physical/chemical functionalization is capable of optimization of mechanical properties, [7] interfacial adhesion, [8] and self-healing ability of hydrogels. [9] These protocols normally introduced functional elements or structures that elicited physical/chemical interactions for the performance improvements of hydrogels. For example, polymeric nanoparticles from crystallization-driven self-assembly enabled mechanical improvements on hydrogel by physical hybridization with matrix. [10] Grafting silica nanoparticles to a double-network polymer also improved the hydrogel mechanical performances. [11] Construction of electrostatic interaction between carboxyl groups and various surfaces resulted in a catechol-chemistrybased hydrogel for the long-term adhesiveness. [12] Treatment by metal ions resulted in a hydrophobic surface that promoted formation of a water-resistant molecular bridge between the hydrogel surface and hydrophobic domains on the substrates, endowing the hydrogels prominent underwater-adhesion capability. [13] Similar adhesive hydrogel could also be achieved by dopamine-modified clay nanosheets. [14] An effective molecular structure design based on acid-ether hydrogen bonding and imine bonds was capable of accelerating hydrogel healing time to 30 min. [15] A dynamic borate bond in network enabled 100% cure of hydrogel in air. [16] Reversible metal-ligand coordination bonding interaction could also be used to construct self-healing hydrogel. [17] These protocols are efficient for the construction of functional hydrogels, yet still challenging to synchronously improve the mechanical strength, self-healing, and interfacial adhesion of a hydrogel, and especially, hard to endow the hydrogel with modular sensitivity to external pressure. Therefore, the development of a new class of protocol is still essential.Herein, we proposed an electrochemistry functionalization protocol, in which the functional improvements on hydrogels were achieved by the electrode reactions, and electrochemistrytriggered ionic and molecular migration. This protocol was capable of enabling the function improvements of the hydrogel in mechanical strength, interfacial adhesion, and self-healing. In the meantime, it allowed generation of various patterns on the hydrogel surface, and endowed the hydrogel modular sensitivity to external pressure. The functional improvements Hydrogels have demonstrated great potential in biomedical and engineering areas. To improve the physical performance, development of efficient physical/chemical protocols is essential. Herein, an electrochemistry functionalization strategy that is capable of enabling the functional improvements of hydrogel is reported. The electrochemistry functionalization is demonstrated on a hydrogel model of polyacrylamide (PAAm)@κ-carrageenan. The electrochemistry reaction generates metal ions (Fe 3+ ) that migrate and coordinate with the sulfate groups of κ-carrageenan resulting in the prominent function improvements. In comparison with untreated PAAm@κcarrageenan hydrogel, it c...
To increase the cellular uptake and drug loading of cellulose nanocrystal (CNC)-based nanomedicines, folate/cis-aconityl-doxorubicin@polyethylenimine@CNC (FA/CAD@PEI@CNC) nanomedicines were built up by the building blocks of folate (FA), cis-aconityl-doxorubicin (CAD), polyethylenimine (PEI), and CNCs via the robust layer-by-layer (LbL) assembly technique. The drug loading content (DLC) of FA/CAD@PEI@CNC hybrids was 11.3 wt %, which was almost 20-fold higher than that of the CNC-based nano-prodrug we reported previously. FA/CAD@PEI@CNC nanomedicines showed lysosomal pH-controlled drug release profiles over 24 h. In detail, the cumulative drug release was over 95% at pH 5.5, while the cumulative drug release was only 17% at pH 7.4. In vitro, FA/CAD@PEI@CNC hybrid nanomedicines had a higher (9.7-fold) mean fluorescent intensity (MFI) than that of DOX·HCl, with enhanced cytotoxicity and decreased IC50 against MCF-7. Thus, FA/CAD@PEI@CNC hybrid nanomedicines displayed efficient targetability and enhanced cellular uptake. In addition, FA/CAD@PEI@CNC nanomedicine could deliver more DOX to the nucleus than the control group, due to the β-carboxylic acid catalyzed breakage of the pH-labile cis-aconityl amide linkages in CAD. These results indicated that FA/CAD@PEI@CNC nanomedicines achieved lysosomal pH-controlled drug release into the nucleus and showed great potential to be high-performance nanomedicines to improve the delivery efficiency and therapy efficacy. This study for CNC-based nanomedicines provided important insights into the bioapplication of CNCs modified by LbL assembly.
Adhesion allows the close contact of wound dressing materials with skin surface. However, the dressing replacement inevitably causes the secondary damage to unhealed wound, so a wound dressing material having physiologically‐regulated adhesion is of high significance. Herein, a hydrogel is reported by covalently introducing cationic moieties into an elastic network. The cationic moieties are capable of electron‐withdrawing that promotes a strong electrostatic interaction with polar groups of protein (high electron cloud density) from the wound skin tissue, enabling the adhesion of hydrogel on the skin surface. With the tissue metabolism, the nucleophilic skin surface forms a lipid layer that gradually destroys the electrostatic interaction and weakens the interfacial affinity. The adhesion energy can be reduced from 60 to <10 J m−2 in 7 days, so that the dressing material can be removed easily. The cationic moieties also endow the hydrogel a high water swelling ratio (reaching 25 200%) and an efficient antibacterial property. The in vivo tests demonstrate that the wound on a mouse back reaches physiological 100% healing after the hydrogel dressing treatment for 12 days. All results show that the introduction of cationic moieties makes the hydrogel more promising as a wound dressing.
Silver nanoparticles synthesized with polymers as coating agents is an effective method to overcome their poor stability and aggregation in solution. Silver-polyethylene glycol (Ag-PEG) nanoparticles were synthesized with the thiol-functionalized polyethylene glycol (SH-PEA) as the coating, reducing and stabilizing agent. The UV irradiation time, polymer and silver nitrate concentration for the synthesis were investigated. The concentration of silver nitrate had significant effect on the morphology of Ag-PEG nanoparticles. When increasing the concentration of silver nitrate, SEM and TEM images showed that Ag-PEG nanoparticles changed from Janus to multi-core shell structure. Meanwhile, pure silver particles in the two hybrid nanoparticles presented spherical shape and had the similar size of 15 nm. The antibacterial activities and cytotoxicity of the two structural Ag-PEG nanoparticles were investigated to understand colloid morphology effect on the properties of AgNPs. The results of antibacterial activities showed that the two structural Ag-PEG nanoparticles exhibited strong antibacterial activities against Staphylococcus aureus, Escherichia coli and Bacillus subtilis. The Janus nanoparticles had larger minimal inhibitory concentration (MIC) and minimum bacterial concentration (MBC) values than the multi-core shell counterparts. The results of cytotoxicity showed the Janus Ag-PEG nanoparticles had lower toxicity than the multi-core shell nanoparticles.
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