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Lignin nanoparticles (LNPs), as one of green and sustainable biological macromolecules, have attracted great attention owing to their promising potentials in many valorized fields. However, the lignin heterogeneity seriously restricts the controllable preparation of LNPs. Herein, a facile nanogrinding activation combining anhydrous ethanol dissolution process was developed to efficiently homogenize lignin prior to gradient ethanol fractionation. Two lignin fractions were obtained from nanogrinding activation/ethanol dissolution followed by gradient ethanol fractionation: L-fractions and S-fractions. Therefore, monodispersed LNPs with unique concave hollow nanostructure and large particle size, and monodispersed LNPs with solid core nanostructure and small particle size were successfully prepared from L-fractions and S-fractions, respectively, via a GVL/water anti-solvent method. The proposed LNPs formation mechanisms facilitated by nanogrinding activation/ethanol dissolution treatment were demonstrated. This study put forwards a facile and green integrated approach for monodispersed LNPs preparation with controllable morphology and particle size.

A cellulose nanocrystal based oxidation system is developed for oxidizing starch in the presence of NaClO, and provides an alternative and green method to improve the oxidizing degree of oxidized starch. The underlying mechanism for the oxidation was studied with confocal laser scanning microscopy. It was found that cellulose nanocrystal would penetrate into the starch microparticles and contribute to oxidation. The function of cellulose nanocrystal on the physicochemical properties of oxidized starch was investigated. With the incorporation of the oxidized starch into starch/polyvinyl alcohol/glyceryl composite films, the mechanical property and transparency of the films improved substantially. The highest oxidation level of starch was attained at 0.5 wt% cellulose nanocrystal dosage and the carboxylate content was 1.10%, the composite film showed the maximum transparency of 0.66 and highest contact angle of 102.0°. Meanwhile, the best film was obtained with oxidized starch containing 1.0 wt% cellulose nanocrystal. Compared to native starch and TEMPO-oxidated starch, the cellulose nanocrystal-based oxidized starch improved the hydrophobicity of film more substanially. In conclusion, cellulose nanocrystal acts as prooxidant and reforcing agent in this starch-based composite film, which makes them promising materials in the preparation of novel composite materials.

In recent years, lignin nanoparticles (LNP) have gained tremendous and deep research in the field of functional composites because of their many advantages such as abundant, non-toxic, affordable, green, eco-friendly, biodegradable and biocompatible features along with antioxidant, antibacterial and UV-absorbing abilities. At present, numerous pioneering works have been devoted to the development of LNP-based composites with multiple functions. Herein, we comprehensively reviewed the latest research progress correlated with LNP-filled functional composites. This overview focused on the application of LNP as reinforcement, crosslinker, UV-protectant, antioxidant, antimicrobial and adhesive agents for functional composites. Additionally, the challenges and future outlooks for further exploiting and utilization of LNP in the functional composites were discussed.

Conductive hydrogels have attracted tremendous attention as a novel generation of wearable devices and body monitoring due to their great stretchability and high flexibility. Here, a multifunctional cellulose nanocrystal @sodium lignosulfonate-silver-poly(acrylamide) nanocomposite hydrogel was prepared by radical polymerization within only a few minutes. This polymerization rapidly occurred by lignosulfonate-silver (Ls-Ag) dynamic catalysis that efficiently activated ammonium persulfate (APS) to initiate the free-radical polymerization. In particular, the hydrogel exhibited excellent tensile strength (406 kPa), ultrahigh stretchability (1880 %), self-recovery, and fatigue resistance. Furthermore, due to the inclusion of Ls-Ag metal ion nanocomposite in the hydrogels, the composite hydrogel presented repeated adhesion to various objects, excellent conductivity (σ ∼ 9.5 mS cm

In this study, an alkaline-catalyzed sulfolane/water solvent system was developed for isolating high-purity and antioxidative lignin from willow (Salix matsudana cv. Zhuliu). Optimization of the pretreatment conditions such as temperature, sulfolane/water ratio, and alkaline catalyst (NaOH) dosage were comprehensively investigated for effective lignin extraction from willow. The 44.4% of lignin was recovered from the biomass with 54% of delignification in 50/50 (w/w) sulfolane/water system at 170 °C. As the addition of the alkaline catalyst (NaOH) increased to 4%, the delignification yield was increased up to 94% with about 70% of lignin recovery yield. The recovered lignin was comparatively investigated with its control, milled wood lignin (MWL). The β-O-4 linkages and phenolic hydroxyl were well preserved in the extracted lignin fractions with the sulfolane/water system. Furthermore, excellent radical scavenging ability was observed with the extracted lignins by sulfolane/water pretreatments owing to rich phenolic hydroxyl groups in the lignins. Hence, systematical investigation on the lignin properties and potential applications under sulfolane organosolv pretreatment would promote the utilization of lignin in biorefinery processes.

The application of industrial kraft lignin is limited by its low molecular weight, dark color, and low solubility. In this work, an efficient crosslinking reaction with N,N-Dimethylformamide (DMF) and 1,6-dibromohexane was proposed for adjusting the molecular weight and color of lignin. The chemical structure of alkylation lignin was systematically investigated by gel permeation chromatography (GPC), ultraviolet spectroscopy, Fourier transform infrared (FT-IR) spectroscopy, and 2D heteronuclear single quantum correlation nuclear magnetic resonance (HSQC NMR) spectra. After the alkylation modification, the molecular weights of the lignin were increased to 1643%. The resinol (β-β), β-aryl ether (β-O-4), and phenylcoumaran (β-5) linkages were still the main types of the linkages. The formation of β-β linkage would be inhibited at high temperatures. The color reduction of lignin can be attributed to the low content of chromophores and low packing density. This alkylation lignin will be a new and general approach for developing molecular weight-controlled and light-colored lignins, which can find more applications in cosmetics, packing, and other fields.

A green and simple lignin nanoparticles (LNPs) production strategy was developed using deep eutectic solvents (DES). The LNPs were formed with corncob alkali lignin by sequential DES dissolution and self-assembling process. Uniform size and spherical shape of LNPs were observed by scanning electron microscopy (SEM), transmission electron microscopy (TEM), dynamic light scattering (DLS), zeta potential analyzer and gel permeation chromatography (GPC). Less than 100 nm of LNPs were formed, and these particles were preserved without significant size-increase or precipitation within 30 days. The nanocomposite films prepared by incorporating the LNPs into biodegradable poly(vinyl alcohol) (PVA) matrix display good mechanical properties (tensile strength of 82.5 MPa and breaking strain of 103.3%), excellent UV-blocking (100% shielding of the UV spectrum region), strong hydrophobicity (static contact angle of 117.0°) and relatively high thermal stability (the maximum thermal weight loss temperature increased by 40 °C). Overall, this study not only facilitates the advancement of lignin-based nanotechnology by DES but also paves the way for the PVA polymer composites as potential food and medical packaging materials.

A novel 3-D biopolymer-based adsorption-photocatalytic composite, polyaniline/dicarboxyl acid cellulose@graphene oxide was synthesized and was employed to remove the reactive brilliant red K-2G from aqueous solution. The addition of dicarboxyl acid cellulose could improve the morphology, structure, stability and dispersity of the nanocomposite, thus providing excellent adsorption and photocatalysis performance to the product. Batch of experiments were conducted in two scenarios: adsorption followed by photocatalysis process and simultaneous adsorption-photocatalysis process. For the first scenario, adsorption equilibrium can be reached within 25 min, the expected adsorption capacity was 447.0 mg·g-1; the subsequent photocatalysis process was carried out under light irradiation and the removal capacity could further improve to 729.0 mg·g-1 under equilibrium state (about 180 min). For the simultaneous adsorption-photocatalytic process, the removal capacity was about 558.1 mg·g-1 at about 25 min and the total removal capacity could reach to 733.3 mg·g-1 under equilibrium state. PANI-DCC@GO exhibited excellent reusability and had potential in the treatment of dyes polluted wastewater.

A novel cationic biosorbent was synthesized by grafting organosolv lignin with GT (also named (2-hydrazinyl-2-oxoethyl)-trimethylazanium chloride, abbreviated as GT) and formaldehyde in an aqueous solution by an eco-friendly way (named QA-g-OL). QA-g-OL was employed as biosorbent to remediate hexavalent chromium polluted water. Research found Cr(VI) removal is a pH-dependence process. It was also found that part of the Cr(VI) was reduced to Cr(III) during the process of adsorption in the range of pH was 2.0 to 7.0. Furthermore, QA-g-OL possess strong absorbability for Cr (VI) in a broad concentration range (from 10 to 100 mg/L). The removal efficiencies of Cr (VI) were 93.40%, 96.70%, 98.78% and 97.84% when initial concentration was 10, 20, 50, 80 and 100 mg/L under optimum pH, respectively. On the other side, the adsorption process exhibited swift equilibrium characteristics, the adsorption equilibrium can be achieved within 10 min. The mechanism of hexavalent chromium removed by QA-g-OL were also discussed, results can be benefit for the application of biomass-based adsorbents in the treatment of hexavalent chromium polluted wastewater.