Biomimetic-Structured Cobalt Nanocatalyst Suppresses Aortic Dissection Progression by Catalytic Antioxidation

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(25), P. 17201 - 17210

Published: June 14, 2024

As one of the most lethal cardiovascular diseases, aortic dissection (AD) is initiated by overexpression reactive oxygen species (ROS) in aorta that damages vascular structure and finally leads to massive hemorrhage sudden death. Current drugs used clinics for AD treatment fail efficiently scavenge ROS a large extent, presenting undesirable therapeutic effect. In this work, nanocatalytic antioxidation concept has been proposed elevate efficacy constructing cobalt nanocatalyst with biomimetic can pathological an efficient sustainable manner. Theoretical calculations demonstrate reaction catalyzed redox transition between hydroxocobalt(III) oxo-hydroxocobalt(V) accompanied inner-sphere proton-coupled two-electron transfer, forming nonassociated activation catalytic cycle. The action region effectively alleviates oxidative stress, which further modulates inflammatory microenvironment promoting phenotype macrophages. Consequently, smooth muscle cells are also protected from inflammation meantime, suppressing progression. This study provides approach other diseases.

Language: Английский

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Pyrene‐Alkyne‐Based Conjugated Porous Polymers with Skeleton Distortion‐Mediated •O2‐ and 1O2 Generation for High‐Selectivity Organic Photosynthesis

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: unknown

Published: May 31, 2024

Abstract Reactive oxygen species (ROS) play a crucial role in determining photocatalytic reaction pathways, intermediate species, and product selectivity. However, research on ROS regulation polymer photocatalysts is still its early stages. Herein, we successfully achieved series of modulations to the skeleton Pyrene‐alkyne‐based (Tetraethynylpyrene (TEPY)) conjugated porous polymers (CPPs) by altering linkers (1,4‐dibromobenzene (BE), 4,4′‐dibromobiphenyl (IP), 3,3′‐dibromobiphenyl (BP)). Experiments combined with theoretical calculations indicate that BE‐TEPY exhibits planar structure minimal exciton binding energy, which favors dissociation followed charge transfer adsorbed O 2 produce ⋅O − . Thus shows optimal activity for phenylboronic acid oxidation [3+2] cycloaddition. Conversely, BP‐TEPY significantly distorted. Its conjugation decreases, intersystem crossing (ISC) efficiency increases, makes it more prone resonance energy generate 1 Therefore, displays best [4+2] cycloaddition thioanisole oxidation. Both above reactant conversion selectivity exceed 99 %. This work systematically reveals intrinsic structure–activity relationship among CPPs, excitonic behavior, selective generation ROS, providing new insights rational design highly efficient CPPs photocatalysts.

Language: Английский

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Oxygen Vacancy Piezoelectric Nanosheets Constructed by a Photoetching Strategy for Ultrasound “Unlocked” Tumor Synergistic Therapy

Nano Letters, Journal Year: 2024, Volume and Issue: 24(26), P. 8008 - 8016

Published: June 24, 2024

Piezoelectric dynamic therapy (PzDT) is an effective method of tumor treatment by using piezoelectric polarization to generate reactive oxygen species. In this paper, two-dimensional Cu-doped BiOCl nanosheets with surface vacancies are produced the photoetching strategy. Under ultrasound, a built-in electric field generated promote electron and hole separation. The separated carriers achieve O

Language: Английский

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Reprogramming Lung Redox Homeostasis by NIR Driven Ultra‐Small Pd Loaded Covalent Organic Framework Inhibits NF‐κB Pathway for Acute Lung Injury Immunotherapy

Advanced Science, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 18, 2025

Abstract Acute lung injury (ALI) refers to damage related cells, typically caused by an uncontrollable inflammatory response, and over‐generated reactive oxygen species (ROS). Increasing evidence suggests that reprogramming redox homeostasis holds significant potentials for the clinical treatment of ALI. Herein, simple synthesis ultra‐small Pd loaded covalent organic framework (COF) (TP@Pd) is reported, which, when combined with near infrared (NIR) irradiation, exhibits nanozyme functionalities, including multiple enzyme mimicking activities broad spectrum ROS scavenging, thereby promoting tissue repair ALI immunotherapy. Mechanistically, through therapeutic strategy TP@Pd+NIR, damaged cells tissues are ameliorated decreasing intracellular levels (total ROS, ·OH ·O 2 − ), downregulating cytokines (IL‐6, TNF‐α IL‐1β), upregulating antioxidant factor level (SOD2), inducing macrophage M2 directional polarization (downregulation iNOS CD86, upregulation IL‐10 CD206), activating immunoregulation (CD4 + /CD8 ratio increase), (upregulation HSP70 CD31), suppressing NF‐κB signaling pathway phosphorylated p65 IκBα). Furthermore, following intravenous (IV) injection in rats, TP@Pd accumulated 6 h, indicating promising efficacy via this administration route. Notably, TP@Pd+NIR demonstrated excellent synergistic effects alleviating inflammation storms, reducing diffuse alveolar damage, accelerating repair. Summarily, work has designed a novel enhancement amelioration, which may serve as approach other diseases.

Language: Английский

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Trilocked Photodynamic Senolytic Inducer Potentiating Immunogenic Senescent Cell Removal for Liver Fibrosis Resolution

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: April 30, 2025

Liver fibrosis is a major global health problem without effective therapies, and targeted elimination of senescent cells beneficial for hepatic function organism survival. We report new trilocked photodynamic senolytic inducer (PDSI) strategy liver resolution using type-I agent immunogenic clearance cells. demonstrate that this PDSI not only facilitates efficient production superoxide anions (O2•-) in lysosomes therapy, but also permits NIR fluorescence photoacoustic (NIRF/PA) imaging Mechanistic investigation reveals the elicited cell predominantly via necroptosis pathway. Moreover, with liver-targeting moiety enables high-contrast NIRF/PA vivo. This exhibits remarkable ablation cells, enhancing dendritic maturation cytotoxic T recruitment fibrosis. Our study highlights potential type I boosting immunity treatment.

Language: Английский

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NADPH Oxidases‐Inspired Reactive Oxygen Biocatalysts with Electron‐Rich Pt Sites to Potently Amplify Immune Checkpoint Blockade Therapy

Advanced Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 14, 2024

Abstract Clinical immune checkpoint blockade (ICB)‐based immunotherapy of malignant tumors only elicits durable responses in a minority patients, primarily due to the highly immunosuppressive tumor microenvironment. Although inducing immunogenic cell death (ICD) through reactive oxygen biocatalyst represents an attractive therapeutic strategy amplify ICB, currently reported biocatalysts encounter insurmountable challenges achieving high ROS‐generating activity induce potent ICD. Here, inspired by natural catalytic characteristics NADPH oxidases, design efficient, robust, and electron‐rich Pt‐based redox centers on non‐stoichiometric W 18 O 49 substrates (Pt─WO x ) serve as bioinspired potently activate ICD, which eventually enhance cancer amplifies ICB‐based is reported. These studies demonstrate that Pt─WO exhibits rapid electron transfer capability can promote formation low oxophilic Pt for superior biocatalysis, enables ‐based inducers trigger endoplasmic reticulum stress directly stimulate amplifying anti‐PD‐L1‐based ICB therapy. This provides straightforward engineer also opens up new avenue create efficient ICD primary/metastatic treatments.

Language: Английский

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Ru induced charge redistribution of MnO2 spheric nanozyme boosted hydrogen sulfide selective detection and cystathionine γ-lyase activity sensitive evaluation

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: unknown, P. 157904 - 157904

Published: Nov. 1, 2024

Language: Английский

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Trends and advances in the development of nanodiamond-graphene core-shell materials in heterogeneous catalysis

Journal of Energy Chemistry, Journal Year: 2025, Volume and Issue: unknown

Published: March 1, 2025

Language: Английский

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Orchestrated electron transfer in reduced polyoxometalate-based coordination architectures for facilitating nitrate-to-ammonia electrosynthesis

Journal of Colloid and Interface Science, Journal Year: 2025, Volume and Issue: 694, P. 137717 - 137717

Published: April 28, 2025

Language: Английский

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Dual‐Functional Artificial Peroxidases with Ferriporphyrin Centers for Amplifying Tumor Immunotherapies via Immunogenic Cell Death

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 34(11)

Published: Nov. 30, 2023

Abstract Constructing highly effective sonosensitizers that integrate tumor microenvironment (TME)‐adaptive and ultrasound (US)‐controllable production of reactive oxygen species (ROS) to amplify immunotherapies is extremely desirable but remains challenging. Here, inspired by the coordination structure biocatalytic effects Fe‐based peroxidase, a dual‐functional artificial peroxidase synthesized with ferriporphyrin networks (FePorNW‐DAP) serve TME‐adaptive US‐controllable ROS‐generator for amplifying in breast cancer via immunogenic cell death. Owing structural advantages ferriporphyrin‐based large d–π‐conjugated monatomic Fe─N 4 center, moderate interaction H 2 O , decreased bandgap, FePorNW‐DAP displays efficient ROS capabilities combat cells immunotherapies, 1) utilize locally produced TME catalytically generate potent •OH other species; simultaneously, 2) external US irradiation can further boost generation 1 . This work provides not only critical evidence proposed peroxidases induce strong antitumor immune response memory also offers essential guidance creating high‐performance biocompatible strategy regulate immunosuppression enhance responses cancer.

Language: Английский

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