In this work, we have developed a novel green nanoparticle platform based on lignin without chemical modification. The alkali lignin (AL) was used to prepare nanoparticles with perfect spheres and well dispersibility via a simple self-assembly method by adding water to a methanol solution of AL. Finally, we showed that self-assembly of AL with the bioactive molecule resveratrol (RSV) and Fe3O4 magnetic nanoparticles led to the formation of stable nanodrug carrier. In cytological and animal tests, the magnetic RSV-loaded lignin nanoparticles (AL/RSV/Fe3O4 NPs) demonstrated good anticancer effects and enhanced in vitro RSV release and stability, drug accumulation, and better tumor reduction, as well lower adverse effects than free drugs, strongly supporting the AL NPs application as a new and highly efficient nanodelivery. Moreover, this renewable green material with its simple preparation technique and easy large-scale production would be a highly potential candidate for many poorly soluble drugs.
Tissue‐engineered hydrogels have received extensive attention as their mechanical properties, chemical compositions, and biological signals can be dynamically modified for mimicking extracellular matrices (ECM). Herein, the synthesis of novel double network (DN) hydrogels with tunable mechanical properties using combinatorial screening methods is reported. Furthermore, nanoengineered (NE) hydrogels are constructed by addition of ultrathin 2D black phosphorus (BP) nanosheets to the DN hydrogels with multiple functions for mimicking the ECM microenvironment to induce tissue regeneration. Notably, it is found that the BP nanosheets exhibit intrinsic properties for induced CaP crystal particle formation and therefore improve the mineralization ability of NE hydrogels. Finally, in vitro and in vivo data demonstrate that the BP nanosheets, mineralized CaP crystal nanoparticles, and excellent mechanical properties provide a favorable ECM microenvironment to mediate greater osteogenic cell differentiation and bone regeneration. Consequently, the combination of bioactive chemical materials and excellent mechanical stimuli of NE hydrogels inspire novel engineering strategies for bone‐tissue regeneration.
Two series of well-defined lignin fractions derived from birch and spruce alkaline lignin (AL) by sequential solvent fractionation (i-PrOH-EtOH-MeOH) were engaged in a structure–property-application relationship study. The bacterial-derived alkaliphilic laccase (MetZyme) extensively catalyzed the oxidation and polymerization of AL fractions in an aqueous alkaline solution (pH 10). Lignin fractions with low molar mass reached a higher polymerization degree due to more phenolic-OH groups serving as reactive sites of oxidation and better lignin-laccase accessibility arose from a lower lignin condensation degree than the high molar mass ones. In comparison, AL fractions from spruce were found to be less reactive toward the laccase-catalyzed polymerization than those from birch, which was attributed to the much pronounced aryl-vinyl moieties’ oxidation. Furthermore, in situ polymerization of birch AL fractions using microfibrillated cellulose as a structural template was conducted in an aqueous medium and a dispersion of nanocellulose with its fiber network evenly coated by aligned lignin nanoparticles was obtained. The present study not only provides fundamental insights on the laccase-assisted oxidation and polymerization of lignin but also presents a new perspective for valorizing lignin in biobased fiber products through green processing of solvent fractionation and enzymatic treatment.
Poly(ether ether ketone) (PEEK) is a promising material in biomedical engineering due to its suitable mechanical properties and excellent chemical resistance and biocompatibility. However, the biological inertness of PEEK limits its applications. In this study, we developed a facile approach of immersion to generate a biocompatible and bioactive PEEK that induced osteodifferentiation. First, micropores on the surface of PEEK were introduced by concentrated sulfuric acid and subsequent water immersion, followed by the hydrothermal treatment to reduce residual sulfuric acid. Subsequently, the sulfonated PEEK surface was activated by the oxygen plasma treatment and then coated with a poly(dopamine) (PDA) layer by immersion into the dopamine solution. Finally, the tripeptide Arg−Gly−Asp (RGD) was integrated onto the PDA-coated surface of PEEK by immersion into the RGD peptide solution. The surface characteristics (physical chemistry and biological properties) and the ability to form bonelike apatite were systematically investigated by scanning electron microscopy, X-ray photoelectron spectroscopy, water contact angle analysis, the Archimedes' fluid saturation method, ellipsometry, a quartz crystal microbalance with dissipation monitoring, cell proliferation, real-time reverse transcription polymerase chain reaction analysis, alizarin red staining, immunocytochemistry staining, and simulated body fluid immersion. Collectively, the modified PEEK showed a significantly improved ability to promote cell proliferation, osteogenic differentiation, and bonelike apatite formation in vitro as compared to the PEEK control. These results demonstrate that combined facile surface modifications for PEEK enhance its bioactivity and biocompatibility, and induce osteodifferentiation. This study presents a strategy for broadening the use of PEEK in the application of orthopedic implants and could be industrially scalable in future.
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