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Enhancing the sorption properties of cellulose is a prerequisite for its efficient use in water purification as an alternative to costly activated carbon. Here, solvent-free phosphorylation of cellulose using environmentally benign and non-toxic chemicals was pursued resulting in a negatively charged material that was used to remove methylene blue (MB) from aqueous solution. Three different cellulose sources were selected, i.e., locally abundant Alfa grass, wood, and microcrystalline cellulose, with the aim to investigate the effect of the cellulose source on the functionalization degree and the removal efficiency of methylene blue. The poor MB adsorption capacity of native cellulose (12–40 mg g−1) reached exceptionally high values after phosphorylation (446–705 mg g−1) resulting in one of the most promising bio-based sorbents reported up-to-date. The highest phosphorylation degree was registered on cellulose from wood conferring it with the maximum adsorption properties. Curve-fitting experimental results revealed that the adsorption data were well described by the Langmuir equation and that the pseudo-second-order kinetic represents well the interactions between cellulose and MB molecules. Finally, we show the possibility to release MB from a used sorbent when it is successively washed with phosphate ions leading to a quasi-total (97%) regeneration.

Alfa fibers (Stipa Tenacissima) were effectively utilized in this study as a promising cellulose source for isolation of carboxy-functionalized cellulose nanofibrils (CNFs) using multiple treatments. Pure cellulose microfibers (CMFs) were firstly extracted by alkali and bleaching treatments. CNFs with an average nanofibrils diameter ranging from 1.4 to 4.6 nm and a crystallinity of 89% were isolated from CMFs by a combination of TEMPO-oxidation and mechanical disintegration processes. The morphology and physico-chemical properties of cellulosic materials were evaluated at different stages of treatments using several characterization techniques. Various CNF loadings (5–15 wt%) were incorporated into PVA polymer to evaluate the nanoreinforcement ability of CNFs and to produce CNF-filled PVA nanocomposite materials. The tensile and optical transmittance properties, as well as the morphological and thermal properties of the as-produced CNF-filled PVA nanocomposite films were investigated. It was found that the tensile modulus and strength of nanocomposites were gradually increased with increasing of CNF loadings, with a maximum increase of 90% and 74% was observed for a PVA nanocomposite containing 15 wt% CNFs, respectively. The optical transmittance was reduced from 91% (at 650 nm) for neat PVA polymer to 88%, 82% and 76% for PVA nanocomposites containing 5, 10 and 15 wt% CNFs, respectively. It was also found that the glass transition temperature was gradually increased from 76 °C for neat PVA to 89 °C for PVA nanocomposite containing 15 wt%. This study demonstrates the importance of Alfa fibers as annual renewable lignocellulosic material to produce CNFs with good morphology and excellent properties. These newly developed carboxy-functionalized CNFs could be considered as a potential nanofiller candidate for the preparation of nanocomposite materials of high transparency and good mechanical properties.

The present work describes the production of novel highly hydrated cellulose microfibrils (CMFs) with unique morphology from coffee pulp waste using specific chemical treatments. The as-produced CMFs were successfully characterized and then used as an adsorbent for removal of methylene blue (MB) from concentrated aqueous solutions. Surprisingly, it was found that the novel CMFs display high water-uptake ability, with a maximum swelling ratio of 265%, and that they form an entangled hydrated network gel in water. The morphological observation and nitrogen adsorption measurement demonstrated that the extracted CMFs exhibit an average fibril diameter of 11.5 µm and mesoporous structure with an average pore size of 6.37 nm. These special features make the as-produced CMFs excellent candidates to be used as adsorbents for removal of MB from concentrated solutions. The performed adsorption studies determined that the adsorption equilibrium was reached within 90 min. The adsorption kinetics data were well fitted to the pseudo-second-order kinetic model, and the adsorption isotherms were well described by the Freundlich isotherm model. In addition, the maximum adsorption capacity was 182.5 mg/g, much higher than that determined for other previously reported cellulose-based adsorbents. Through this study, we have demonstrated a possible strategy to give an added value to the coffee pulp waste, a by-product of the coffee processing industry, which is rich in cellulose, inexpensive and renewable source. Indeed, the extracted CMFs are very attractive for developing a sustainable and economically viable bio-sourced material for future growth of cellulose use in advanced applications.

Cellulose nanocrystals (CNC) were extracted from Miscanthus (MST) fibers using a sulfuric acid hydrolysis process. The results showed that the obtained CNC exhibit a needle-like shape with an average aspect ratio of 37. The surface charge density was measured at 1.99 sulfate groups per 100 anhydroglucose units while the zeta potential value was found to be -38 mV. The crystallinity of the extracted CNC was 76%, and the cellulose I type crystal structure was predominant. Due to its high importance for potential application of CNC in aqueous systems, the rheological behavior of CNC aqueous suspensions at various CNC concentrations was determined. The CNC suspensions showed gel-like behavior at very low CNC concentrations ranging from 0.1 wt% up to 0.6 wt%, as confirmed by the steady shear viscosity measurements and the oscillatory dynamic tests. The dynamic rheological parameters of CNC suspensions were slightly affected by the temperature profile. At high temperature up to 80 °C a stronger CNC network is formed by increasing the relative motion resistance of CNC macromolecules and the entanglement. In order to identify the reinforcing ability of the newly extracted CNC, starch-based nanocomposite films were produced with various CNC contents (1, 3, 5 and 8 wt%) and their tensile properties were investigated. It was found that the addition 8 wt% CNC within starch matrix increased the Young’s modulus by 150% and the tensile strength by 118%, resulting in mechanically strong and eco-friendly nanocomposite materials.