RESUMO
Nitric oxide (NO) has received growing attention as an effective antibacterial agent with broad-spectrum activity and a low risk of resistance. However, it remains challenging to develop effective, controllable, and biocompatible NO-releasing materials. Here, we report a novel NO nanogenerator (AL-BNN6-PEG) self-assembled by lignin, a UV-absorbing and hydrophobic NO donor (N,N'-disec-butyl-N,N'-dinitroso-1,4-phenylenediamine, BNN6), and PEG-DSPE2000. It was discovered that upon visible light irradiation (450-460 nm), BNN6 can be decomposed by lignin within micellar nanoparticles via a photoinduced electron transfer mechanism in the aqueous medium. Lignin not only served as a sustainable carrier, enhancing the water dispersity of BNN6, but also acted as a biocompatible photosensitizer, triggering BNN6 decomposition with the concomitant release of NO. As a result, the micellar nanoparticles displayed superior antibacterial effects against Gram-negative and Gram-positive bacteria upon visible light illumination. Moreover, MTT assay revealed the negligible cytotoxic effect of the micellar nanoparticles to the mouse fibroblast cells (L929). This research provides more insight into the BNN6 decomposition mechanism and demonstrates a straightforward, effective, and biocompatible strategy for controlled NO-mediated antibacterial applications.
Assuntos
Antibacterianos , Luz , Lignina , Nanopartículas , Óxido Nítrico , Antibacterianos/farmacologia , Antibacterianos/química , Óxido Nítrico/química , Lignina/química , Lignina/farmacologia , Camundongos , Animais , Nanopartículas/química , Micelas , Doadores de Óxido Nítrico/química , Doadores de Óxido Nítrico/farmacologia , Polietilenoglicóis/químicaRESUMO
Antibiotic resistance and the rise of untreatable bacterial infections pose severe threats to human health. Silver nanoparticles (AgNPs) have emerged as a promising antibacterial solution due to their broad-spectrum effectiveness. However, their relatively high cytotoxicity has limited their widespread application. In this study, ferulic acid (FA) was used as a reducing agent, while silver oxide served as a silver precursor to rapidly prepare FA-derived lignin (FAL) coated AgNPs (AgNPs@FAL) with a size ranging from 34.8 to 77.1 nm. Density functional theory (DFT) calculations indicated that the coating of FAL endowed AgNPs@FAL with high stability, preventing the oxidation of AgNPs prior to antibacterial applications. Cell experiments further indicated that AgNPs@FAL exhibited lower cell toxicity (â¼80 % viability of normal kidney cells cultured at 25 µg/mL AgNPs@FAL) compared to fully exposed commercially available citrate-modified AgNPs (AgNPs@CA). Antibacterial experiments revealed that the minimum inhibitory concentrations (MIC) of AgNPs@FAL against E. coli and S. aureus were 12.5 µg/mL and 25 µg/mL, respectively, surpassing the antibacterial effect of AgNPs@CA, as well as ampicillin and penicillin. Additionally, AgNPs@FAL was capable of disrupting E. coli and S. aureus biofilm formation. This novel AgNPs@FAL formulation presents a promising antibacterial solution, addressing limitations observed in conventional drugs.
Assuntos
Antibacterianos , Ácidos Cumáricos , Escherichia coli , Lignina , Nanopartículas Metálicas , Testes de Sensibilidade Microbiana , Prata , Prata/química , Prata/farmacologia , Nanopartículas Metálicas/química , Antibacterianos/farmacologia , Antibacterianos/química , Antibacterianos/síntese química , Ácidos Cumáricos/química , Ácidos Cumáricos/farmacologia , Lignina/química , Lignina/farmacologia , Escherichia coli/efeitos dos fármacos , Staphylococcus aureus/efeitos dos fármacos , Humanos , Biofilmes/efeitos dos fármacos , Sobrevivência Celular/efeitos dos fármacosRESUMO
Ligand-receptor recognition serves as the fundamental driving force for active targeting, yet it is still constrained by off-target effects. Herein, we demonstrate that circumventing or blocking the mononuclear phagocyte system (MPS) are both viable strategies to address off-target effects. Naturally derived lignin nanoparticles (LNPs) show great potential to block MPS due to its good stability, low toxicity, and degradability. We further demonstrate the impact of LNPs dosage on in vivo tumor targeting and antitumor efficacy. Our results show that a high dose of LNPs (300 mg/kg) leads to significant accumulation at the tumor site for a duration of 14 days after intravenous administration. In contrast, the low-dose counterparts (e.g., 50, 150 mg/kg) result in almost all LNPs accumulating in the liver. This discovery indicates that the liver is the primary site of LNP capture, leaving only the surplus LNPs the chance to reach the tumor. In addition, although cell membrane-engineered LNPs can rapidly penetrate tumors, they are still prone to capture by the liver during subsequent circulation in the bloodstream. Excitingly, comparable therapeutic efficacy is obtained for the above two strategies. Our findings may offer valuable insights into the targeted delivery of drugs for disease treatment.
Assuntos
Células de Kupffer , Lignina , Fígado , Nanopartículas , Fagocitose , Animais , Lignina/farmacologia , Lignina/química , Nanopartículas/química , Células de Kupffer/efeitos dos fármacos , Células de Kupffer/metabolismo , Camundongos , Fígado/metabolismo , Fígado/efeitos dos fármacos , Fígado/patologia , Fagocitose/efeitos dos fármacos , Humanos , Linhagem Celular Tumoral , Neoplasias/tratamento farmacológico , Neoplasias/metabolismo , Neoplasias/patologiaRESUMO
Lignin is the most abundant natural phenolic polymer. However, the severe condensations of industrial lignin resulted in an undesirable apparent morphology and darker color, which hindered its application in the field of daily chemicals. Therefore, a ternary deep eutectic solvent is used to obtain lignin with light-color and low condensations from softwood. The results showed that the brightness value of lignin extracted from aluminum chloride-1,4-butanediol-choline chloride at 100 °C and 1.0 h was 77.9, and the lignin yield was 32.2 ± 0.6%. It is important that 95.8% of ß-O-4 linkages (ß-O-4 and ß-O-4') was retained. Lignin is used to prepare sunscreens and is added to physical sunscreens at 5%, with SPF up to 26.95 ± 4.20. Meanwhile, enzyme hydrolysis experiments and reaction liquid composition tests were also conducted. In conclusion, a systematic understanding of this efficient process could facilitate high-value utilization of lignocellulosic biomass in industrial processes.
Assuntos
Solventes Eutéticos Profundos , Lignina , Lignina/química , Ácidos de Lewis , Solventes/química , Protetores Solares , Biomassa , HidróliseRESUMO
Co-based catalysts play a crucial role in the activation of peroxymonosulfate (PMS) for degradation contaminants. However, the practical application of such catalysts is hindered by challenges like the self-aggregation of Co nanoparticles and leaching of Co2+. In this study, the Co-based catalyst Co-N/C@CL was synthesized from carboxymethylated lignin obtained by grafting abundant carboxymethyl groups into alkali lignin, in which the presence of these carboxymethyl groups enhanced its water solubility and allowed the formation of stable macromolecular complexes with Co2+. This catalyst exhibited a high specific surface area (521.8 m2·g-1) and a uniform distribution of Co nanoparticles. Consequently, the Co-N/C@CL/PMS system could completely remove 20 ppm tetracycline (TC) in 2 min at a rate of 2.404 min-1. Experimental results and DFT calculations revealed that the synergistic effect of lignin carbon and Co NPs accelerated the cleavage and electron transfer of OO bonds, thus promoting the formation of 1O2, OH and SO4-, with 1O2 emerging as the predominant contributor. Moreover, Co-N/C@CL displayed excellent cycling stability and low Co2+ leaching. This work not only provides a feasible strategy for the preparation of highly active and stable Co-based carbon materials but also offers a promising catalyst for the efficient degradation of TC.
Assuntos
Antibacterianos , Lignina , Tetraciclina , Carbono , NitrogênioRESUMO
Facile strategy to construct a cellulose nanocomposite hydrogel with self-healing and biocompatible properties is reported by crosslinking dialdehyde cellulose nanocrystals with acylhydrazine-terminated polyethylene glycol via dynamic reversible acylhydrazone for the first time. The effects of process variables on gelation time, mechanical strength and self-healing efficiency of hydrogels were investigated. It was found that gelation time shortened from hours to seconds by adjusting gelator and catalyst concentration. Tensile and compressive strength of hydrogel could reach 141 K Pa and 580 K Pa at 20.1% gelator concentration, respectively. Interestingly, the as-prepared hydrogel presented excellent self-healing ability without additional stimuli whose healing efficiency was higher than 90% even at higher gelator concentration. Furthermore, Cytotoxicity test showed that cell viability almost reached 100% after culturing with hydrogel, which revealed the hydrogel was biocompatible.
Assuntos
Materiais Biocompatíveis/química , Celulose/química , Hidrazonas/química , Hidrogéis/química , Nanocompostos/química , Animais , Materiais Biocompatíveis/síntese química , Materiais Biocompatíveis/toxicidade , Linhagem Celular , Celulose/síntese química , Celulose/toxicidade , Força Compressiva , Hidrazonas/síntese química , Hidrazonas/toxicidade , Hidrogéis/síntese química , Hidrogéis/toxicidade , Concentração de Íons de Hidrogênio , Camundongos , Nanocompostos/toxicidade , Polietilenoglicóis/química , Polietilenoglicóis/toxicidade , Resistência à TraçãoRESUMO
Pretreatment combining FeCl3 and Tween80 was performed for cellulose-to-ethanol conversion of eucalyptus alkaline peroxide mechanical pulping waste fibers (EAWFs). The FeCl3 pretreatment alone showed a good effect on the enzymatic hydrolysis of EAWFs, but inhibited enzyme activity to some extent. A surfactant, Tween80, added during FeCl3 pretreatment was shown to significantly enhance enzyme reaction by eluting enzymatic inhibitors such as iron(III) that are present at the surface of the pretreated biomass. Treatment temperature, liquid-solid ratio, treatment time, FeCl3 concentration, and Tween80 dosage for pretreatment were optimized as follows: 180 °C, 8:1, 30 min, 0.15 mol/L, and 1% (w/v). Pretreated EAWFs under such optimal conditions provided enzymatic glucose (based on 100 g of oven-dried feedstock) and substrate enzymatic digestibility of EAWFs of 34.8 g and 91.3% after 72 h of enzymatic hydrolysis, respectively, with an initial cellulase loading of 20 FPU/g substrate.