Chitin-glucan complex (CGC) hydrogels were fabricated through a freeze–thaw procedure for biopolymer dissolution in NaOH 5 mol/L, followed by a dialysis step to promote gelation. Compared to a previously reported methodology that included four freeze–thaw cycles, reducing the number of cycles to one had no significant impact on the hydrogels’ formation, as well as reducing the total freezing time from 48 to 18 h. The optimized CGC hydrogels exhibited a high and nearly spontaneous swelling ratio (2528 ± 68%) and a water retention capacity of 55 ± 3%, after 2 h incubation in water, at 37 °C. Upon loading with caffeine as a model drug, an enhancement of the mechanical and rheological properties of the hydrogels was achieved. In particular, the compressive modulus was improved from 23.0 ± 0.89 to 120.0 ± 61.64 kPa and the storage modulus increased from 149.9 ± 9.8 to 315.0 ± 76.7 kPa. Although the release profile of caffeine was similar in PBS and NaCl 0.9% solutions, the release rate was influenced by the solutions’ pH and ionic strength, being faster in the NaCl solution. These results highlight the potential of CGC based hydrogels as promising structures to be used as drug delivery devices in biomedical applications.

In line with environmental awareness movements and social concerns, the textile industry is prioritizing sustainability in its strategic planning, product decisions, and brand initiatives. The use of non-biodegradable materials, obtained from non-renewable sources, contributes heavily to environmental pollution throughout the textile production chain. As sustainable alternatives, considerable efforts are being made to incorporate biodegradable biopolymers derived from residual biomass, with reasonable production costs, to replace or reduce the use of synthetic petrochemical-based polymers. However, the commercial deployment of these biopolymers is dependent on high biomass availability and a cost-effective supply. Residual forest biomass, with lignocellulosic composition and seasonably available at low cost, constitutes an attractive renewable resource that might be used as raw material. Thus, this review aims at carrying out a comprehensive analysis of the existing literature on the use of residual forest biomass as a source of new biomaterials for the textile industry, identifying current gaps or problems. Three specific biopolymers are considered: lignin that is recovered from forest biomass, and the bacterial biopolymers poly(hydroxyalkanoates) (PHAs) and bacterial cellulose (BC), which can be produced from sugar-rich hydrolysates derived from the polysaccharide fractions of forest biomass. Lignin, PHA, and BC can find use in textile applications, for example, to develop fibers or technical textiles, thus replacing the currently used synthetic materials. This approach will considerably contribute to improving the sustainability of the textile industry by reducing the amount of non-biodegradable materials upon disposal of textiles, reducing their environmental impact. Moreover, the integration of residual forest biomass as renewable raw material to produce advanced biomaterials for the textile industry is consistent with the principles of the circular economy and the bioeconomy and offers potential for the development of innovative materials for this industry.

Chitin-glucan complex (CGC) hydrogels were fabricated by coagulation of the biopolymer from an aqueous alkaline solution, and their morphology, swelling behavior, mechanical, rheological, and biological properties were studied. In addition, their in vitro drug loading/release ability and permeation through mimic-skin artificial membranes (Strat-M) were assessed. The CGC hydrogels prepared from 4 and 6 wt% CGC suspensions (Na5₁*⁴ and Na5₁*⁶ hydrogels, respectively) had polymer contents of 2.40 ± 0.15 and 3.09 ± 0.22 wt%, respectively, and displayed a highly porous microstructure, characterized by compressive moduli of 39.36 and 47.30 kPa and storage moduli of 523.20 and 7012.25 Pa, respectively. Both hydrogels had a spontaneous and almost immediate swelling in aqueous media, and a high-water retention capacity (>80%), after 30 min incubation at 37 °C. Nevertheless, the Na5₁*⁴ hydrogels had higher fatigue resistance and slightly higher-water retention capacity. These hydrogels were loaded with caffeine, ibuprofen, diclofenac, or salicylic acid, reaching entrapment efficiency values ranging between 13.11 ± 0.49% for caffeine, and 15.15 ± 1.54% for salicylic acid. Similar release profiles in PBS were observed for all tested APIs, comprising an initial fast release followed by a steady slower release. In vitro permeation experiments through Strat-M membranes using Franz diffusion cells showed considerably higher permeation fluxes for caffeine (33.09 µg/cm²/h) and salicylic acid (19.53 µg/cm²/h), compared to ibuprofen sodium and diclofenac sodium (4.26 and 0.44 µg/cm²/h, respectively). Analysis in normal human dermal fibroblasts revealed that CGC hydrogels have no major effects on the viability, migration ability, and morphology of the cells. Given their demonstrated features, CGC hydrogels are very promising structures, displaying tunable physical properties, which support their future development into novel transdermal drug delivery platforms.

In recent years, polyhydroxyalkanoates (PHAs) have gained notoriety because of their desirable properties that include proven biodegradability, biocompatibility, and thermal stability, which make them suitable alternatives to fossil-based polymers. However, the widespread use of PHAs is still challenging because of their production costs, which are greatly associated with the cultivation medium used for bacterial cultivation. In Portugal, one-quarter of the forest area is covered by Eucalyptus globulus wood, making its residues a cheap, abundant, and sustainable potential carbon source for biotechnological uses. In this work, eucalyptus bark was used as the sole feedstock for PHA production in a circular bioeconomic approach. Eucalyptus bark hydrolysate was obtained after enzymatic saccharification using Cellic^® CTec3, resulting in a sugar-rich solution containing glucose and xylose. Although with differing performances, several bacteria were able to grow and produce PHA with distinct compositions, using the enzymatic hydrolysate as the sole carbon source. Pseudomonas citronellolis NRRL B-2504 achieved a high cellular growth rate in bioreactor assays (24.4 ± 0.15 g/L) but presented a low accumulation of a medium-chain-length PHA (mcl-PHA) comprising the monomers hydroxydecanoate (HD, 65%), hydroxydodecanoate (HDd, 25%), and hydroxytetradecanoate (HTd, 14%). Burkholderia thailandensis E264, on the other hand, reached a lower cellular growth rate (8.87 ± 0.34 g/L) but showed a higher biopolymer accumulation, with a polyhydroxybutyrate (PHB) content in the cells of 12.3 wt.%. The new isolate, Pseudomonas sp., revealed that under nitrogen availability, it was able to reach a higher accumulation of the homopolymer PHB (31 wt.%). These results, although preliminary, demonstrate the suitability of eucalyptus bark’s enzymatic hydrolysate as a feedstock for PHA production, thus offering an exciting avenue for achieving sustainable and environmentally responsible plastic products from an undervalued forestry waste.