Tailored Metal‐Organic Framework‐Based Nanozymes for Enhanced Enzyme‐Like Catalysis

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

Published: Nov. 19, 2024

Abstract The global crisis of bacterial infections is exacerbated by the escalating threat microbial antibiotic resistance. Nanozymes promise to provide ingenious solutions. Here, we reported a homogeneous catalytic structure Pt nanoclusters with finely tuned metal–organic framework (ZIF‐8) channel structures for treatment infected wounds. Catalytic site normalization showed that active aggregates fine‐tuned pore modifications had capacity 14.903×10 5 min −1 , which was 18.7 times higher than particles in monodisperse state ZIF‐8 (0.793×10 ). In situ tests revealed change from homocleavage heterocleavage hydrogen peroxide at interface nanozyme one key reasons improvement activity. Density‐functional theory and kinetic simulations reaction jointly determine role center substrate together. Metabolomics analysis developed nanozyme, working conjunction reactive oxygen species, could effectively block energy metabolic pathways within bacteria, leading spontaneous apoptosis rupture. This pioneering study elucidates new ideas regulation artificial enzyme activity provides perspectives development efficient substitutes.

Language: Английский

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Surface Engineering‐Induced d‐Band Center Down‐Regulation in High‐Entropy Alloy Nanowires for Enhanced Nanozyme Catalysis

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

Published: April 7, 2025

Abstract High‐entropy alloys (HEAs) have garnered extensive attention owing to their broad compositional tunability and high catalytic activity. However, precisely modulating the enzyme‐like activity of HEAs enhancing biocompatibility for biological applications remain severely challenging. Herein, PtRuFeCoNi HEA nanowires (NWs) are synthesized by adjusting metal composition surface‐engineered with polydopamine (PDA) form NWs@PDA nanozymes (HEzymes@PDA) superior photothermal properties. Density functional theory calculations Sabatier principle reveal that self‐polymerized PDA surface engineering moderately lowers d‐band center HEAs, optimizes charge distribution, enhances adsorption–desorption efficiency substrates. As a proof‐of‐concept, HEzymes@PDA synergistically integrated hydrogels biosensing analysis. This study presents an innovative paradigm designing highly active via demonstrates immense potential in sensing applications.

Language: Английский

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High-Performance Biosensing Platforms Based on Enzyme-Linked Nucleic Acid Amplification Regulated by Synergistic Allosteric Hairpin Catalysis of Bimetallic Nanozymes and Its Mechanisms

Analytical Chemistry, Journal Year: 2025, Volume and Issue: unknown

Published: April 7, 2025

Sugar cane smut disease can greatly decrease both the production and quality of sugar cane, its early diagnosis is an effective strategy to ensure increase income cane. Therefore, developing high-precision detection methods has major implications for actual Herein, we synthesize bimetallic nanozymes Fe3O4@AuNPs with excellent glucose oxidase-like activity nitrogen-doped graphdiyne (N-GDY) conductivity interfacial loading capacity, which are used as catalysts biofuel cells flexible electrode substrates, respectively. An allosteric hairpin-regulated enzymatic cascade nucleic acid amplification employed construct a novel biosensing platform precise highly sensitive analysis pathogen causing disease, catalytic mechanism studied. The specifically cause complementary region hairpin migrate form new functional hairpin. Under promotion enzymes, dual occurs using template outputs large amount double-stranded products, captured by RCA long chain on biocathode. At cathode, DNA double strands capable holding quantity Ru[(NH3)6]3+ through electrostatic attraction. anode catalyze oxidation produce electrons, AuNPs/N-GDY efficiently transfer electrons cathode obtain strong open-circuit voltage signal, exhibits linear correlation in range 0.0001-10000 pM, limit 53.29 aM (S/N = 3). sensing offers reliable method that allows accurate great application development potential identification on-site rapid detection.

Language: Английский

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Cell-Inspired Microreactor with Compartmentalized Active Sites for Development of Cascade Catalysis System in Biosensing

Analytical Chemistry, Journal Year: 2024, Volume and Issue: 96(47), P. 18736 - 18744

Published: Nov. 13, 2024

Enzymatic cascade reactions with high activity and specificity in living cells always benefit from multicompartmentalized organelles that provide separately confined spaces for enzymes, avoiding their mutual interference to ensure the high-efficiency operation of necessary vital movements. Inspired by this, we designed a 3D spherical microreactor (Au@H-APF@Pt) biomimetic catalysis glucose detection. First, ultrasmall gold nanoparticles were immobilized situ on internal cavities hollow 3-aminophenol formaldehyde resin (H-APF) nanospheres, along oxidase activity. Then, platinum (PtNPs) peroxide-like reduced surrounding outer layer H-APF nanospheres. Similar cell structure, different metal sites this bifunctional operated independently, bringing higher catalytic selectivity thus being synergistically capable reaction catalyze substrate This cell-mimicking was successfully applied colorimetric detection, showing 1.9-fold enhancement compared direct mixing (Au/Pt). The observed low attributed extended time transferring hydrogen peroxide (H

Language: Английский

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