We have produced foams from cellulose nanofibrils from upcycled cotton (upCNF) and wood (wCNF) through unidirectional (UIT) and multidirectional ice-templating (MIT) and investigated the structural humidity response through in-situ WAXS, SAXS, and micro tomography (μCT) between 10 and 95 % relative humidity (RH). The upCNF and wCNF WAXS patterns displayed a shape- and position shift as the RH was increased, with a compression in the (200) direction and an elongation in the (004) direction. The average separation distance extracted from the 1D SAXS patterns revealed no significant change for the upCNF foams regardless of RH and processing route, while a significant increase was observed for the wCNF foams. The μCT measurements of the upCNF foams showed a slight shift in macropore distribution towards larger pores between 50 and 80 % RH which can be attributed to the weakening and partial disintegration of the pore wall as more moisture is introduced. The humidity-induced structural alterations of the upCNF foam were significantly lower compared to the wCNF foams, confirming our claim of upCNF being more moisture resistant than wCNF foams.

The expanding field of lignin-containing nanocellulose offers a sustainable alternative to fossil-based substances in applications such as packaging, coatings, and composites. This has underscored the importance to explore the impact of raw materials due to the complexities of lignin structures and different raw fiber characteristics, which plays a significant role in determining the properties of the resultant lignin-rich cellulose materials. This study presents a detailed investigation and comparison on the production and structure-property relationships of lignin-containing microfibrillated cellulose (LMFC) fibers prepared from unbleached softwood and hardwood kraft pulps. The microfibrillation process was analyzed for both softwood and hardwood pulps, comparing the results across various stages of fibrillation. Distinguishing features of lignin structures in softwood and hardwood pulps were identified through Py-GC/MS analysis. Additionally, Digital Image Correlation was employed to investigate the varying failure patterns in LMFC films derived from different wood species. Softwood-derived LMFC films demonstrate less strain-concentrated regions and strain variation, attributed to the formation of more physical crosslinking joints by the elongated fibers. Consequently, softwood-origin LMFC films displayed superior load-sharing and enhanced tensile strength (287 MPa) compared to those derived from hardwood. Additionally, the denser lignin structures in unbleached softwood pulp further boosted the stiffness of resultant softwood-derived films. Upon recycling, LMFC films exhibited superior recovery of mechanical properties following drying, suggesting their significant potential for widespread commercial use.

The upcycling of discarded garments can help to mitigate the environmental impact of the textile industry. Here, we fabricated hybrid anisotropic foams having cellulose nanocrystals (CNCs), which were isolated from discarded cotton textiles and had varied surface chemistries as structural components, in combination with xanthan gum (XG) as a physical crosslinker of the dispersion used for foam preparation. All CNCs had crystallinity indices above 85 %, zeta potential values below -40 mV at 1 mM NaCl, and true densities ranging from 1.61 to 1.67 g center dot cm(-3). Quartz crystal microbalance with dissipation (QCM-D) measurements indicated weak interactions between CNC and XG, while rheology measurements showed that highly charged CNCs caused the XG chains to change from an extended to a helicoidal conformation, resulting in changes the in viscoelastic properties of the dispersions. The inclusion of XG significantly enhanced the compression mechanical properties of the freeze-casted foams without compromising their thermal properties, anisotropy, or degree of alignment. CNC-XG foams maintained structural integrity even after exposure to high humidity (91 %) and temperatures (100 degrees C) and displayed very low radial thermal conductivities. This research provides a viable avenue for upcycling cotton-based clothing waste into high-performance materials.

Nitric oxide (NO) holds promise for wound healing due to its antimicrobial properties and role in promoting vasodilation and tissue regeneration. The local delivery of NO to target cells or organs offers significant potential in numerous biomedical applications, especially when NO donors are integrated into nontoxic viscous matrices. This study presents the development of robust cellulose nanofibril (CNF) hydrogels designed to control the release of nitric oxide (NO) generated in situ from a NO-donor molecule (S-nitrosoglutathione, GSNO) obtained from the nitrosation of its precursor molecule glutathione (GSH). CNF, efficiently isolated from sugar cane bagasse, exhibited a high aspect ratio and excellent colloidal stability in water. Although depletion forces could be observed upon the addition of GSH, this effect did not significantly alter the morphology of the CNF network at low GSH concentrations (<20 mM). Ionic cross-linking with Ca²⁺ resulted in nontoxic and robust hydrogels (elastic moduli ranging from 300 to 3000 Pa) at low CNF solid content. The release rate of NO from GSNO decreased in CNF from 1.61 to 0.40 mmol. L^–1·h^–1 when the nanofibril content raised from 0.3 to 1.0 wt %. The stabilization effect monitored for 16 h was assigned to hydrogel mesh size, which was easily tailored by modifying the concentration of CNF in the initial suspension. These results highlight the potential of CNF-based hydrogels in biomedical applications requiring a precise NO delivery.

Bone defect repair, particularly in the alveolar region, remains a significant hurdle in periodontics. In recent years, the spotlight in regenerative medicine has fallen on 3D-printed bone scaffolds, especially those constructed of polylactic acid (PLA) infused with hydroxyapatite. This research introduced a novel approach by developing a 3D-printed PLA scaffold enriched with hydroxyapatite derived from fish skin waste (FSHA). Mechanical compression tests revealed that the 3D-printed PLA-FSHA scaffolds had a compressive strength (13.4 ± 5.53 MPa) in the same ballpark as their reference PLA counterparts (20.3 ± 1.08 MPa). Scanning electron micrographs highlighted an average pore size in the scaffold (572 ± 33 μm) conducive to angiogenesis and facilitating cell migration and proliferation. In vitro, cytotoxicity was ascertained using the MTT assay on L929 fibroblast cells. Further in vitro cytocompatibility assessments through actin-DAPI staining and measurements of bone regeneration markers - alkaline phosphatase, osteocalcin and osteopontin-demonstrated that the PLA-FSHA scaffolds not only were biocompatible but also showcased performance on par with the commercial graft, osseograft. This lays the foundation for future in vivo evaluations of bone regenerative capabilities.

The linear lifecycle of the textile industry contributes to the enormous waste generation of post-consumer garments. Recycling or repurposing of post-consumer garments typically requires separation of the individual components. This study describes a novel and facile chemo-thermo-mechanical method for producing extrudable pellets, involving one-pot, 2,2,6,6-Tetramethylpiperidine-1-oxyl (TEMPO)-mediated oxidation of post-consumer polycotton textiles, followed by mild mechanical treatment, all without isolating the constituents of the polycotton blend. The oxidized blend with high cellulose and carboxylate content of 1221 ± 82 mmol COO− per kg of cotton, is pelletised into a masterbatch and further in situ extruded into nanocomposite filaments for 3D printing. The carboxyl groups introduced on the polycotton-based filters enable cotton fibrillation into nanoscaled fibers during mechanical treatment and extrusion resulting to a variety of functional and high surface-finish quality models, including filters and fashion accessories. The electrostatic interactions with positively charged species, such as methylene blue (MB), facilitate their adsorption from water while exhibiting promising adsorption capacities. The adsorption of MB follows the Freundlich model and depends on the printed porosity of the filter. A “trash to treasure” concept for textile waste is further corroborated through the use of the developed 3D printing filament into commodity products.

Bionanocomposites comprising biobased polymers and nanosized bio-based fillers are novel materials with tunable properties and have diverse applications in packaging, environmental remediation and the biomedical sector. Bionanocomposite materials also have a significant role to play in the implementation of a functional circular economy.

In this themed issue, leading researchers from academia and industry were invited to submit reviews or their latest research on topics aligned to the development of bionanocomposites from renewable resources. Studies dealing with waste conversion to bio-based products and the development of bionanocomposites have been included in this issue. This issue consists of 7 research articles.

As guest editors of this themed issue, we acknowledge all the authors and reviewers who have contributed to its publication. We would also like to thank the technical support team at the Royal Society of Chemistry for their assistance in preparing this themed issue.

As a versatile nanomaterial derived from renewable sources, nanocellulose has attracted considerable attention for its potential applications in various sectors, especially those focused on water treatment and remediation. Here, we have combined atomic force microscopy (AFM) and reactive molecular dynamics (RMD) simulations to characterize the interactions between cellulose nanofibers modified with carboxylate or phosphate groups and the protein foulant model bovine serum albumin (BSA) at pH 3.92, which is close to the isoelectric point of BSA. Colloidal probes were prepared by modification of the AFM probes with the nanofibers, and the nanofiber coating on the AFM tip was for the first time confirmed through fluorescence labeling and confocal optical sectioning. We have found that the wet-state normalized adhesion force is approximately 17.87 +/- 8.58 pN/nm for the carboxylated cellulose nanofibers (TOCNF) and about 11.70 +/- 2.97 pN/nm for the phosphorylated ones (PCNF) at the studied pH. Moreover, the adsorbed protein partially unfolded at the cellulose interface due to the secondary structure's loss of intramolecular hydrogen bonds. We demonstrate that nanocellulose colloidal probes can be used as a sensitive tool to reveal interactions with BSA at nano and molecular scales and under in situ conditions. RMD simulations helped to gain a molecular- and atomistic-level understanding of the differences between these findings. In the case of PCNF, partially solvated metal ions, preferentially bound to the phosphates, reduced the direct protein-cellulose connections. This understanding can lead to significant advancements in the development of cellulose-based antifouling surfaces and provide crucial insights for expanding the pH range of use and suggesting appropriate recalibrations.

Recycled textiles are becoming widely available to consumers as manufacturers adopt circular economy principles to reduce the negative impact of garment production. Still, the quality of the source material directly impacts the final product, where the presence of harmful chemicals is of utmost concern. Here, we develop a risk-based suspect and non-targeted screening workflow for the detection, identification, and prioritization of the chemicals present in consumer-based recycled textile products after manufacture and transport. We apply the workflow to characterize 13 recycled textile products from major retail outlets in Sweden. Samples were extracted and analyzed by liquid chromatography coupled with high-resolution mass spectrometry (LC-HRMS). In positive and negative ionization mode, 20,119 LC-HRMS features were detected and screened against persistent, mobile, and toxic (PMT) as well as other textile-related chemicals. Six substances were matched with PMT substances that are regulated in the European Union (EU) with a Level 2/3 confidence. Forty-three substances were confidently matched with textile-related chemicals reported for use in Sweden. For estimating the relative priority score, aquatic toxicity and concentrations were predicted for 7416 features with tandem mass spectra (MS2) and used to rank the non-targeted features. The top 10 substances were evaluated due to elevated environmental risk linked to the recycling process and potential release at end-of-life.

Polyethylene terephthalate (PET) is one of the most common plastics and can be cascaded mechanically during its life cycle. However, recycling affects the mechanical properties of the material, and the virgin material is constantly in demand. If a worn material could be depolymerized to its chemical building blocks, then a virgin polymer could be generated from old fibers. In this work, we have developed a benign organo-catalytic depolymerization of PET to yield dimethyl terephthalate (DMT) and ethylene glycol (EG) without the need for purification of generated monomers. By recirculating the solvent and organo-catalyst, a solvent/substrate ratio of 3:1 was achieved. The depolymerization was successfully applied to other polyesters, polycarbonates, and polycotton. The cotton isolated from the polycotton depolymerization was successfully processed into viscose fibers with a tenacity in the range of nonwaste cotton-derived viscose filaments. The global warming potential (GWP) of PET depolymerization was evaluated by using life cycle assessment (LCA). The GWP of 1 kg PET recycling is 2.206 kg CO₂ equivalent, but the process produces DMT, EG, and heat, thereby avoiding the emissions equivalent to 4.075 kg CO₂ equivalent from the DMT, EG, and steam-energy production through conventional pathways. Thus, the net result potentially avoids the emission of 1.88 kg of CO₂ equivalent. The impact of this process is lower than that of waste PET incineration and conventional PET recycling technologies.