Atomically Dispersed Metal Interfaces for Analytical Chemistry

Accounts of Chemical Research, Год журнала: 2025, Номер unknown

Опубликована: Апрель 17, 2025

ConspectusEngineering sensing interfaces with functional nanomaterials have aroused great interest in constructing novel analytical platforms. The good catalytic abilities and physicochemical properties allow to perform signal transductions synergistically amplify biorecognition events for efficient target analysis. However, further boosting their performances poses grand challenges achieving more sensitive selective sample assays. Besides, abundant atomic compositions complex structural characteristics bring about difficulties understanding the underlying mechanism of amplification. Atomically dispersed metal catalysts (ADMCs), as an emerging class heterogeneous catalysts, feature support-stabilized isolated sites, showing maximum utilization a strong metal-support interfacial interaction. These unique are akin those homogeneous which well-defined coordination structures between sites synthetic or biological ligands. By integrating advantages ADMCs present superior activity specificity relative nanoparticles formed by nonuniform aggregation active sites. ADMC-enabled platforms been demonstrated realize advanced applications various fields. Notably, easily tunable opportunities improve performance, moving toward transduction ability. leveraging inherent detection strategies, not only achieve enhanced but also show diversified output models. Such functions access goal high-performance trace targets making significant progress chemistry.In this Account, we provide overview recent atomically metal-involved chemistry. engineering strategies focused on regulating centers, multisite synergy, tuning charge transport pathways discussed boost well expand multifunctionality. Combined models, including colorimetry, electrochemistry, chemiluminescence, electrochemiluminescence, photoelectrochemistry, ADMC-based sensors diverse analytes. Specifically, mechanisms highlighted. Finally, perspective interface chemistry proposed. We hope that Account will afford inspiration design decoding improved interfaces.

Язык: Английский

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High-Throughput Screening of Selective Bimetallic Atomic Catalysts for Self-Adaptive Matched Electrochemical Reduction

Nano Letters, Год журнала: 2025, Номер unknown

Опубликована: Фев. 7, 2025

Due to the impediments of spatial and temporal resolution, comprehension microdynamic processes still remains limited, which seriously hinders advancement catalyst regulating expansion application. Herein, efficient selective bimetallic atomic electrode interface was cultivated via high-throughput screening, achieving self-adaptive parallel electrochemical reduction Cu(II) As(III). Combined in situ X-ray absorption fine structure (XAFS) spectroscopy coordination field theory verified Ni-Cu specific energy level matching promoted by permitted d-d transition also reproduced microscopic dynamic process. Additionally, it discovered that Fe-As bonding barrier smallest potential-determining step (1.40 eV) were derived from linear shift main s p peaks key arsenic intermediates high-energy orbital. This work offers insights into transient reaction dynamics methods theoretical simulations, broadens design multisite catalysts.

Язык: Английский

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Boosting Peroxidase-Mimetic Activity of FeMn-NC_e Dual-Atom Radiosensitizing Nanozymes for Augmented Radiodynamic Immunotherapy

ACS Nano, Год журнала: 2025, Номер unknown

Опубликована: Март 7, 2025

Dual-atom nanozymes (DAzymes) have garnered considerable attention as catalysts for reactive oxygen species (ROS)-based therapies, effectively leveraging ROS generation within the tumor microenvironment (TME). Herein, we introduce FeMn-NCe DAzymes, which are meticulously engineered enhanced peroxidase (POD)-mimetic activity and potent radiosensitization to advance radioimmunotherapy. Density functional theory (DFT) calculations reveal that DAzymes lower energy barrier increase substrate affinity, enabling highly efficient catalytic performance. Within TME, these efficiently convert overexpressed hydrogen peroxide (H2O2) into hydroxyl radicals (•OH), potentially activating cGAS-STING immune pathway. This POD-mimetic catalysis is further accelerated under X-ray irradiation, significantly enhancing radiosensitization. Additionally, a uniform coating of ultrasmall gold nanoparticles on enhances absorption cancer cells. The incorporation STING agonist diABZI onto induces long-term antitumor immunity, reprograms immunosuppressive suppresses growth metastasis following single low-dose treatment. work highlights valuable strategy designing radiodynamic immunotherapy.

Язык: Английский

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f-p-d Orbital Hybridization Promotes Hydroxyl Intermediate Adsorption for Electrochemical Biomolecular Oxidation and Identification

Analytical Chemistry, Год журнала: 2025, Номер unknown

Опубликована: Янв. 3, 2025

The rational design of efficient hydroxyl intermediate (*OH) adsorption catalysts for dopamine electrooxidation still faces a major challenge. To address this challenge, CeO2-loaded CuO catalyst inspired by the f-p-d orbital hybridization strategy is designed to achieve *OH and improve oxidation. experimental results theoretical calculations demonstrate that regulates electron distribution at Ce–O–Cu interface, which facilitates transfer optimizes *OH, thereby promoting electrochemical sensor exhibits excellent catalytic activity sensitivity, reaching limit detection 3.22 nM. This work provides promising approach designing highly active electrocatalysts with

Язык: Английский

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Accurate electrochemical paracetamol sensor for drug control through catalytic roles of single Fe atoms

Rare Metals, Год журнала: 2025, Номер unknown

Опубликована: Апрель 11, 2025

Язык: Английский

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Jahn–Teller-Driven Electronic Modulation of Bio-Heterojunction for Wound Regeneration after Postoperative Tumor Resection

Nano Letters, Год журнала: 2025, Номер unknown

Опубликована: Апрель 12, 2025

Abundant ·OH, 1O2, and ·O2- provide an efficient methodology for rapid tumor bacteria killing, whereas a limitation focuses on the catalytic efficiency. Thus, Jahn-Teller-driven electronic modulation of bioheterojunction (bioHJ) platform is developed remedy in diabetic infectious wound regeneration after postoperative resection. The bioHJ composed MoTe2/MnO2 glucose oxidase (GOx). GOx depletes to H2O2, which intercepts their metabolism. H2O2 can be further converted into highly lethal ·OH owing peroxidase-mimetic activity via Jahn-Teller effect, while GSH consumed due its GPx-mimetic activity. Both amplified upon NIR irradiation as NIR-activatable enzyme-mimetic activities. In vivo studies subcutaneous model authenticate ability kill tumor, defeat bacterial infection, accelerate regeneration. This work enlightens powerful resection using engineered bioHJ.

Язык: Английский

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Interfacial engineering of VS2/Ti3C2Tx MXene heterojunctions for portable electrochemical sensing of nitrofurantoin residues in food and water samples

Food Chemistry, Год журнала: 2025, Номер 486, С. 144624 - 144624

Опубликована: Май 3, 2025

Язык: Английский

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Single–Atom Supported Catalysts and Beyond

Advanced Materials, Год журнала: 2025, Номер unknown

Опубликована: Июнь 4, 2025

Abstract Tuning electronic configurations of active components in supported metal catalysts can be achieved via strong metal–support interaction (SMSI) between loaded species and support, which has a profound effect on catalytic efficiency. Distinct from conventional supports, single–atom catalysts, due to their rich unsaturated coordination sites versatile states, are employed as supports load species, manipulate the SMSI thereby regulate performance. Although have demonstrated remarkable advance capabilities, this field is still its infancy with large room for improvement. Here, definition, classification, state‐of‐the‐art characterization techniques summarily demonstrated. The enhancement mechanisms influenced by site‐specific metal‐support within including interactions synergistic catalysis highlighted present potentials advantages community. Moreover, various advanced summarized discuss relationships properties. Finally, challenges perspectives directions future development provided.

Язык: Английский

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Engineering Interference-Removal and Target-Response Cascade Zones on Wood Channels for Straightforward Detection of Uric Acid in Saliva

Analytica Chimica Acta, Год журнала: 2024, Номер 1336, С. 343522 - 343522

Опубликована: Дек. 4, 2024

Язык: Английский

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