Intrinsic Anti‐Freezing and Unique Phosphorescence of Glassy Hydrogels with Ultrahigh Stiffness and Toughness at Low Temperatures

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(21)

Published: Feb. 23, 2023

Most hydrogels become frozen at subzero temperatures, leading to degraded properties and limited applications. Cryoprotectants are massively employed improve anti-freezing property of hydrogels; however, there accompanied disadvantages, such as varied networks, reduced mechanical properties, the risk cryoprotectant leakage in aqueous conditions. Reported here is glassy hydrogel having intrinsic capacity excellent optical ultra-low temperatures. Supramolecular poly(acrylamide-co-methacrylic acid) with moderate water content (≈50 wt.%) dense hydrogen-bond associations a state room temperature. Since hydrogen bonds strengthened temperature decreases, this gel becomes stronger stiffer, yet still ductile, Young's modulus 900 MPa, tensile strength 30 breaking strain 35% -45 °C. This retains high transparency even liquid nitrogen. It also exhibits unique phosphorescence due presence carbonyl clusters, which further enhanced Further investigations elucidate that related fact most molecules tightly bound confined matrix non-freezable. correlation, validated several systems, provides roadmap develop for widespread applications extreme

Language: Английский

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A NIR‐II AIEgen‐Based Supramolecular Nanodot for Peroxynitrite‐Potentiated Mild‐Temperature Photothermal Therapy of Hepatocellular Carcinoma

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(19)

Published: Feb. 13, 2023

Abstract Compared to conventional photothermal therapy (PTT) which requires hyperthermia higher than 50 °C, mild‐temperature PTT is a more promising antitumor strategy with much lower phototoxicity neighboring normal tissues. However, the therapeutic efficacy of always restricted by thermoresistance cancer cells. To address this issue, supramolecular drug nanocarrier fabricated co‐deliver nitric oxide (NO) and agent DCTBT NIR‐II aggregation‐induced emission (AIE) characteristic for PTT. NO can be effectively released from nanocarriers in intracellular reductive environment capable simultaneously producing reactive oxygen species (ROS) upon 808 nm laser irradiation. The generated ROS further react produce peroxynitrite (ONOOˉ) bearing strong oxidization nitration capability. ONOOˉ inhibit expression heat shock proteins (HSP) reduce cells, necessary achieve excellent DCTBT‐based at mild temperature (<50 °C). performance ONOOˉ‐potentiated validated on subcutaneous orthotopic hepatocellular carcinoma (HCC) models. This research puts forward an innovative overcome PTT, provides new inspirations explore ONOOˉ‐sensitized tumor strategies.

Language: Английский

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Nanoarchitectonics of in Situ Antibiotic-Releasing Acicular Nanozymes for Targeting and Inducing Cuproptosis-like Death to Eliminate Drug-Resistant Bacteria

ACS Nano, Journal Year: 2024, Volume and Issue: 18(35), P. 24327 - 24349

Published: Aug. 22, 2024

A series of progress has been made in the field antimicrobial use nanozymes due to their superior stability and decreased susceptibility drug resistance. However, catalytically generated reactive oxygen species (ROS) are insufficient for coping with multidrug-resistant organisms (MDROs) complex wound environments low targeting ability catalytic activity. To address this problem, chemically stable copper-gallic acid-vancomycin (CuGA-VAN) nanoneedles were successfully constructed by a simple approach bacteria; these exhibit OXD-like GSH-px-like dual enzyme activities produce ROS induce bacterial cuproptosis-like death, thereby eliminating MDRO infections. The results

Language: Английский

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Organoboron-mediated polymerizations

Chemical Society Reviews, Journal Year: 2024, Volume and Issue: 53(7), P. 3384 - 3456

Published: Jan. 1, 2024

The scientific community has witnessed extensive developments and applications of organoboron compounds as synthetic elements metal-free catalysts for the construction small molecules, macromolecules, functional materials over last two decades. This review highlights achievements organoboron-mediated polymerizations in past several decades alongside mechanisms underlying these transformations from standpoint polymerization mode. Emphasis is placed on free radical polymerization, Lewis pair ionic (cationic anionic) polyhomologation. Herein, alkylborane/O

Language: Английский

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Inhibiting Quorum Sensing by Active Targeted pH-Sensitive Nanoparticles for Enhanced Antibiotic Therapy of Biofilm-Associated Bacterial Infections

ACS Nano, Journal Year: 2023, Volume and Issue: 17(11), P. 10019 - 10032

Published: May 26, 2023

Inhibition of quorum sensing (QS) is considered as an effective strategy in combatting biofilm-associated bacterial infections. However, the application inhibitors (QSI) strongly restricted by poor water-solubility and low bioavailability. We herein fabricate pH-sensitive curcumin (Cur) loaded clustered nanoparticles with active targeting ability (denoted anti-CD54@Cur-DA NPs) to inhibit QS for enhanced antibiotic therapy. Cur-DA NPs are first prepared through electrostatic interaction between Cur amino-ended poly(amidoamine) dendrimer (PAMAM) 2,3-dimethyl maleic anhydride (DA) modified biotin-poly(ethylene glycol)-polylysine (biotin-PEG-PLys). Anti-CD54@Cur-DA then obtained modification anti-CD54. PAMAM can be released from acidic pH, leading simultaneous charge reversal size decrease, which beneficial biofilm penetration. hence much better inhibiting than free due Compared Cur, exhibit stronger capability development architecture maturation, thus downregulating efflux pump-related genes improving bactericidal performance multiple antibiotics, including Penicillin G, ciprofloxacin, tobramycin. Moreover, since anti-CD54 selectively bind inflamed endothelial cells, targeted accumulated bacteria-infected tissues. The sequential treatment using antibiotics effectively reduce burden alleviate inflammation a chronic lung infection model vivo. This research provides way improve therapeutic QSI enhance anti-biofilm effects radiate vitality conventional treating

Language: Английский

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A Facile Strategy to Fabricate Tough and Adhesive Elastomers by In Situ Formation of Coordination Complexes as Physical Crosslinks

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(51)

Published: Aug. 11, 2023

Abstract Coordination bonds with a dynamic nature and wide‐spectrum bond energy have gained great popularity in use for fabricating tough soft materials. However, most existing coordination‐based elastomers are prepared through complicated procedures, usually involving elaborate synthesis of ligand‐containing monomers or polymers, ion diffusion to form coordination complexes, removal organic solvent during the synthesis, which neither easy operation nor environmentally friendly. Here, facile effective strategy is demonstrated fabricate metallosupramolecular by one‐pot polymerization aqueous precursor solutions containing commercial agents, 2‐acrylamido‐2‐methyl‐1‐propanesulfonic acid, 2‐[2‐(2‐methoxyethoxy)ethoxy]ethyl acrylate, Zr 4+ ions. After (i.e. water) evaporation, obtained transparent extremely owing presence sulfonate‐Zr complexes as physical crosslinks. Their mechanical properties tunable over wide spectrum adjusting composition copolymers density bonds. This eco‐friendly further extended various monomers, manifesting good universality toughen elastomers. Furthermore, abundant functional groups make adhesive substrates including themselves, favoring applications such interfacial adhesion encapsulations. The fabrication, properties, ability endow potential substrate wearable electronics.

Language: Английский

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Catalytic Amounts of an Antibacterial Monomer Enable the Upcycling of Poly(Ethylene Terephthalate) Waste

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(20)

Published: Feb. 21, 2023

Poly(ethylene terephthalate) (PET) is an important polymer with annual output second only to polyethylene. The development of PET recycling technologies therefore necessary not eliminate the harm associated white pollution and microplastics, but also reduce carbon emissions. Antibacterial PET, one most high-value advanced materials, has improved ability treat bacterial infections. However, current methods manufacturing commercial antibacterial require blending excess metal-based agents, which leads biotoxicity a nonpersistent activity. In addition, high-efficiency organic agents have yet be employed in due their poor thermal stabilities. Herein, solid-state reaction for upcycling waste using novel hyperthermostable monomer described. This catalyzed by residual catalyst present waste. It found that catalytic amount enabled low-cost produce recycled strong persistent activity, as well similar properties virgin PET. work provides feasible economic strategy large-scale exhibits potential application industry.

Language: Английский

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NIR Clusteroluminescence of Non‐conjugated Phenolic Resins Enabled by Through‐Space Interactions

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(30)

Published: May 30, 2023

Clusteroluminescence (CL) and through-space interactions (TSIs) of non-conjugated molecules have drawn more attention due to their unique photophysical behaviors that are different from largely conjugated luminogens. However, achieving red even near-infrared (NIR) emission such systems is still challenging the intrinsic drawbacks lack theories for structure-property relationships. In this work, six phenolic resins designed synthesized based on two molecule-engineering strategies: increasing number TSIs units introducing electron-donating/-withdrawing groups. All verified as luminogens with CL property (CLgens), first example CLgens NIR (maximum wavelength ≥680 nm) high absolute quantum yield (47 %) reported. Experiments theoretical analysis reveal types, locally excited state charge transfer state, play essential roles in these polymers, which could be manipulated via changing structural conformation electron density or altering transition behaviors. This work not only provides an approach manipulate polymers but also endows commercially available practical value luminescence materials.

Language: Английский

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Facile Synthesis of Self‐Targeted Zn²⁺‐Gallic acid Nanoflowers for Specific Adhesion and Elimination of Gram‐Positive Bacteria

Small, Journal Year: 2023, Volume and Issue: 19(43)

Published: June 27, 2023

Transition metal ions are served as disinfectant thousand years ago. However, the in vivo antibacterial application of is strongly restricted due to its high affinity with proteins and lack appropriate bacterial targeting method. Herein, for first time, Zn2+ -gallic acid nanoflowers (ZGNFs) synthesized by a facile one-pot method without additional stabilizing agents. ZGNFs stable aqueous solution while can be easily decomposed acidic environments. Besides, specifically adhere onto Gram-positive bacteria, which mediated interaction quinone from amino groups teichoic bacteria. exhibit bactericidal effect toward various bacteria multiple environments, ascribed situ release on surface. Transcriptome studies reveal that disorder basic metabolic processes Methicillin-resistant Staphylococcus aureus (MRSA). Moreover, MRSA-induced keratitis model, long-term retention infected corneal site prominent MRSA elimination efficacy self-targeting ability. This research not only reports an innovative prepare metal-polyphenol nanoparticles, but also provides novel nanoplatform targeted delivery combating infections.

Language: Английский

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Closed‐Loop Polymer‐to‐Polymer Upcycling of Waste Poly (Ethylene Terephthalate) into Biodegradable and Programmable Materials

ChemSusChem, Journal Year: 2024, Volume and Issue: 17(13)

Published: Feb. 27, 2024

Abstract Poly(ethylene terephthalate) (PET), extensively employed in bottles, film, and fiber manufacture, has generated persistent environmental contamination due to its non‐degradable nature. The resolution of this issue requires the conversion waste PET into valuable products, often achieved through depolymerization monomers. However, laborious purification procedures involved extraction monomers pose challenges constraints on complete utilization PET. Herein, a strategy is demonstrated for polymer‐to‐polymer upcycling high‐value biodegradable programmable materials named PEXT. This process involves reversible transesterifications dependent ester bonds, wherein commercially available X‐monomers from aliphatic diacids diols are introduced, utilizing existing industrial equipment utilization. PEXT features molecular structure, delivering tailored mechanical, thermal, biodegradation performance. Notably, exhibits superior mechanical performance, with maximal elongation at break 3419.2 % toughness 270.79 MJ m −3 . These characteristics make suitable numerous applications, including shape‐memory materials, transparent films, fracture‐resistant stretchable components. Significantly, allows closed‐loop recycling within specific analogs by reprograming or X‐monomers. not only offers cost‐effective advantages large‐scale advanced but also demonstrates enormous prospect conservation.

Language: Английский

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