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

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(14), P. 10023 - 10031

Published: March 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.

Language: Английский

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Single-Atom-Based Nanoenzyme in Tissue Repair

ACS Nano, Journal Year: 2024, Volume and Issue: 18(20), P. 12639 - 12671

Published: May 8, 2024

Since the discovery of ferromagnetic nanoparticles Fe3O4 that exhibit enzyme-like activity in 2007, research on nanoenzymes has made significant progress. With in-depth study various and rapid development related nanotechnology, have emerged as a promising alternative to natural enzymes. Within nanozymes, there is category metal-based single-atom nanozymes been rapidly developed due low cast, convenient preparation, long storage, less immunogenicity, especially higher efficiency. More importantly, possess capacity scavenge reactive oxygen species through mechanisms, which beneficial tissue repair process. Herein, this paper systemically highlights types metal their catalytic recent applications repair. The existing challenges are identified prospects future composed metallic nanomaterials proposed. We hope review will illuminate potential repair, encouraging sequential clinical translation.

Language: Английский

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Multi‐Enzyme Mimetic MoCu Dual‐Atom Nanozyme Triggering Oxidative Stress Cascade Amplification for High‐Efficiency Synergistic Cancer Therapy

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 64(1)

Published: Aug. 22, 2024

Single-atom nanozymes (SAzymes) with ultrahigh atom utilization efficiency have been extensively applied in reactive oxygen species (ROS)-mediated cancer therapy. However, the high energy barriers of reaction intermediates on single-atom sites and overexpressed antioxidants tumor microenvironment restrict amplification oxidative stress, resulting unsatisfactory therapeutic efficacy. Herein, we report a multi-enzyme mimetic MoCu dual-atom nanozyme (MoCu DAzyme) various catalytic active sites, which exhibits peroxidase, oxidase, glutathione (GSH) nicotinamide adenine dinucleotide phosphate (NADPH) oxidase mimicking activities. Compared Mo SAzyme, introduction Cu atoms, formation synergetic effects among enhance substrate adsorption reduce barrier, thereby endowing DAzyme stronger Benefiting from above enzyme-like activities, can not only generate multiple ROS, but also deplete GSH block its regeneration to trigger cascade stress. Additionally, strong optical absorption near-infrared II bio-window endows remarkable photothermal conversion performance. Consequently, achieves high-efficiency synergistic treatment incorporating collaborative therapy This work will advance applications DAzymes provide valuable insights for nanocatalytic

Language: Английский

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Rational Design of Nanozymes for Engineered Cascade Catalytic Cancer Therapy

Chemical Reviews, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 27, 2025

Nanozymes have shown significant potential in cancer catalytic therapy by strategically catalyzing tumor-associated substances and metabolites into toxic reactive oxygen species (ROS) situ, thereby inducing oxidative stress promoting cell death. However, within the complex tumor microenvironment (TME), rational design of nanozymes factors like activity, reaction substrates, TME itself significantly influence efficiency ROS generation. To address these limitations, recent research has focused on exploring that affect activity developing nanozyme-based cascade systems, which can trigger two or more processes tumors, producing therapeutic achieving efficient stable with minimal side effects. This area remarkable progress. Perspective provides a comprehensive overview nanozymes, covering their classification fundamentals. The regulation nanozyme strategies are discussed detail. Furthermore, representative paradigms for successful construction systems treatment summarized focus revealing underlying mechanisms. Finally, we current challenges future prospects development biomedical applications.

Language: Английский

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Tuning Atomically Dispersed Metal Sites in Nanozymes for Sensing Applications

Angewandte Chemie International Edition, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 12, 2025

Abstract Nanozymes with atomically dispersed metal sites (ADzymes), especially single‐atom nanozymes, have attracted widespread attention in recent years due to their unique advantages mimicking the active of natural enzymes. These nanozymes not only maximize exposure catalytic but also possess superior activity performance, achieving challenging reactions. position ADzymes as highly promising candidates field sensing and biosensing. This review summarizes classification properties ADzymes, systematically highlighting some typical regulation strategies involving central metal, coordination environment, etc., achieve catalytical activity, specificity, multifunctionality. Then, we present advances different fields, including colorimetry, fluorescence, electrochemistry, chemiluminescence, photoelectrochemistry, electrochemiluminescence. Taking advantage resultant show great potential goal sensitivity, selectivity accuracy for detection various targets. Specifically, underlying mechanisms terms signal amplification were discussed detail. Finally, current challenges perspectives on development advanced are discussed.

Language: Английский

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Heteroatoms Modulate the Copper Single Atom Catalytic Host Materials for Promoting the Redox Reaction in Aqueous Zinc‐Selenium Batteries

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

Published: Oct. 18, 2024

Abstract Aqueous zinc‐selenium (Zn‐Se) batteries have garnered much attention due to their inherent safety and high specific capacity. Unfortunately, the problem of sluggish redox reaction represents a significant obstacle development aqueous Zn‐Se batteries. Here, nitrogen‐phosphorus asymmetrically coordinated copper single atom catalytic host material (CuN 3 P 1 @C) is synthesized for an battery. The CuN @C exhibits rich porous structure, high‐loading Cu atoms, unique asymmetric coordination environment, which significantly reduces energy barrier between Se Zn, enhancing electrochemical performance Consequently, Se/CuN cathode achieves capacity 756 mAh g −1 at 0.2 A cycling stability 4 000 cycles 5.0 (capacity decay 0.0044% per cycle). Meanwhile, conversion mechanism battery systematically explored via systematical characteristics density functional theory calculations. This work opens up novel approach boosting by modulating atom‐based materials heteroatoms.

Language: Английский

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Nitrogen Vacancy Modulation of Tungsten Nitride Peroxidase-Mimetic Activity for Bacterial Infection Therapy

ACS Nano, Journal Year: 2024, Volume and Issue: 18(35), P. 24469 - 24483

Published: Aug. 22, 2024

Bacterial infections claim millions of lives every year, with the escalating menace microbial antibiotic resistance compounding this global crisis. Nanozymes, poised as prospective substitutes for antibiotics, present a significant frontier in antibacterial therapy, yet their precise enzymatic origins remain elusive. With continuous development nanozymes, applications elemental N-modulated nanozymes have spanned multiple fields, including sensing and detection, infection cancer treatment, pollutant degradation. The introduction nitrogen into not only broadens application range but also holds importance design catalysts biomedical research. synergistic interplay between W N induces pivotal alterations electronic configurations, endowing tungsten nitride (WN) peroxidase-like functionality. Furthermore, vacancies augments nanozyme activity, thus amplifying catalytic potential WN nanostructures. Rigorous theoretical modeling empirical validation corroborate genesis enzyme activity. meticulously engineered nanoflower architecture exhibits an exceptional ability traversing bacterial surfaces, exerting potent bactericidal effects through direct physical interactions. Additionally, topological intricacies these nanostructures facilitate targeting generated radicals on culminating efficacy against both Gram-negative Gram-positive strains along notable inhibition biofilm formation. Importantly, assessments using skin model underscore proficiency nanoflowers effectively clearing fostering wound healing. This pioneering research illuminates realm pseudoenzyme activity capture-killing strategies, promising fertile ground innovative, high-performance artificial peroxidases.

Language: Английский

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Asymmetrically Coordinated Cu Dual‐Atom‐Sites Enables Selective CO₂ Electroreduction to Ethanol

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

Published: Oct. 6, 2024

Abstract Electrochemical reduction of CO 2 (CO RR) to value‐added liquid fuels is a highly attractive solution for carbon‐neutral recycling, especially C 2+ products. However, the selectivity control preferable products great challenge due complex multi‐electron proton transfer process. In this work, series Cu atomic dispersed catalysts are synthesized by regulating coordination structures optimize RR selectivity. ‐SNC catalyst with uniquely asymmetrical coordinated CuN ‐CuNS site shows high ethanol selective FE 62.6% at −0.8 V versus RHE and 60.2% 0.9 in H‐Cell Flow‐Cell test, respectively. Besides, nest‐like structure beneficial mass process selection catalytic situ experiments theory calculations reveal reaction mechanisms such ethanol. The S atoms weaken bonding ability adjacent carbon atom, which accelerates from *CHCOH generate *CHCHOH, resulting This work indicates promising strategy rational design asymmetrically single, dual, or tri‐atom provides candidate material produce

Language: Английский

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Coordination engineering of FeCo dual single-atom nanozymes with photothermal-enhanced cascaded catalysis for efficient pancreatic cancer immunotherapy

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 496, P. 154203 - 154203

Published: July 21, 2024

Language: Английский

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A Core-Shell Confinement Strategy Towards Single-Atom Fe-N/S-C Bifunctional Catalyst for Selective Nitroarene Reduction and Olefin Epoxidation

Journal of Alloys and Compounds, Journal Year: 2025, Volume and Issue: 1012, P. 178488 - 178488

Published: Jan. 1, 2025

Language: Английский

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