Reprogram Local Electronic Configuration in Multicomponent Covalent–Organic Frameworks for Efficient Hydrogen Peroxide Photoproduction

Chemistry of Materials, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 19, 2025

Covalent organic frameworks (COFs) have recently demonstrated significant potential for photocatalysis. Optimizing the local electronic environment in COFs has been considered to be critical enhancing photocatalytic activity. Here, we report a one-pot "grafting-to" strategy reprogram configurations of series isoreticular multicomponent by introducing electron-donating or electron-withdrawing groups into pores transform photoinert photoactive and form intramolecular donor–acceptor (D-A) structures. Such D-A structures enhanced overall hydrogen peroxide photoproduction facilitating charge carrier separation optimizing band achieve oxygen reduction reaction water oxidation simultaneously. Notably, one incorporated with 2-aminothiazole exhibits production rate 3701 μmol g–1 h–1 solar-to-chemical conversion efficiency 0.13% without use any sacrificial reagents, it 100% bacterial killing rates remarkable >90% biofilm removal capability. This COF modification strategy, which not reported before, offers unique approach constructing highly active photocatalysts containing great future design antibacterial therapies.

Language: Английский

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Porphyrin-Based Covalent Organic Framework Encapsulating Multiwalled Carbon Nanotubes: A High-Performance Electrocatalyst for Oxygen Reduction Reaction

Langmuir, Journal Year: 2025, Volume and Issue: unknown

Published: April 17, 2025

The development of efficient and cost-effective oxygen reduction reaction (ORR) catalysts is crucial for advancing fuel cell technologies, given the limitations platinum-based catalysts. Here, we present a novel nanocomposite, cobalt-based porphyrinic covalent organic framework wrapped on multiwalled carbon nanotubes (Co-pCOF@MWCNTs), synthesized via template-directed in situ polymerization. This composite combines high porosity tunable catalytic properties COFs with excellent electrical conductivity MWCNTs. Co-pCOF@MWCNT demonstrates superior ORR activity, exhibiting an onset potential (Eonset) 0.86 V vs RHE 0.1 M KOH, surpassing performance its individual components (Co-pCOF MWCNT) other related materials. enhanced efficiency attributed to synergistic interactions between conductive MWCNT scaffold active COF nanolayers, which facilitate charge transfer increase site exposure. Furthermore, nanocomposite exhibits stability methanol tolerance, establishing as cathodic material cells. work highlights promise integrating materials opens new avenues design advanced energy conversion applications.

Language: Английский

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Bacteriophage-like Nanobiocatalysts with Spiky Topography and Dual-Atom Sites for Treating Drug-Resistant Bacteria

ACS Nano, Journal Year: 2024, Volume and Issue: unknown

Published: Sept. 12, 2024

Overuse of antibiotics leads to the proliferation drug-resistant bacterial strains, worsening global morbidity, and mortality rates. Bioinspired nanomaterials present a promising avenue for developing nonantibiotic strategies against bacteria. Here, we engineer bacteriophage-inspired artificial nanobiocatalyst via nonstoichiometric W

Language: Английский

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Progress in the Computer‐aided Analysis in Multiple Aspects of Nanocatalysis Research

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

Published: June 27, 2024

Making the utmost of differences and advantages multiple disciplines, interdisciplinary integration breaks science boundaries accelerates progress in mutual quests. As an organic connection material science, enzymology, biomedicine, nanozyme-related research is further supported by computer technology, which injects new vitality, contributes to in-depth understanding, unprecedented insights, broadened application possibilities. Utilizing computer-aided first-principles method, high-speed high-throughput mathematic, physic, chemic models are introduced perform atomic-level kinetic analysis for nanocatalytic reaction process, theoretically illustrate underlying nanozymetic mechanism structure-function relationship. On this basis, nanozymes with desirable properties can be designed demand-oriented synthesized without repeated trial-and-error experiments. Besides that, computational device also play indispensable role nanozyme-based detecting methods realize automatic readouts improved accuracy reproducibility. Here, work focuses on crossing nanocatalysis inspire nanozyme field a greater extent.

Language: Английский

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Persistent Luminescence-Based Nanoreservoir for Benign Photothermal-Reinforced Nanozymatic Therapy

ACS Applied Materials & Interfaces, Journal Year: 2024, Volume and Issue: 16(37), P. 49114 - 49123

Published: Sept. 6, 2024

Adjusting the catalytic activity of nanozymes for enhanced oncotherapy has attracted significant interest. However, it remains challenging to engineer regulatory tactics with a minimal impact on normal tissues. By exploiting advantages energy storage, photostimulated, and long afterglow luminescence persistent nanoparticles (PLNPs), luminescence-based nanoreservoir was produced improve its benign oncotherapy. In study, PLNPs in ability store photons served as self-illuminant promote peroxidase-like therapeutic efficacy by persistently motivating photothermal effect before after external irradiation ceased. The photostimulated spatiotemporal controllability exogenous light jointly alleviated adverse effects induced prolonged elevated capability nanoreservoir. Ultimately, system fulfilled photothermal-intensive nanozymatic therapy. This work provides new insights into boosting secure disease treatment.

Language: Английский

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Oxygen‐Bonded Amorphous Transition Metal Dichalcogenides with pH‐Responsive Reactive Oxygen Biocatalysis for Combined Antibacterial and Anti‐inflammatory Therapies in Diabetic Wound Healing

Small, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 29, 2024

Diabetic wound healing is a formidable challenge, often complicated by biofilms, immune dysregulation, and hindered vascularization within the environments. The intricate interplay of these microenvironmental factors has been significant oversight in evolution therapeutic strategies. Herein, design an efficient versatile oxygen-bonded amorphous transition metal dichalcogenide biocatalyst (aRuS-O

Language: Английский

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Upgrading the Bioinspired Iron-Polyporphyrin Structures by Abiological Metals Toward New-Generation Reactive Oxygen Biocatalysts

Nano Letters, Journal Year: 2024, Volume and Issue: unknown

Published: Dec. 27, 2024

Developing artificial enzymes based on organic molecules or polymers for reactive oxygen biocatalysis has broad applicability. Here, inspired by heme-based enzyme systems, we construct the abiological iron group metal-based polyporphyrin (Ru/Os-coordinated porphyrin-based biocatalyst, Ru/Os-PorBC) to serve as a new generation of efficient and versatile species (ROS)-related biocatalyst. Due structural benefits, including excellent electron configuration, appropriate bandgap, optimized adsorption activation reaction intermediates, Ru/Os-PorBC shows unparalleled ROS-production activities regarding maximum rate turnover numbers, which also demonstrates superior pH temperature adaptability compared natural enzymes. Impressively, Os-PorBC manifests most efficacious capabilities, surpassing not only Ru/Fe-PorBC but existing state-of-the-art ROS-related Our findings provide pivotal direction developing next-generation polyporphyrin-based biocatalysts, setting stage era upgrading metalloenzymes metals.

Language: Английский

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Vanadium Single-Atoms Coordinated Artificial Peroxidases as Biocatalyst-Linked Immunosorbent Assay for Highly-Sensitive Carcinoembryonic Antigen Immunoassay

Biomaterials, Journal Year: 2024, Volume and Issue: 316, P. 123008 - 123008

Published: Dec. 14, 2024

Language: Английский

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