Narrow-Bandgap Iridium(III)-C₃N₅ Nanocomplex as an Oxygen Self-Sufficient Piezo-Sonosensitizer for Hypoxic Tumor Sonodynamic Immunotherapy

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

Опубликована: Апрель 28, 2025

Low immunogenicity and insufficient infiltration of immune cells are the main factors affecting therapeutic efficacy melanoma immunotherapy. Ultrasound-triggered sonodynamic therapy (SDT) based on piezoelectric materials has attracted substantial attention due to its high efficiency catalytic generation reactive oxygen species (ROS) induce immunogenic cell death (ICD). However, hypoxic environment in solid tumors hinders limits SDT effect. Herein, we construct a novel Ir-C3N5 nanocomplex that uses nitrogen-rich carbon nitride (C3N5) nanosheets as nanoligands Ir(tpy)Cl3 precursor. The newly formed exhibits narrowed band gap an enlarged dipole moment, resulting better electron-hole pair separation bending, contributing ROS burst upon ultrasonic activation. In addition, Ir(III) enables C3N5 catalyze degradation H2O2 O2, alleviating tumor hypoxia reinforcing efficacy. Mechanistically, by catalysis, can target lysosomes trigger autophagy inhibition caused lysosome rupture evoke pyroptosis. More importantly, cleaved caspase-1/GSDMD-N pyroptosis pathway activated was associated with ICD, effectively initiating innate adaptive immunity body for suppressing metastasis relapse.

Язык: Английский

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Unveiling Mechanically Driven Catalytic Processes: Beyond Piezocatalysis to Synergetic Effects

ACS Nano, Год журнала: 2025, Номер unknown

Опубликована: Май 6, 2025

Mechanically driven catalysis (MDC) has emerged as an effective strategy for environmental remediation, renewable energy conversion, and cancer therapy; this functions by converting mechanical forces to drive catalytic reactions. This review examines four primary mechanisms, namely, piezocatalysis, flexocatalysis, tribocatalysis, sonocatalysis, each involving specific pathways harnessing at the nanoscale. However, significant challenges arise in decoupling effects related individual mechanism order better understand manipulate their synergies. In review, fundamental principles underpinning MDC are systematically interpreted. Beyond mechanistic insights, recent advancements performance enhancement strategies these catalysts highlighted. Potential applications using approaches remediation (pollutant antibiotic degradation microbial disinfection), conversion (hydrogen production greenhouse gas conversion), biomedical treatments (particularly therapy) discussed. Finally, synergies limiting factors explored, addressing overlooked combined of ultrasound activation source, complexities force interactions nanoscale, need targeted application strategies. Additionally, industrial potential processes with consideration scalability practical deployment is evaluated. While remain, provides a roadmap advancing mechanically catalyst design implementation toward real-world applications, offering into its future trajectory transformative impact across numerous fields.

Язык: Английский

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Accelerated C-F bond cleavage on sulfur vacancy-contained CoS2/MoS2 electrode featuring rich H*

Journal of Hazardous Materials, Год журнала: 2025, Номер 494, С. 138566 - 138566

Опубликована: Май 15, 2025

Язык: Английский

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In-situ synthesis of Zn ion-implanted ZIF-67-derived sulfide CoS2 for advanced supercapacitor applications

Journal of Electroanalytical Chemistry, Год журнала: 2025, Номер unknown, С. 119203 - 119203

Опубликована: Май 1, 2025

Язык: Английский

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Piezoelectric catalysts for water pollutant remediation: Achievements, challenges, and perspectives

Materials Today, Год журнала: 2025, Номер unknown

Опубликована: Май 1, 2025

Язык: Английский

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Assisting a Type-II Heterojunction with the LSPR Effect for Realizing Photocatalytic Hydrogen Peroxide Evolution with NIR Apparent Quantum Efficiency Exceeding 0.5%

Nano Letters, Год журнала: 2025, Номер unknown

Опубликована: Май 21, 2025

Designing heterojunction catalysts for the production of hydrogen peroxide is a crucial strategy advancing field artificial photosynthesis. However, conventional type-II often face challenges weak redox ability and utilization charge carriers. Herein, distinct proposed that combines heterojunctions with localized surface plasmon resonance (LSPR) effect, thereby cooperatively enhancing high-energy electrons through hot electron injection process. The optimized catalyst MoO3-x-ZnIn2S4 (VMZS) exhibits H2O2 (47.2 μmol g-1 min-1) under simulated sunlight (AM1.5G, 100 mW cm-2) filter (λ > 350 nm) an apparent quantum efficiency 0.5% at 940 nm, significantly exceeding previously reported state-of-the-art catalysts. Moreover, prepared film VMZS enables rate 338.1 μM h-1. This work provides new insight on designing systems synergistic contribution carrier transfer route LSPR effect.

Язык: Английский

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NIR‐II‐Responsive Chainmail Nanocatalysts for Spatiotemporally Controlled Enzymatic Tumor Therapy

Advanced Healthcare Materials, Год журнала: 2025, Номер unknown

Опубликована: Май 20, 2025

Abstract The clinical translation of metal‐based peroxidase‐like nanozymes for antitumor therapy faces two critical challenges: off‐target catalytic activation and suboptimal hydroxyl radical (•OH) generation efficiency. To address these limitations, an innovative chainmail nanocatalyst featuring nitrogen‐doped carbon‐encapsulated nanoceria is developed, which combines spatial confinement effects with photo‐trigger enhancement. graphitic carbon shell serves as a physical barrier that effectively isolates metallic cerium from the biological environment, reducing nonspecific by 100% compared to bare nanoceria. Remarkably, under 1064 nm laser irradiation, electrons species can penetrate through quantum tunneling effects, activating multiple enzymatic pathways. Vacancy engineering further optimizes Ce 3+ /Ce 4+ redox pair ratio (1.75 vs 0.44 in pristine nanoceria), establishing electron reservoir facilitates amplification H 2 O ‐to‐•OH conversion glutathione oxidase‐mimicking activity tumor microenvironment remodeling. This dual mechanism synergistically elevates intracellular oxidative stress while preserving normal tissue viability. In vivo evaluations demonstrate photoactivated exhibits remarkable suppression efficacy, prolonging survival duration tumor‐bearing mice 33 days 70 days. light‐gated architecture provides paradigm spatiotemporally controlled therapy, resolving dilemma between potency specificity nanozyme design.

Язык: Английский

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A Needle‐Like H₂S‐Releasing and H₂O₂ Self‐Replenishing Nanoplatform for Enhanced Chemodynamic Tumor Immunotherapy

Advanced Science, Год журнала: 2025, Номер unknown

Опубликована: Май 22, 2025

Abstract The tumor microenvironment (TME) significantly restricts chemodynamic therapy (CDT) efficacy through hypoxia and antioxidant defenses. An intelligent cascade nanosystem, PTA‐SnS 2 @GOx, is developed by integrating a tannic acid‐modified Prussian blue analogue core, SnS shell, glucose oxidase (GOx) activation module. needle‐like nanostructure enhanced accumulation cellular uptake. GOx‐mediated oxidation generated H O gluconic acid, triggering pH‐responsive S release from . This gas disrupted mitochondrial respiration catalase activity, alleviating while elevating intracellular levels. oxygenated TME subsequently amplified GOx biocatalysis, establishing self‐sustaining cycle of production acidification. Concurrently, Sn 4+ ions depleted glutathione, synergistically enhancing Fenton‐like reactions in the PTA core for reinforced ROS generation. multi‐tiered strategy achieved effective CDT coordinated mechanisms: continuous self‐supply, pH reduction, redox homeostasis disruption. Notably, nanosystem induced immunogenic cell death, promoting dendritic maturation repolarizing tumor‐associated macrophages M2 to M1 phenotype, thereby remodeling immunosuppressive activating systemic antitumor immunity. synergistic integration self‐amplifying with immune sensitization demonstrates superior suppression vivo. study provided an paradigm cancer theranostics combining self‐supplying S/H ‐enhanced sensitized immunotherapy.

Язык: Английский

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Augmenting Antioxidant Enzyme‐Like Activity and Hydrogen Evolution of MoS₂@Bi₂S₃ Heterojunction via Ultrasound‐Evoked Piezoelectricity for Anti‐Inflammation

Small, Год журнала: 2025, Номер unknown

Опубликована: Май 23, 2025

Abstract Inorganic piezoelectric biomaterials exhibit significant potential for diverse biomedical applications, yet their limited effect has hindered broader utilization. To address this challenge, the study successfully fabricates a heterojunction MoS 2 @Bi S 3 with exceptional properties through doping engineering. Comprehensive studies reveal that efficiently converts mechanical energy into electrical energy, facilitates hydrogen (H ) evolution, and enhances antioxidant enzyme‐like performances under ultrasonic irradiation. Moreover, GSH GSSG switch cycle is established during piezocatalytic process, which conducive to augment piezoelectricity of in biological environment. Further investigations demonstrate deformation significantly reduced free required •OH adsorption, thereby dramatically enhancing its scavenging ability. Both experimental theoretical results verify narrowed bandgap or without deformation, indicating alteration fundamentally responsible enhanced effect, properties, H evolution. Capitalizing on capability itself, developed exhibits anti‐inflammation activity both vitro vivo, suggesting treatment rheumatoid arthritis other inflammatory diseases.

Язык: Английский

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Antimony Component Schottky Nanoheterojunctions as Ultrasound‐Heightened Pyroptosis Initiators for Sonocatalytic Immunotherapy

Angewandte Chemie, Год журнала: 2024, Номер unknown

Опубликована: Сен. 21, 2024

Abstract Pyroptosis, an inflammatory modality of programmed cell death associated with the immune response, can be initiated by bioactive ions and reactive oxygen species (ROS). However, ion‐induced pyroptosis lacks specificity, further exploration other that induce in cancer cells is needed. Sonocatalytic therapy (SCT) holds promise due to its exceptional penetration depth; however, rapid recombination electron‐hole (e − ‐h + ) pairs complex tumor microenvironment (TME) impede broader application. Herein, we discovered antimony (Sb)‐based nanomaterials induced cells. Therefore, Schottky heterojunctions containing Sb component (Sb 2 Se 3 @Pt) were effectively designed constructed via situ growth platinum (Pt) nanoparticles (NPs) on semiconductor narrow band gaps, which utilized as US‐heightened initiators highly effective boost SCT‐immunotherapy. Under US irradiation, excited electrons transferred from nanorods (NRs) co‐catalyst Pt junctions, bending prevented electron backflow achieved efficient ROS generation. Moreover, pores oxidized depleted overexpressed GSH TME, potentially amplifying The biological effects @Pt nanoheterojunction itself combined sonocatalytic amplification oxidative stress significantly Caspase‐1/GSDMD‐dependent SCT treatment not only restrained proliferation but also potent memory responses suppressed recurrence. Furthermore, integration this innovative strategy checkpoint blockade (ICB) elicited a systemic augmenting therapeutic impeding abscopal tumors. Overall, study provides opportunities explore pyroptosis‐mediated

Язык: Английский

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