NiCo‐LDH Hollow Nanocage Oxygen Evolution Reaction Promotes Luminol Electrochemiluminescence

Small, Год журнала: 2023, Номер 20(11)

Опубликована: Ноя. 5, 2023

Abstract Conventional luminol co‐reactant electrochemiluminescence (ECL) systems suffer from low stability and accuracy due to factors such as the ease of decomposition hydrogen peroxide inefficient generation reactive oxygen species (ROS) dissolved oxygen. Inspired by ECL mechanism mediated evolution reaction (OER), nickel‐cobalt layered double hydroxide (NiCo‐LDH) hollow nanocages with structure defect state are used co‐reaction promoters enhance emission luminol‐H 2 O system. Thanks state, NiCo‐LDH show excellent OER catalytic activity, which can stabilize efficiently produce ROS emission. Additionally, mechanistic exploration suggests that involved in system derived process, there is a positive correlation between intensity activity promoter. The selection catalysts key factor improving Finally, dual‐mode immunosensor constructed for detection analysis alpha‐fetoprotein (AFP) based on promoting effect

Язык: Английский

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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

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Electroless Deposition of Palladium Nanoparticles on Graphdiyne Boosts Electrochemiluminescence

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(6), С. 3836 - 3843

Опубликована: Фев. 2, 2024

Modulating the electronic structure of metal nanoparticles via metal–support interaction has attracted intense interest in field catalytic science. However, roles supporting substrates regulating properties electrochemiluminescence (ECL) remain elusive. Here, we find that use graphdiyne (GDY) as substrate for electroless deposition Pd (Pd/GDY) produces most pronounced anodic signal enhancement luminol–dissolved oxygen (O2) ECL system co-reactant accelerator over other carbon-based composite nanomaterials. Pd/GDY exhibits electrocatalytic activity reduction O2 through a four-electron pathway at approximately −0.059 V (vs Ag/AgCl) neutral solution forming reactive species (ROS) intermediates. The study shows and GDY increases amount stability ROS on electrode surface promotes reaction luminol anion radical to generate excited luminol, which significantly boosts emission. Based quenching consumption by antioxidants, develop platform detection intracellular antioxidants. This provides an avenue development efficient systems media expands biological application systems.

Язык: Английский

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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

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Bioinspired Single‐Atom Sites Enable Efficient Oxygen Activation for Switching Anodic/Cathodic Electrochemiluminescence

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(29)

Опубликована: Апрель 21, 2023

Abstract Exploring advanced co‐reaction accelerators with superior oxygen reduction activity that generate rich reactive species (ROS) has attracted great attention in boosting luminol‐O 2 electrochemiluminescence (ECL). However, tuning for efficient and selective catalytic O activation to switch anodic/cathodic ECL is very challenging. Herein, we report enzyme‐inspired Fe‐based single‐atom catalysts axial N/C coordination structures (FeN 5 , FeN 4 © SACs) can specific ROS cathodic/anodic conversion. Mechanistic studies reveal sites prefer produce highly active hydroxyl radicals afford direct cathodic luminescence by promoting the cleavage of O−O bonds through N‐induced electron redistribution. In contrast, tend superoxide radicals, resulting inefficient anodic ECL. Benefiting from enhanced ECL, SAC‐based immunosensor was constructed sensitive detection cancer biomarkers.

Язык: Английский

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A novel bimetallic MXene derivative QD-based ECL sensor for miRNA-27a-3p detection

Biosensors and Bioelectronics, Год журнала: 2023, Номер 228, С. 115225 - 115225

Опубликована: Март 11, 2023

Язык: Английский

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Ultrasensitive Electrochemiluminescence Biosensor Based on Efficient Signal Amplification of Copper Nanoclusters Induced by CaMnO₃ for CD44 Trace Detection

Analytical Chemistry, Год журнала: 2024, Номер 96(12), С. 4969 - 4977

Опубликована: Март 15, 2024

Metal nanoclusters (Me NCs) have become a research hotspot in the field of electrochemiluminescence (ECL) sensing analysis. This is primarily attributed to their excellent luminescent properties and biocompatibility along with easy synthesis labeling characteristics. At present, application Me NCs ECL mainly focuses on precious metals, whose high cost, some extent, limits widespread application. In this work, Cu cathode emissions persulfate (S2O82–) were prepared as signal probes using glutathione ligands, which exhibited stable luminescence signals efficiency. same time, CaMnO3 was introduced co-reaction promoter increase responses NCs, thereby further expanding potential biochemical Specifically, reversible conversion Mn3+/Mn4+ greatly promoted generation sulfate radicals (SO4•–), providing guarantee for improving NCs. Furthermore, short peptide (NARKFYKGC) enable fixation antibodies specific targets, preventing occupancy antigen-binding sites (Fab fragments). Therefore, sensitivity biosensor could be significantly enhanced by releasing additional Fab fragments. Considering approaches discussed above, constructed achieve sensitive detection CD44 over broad range (10 fg/mL–100 ng/mL), an ultralow limit 3.55 fg/mL (S/N = 3), had valuable implications nonprecious biosensing

Язык: Английский

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Electrogenerated Chemiluminescence Imaging of Single‐Atom Nanocatalysts

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(16)

Опубликована: Фев. 20, 2024

Abstract Single‐atom catalysts (SACs), distinguished by their maximum atom efficiency and precise control over the coordination electronic properties of individual atoms, show great promise in electrocatalysis. Gaining a comprehensive understanding electrochemical performance SACs requires screening electron transfer process at micro/nano scale. This research pioneers use electrogenerated chemiluminescence microscopy (ECLM) to observe electrocatalytic reactions SACs. It boasts sensitivity single photon level temporal resolution down 100 ms, enabling real‐time capture behavior during potential sweeping. Leveraging direct correlation between ECL emission heterogeneous processes, we introduced flux density for quantitative analysis, unveiling approach systematically reveals relationship based on different metal atoms peroxidase (POD)‐like activity. The outcomes contribute fundamental pave way designing with diverse technological industrial applications.

Язык: Английский

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Lattice Strained Induced Spin Regulation in Co−N/S Coordination‐Framework Enhanced Oxygen Reduction Reaction

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(16)

Опубликована: Фев. 23, 2024

Abstract Oxygen reduction reaction (ORR) is the bottleneck of metal‐air batteries and fuel cells. Strain regulation can change geometry adjust surface charge distribution catalysts, which a powerful strategy to optimize ORR activity. The introduction controlled strain material still difficult achieve. Herein, we present temperature‐pressure‐induced achieve lattice for metal coordination polymers. Through systematic study effect on performance, relationship between geometric electronic effects further understood confirmed. strained Co‐DABDT (DABDT=2,5‐diaminobenzene‐1,4‐dithiol) with 2 % compression exhibits superior half‐wave potential 0.81 V. Theoretical analysis reveals that changes spin‐charge densities around S atoms Co‐DABDT, then regulates hydrogen bond interaction intermediates promote catalytic process. This work helps understand mechanism from atomic level.

Язык: Английский

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Cu Single-Atom Nanozyme-Mediated Electrochemiluminescence Biosensor for Highly Sensitive Detection of MicroRNA-622

Analytical Chemistry, Год журнала: 2024, Номер 96(31), С. 12838 - 12845

Опубликована: Июль 25, 2024

MicroRNA (miRNA) detection is a critical aspect of disease diagnosis, and recent studies indicate that miRNA-622 could be potential target for lung cancer. Herein, Cu single atoms were anchored on graphitic carbon nitride (Cu SAs@CN) as coreaction accelerator applied in luminol-H

Язык: Английский

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