A deep eutectic solvent (DES) composed of sulfamic acid and glycerol allowed for the sustainable preparation of cellulose nanofibrils (CNF) with simultaneous sulfation. The reaction time and the levels of sulfamic acid demonstrated that fibers could be swelled and sulfated simultaneously by a sulfamic acid-glycerol-based DES and swelling also promoted sulfation with a high degree of substitution (0.12). The DES-pretreated fibers were further nanofibrillated by a grinder producing CNF with diameters from 10 nm to 25 nm. The crystallinity ranged from 53–62%, and CNF maintained the original crystal structure. DES pretreatment facilitated cellulose nano-fibrillation and reduced the energy consumption with a maximum reduction of 35%. The films prepared from polyvinyl alcohol (PVA) and CNF showed good UV resistance ability and mechanical properties. This facile and efficient method provided a more sustainable strategy for the swelling, functionalization and nano-fibrillation of cellulose, expanding its application to UV-blocking materials and related fields.

To improve the physical strength of regenerated cellulose fibers, cellulose dissolution was analyzed with a conductor-like screening model for real solvents in which 1-allyl-3-methylimidazolium chloride (AMIMCl) worked only as a hydrogen bond acceptor while dissolving the cellulose. This process could be promoted by the addition of urea, glycerol, and choline chloride. The dissolution and regeneration of cellulose was achieved through dry-jet and wet-spinning. The results demonstrated that the addition of hydrogen bond donors and acceptors either on their own or in combination can enhance the tensile strength, but their effects on the crystallinity of the regenerated fibers were quite limited. Compared with the regenerated fibers without any additives, the tensile strength was improved from 54.43 MPa to 139.62 MPa after introducing the choline chloride and glycerol, while related the crystallinity was only changed from 60.06% to 62.97%. By contrast, a more compact structure and fewer pores on the fiber surface were identified in samples with additives along with well-preserved cellulose frameworks. Besides, it should be noted that an optimization in the overall thermal stability was obtained in samples with additives. The significant effect of regenerated cellulose with the addition of glycerol was attributed to the reduction of cellulose damage by slowing down the dissolution and cross-linking in the cellulose viscose. The enhancement of the physical strength of regenerated cellulose fiber can be realized by the appropriate adjustment of the hydrogen bond distribution in the ionic liquid system with additives.

In this study, a novel type of high-strength regenerated cellulose composite fiber reinforced with cellulose nanofibrils (CNFs) and nanosilica (nano-SiO₂) was prepared. Adding 1% CNF and 1% nano-SiO₂ to pulp/AMIMCl improved the tensile strength of the composite cellulose by 47.46%. The surface of the regenerated fiber exhibited a scaly structure with pores, which could be reduced by adding CNF and nano-SiO₂, resulting in the enhancement of physical strength of regenerated fibers. The cellulose/AMIMCl mixture with or without the addition of nanomaterials performed as shear thinning fluids, also known as “pseudoplastic” fluids. Increasing the temperature lowered the viscosity. The yield stress and viscosity sequences were as follows: RCF-CNF² > RCF-CNF²-SiO₂² > RCF-SiO₂² > RCF > RCF-CNF¹-SiO₂¹. Under the same oscillation frequency, G’ and G” decreased with the increase of temperature, which indicated a reduction in viscoelasticity. A preferred cellulose/AMIMCl mixture was obtained with the addition of 1% CNF and 1% nano-SiO₂, by which the viscosity and shear stress of the adhesive were significantly reduced at 80 °C.

A novel choline-based deep eutectic solvent (DES) with low halogen content—namely choline lactate-lactic acid (CLL)—was synthesized by replacing the chloride anion with lactate anion in choline chloride-lactic acid (CCL). CLL and CCL treatments were conducted at 140 °C for 12 h with hydrogen bond acceptor/hydrogen bond donor =1/10, thereafter composition analysis and characterizations of the lignin extracted by DES treatment (DES lignin) and the solid residue were carried out. The proposed low halogen content DES presented an improved lignin extraction efficiency. The CLL treatment extracted 90.13% of initial lignin from poplar, while CCL extracted 86.02%. In addition, the CLL treatment also provided DES lignin with an improved purity (91.17%), lower molecular weight (Mw/Mn=1805/971 g/mol) and more concentrated distribution (polydispersity index=1.86). The efficient lignin extraction was mainly ascribed to the cleavage of β-O-4 bonds in lignin macromolecule, especially in the guaiacyl units, thereby breaking them into smaller molecules, facilitating the lignin extraction. The replacement of chloride anion allowed CLL acting as a more efficient DES to interact with lignin macromolecules, thus providing lignin with higher uniformity and suitable molecular weight. The low halogen content DES system proposed in present work could benefit the fractionation of biomass, improve the valorization of lignin compounds and facilitate industrial process in the downstream.

Hydrogels have attracted much attraction for promising flexible electronics due to the versatile tunability of the properties. However, there is still a big obstacle to balance between the multi-properties and performance of wearable electronics. Herein, we propose a salt-percolated nanocellulose composite hydrogel which was fabricated via radical polymerization with acrylic acid as polymer networks (NaCl-CNCs-PAA). CNCs were utilized as a reinforcing agent to enhance the mechanical properties of the hydrogel. Moreover, the abundant hydroxyl groups endow the hydrogel with noncovalent interactions, such as hydrogen bonding, and the robustness of the hydrogel was thus improved. NaCl incorporation induced the electrostatic interaction between CNCs and PAA polymer blocks, thus facilitating the improvement of the stretchability of the hydrogel. The as-obtained hydrogel exhibited excellent stretchability, ionic conductivity, mechanical robustness and anti-freezing properties, making it suitable for self-powered sensing applications. A single-mode triboelectric nanogenerator (C-TENG) was fabricated by utilizing the composite hydrogel as electrodes. This C-TENG could effectively convert biomechanical energy to electricity (89.2 V, 1.8 µA, 32.1 nC, and the max power density of 60.8 mW m⁻² at 1.5 Hz.) Moreover, the composite hydrogel was applied for strain sensing to detect human motions. The nanocellulose composite hydrogel can achieve the application as a power supply in integrated sensing systems and as a strain sensor for human motion detection.

Deep eutectic solvents (DESs) are promising for lignin dissolution and extraction. However, they usually possess high polarity and are difficult to recycle. To overcome this drawback, a variety of switchable ionic liquids (SILs) composed of 1,8-diazabicyclo[5.4.0]undec-7-ene (DBU) and alcohols was synthesized and screened. According to the thermodynamic modeling suggestions, the selected DBU–HexOH SIL was coupled with hydrogen-bond donors to form switchable-DES (SDES) systems with moderated viscosity, conductivity, and pH while maintaining switchability. The SDESs produced a well-improved lignin and lignin model compound solubility compared with those of SILs; charging CO₂ into SDES (SDES_CO2) caused a further increase in solubility. The solubility (25 °C) of syringic acid, ferulic acid, and milled wood lignin in SDES_CO2 reached 230.57, 452.17, and 279.12 mg/g, respectively. Such SDES-dissolved lignin can be regenerated using acetone as an anti-solvent. The SDES-regenerated lignin exhibited a well-preserved structure with no noticeable chemical modifications. Furthermore, the SDES_CO2 lignin possessed a higher molecular weight (Mw = 10,340 g/mol; Mn = 7672 g/mol), improved uniformity (polydispersity index = 1.35), and a higher guaiacyl lignin unit content compared with the original milled wood lignin. The SDES system proposed in the present work could benefit the fractionation of lignin compounds and facilitate downstream industrial processes.