Oxygen‐Bonded Amorphous Transition Metal Dichalcogenides with pH‐Responsive Reactive Oxygen Biocatalysis for Combined Antibacterial and Anti‐inflammatory Therapies in Diabetic Wound Healing

Small, Год журнала: 2024, Номер unknown

Опубликована: Окт. 29, 2024

Diabetic wound healing is a formidable challenge, often complicated by biofilms, immune dysregulation, and hindered vascularization within the environments. The intricate interplay of these microenvironmental factors has been significant oversight in evolution therapeutic strategies. Herein, design an efficient versatile oxygen-bonded amorphous transition metal dichalcogenide biocatalyst (aRuS-O

Язык: Английский

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Reprogram Local Electronic Configuration in Multicomponent Covalent–Organic Frameworks for Efficient Hydrogen Peroxide Photoproduction

Chemistry of Materials, Год журнала: 2025, Номер unknown

Опубликована: Фев. 19, 2025

Covalent organic frameworks (COFs) have recently demonstrated significant potential for photocatalysis. Optimizing the local electronic environment in COFs has been considered to be critical enhancing photocatalytic activity. Here, we report a one-pot "grafting-to" strategy reprogram configurations of series isoreticular multicomponent by introducing electron-donating or electron-withdrawing groups into pores transform photoinert photoactive and form intramolecular donor–acceptor (D-A) structures. Such D-A structures enhanced overall hydrogen peroxide photoproduction facilitating charge carrier separation optimizing band achieve oxygen reduction reaction water oxidation simultaneously. Notably, one incorporated with 2-aminothiazole exhibits production rate 3701 μmol g–1 h–1 solar-to-chemical conversion efficiency 0.13% without use any sacrificial reagents, it 100% bacterial killing rates remarkable >90% biofilm removal capability. This COF modification strategy, which not reported before, offers unique approach constructing highly active photocatalysts containing great future design antibacterial therapies.

Язык: Английский

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Porphyrin-Based Covalent Organic Framework Encapsulating Multiwalled Carbon Nanotubes: A High-Performance Electrocatalyst for Oxygen Reduction Reaction

Langmuir, Год журнала: 2025, Номер unknown

Опубликована: Апрель 17, 2025

The development of efficient and cost-effective oxygen reduction reaction (ORR) catalysts is crucial for advancing fuel cell technologies, given the limitations platinum-based catalysts. Here, we present a novel nanocomposite, cobalt-based porphyrinic covalent organic framework wrapped on multiwalled carbon nanotubes (Co-pCOF@MWCNTs), synthesized via template-directed in situ polymerization. This composite combines high porosity tunable catalytic properties COFs with excellent electrical conductivity MWCNTs. Co-pCOF@MWCNT demonstrates superior ORR activity, exhibiting an onset potential (Eonset) 0.86 V vs RHE 0.1 M KOH, surpassing performance its individual components (Co-pCOF MWCNT) other related materials. enhanced efficiency attributed to synergistic interactions between conductive MWCNT scaffold active COF nanolayers, which facilitate charge transfer increase site exposure. Furthermore, nanocomposite exhibits stability methanol tolerance, establishing as cathodic material cells. work highlights promise integrating materials opens new avenues design advanced energy conversion applications.

Язык: Английский

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Injectable Spiky Artificial Peroxidase‐Encapsulated Hydrogels for Bioadaptively and Synergistically Combating Endometrial Infections

Advanced Functional Materials, Год журнала: 2025, Номер unknown

Опубликована: Май 5, 2025

Abstract Endometrial infections can lead to acute endometritis and persistent inflammation of the uterus, which may further infertility in severe cases. It is a great challenge develop localized antimicrobial therapeutic strategy that exploits infected microenvironment for effectively combating endometrial facilitating repair. Here, an injectable spiky artificial Cu‐polyphthalocyanine peroxidase‐encapsulated thermosensitive hydrogel engineered bioadaptively synergistically infection. The comprehensive investigations have elucidated network‐based spike‐linked enzyme‐mimics (SLE‐CuPPc) possess dual functionalities nanostructure enables efficient capture kill action bacteria simultaneously generates substantial quantity reactive oxygen species (ROS). attachment SLE‐CuPPc bacterial surfaces constricts ROS radius, thereby potentiating its bactericidal efficacy. encapsulated into clinically approved hydrogel, yielding composite G‐SLE‐CuPPc. infection models demonstrate this formulation not only eradicates S. aureus but also stimulates vascular proliferation, curbs fibrosis, fosters This work demonstrates pivotal role G‐SLE‐CuPPc eradicating antibiotic‐resistant paves way developing next‐generation hydrogels clinical treatment.

Язык: Английский

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Construction of Active Sites‐Accessible Au₈ Clusters for Intensive Tumor Pyroptosis

Aggregate, Год журнала: 2025, Номер unknown

Опубликована: Май 8, 2025

ABSTRACT Atomically precise gold nanoclusters (NCs), possessing characteristics of molecules and nanoparticles, offer a promising solution to the challenges faced by existing pyroptosis inducers. Their abilities catalyze generation reactive oxygen species enhance radiosensitization position them as effective agents for activating pyroptosis. However, their catalytic efficiency is often compromised limited geometrically accessible spaces around active sites lack suitable ligands. Leveraging exposed metal centers in mononuclear organometallic catalysts tunable ligand NCs, herein, ethynylferrocene (EFc) was utilized amplify peroxidase (POD)‐like activity NCs establishing unshielded center electron donor‐acceptor interaction between EFc Au core. The resulting 8 Fe 2 with excellent POD‐mimicking could efficiently trigger inducing intracellular oxidative stress. Moreover, potential deplete glutathione enable magnetic resonance imaging, also induce ferroptosis serve diagnostic tool tumors. All these processes can be further potentiated X‐ray radiation, taking advantage high atomic number gold. This work opens new avenues engineering properties broadens applications biomedicine.

Язык: Английский

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Engineering sulfur vacancies in NiCo2S4 flower-like structure to achieve exceptional peroxidase activity for advanced colorimetric biomedical diagnostics

Journal of Alloys and Compounds, Год журнала: 2025, Номер 1030, С. 180924 - 180924

Опубликована: Май 1, 2025

Язык: Английский

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Spatial Configuration-Guided Design of Covalent Organic Framework-Based Artificial Metalloantioxidases for Inhibiting Inflammatory Cascades and Regulating Bone Homeostasis

Journal of the American Chemical Society, Год журнала: 2025, Номер unknown

Опубликована: Май 22, 2025

Intense oxidative stress in bone tissues can trigger the hyperactivation of neutrophils, thereby causing inflammatory cascades to deteriorate homeostasis. Here, inspired by catalytic centers natural antioxidases, we introduce spatial configuration-guided design covalent organic framework (COF)-based artificial metalloantioxidases for inhibiting and regulating Specifically, hexaiminohexaazatrinaphthalene COF with ruthenium coordination (S-HACOF-Ru), featuring electron-rich a configuration, demonstrates exceptional antioxidase-like reactive oxygen species (ROS) scavenging capabilities efficiently mitigating stress. As result, S-HACOF-Ru prevents generation neutrophil extracellular traps inhibits release myeloperoxidase (MPO). By preventing MPO-induced activation nuclear factor-kappa B proinflammatory macrophage polarization, successfully blocks neutrophil-macrophage cascades. This intervention promotes homeostasis shift from resorption tissue regeneration, which inhibit alveolar loss periodontal reverse cartilage damage ankle joint cavities. We propose that this strategy provides an intriguing avenue developing new antioxidases biocatalytic materials potential applications treating wide range chronic diseases.

Язык: Английский

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Tuning ligand substituents of metal-organic frameworks enhances laccase-like activity for pesticide detection

Food Chemistry, Год журнала: 2025, Номер 488, С. 144892 - 144892

Опубликована: Май 23, 2025

Язык: Английский

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Neuroblastoma‐Targeting π‐Conjugated COP Nanostructure with Multiple Enzyme‐Mimetic Actions for Sonochemodynamic Immunotherapies

Advanced Materials, Год журнала: 2025, Номер unknown

Опубликована: Май 30, 2025

Abstract Sonodynamic therapy (SDT) has emerged as a promising strategy for neuroblastoma treatment, leveraging ultrasound to induce the production of reactive oxygen species (ROS) at tumor sites, thereby enhancing efficacy immunotherapy. However, major challenge in SDT is efficiency ROS generation, particularly context hypoxia within microenvironment. Herein, inspired by natural peroxidase, an imide‐linked metal‐phthalocyanine‐based conjugated organic polymer (COP) (COP TPcFe ) been designed with well‐defined π‐conjugated nanostructure and peroxidase‐mimetic atomic Fe‐N sites sonochemodynamic immunotherapy against neuroblastoma. This work demonstrates that COP can efficiently produce potent (•OH •O 2 − utilizing localized H O effects ultrasound, achieving efficient synergistic tumoricidal activity. Notably, highly structure endows excellent electron transport capabilities, enabling rapid catalysis , thus alleviating hypoxic conditions tumors. Moreover, encapsulating cell membranes, this study achieveshomologous targeting cells tissues, leading accumulation cells, mitochondrial disruption, apoptosis. Additionally, proposed effectively activates killer reverses immunosuppressive microenvironment, significantly therapeutic treatment.

Язык: Английский

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Biocatalytic and Redox‐Regulated Nanoarchitectures for Precision Inflammation and Immune Homeostasis Modulation to Combat Rheumatoid Arthritis

Advanced Materials, Год журнала: 2025, Номер unknown

Опубликована: Июнь 1, 2025

Abstract The chronic inflammatory milieu of rheumatoid arthritis (RA), marked by elevated reactive oxygen species (ROS), perpetually activated pro‐inflammatory macrophages (M1) and osteoclasts, significant infiltration cytokines contributes to abnormal articular redox imbalance, severe synovitis, progressive joint erosion. In this study, the rational design a biocatalytic redox‐regulated nanoarchitecture comprising Ru cluster‐anchored hydroxylated Fe 2 O 3 (Ru‐HFO) encapsulated within bone marrow stem cell‐derived extracellular vesicles (BEVs), for precision inflammation modulation combat RA is proposed. When combined with ultrasound (US) stimulation, inflammation‐targeting (BEVs@Ru‐HFO) can reprogram osteoclasts restore immune homeostasis, thereby alleviating RA. findings reveal that hydroxylation strategy enhances electron density at centers fine‐tunes binding affinity intermediates, ensuring exceptional multi‐enzymatic ROS‐scavenging activities. Notably, under ultrasonic irradiation, BEVs@Ru‐HFO targets inflamed joints, promotes local accumulation anti‐inflammatory macrophages, downregulates cytokines, ameliorates hypoxic microenvironment inhibit osteoclastogenesis. This ultimately confers cartilage protection restores function. It posit nanoarchitecture, its superior antioxidant immunomodulatory capabilities, represents promising engineering ROS‐catalytic materials treat potentially many other autoimmune diseases.

Язык: Английский

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