A novel multi-performance SHNC/SA/CaCl2 hydrogel with multi-performance was prepared via ultra-low-temperature freeze-thaw cycling and Ca2+ cross-linking for the removal of methylene blue (MB) from industrial wastewater. Various methods were used to characterize the structure and properties of hydrogel, and the internal structure of hydrogel showed a three-dimensional network with hydrogen and ester bonds. The SHNC/SA/CaCl2-15 hydrogel exhibited the highest tensile properties (elongation = 800 %), viscoelasticity (90 kPa), compressive strength (0.45 MPa), tensile strength (0.47 MPa) and ionic conductivity (4.34 S/cm). The maximum adsorption capacity of 2 g SHNC/SA/CaCl2-15 hydrogel was 608.49 mg/g at 40 °C, pH = 8 and adsorption 24 h. The adsorption process of hydrogel toward MB was more consistent with the second-order kinetic model and Langmuir isothermal adsorption model. According to the Langmuir isotherm model, the maximum monolayer adsorption capacity of SHNC/SA/CaCl2-15 hydrogel toward MB can reach 613.88 mg/g. Finally, it was found that the removal rate of SHNC/SA/CaCl2-15 hydrogel for MB was still as high as 90 % after five cycles of the adsorption-desorption test, and it could be reused. The hydrogel can be used as cheap and reusable adsorption material for cationic dyes. Our study provides a new perspective for the development of multifunctional cellulose hydrogel adsorbent materials.

As the most abundant and renewable natural resource, cellulose has attracted significant attention and research interest for the production of hydrogels (HGs). To address environmental issues and emerging demands, the benefits of naturally produced HGs include excellent mechanical properties and superior biocompatibility. HGs are three-dimensional networks created by chemical or physical cross-linking of linear or branched hydrophilic polymers and have high capacity for absorption of water and biological fluids. Although widely used in the food and biomedical fields, most HGs are not biodegradable. Nanocellulose hydrogels (NC-HGs) have been extensively applied in the food industry for detection of freshness, chemical additives, and substitutes, as well as the biomedical field for use as bioengineering scaffolds and drug delivery systems owing to structural interchangeability and stimuli-responsive properties. In this review article, the sources, structures, and preparation methods of NC-HGs are described, applications in the food and biomedical industries are summarized, and current limitations and future trends are discussed.

Enormous amounts of food resources are annually wasted because of microbial contamination, highlighting the critical role of effective food packaging in preventing such losses. However, traditional food packaging faces several limitations, such as low mechanical strength, poor fatigue resistance, and low water retention. In this study, we aimed to prepare nanocellulose hydrogels with enhanced stretchability, fatigue resistance, high water retention, and antibacterial properties using soy hull nanocellulose (SHNC), polyvinyl alcohol (PVA), sodium alginate (SA), and tannic acid (TA) as raw materials. These hydrogels were applied in food packaging to extend the shelf life of refrigerated chicken. The structure and properties (e.g., mechanical, antibacterial, and barrier properties) of these hydrogels were characterized using different techniques. Fourier-transform infrared spectroscopy revealed the presence of hydrogen and ester bonds in the hydrogels, whereas scanning electron microscopy revealed the three-dimensional network structure of the hydrogels. Mechanical testing demonstrated that the SHNC/PVA/SA/TA-2 hydrogel exhibited excellent tensile properties (elongation = 160 %), viscoelasticity (storage modulus of 1000 Pa), and mechanical strength (compressive strength = 10 kPa; tensile strength = 0.35 MPa). Moreover, under weak acidic and alkaline conditions, the ester bonds of the hydrogel broke down with an increase in pH, improving its swelling and release properties. The SHNC/PVA/SA/TA-2 hydrogel displayed an equilibrium swelling ratio exceeding 300 %, with a release rate of >80 % for the bioactive substance TA. Notably, antibacterial testing showed that the SHNC/PVA/SA/TA-2 hydrogel effectively deactivated Staphylococcus aureus and Escherichia coli, prolonging the shelf life of refrigerated chicken to 10 d. Therefore, the SHNC/PVA/SA/TA hydrogels can be used in food packaging to extend the shelf life of refrigerated meat products. Their cost-effectiveness and simple preparation make them suitable for various applications in the food industry.

Developing an environment-friendly preparation method for silver nanoparticles (AgNPs) composite is significant. However, it remains challenges in size adjustment and content improvement of AgNPs. Here, the NaIO4 oxidation and TEMPO-mediated oxidation were applied to bagasse pulp to prepare nanocellulose (NC) with both carboxyl and aldehyde groups. The aldehyde content of NC could be adjusted in the range of 0.21-1.45 mmol/g by different NaIO4 oxidation times. When the carboxyl groups were protonated, NC with a high length-diameter ratio could construct stable hydrogels in a low concentration at 0.5 wt%. The NC hydrogels showed excellent in situ synthesis ability of AgNPs with abundant pore structure. By regulating the carboxyl group content of NC, the size distribution of synthesized AgNPs could be controlled in the range of 7.14-28.6 nm with high content of 6.79-11.0 %. The NC/AgNPs composite hydrogel exhibited high catalytic degradation activity for 4-nitrophenol and antibacterial activity. This approach for constructing NC hydrogel paves the way for AgNPs composite products with adjustable sizes and high contents.

In nature, many biological tissues are composed of oriented structures, which endow tissues with special properties and functions. Although traditional hydrogels can achieve a high level of biomimetic composition, the orderly arrangement of internal structures remains a challenge. Therefore, it is of great significance to synthesize hydrogels with oriented structures easily and quickly. In this study, we first proposed and demonstrated a fabrication process for producing a well-ordered and dual-responsive cellulose nanofibers + hyaluronic acid methacrylate (CN+HAMA) hydrogels through an extrusion-based three-dimensional (3D) printing process. CN in the CN+HAMA hydrogels are directionally aligned after extrusion due to shear stress. In addition, the synthesized hydrogels exhibited responsive behaviors to both temperature and ultraviolet light. Since the temperature-responsiveness is reversible, the hydrogels can transit between the gelation and solution states while retaining their original qualities. Furthermore, the developed well-oriented CN+HAMA hydrogels induced directional cell growth, paving the way for potential applications in ordered biological soft-tissue repair.

Hydrogel was recognized as one of the most promising materials for adsorption of pharmaceuticals and personal care products (PPCPs). The highly efficient bio-based nanocelluloses fine-tuned poly(acrylic acid) hydrogel (PAA/NC) adsorbent was constructed by adjusting aspect ratio, surface charge and crystallinity of NC. The cross-linked networks were fabricated through a single-step free-radical polymerization via steric effect and hydrogen bonds. The uniform three-dimensional structures with abundant macropores and mesopores were in-situ visualized by the cryogenic-scanning electron microscopy (Cryo-SEM). The diclofenac adsorption capacity of TEMPO oxidized cellulose nanofibers (TCNF) incorporated PAA hydrogel (PAA/TCNF, 559.8 mg·g-1) was circa 2.1 times higher than pristine PAA (293.5 mg·g-1) due to the elevated specific surface area, favorable spatial structure with unimpeded channels and abundant surface-charged carboxylic groups. Moreover, PAA/NC hydrogel exhibited a wide-pH applicability and high salinity tolerance. The adsorption was predominantly determined by hydrogen bonds, validated by XPS and FT-IR analysis. It was demonstrated developed PAA/NC hydrogel with unique porous structure significantly enhanced adsorption capacity for potential application in the purification of refractory organic pollutants-containing wastewater.

A sugarcane bagasse nanocellulose-based hydrogel was developed as a colourimetric freshness indicator for monitoring spoilage of chicken breast. Nanocellulose was prepared from sugarcane bagasse cellulose filaments by TEMPO-mediated oxidation, and then used to form a strong self-standing hydrogel matrix through Zn2+ cross-linking. The hydrogel worked as a carrier for pH-responsive dyes (bromothymol blue/methyl red), which changed colour according to the freshness of the chicken sample. CO2 levels were found to increase with the spoilage of chicken, relative to rising levels of micro-organisms. The indicator hydrogel optical colour changed from green to red on the third day, as the log CFU/g passed the limit of acceptability for human consumption and emission of complicated volatiles. This new design of colourimetric freshness indicator made with a nanocellulose hydrogel has a quick response to chicken spoilage and is expected to facilitate the utilisation of bagasse nanocellulose as a value-added material in intelligent packaging.

Artificial stimuli-responsive hydrogels that can mimic natural extracellular matrix for growth and release of cancer spheroids (CSs) have attracted much attention. However, such hydrogels still face a challenge in regulating CSs growth and controlled release as well as keeping CSs integrity. Herein, a new class of ClO-/SCN- reversibly responsive nanocellulose hydrogel with fluorescence on-off reporter is developed. Upon addition of ClO-, the gel network of nanocellulose hydrogel was destructed, accompanying by the fluorescent quenching. Notably, when introducing of SCN-, a red fluorescence filamentous hydrogel was recovered by coordination cross-linking. The hydrogel reforms in a completely reversible process through the regulation of ClO-/SCN-. Benefit from the above response features of the hydrogel, the growth of cancer spheroids (CSs) in the hydrogel and on demand release of CSs from the hydrogel could be easily achieved through ClO-/SCN- regulation. Importantly, the growth and release of CSs can be monitored in real time by fluorescence imaging. Overall, such design strategy based on ClO-/SCN--responsive fluorescent hydrogels provided a new type of multi-responsive hydrogels as main scaffolds for cancer research and cancer drug screening.