Atomically Site Synergistic Effects of Dual-Atom Nanozyme Enhances Peroxidase-like Properties

Nano Letters, Год журнала: 2023, Номер 23(13), С. 6073 - 6080

Опубликована: Июнь 26, 2023

Pursuing effective and generalized strategies for modulating the electronic structures of atomically dispersed nanozymes with remarkable catalytic performance is exceptionally attractive yet challenging. Herein, we developed a facile "formamide condensation carbonization" strategy to fabricate library single-atom (M1-NC; 6 types) dual-atom (M1/M2-NC; 13 metal-nitrogen-carbon (M = Fe, Co, Ni, Mn, Ru, Cu) reveal peroxidase- (POD-) like activities. The Fe1Co1-NC nanozyme Fe1-N4/Co1-N4 coordination displayed highest POD-like activity. Density functional theory (DFT) calculations revealed that Co atom site synergistically affects d-band center position Fe served as second reaction center, which contributes better Finally, Fe1Co1 NC was shown be in inhibiting tumor growth both vitro vivo, suggesting diatomic synergy an developing artificial novel nanocatalytic therapeutics.

Язык: Английский

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Biomedicine meets nanozyme catalytic chemistry

Coordination Chemistry Reviews, Год журнала: 2023, Номер 491, С. 215245 - 215245

Опубликована: Май 22, 2023

Язык: Английский

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Recent advances in the development and analytical applications of oxidase-like nanozymes

TrAC Trends in Analytical Chemistry, Год журнала: 2023, Номер 166, С. 117220 - 117220

Опубликована: Авг. 3, 2023

Язык: Английский

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Copper Single-Atom Jellyfish-like Nanomotors for Enhanced Tumor Penetration and Nanocatalytic Therapy

ACS Nano, Год журнала: 2023, Номер 17(7), С. 6789 - 6799

Опубликована: Март 29, 2023

Single-atom catalysts with extraordinary catalytic activity have been receiving great attention in tumor therapy. However, most single-atom lack self-propulsion properties, restricting them from actively approaching cancer cells or penetrating the interior of tumors. Herein, we design N-doped jellyfish-like mesoporous carbon nanomotors coordinated copper (Cu-JMCNs). It is a combination nanocatalytic medicine and nanomotor for The Cu single atom can catalyze H2O2 into toxic hydroxyl radical (•OH) chemodynamic therapy (CDT). Near-infrared light triggers Cu-JMCNs to achieve self-thermophoretic motion because asymmetric structure photothermal property carbon, which significantly improves cellular uptake penetration three-dimensional In vivo experiments indicate that CDT near-infrared propulsion over 85% inhibition rate. This work sheds on development advanced biomedical applications.

Язык: Английский

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Spatial Position Regulation of Cu Single Atom Site Realizes Efficient Nanozyme Photocatalytic Bactericidal Activity

Advanced Materials, Год журнала: 2023, Номер 35(46)

Опубликована: Июль 27, 2023

Recently, single-atom nanozymes have made significant progress in the fields of sterilization and treatment, but their catalytic performance as substitutes for natural enzymes drugs is far from satisfactory. Here, a method reported to improve enzyme activity by adjusting spatial position site on nanoplatforms. Two types Cu are synthesized interlayer (CuL /PHI) in-plane (CuP poly (heptazine imide) (PHI) through different synthesis pathways. Experimental theoretical analysis indicates that PHI can effectively adjust coordination number, bond length, electronic structure single atoms compared position, thereby promoting photoinduced electron migration O2 activation, enabling effective generate reactive oxygen species (ROS). Under visible light irradiation, photocatalytic bactericidal CuL /PHI against aureus ≈100%, achieving same antibacterial effect antibiotics, after 10 min low-dose exposure 2 h incubation.

Язык: Английский

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Single‐Atom Nanozymes for Catalytic Therapy: Recent Advances and Challenges

Advanced Functional Materials, Год журнала: 2024, Номер 34(16)

Опубликована: Янв. 4, 2024

Abstract As a powerful tool, nanozyme catalysts broaden the avenues to implement bio‐inspired solutions for addressing many important concerns, covering energy, healthcare, environment, and more. Recent endeavors, characterized by atomic precision, have enabled extensive exploration of single‐atom nanozymes (SAzymes) with high catalytic activity, superior substrate selectivity, integrated multifunctionalities, thus becoming an emerging field that bridges nanotechnology biology. This review provides brief outline progress summarizes latest research advances regarding SAzymes in biomedical therapeutics, mainly including tumor therapy, wound antibacterial tissue anti‐inflammatory focus on their prototypical synthesis therapeutic mechanisms. Finally, current challenges future perspectives engineering advanced are also discussed outlooked. It is anticipated this area shall provide useful guidance therapy.

Язык: Английский

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Boosting Ferroptosis Therapy with Iridium Single‐Atom Nanocatalyst in Ultralow Metal Content

Advanced Materials, Год журнала: 2023, Номер 35(17)

Опубликована: Янв. 31, 2023

Nanocatalysts are promising tumor therapeutics due to their ability induce reactive oxygen species in the microenvironment. Although increasing metal loading can improve catalytic activity, quandary of high content versus potential systemic biotoxicity remains challenging. Here, a fully exposed active site strategy by site-specific anchoring single iridium (Ir) atoms on outer surface nitrogen-doped carbon composite (Ir single-atom catalyst (SAC)) is reported achieve remarkable performance at ultralow (≈0.11%). The Ir SAC exhibits prominent dual enzymatic activities mimic peroxidase and glutathione peroxidase, which catalyzes conversion endogenous H2 O2 into •OH acidic TME depletes (GSH) simultaneously. With an advanced support GSH-trapping platinum(IV) encapsulation with red-blood-cell membrane, this nanocatalytic agent (Pt@IrSAC/RBC) causes intense lipid peroxidation that boosts cell ferroptosis. Pt@IrSAC/RBC demonstrates superior therapeutic efficacy mouse triple-negative mammary carcinoma model, resulting complete ablation treatment session negligible side effects. These outcomes may provide valuable insights design nanocatalysts biosafety for biomedical applications.

Язык: Английский

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Single-Site Nanozymes with a Highly Conjugated Coordination Structure for Antitumor Immunotherapy via Cuproptosis and Cascade-Enhanced T Lymphocyte Activity

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(6), С. 3675 - 3688

Опубликована: Фев. 2, 2024

The extracellular matrix (ECM) in the tumor microenvironment (TME) and upregulated immune checkpoints (ICs) on antitumor cells impede infiltration killing effect of T cells, creating an immunosuppressive TME. Herein, a cholesterol oxidase (CHO) lysyl inhibitor (LOX-IN-3) co-delivery copper-dibenzo-[g,p]chrysene-2,3,6,7,10,11,14,15-octaol single-site nanozyme (Cu-DBCO/CL) was developed. conjugated organic ligand well-distributed Cu-O4 sites endow Cu-DBCO with unique redox capabilities, enabling it to catalyze O2 H2O2 ·O2– ·OH. This surge reactive oxygen species (ROS) leads impaired mitochondrial function insufficient ATP supply, impacting copper-transporting ATPase-1 causing dihydrolipoamide S-acetyltransferase oligomerization-mediated cuproptosis. Moreover, multiple ROS storms glutathione peroxidase 4 depletion also induce lipid peroxidation trigger ferroptosis. Simultaneously, ROS-triggered release LOX-IN-3 reshapes ECM by inhibiting activity further enhances cytotoxic lymphocytes (CD8+ cells). CHO-triggered not only increases ·OH generation but downregulates expression ICs such as PD-1 TIM-3, restoring tumor-infiltrating CD8+ cells. Therefore, Cu-DBCO/CL exhibits efficient properties activating potent response cascade-enhanced cell viability. More importantly, remodeling could suppress metastasis proliferation In short, this nanoremodeler can greatly enhance enhancing immunogenicity, ECM, downregulating ICs, thus achieving effective inhibition growth metastasis.

Язык: Английский

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Programmed Targeting Pyruvate Metabolism Therapy Amplified Single‐Atom Nanozyme‐Activated Pyroptosis for Immunotherapy

Advanced Materials, Год журнала: 2024, Номер 36(24)

Опубликована: Фев. 7, 2024

Abstract Increasing cellular immunogenicity and reshaping the immune tumor microenvironment (TME) are crucial for antitumor immunotherapy. Herein, this work develops a novel single‐atom nanozyme pyroptosis initiator: UK5099 pyruvate oxidase (POx)‐co‐loaded Cu‐NS (Cu‐NS@UK@POx), that not only trigger through cascade biocatalysis to boost of cells, but also remodel immunosuppressive TME by targeting metabolism. By replacing N with weakly electronegative S, original spatial symmetry Cu‐N 4 electron distribution is changed enzyme‐catalyzed process effectively regulated. Compared spatially symmetric nanozymes (Cu‐N SA), S‐doped asymmetric (Cu‐NS SA) exhibit stronger activities, including peroxidase (POD), nicotinamide adenine dinucleotide (NADH) (NOx), L ‐cysteine (LCO), glutathione (GSHOx), which can cause enough reactive oxygen species (ROS) storms pyroptosis. Moreover, synergistic effect SA, UK5099, POx target metabolism, improves increases degree This study provides two‐pronged treatment strategy significantly activate immunotherapy effects via ROS storms, NADH/glutathione/ consumption, oxidation, lactic acid (LA)/ATP depletion, triggering regulating broad vision expanding

Язык: Английский

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Single-Atom Nanozymes: From Precisely Engineering to Extensive Applications

Accounts of Materials Research, Год журнала: 2024, Номер 5(3), С. 347 - 357

Опубликована: Фев. 3, 2024

ConspectusNanozymes are nanomaterials with intrinsic enzyme-like properties that can overcome the current limitations of natural enzymes, such as high preparation cost, instability, restricted application scenarios, etc. Since Fe3O4 nanoparticles (NPs) were shown to possess peroxidase (POD)-like activity in 2007, thousands reported mimic catalytic various types enzymes including catalase (CAT), haloperoxidase, superoxide dismutase (SOD), glucose oxidase, glutathione peroxidase, hydrolase, nuclease, nitroreductase, and others. Particularly, some nanozymes showed multienzyme-like activities regarding changes scenarios temperature, pH, Benefiting from their distinct physical-chemical characteristics properties, have been widely applied biomedical related fields vitro detections vivo therapeutic treatments. However, currently ambiguous structure–function correlations relatively inferior compared promote extensive efforts for modifications on development novel alternative nanozymes. The single-atom (SAzymes) present a unique way highly evolved enzyme active centers, because atomically dispersed sites, which leads atom utilization efficiency and, thus, potentially extraordinary activity. Also, abilities modify centers and/or tune interactions between metal supporting ligands provide precise engineer SAzymes at atomic levels. Given well-defined geometric electronic structures, thus serve exceptional templates deciphering relationships, is beneficial further improving performances.In this Account, we will review our recent other notable works developments effective mimics applications areas. We begin brief introduction why emergence SAzymes, artificial enzyme, tackles challenges facing. Next, focus systematic design, synthesis optimization especially impacts engineering environment an enzymologist perspective. For example, alternations first-shell ligand N P/S, SAzymes' CAT-like increased more than 4-fold. coordination numbers (x) Co–Nx(C) SAzyme significantly altered its oxidase (OXD)-like kinetics Then, discuss ways standardization specific kinetics. also wide ranges colorimetric biologicals, antibiosis treatments, cancer therapies. Finally, address future perspectives

Язык: Английский

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