1, 2024

The successful integration of the SPECM measurement technique to provide deeper insights into underlying mechanisms responsible for improved ECL performance is reported.

Язык: Английский

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Enhanced Aggregation-Induced Delayed Electrochemiluminescence Triggered by Spatial Perturbation of Organic Dots

Analytical Chemistry, Год журнала: 2024, Номер 96(19), С. 7780 - 7786

Опубликована: Май 2, 2024

Development of highly efficient, heavy-metal-free electrochemiluminescence (ECL) materials is attractive but still challenging. Herein, we report an aggregation-induced delayed ECL (AIDECL) active organic dot (OD) composed a tert-butoxy-group-substituted benzophenone-dimethylacridine compound, which shows high efficiency. The resultant ODs exhibit 2.1-fold higher efficiency compared to control AIDECL-active ODs. Molecular stacking combined with theoretical calculations suggests that tert-butoxy groups effectively participate in the intermolecular interactions, further inhibiting molecular motions aggregated states and thus accelerating radiative decay. On basis these exhibiting excellent performance, proof-of-concept biosensor constructed for detection miR-16 associated Alzheimer's disease, demonstrates ability limit 1.7 fM. This work provides new approach improve enriches fundamental understanding structure–property relationship.

Язык: Английский

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