In temperature sensitive hydrogels, the swelling degree or light transmittance of the gel itself changes with variations in ambient temperature, prompting its wide application in controlled drug release, tissue engineering, and material separation. Considering the amphiphilic structure of β-cyclodextrin (β-CD), a cellulose-based supramolecular hydrogel with superior temperature sensitivity was synthesized based on a combination of cellulose and β-CD as well as the host–guest interaction between β-CD and polypropylene glycol (PPG). In the one-pot tandem reaction process, chemical grafting of β-CD on cellulose and the inclusion complexation of β-CD with PPG were performed simultaneously in a NaOH/urea/water system. The obtained supramolecular hydrogel had a lower critical solution temperature (LCST) of 34 °C. There existed covalent bonding between the cellulose and β-CD, host–guest complexation between the β-CD and PPG, and hydrogen bonding and hydrophobic interactions between the components in the network structure of the supramolecular hydrogel. The combination of various covalent and non-covalent bonds endowed the resulting supramolecular hydrogel with good internal network structure stability and thermal stability, as well as sensitive temperature responsiveness within a certain range—implying its potential as a smart material in the fields of medicine, biology, and textiles. This work is expected to bring new strategies for the fabrication of cellulose-based thermosensitive materials, benefitting the high-value utilization of cellulose.

The high mechanical strength, large specific surface area, favorable biocompatibility, and degradability of nanocellulose (CNC) enable it to be a potential alternative to petroleum-based materials. However, the traditional preparation of CNCs requires a large amount of strong acid, which poses a serious challenge to equipment maintenance, waste liquid recycling, and economics. In this study, a solid and easily recoverable zirconium phosphate (ZrP) was used to assist in the phosphoric acid co-catalyzed hydrolysis of lignocellulose for extracting CNCs. Due to the presence of acidic phosphate groups, ZrP has a strong active center with a high catalytic activity. With the assistance of ZrP, the amount of phosphoric acid used in the reaction is significantly reduced, improving the equipment’s durability and economic efficiency. The effects of the process conditions investigated were the phosphate acid concentration, reaction temperature, and reaction time on the yield of CNCs. The Box–Behnken design (BBD) method from the response surface methodology (RSM) was applied to investigate and optimize the preparation conditions. The optimized pre-treatment conditions were 49.27% phosphoric acid concentration, 65.38 °C reaction temperature, and 5 h reaction time with a maximal cellulose yield (48.33%). The obtained CNCs show a granular shape with a length of 40~50 nm and a diameter of 20~30 nm, while its high zeta potential (−24.5 mV) make CNCs present a stable dispersion in aqueous media. Moreover, CNCs have a high crystallinity of 78.70% within the crystal type of cellulose Ⅰ. As such, this study may pioneer the horizon for developing a green method for the efficient preparation of CNC, and it is of great significance for CNCs practical production process.

Based on the self-passivation function of chitosan, an efficient, and green synthesis strategy was applied to prepare chitosan carbon dots (CDs). The quantum yield of carbon dots reached 35% under the conditions of hydrothermal temperature of 200 °C, hydrothermal time of 5 h, and chitosan concentration of 2%. Moreover, the obtained carbon dots had high selectivity and sensitivity to Fe³⁺. Based on the Schiff base reaction between the aldehyde groups of dialdehyde cellulose nanofibrils (DNF) and the amino groups of CDs, a chemically cross-linked, novel, fluorescent composite film, with high transparency and high strength, was created using one-pot processing. Knowing that the fluorescence effect of the composite film on Fe³⁺ had a linear relationship in the concentration range of 0–100 μM, a fluorescent probe can be developed for quantitative analysis and detection of Fe³⁺. Owing to their excellent fluorescent and mechanical properties, the fluorescent nanocomposite films have potential applications in the fields of Fe³⁺ detection, fluorescent labeling, and biosensing.

The high strength, high specific surface area, excellent biocompatibility, and degradability of nanocellulose (NCC) make it a potential reinforcing phase for composite materials. However, the polyhydroxyl property of NCC renders it prone to self-aggregation and it has weak interfacial compatibility with non-polar substrates, limiting its enhancement performance for composite materials. Therefore, based on the high reactivity of NCC, the chemical modification of NCC to introduce functional groups is the basis for effectively reducing its self-aggregation, improving its interfacial compatibility with the polymer matrix, and creating nanocellulose-based functional materials. The existing functional modifications of NCC have limitations; they require cumbersome steps, generate low yields, and are environmentally unfriendly. Herein, ureido-pyrimidinone (UPy) was introduced to NCC through a sustainable and high-efficiency avenue formed by the mechanochemical synergy of microwaves and ultrasonication. The obtained UPy-modified nanocellulose (NCC-UPy) exhibited a rod-like shape, with a length of 200–300 nm and a width of 20–30 nm, which presented oriented and stable dispersion in an aqueous medium, and the zeta potential reached −40 mV. Moreover, NCC-UPy had good thermostability (>350 °C) and high crystallinity (82.5%) within the crystal type of cellulose I. Using the as-prepared NCC-UPy as a molecular bridge, it was organically combined with epoxy resin through multiple hydrogen bonds to construct a nanocomposite membrane with superior mechanical strength and thermal stability. The results revealed that NCC-UPy dispersed uniformly in the epoxy matrix without aggregating and that the interfacial compatibility was good, leading to an 87% increase in the tensile strength of the formed nanocomposite membrane when 0.5 wt.% NCC-UPy was loaded. It was proved that NCC-UPy had remarkable reinforcing potential and effective stress transfer capacity for composites. Consequently, this study may open the door to the development of a one-pot green approach for undertaking the functional modification of NCC, and it is of great significance for the development of NCC-based nanocomposites.

Fluorescent cellulose nanofibers (FCNFs), with a high yield, were prepared via one-pot hydrolysis and the grafting reaction of cellulose with thiazolipyridine carboxylic acid (TPCA). The hydrolysis and Fischer esterification of cellulose were conducted under microwave-hydrothermal conditions; meanwhile, TPCA formation was induced by the dehydration reaction between L-cysteine and citric acid. The effects of the reaction temperature and reaction time on the yield and performance of FCNF were investigated. The morphology and size, surface chemical property, crystal structure, thermostability, and fluorescent performance of FCNF were characterized. The results revealed that the yield of FCNF reached 73.2% under a microwave power of 500 W, reaction temperature of 110 °C, and reaction time of 5 h. The FCNF obtained presents a short rod-like morphology. The crystallinity of the FCNFs is 80%, and their thermal stability did not decline significantly. Additionally, the fluorescent performance of the FCNFs is excellent, which results in them having good sensitivity to chloride ions. The good fluorescent performance and significant responsiveness to chloride ions of FCNFs lead to them having broad prospects in bio-labeling, biosensing, information storage, chloride ion detection, among others.