Composite polymer hydrogels are of significant interests for high optical transparency and mechanical performance. In this work, a strong and transparent composite hydrogel is developed from a highly mesoporous cellulose network prepared from wood via top-down delignification followed by TEMPO-mediated oxidation and in situ polymerization of PNIPAM. Individualization of cellulose microfibrils inside the wood cell wall is critical for the fabrication of free-standing composite hydrogel with high water content of 94.9 wt% and high optical transmittance of 85.8% with anisotropic light scattering behavior. The composite hydrogel also showed anisotropic mechanical properties with a tensile strength, Young's modulus and toughness of 317 kPa, 5.4 MPa, and 39.2 kJ m- 3 in axial direction, and 152 kPa, 0.31 MPa and 57.1 kJ m- 3 in the transverse direction, respectively. It also showed thermochromic behavior, i.e., reversibly changing between transparent and brightly white by a temperature change between 25 and 40 degrees C, demonstrating great potential for optical applications.

Protein immobilization on a stationary phase, such as nanocelluloses, is widely used in biodiagnostic, biocatalytic, and bioseparation applications. With the top-down approach which utilizes the native hardwood honeycomb structure, mesoporous cellulose scaffolds can be fabricated without the need for energy-consuming production and bottom-up assembly of nanocelluloses. However, this approach is difficult for preparing softwood-based cellulose scaffolds due to the disintegration of wood cells after complete delignification. Herein, for the first time the use of spruce softwood with a homogenous cellular structure of longitudinally positioned and top-to-bottom joined tracheids is explored as a scaffold for protein immobilization. 1,4-butanediol diglycidyl ether is utilized to crosslink cell wall polysaccharides before the delignification step, thus improving the adhesion between tracheids. The native cellular structure of spruce is well preserved after the complete removal of lignin, enabling the successful production of a highly mesoporous and mechanically robust spruce-derived cellulose scaffold with exceptionally high specific surface area (219 m² g⁻¹). Further amination of the cellulose scaffold allows covalent immobilization of functional biomolecules, such as a lectin protein concanavalin A (Con A) and biotin, on the lumen surfaces and inside the porous cell wall. The Con A immobilized scaffold demonstrates native glycoprotein-binding activity and possible glycoprotein separation application.

A delignified wood template with hydrophilic characteristics and high porosity was obtained by removal of lignin. Gelatin was infiltrated into the delignified wood and further crosslinked with a natural crosslinker genipin to form hydrogels. The composite hydrogels showed high mechanical strength under compression and low swelling in physiological condition. The effect of genipin concentrations (1, 50 and 100 mM) on structure and properties of the composite hydrogels were studied. A porous honeycomb structure with tunable pore size and porosity was observed in the freeze-dried composite hydrogels. High elastic modulus of 11.82 +/- 1.51 MPa and high compressive yield stress of 689.3 +/- 34.9 kPa were achieved for the composite hydrogel with a water content as high as 81%. The equilibrium water uptake of the freeze-dried hydrogel in phosphate buffered saline at 37 degrees C was as low as 407.5%. These enables the delignified wood structure an excellent template in composite hydrogel preparation by using infiltration and in-situ synthesis, particularly when high mechanical strength and stiffness are desired.

In the native wood cell wall, cellulose microfibrils are highly aligned and organized in the secondary cell wall. A new preparation strategy is developed to achieve individualization of cellulose microfibrils within the wood cell wall structure without introducing mechanical disintegration. The resulting mesoporous wood structure has a high specific surface area of 197 m2 g−1 when prepared by freeze‐drying using liquid nitrogen, and 249 m2 g−1 by supercritical drying. These values are 5 to 7 times higher than conventional delignified wood (36 m2 g−1) dried by supercritical drying. Such highly mesoporous structure with individualized cellulose microfibrils maintaining their natural alignment and organization can be processed into aerogels with high porosity and high compressive strength. In addition, a strong film with a tensile strength of 449.1 ± 21.8 MPa and a Young's modulus of 51.1 ± 5.2 GPa along the fiber direction is obtained simply by air drying owing to the self‐densification of cellulose microfibrils driven by the elastocapillary forces upon water evaporation. The self‐densified film also shows high optical transmittance (80%) and high optical haze (70%) with interesting biaxial light scattering behavior owing to the natural alignment of cellulose microfibrils.

The production of cellulose nanofibres (CNFs) typically requires harsh chemistry and strong mechanical fibrillation, both of which have negative environmental impacts. A possible solution is offered by lytic polysaccharide monooxygenases (LPMOs), oxidative enzymes that boost cellulose fibrillation. Although the role of LPMOs in oxidative modification of cellulosic substrates is rather well established, their use in the production of cellulose nanomaterials is not fully explored, and the effect of the carbohydrate-binding module (CBM) on nanofibrillation has not yet been reported. Herein, we studied the activity of two LPMOs, one of which was appended to a CBM, on delignified softwood fibres for green and energy-efficient production of CNFs. The CNFs were used to prepare cellulose nanopapers, and the structure and properties of both nanofibres and nanopapers were determined. Both enzymes were able to facilitate nanocellulose fibrillation and increase colloidal stability of the produced CNFs. However, the CBM-lacking LPMO was more efficient in introducing carboxyl groups (0.53 mmol/g) on the cellulose fibre surfaces and releasing CNFs with thinner width (4.3 ± 1.5 nm) from delignified spruce fibres than the modular LPMO (carboxylate content of 0.38 mmol/g and nanofibre width of 6.7± 2.5 nm through LPMO pretreatment followed by mild homogenisation. The prepared nanopapers showed improved mechanical properties (tensile strength of 262 MPa, and modulus of 16.2 GPa) compared to conventional CNFs preparation methods, demonstrating the potential of LPMOs as green alternatives for cellulose nanomaterials preparation.