Dimensionality Engineering of Single-Atom Nanozyme for Efficient Peroxidase-Mimicking

Journal of the American Chemical Society, Год журнала: 2023, Номер 145(30), С. 16835 - 16842

Опубликована: Июль 24, 2023

In nature, enzymatic reactions occur in well-functioning catalytic pockets, where substrates bind and react by properly arranging the sites amino acids a three-dimensional (3D) space. Single-atom nanozymes (SAzymes) are new type of with active similar to those natural metalloenzymes. However, centers current SAzymes two-dimensional (2D) architectures lack collaborative substrate-binding features limits their activity. Herein, we report dimensionality engineering strategy convert conventional 2D Fe–N-4 into 3D structures integrating oxidized sulfur functionalities onto carbon plane. Our results suggest that could serve as binding for assisting substrate orientation facilitating desorption H2O, resulting an outstanding specific activity up 119.77 U mg–1, which is 6.8 times higher than FeN4C SAzymes. This study paves way rational design highly single-atom nanozymes.

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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Bioinspired porous three-coordinated single-atom Fe nanozyme with oxidase-like activity for tumor visual identification via glutathione

Nature Communications, Год журнала: 2023, Номер 14(1)

Опубликована: Ноя. 6, 2023

Inspired by structures of natural metalloenzymes, a biomimetic synthetic strategy is developed for scalable synthesis porous Fe-N3 single atom nanozymes (pFeSAN) using hemoglobin as Fe-source and template. pFeSAN delivers 3.3- 8791-fold higher oxidase-like activity than Fe-N4 Fe3O4 nanozymes. The high catalytic performance attributed to (1) the suppressed aggregation atomically dispersed Fe; (2) facilitated mass transfer maximized exposure active sites created mesopores thermal removal (2 ~ 3 nm); (3) unique electronic configuration oxygen-to-water oxidation pathway (analogy with cytochrome c oxidase). successfully demonstrated rapid colorimetric detection glutathione low limit (2.4 nM) wide range (50 nM-1 mM), further real-time, facile, (~6 min) precise visualization analysis methodology tumors via level, showing its potentials diagnostic clinic 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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Facile synthesis of 2D Al-TCPP MOF nanosheets for efficient sonodynamic cancer therapy

Materials Chemistry Frontiers, Год журнала: 2023, Номер 7(8), С. 1684 - 1693

Опубликована: Янв. 1, 2023

2D Al-TCPP MOF nanosheets were prepared via a simple solvothermal synthesis method without the need for any surfactants and found to be an effective sonosensitizer sonodynamic cancer therapy.

Язык: Английский

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Deep Insight of Design, Mechanism, and Cancer Theranostic Strategy of Nanozymes

Nano-Micro Letters, Год журнала: 2023, Номер 16(1)

Опубликована: Ноя. 21, 2023

Since the discovery of enzyme-like activity Fe

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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Precise Tuning of the D-Band Center of Dual-Atomic Enzymes for Catalytic Therapy

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(14), С. 10023 - 10031

Опубликована: Март 30, 2024

Single-atom nanozyme-based catalytic therapy is of great interest in the field tumor therapy; however, their development suffers from low affinity nanozymes to substrates (H2O2 or O2), leading deficient activity microenvironment. Herein, we report a new strategy for precisely tuning d-band center dual-atomic sites enhance metal atomic and on class edge-rich N-doped porous carbon Fe–Mn (Fe1Mn1–NCe) greatly boosting multiple-enzyme-like activities. The as-made Fe1Mn1–NCe achieved much higher efficiency (Kcat/Km = 4.01 × 105 S–1·M–1) than Fe1–NCe 2.41 104 with an outstanding stability over 90% retention after 1 year, which best among reported dual-atom nanozymes. Theoretical calculations reveal that synergetic effect Mn upshifts Fe −1.113 −0.564 eV enhances adsorption capacity substrate, thus accelerating dissociation H2O2 weakening O–O bond O2. We further demonstrated superior enzyme-like combined photothermal could effectively inhibit growth vivo, inhibition rate up 95.74%, highest value artificial enzyme therapies so far.

Язык: Английский

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Using Cu‐Based Metal–Organic Framework as a Comprehensive and Powerful Antioxidant Nanozyme for Efficient Osteoarthritis Treatment

Advanced Science, Год журнала: 2024, Номер 11(13)

Опубликована: Янв. 26, 2024

Abstract Developing nanozymes with effective reactive oxygen species (ROS) scavenging ability is a promising approach for osteoarthritis (OA) treatment. Nonetheless, numerous lie in their relatively low antioxidant activity. In certain circumstances, some of these may even instigate ROS production to cause side effects. To address challenges, copper‐based metal–organic framework (Cu MOF) nanozyme designed and applied OA Cu MOF exhibits comprehensive powerful activities (i.e., SOD‐like, CAT‐like, •OH activities) while negligible pro‐oxidant (POD‐ OXD‐like activities). Collectively, more at various types than other Cu‐based antioxidants, such as commercial CuO single‐atom nanozyme. Density functional theory calculations also confirm the origin its outstanding enzyme‐like activities. vitro vivo results demonstrate that an excellent decrease intracellular levels relieve hypoxic microenvironment synovial macrophages. As result, can modulate polarization macrophages from pro‐inflammatory M1 anti‐inflammatory M2 subtype, inhibit degradation cartilage matrix efficient The biocompatibility protective properties make it valuable asset treating ROS‐related ailments beyond OA.

Язык: Английский

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Synergistic Interaction between Metal Single‐Atoms and Defective WO_3−x Nanosheets for Enhanced Sonodynamic Cancer Therapy

Advanced Materials, Год журнала: 2024, Номер 36(23)

Опубликована: Фев. 27, 2024

Abstract Although metal single‐atom (SA)‐based nanomaterials are explored as sonosensitizers for sonodynamic therapy (SDT), they normally exhibit poor activities and need to combine with other therapeutic strategies. Herein, the deposition of SAs on oxygen vacancy (OV)‐rich WO 3− x nanosheets generate a synergistic effect efficient SDT is reported. Crystalline 3 OV‐rich first prepared by simple calcination ·H 2 O under an air N atmosphere, respectively. Pt, Cu, Fe, Co, Ni then deposited obtain SA‐decorated nanocomposites (M‐WO ). Importantly, Cu‐WO sonosensitizer exhibits much higher activity ultrasound (US)‐induced production reactive species than that Cu , which also M‐WO nanosheets. Both experimental theoretical results suggest excellent performance should be attributed between OVs. Therefore, after polyethylene glycol modification, can quickly kill cancer cells in vitro effectively eradicate tumors vivo US irradiation. Transcriptome sequencing analysis further molecular validation ‐mediated SDT‐activated apoptosis TNF signaling pathways potential drivers tumor induction.

Язык: Английский

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