Multivalent ion-induced re-entrant transition of carboxylated cellulose nanofibrils and its influence on nanomaterials’ properties

Valencia, Luis; Nomena, Emma M.; Monti, Susanna; Rosas-Arbelaez, Walter; Mathew, Aji P.; Kumar, Sugam; Velikov, Krassimir P.

doi:10.1039/d0nr02888f

Cited by 34 publications

(28 citation statements)

References 54 publications

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“…Grafting onto cellulose has also been extended to produce hybrid materials based on CNs such as cellulose-metal-organic frameworks (celloMOFs) [42,43], TiO 2 / nanocellulose [44], graphene oxide/nitrocellulose [45]. For example, Aji P. Mathew et al reported the ability to use nanocellulose as a platform for the in-situ formation of metal oxide nanoparticles on its surface as illustrated in Figure 5 [46,47]. The authors demonstrated that carboxylated cellulose nanofibril-based films can spontaneously grow functional metal oxide nanoparticles, for example, Cu 2 O, during the adsorption of Cu(II) ions, without any further chemical or temperature treatment.…”

Section: Grafting On Cellulosementioning

confidence: 99%

Cellulose Nanomaterials as a Future, Sustainable and Renewable Material

et al. 2022

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Cellulose nanomaterials (CNs) are renewable, bio-derived materials that can address not only technological challenges but also social impacts. This ability results from their unique properties, for example, high mechanical strength, high degree of crystallinity, biodegradable, tunable shape, size, and functional surface chemistry. This minireview provides chemical and physical features of cellulose nanomaterials and recent developments as an adsorbent and an antimicrobial material generated from bio-renewable sources.

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Section: Grafting On Cellulosementioning

confidence: 99%

Cellulose Nanomaterials as a Future, Sustainable and Renewable Material

et al. 2022

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“…Among all the different methods to obtain cellulose nanofibers (CNFs) proposed in the literature, the selective oxidation of C6 cellulose hydroxyls catalyzed by the stable radical 2,2,6,6-Tetramethyl-1-piperidinyloxy (TEMPO) represents one of the most diffused approaches [ 10 , 11 , 12 , 13 , 14 ]. From TEMPO-oxidized CNFs (TOCNFs) aqueous dispersions it is possible to obtain physically crosslinked hydrogels by means of divalent cation addition [ 15 , 16 , 17 , 18 ]. Recently, cellulose and its derivative have been widely investigated leading to different applications in the biomedical field [ 19 ].…”

Section: Introductionmentioning

confidence: 99%

Bioactive Hydrogels: Design and Characterization of Cellulose-Derived Injectable Composites

et al. 2021

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Cellulose represents a low cost, abundant, and renewable polysaccharide with great versatility; it has a hierarchical structure composed of nanofibers with high aspect ratio (3–4 nm wide, hundreds of μm long). TEMPO-mediated oxidation represents one of the most diffused methods to obtain cellulose nanofibers (CNFs): It is possible to obtain physically crosslinked hydrogels by means of divalent cation addition. The presence of inorganic components, such as calcium phosphates (CaP), can improve not only their mechanical properties but also the bioactivity of the gels. The aim of this work is to design and characterize a TEMPO-oxidized cellulose nanofibers (TOCNFs) injectable hydrogel embedded with inorganic particles, CaP and CaP-GO, for bone tissue regeneration. Inorganic particles act as physical crosslinkers, as proven by rheological characterization, which reported an increase in mechanical properties. The average load value registered in injection tests was in the range of 1.5–4.4 N, far below 30 N, considered a reasonable injection force upper limit. Samples were stable for up to 28 days and both CaP and CaP-GO accelerate mineralization as suggested by SEM and XRD analysis. No cytotoxic effects were shown on SAOS-2 cells cultured with eluates. This work demonstrated that the physicochemical properties of TOCNFs-based dispersions could be enhanced and modulated through the addition of the inorganic phases, maintaining the injectability and bioactivity of the hydrogels.

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“…For example, 2,2,6,6-tetramethyl-piperidin-1-yl)oxyl (TEMPO) mediated oxidation is commonly used to introduce negatively charged carboxyl groups to the cellulose surface, which is key to enhance the stability of particle dispersions in aqueous media due to electrostatic repulsion forces [4,5]. Cellulose nanofibrils have been extensively used to form hydrogels where the properties can be modulated by various factors such as salts [6,7], pH [8,9], concentration [10,11], temperature [12], and surfactants [13][14][15]. In addition, OCNF hydrogels have been reported to have excellent shear-thinning properties, which is desirable for 2 of 17 some formulation-based products, especially in health and personal care applications [13].…”

Section: Introductionmentioning

confidence: 99%

“…Both OCNF and starch are anionic hydrocolloids with different charge densities; therefore, understanding the interactions between these two species during gelation is important to describe their rheological properties. The addition of counter-ions (for example, salts) can be utilised to screen the repulsive forces between the OCNF fibrils [6,7] and starch [33]. However, excess counter-ions can lead to complete screening of the repulsive interactions, leading to stronger attractive forces, which often cause gel precipitation and syneresis.…”

Section: Introductionmentioning

confidence: 99%

Monovalent Salt and pH-Induced Gelation of Oxidised Cellulose Nanofibrils and Starch Networks: Combining Rheology and Small-Angle X-ray Scattering

et al. 2021

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Water quality parameters such as salt content and various pH environments can alter the stability of gels as well as their rheological properties. Here, we investigated the effect of various concentrations of NaCl and different pH environments on the rheological properties of TEMPO-oxidised cellulose nanofibril (OCNF) and starch-based hydrogels. Addition of NaCl caused an increased stiffness of the OCNF:starch (1:1 wt%) blend gels, where salt played an important role in reducing the repulsive OCNF fibrillar interactions. The rheological properties of these hydrogels were unchanged at pH 5.0 to 9.0. However, at lower pH (4.0), the stiffness and viscosity of the OCNF and OCNF:starch gels appeared to increase due to proton-induced fibrillar interactions. In contrast, at higher pH (11.5), syneresis was observed due to the formation of denser and aggregated gel networks. Interactions as well as aggregation behaviour of these hydrogels were explored via ζ-potential measurements. Furthermore, the nanostructure of the OCNF gels was probed using small-angle x-ray scattering (SAXS), where the SAXS patterns showed an increase of slope in the low-q region with increasing salt concentration arising from aggregation due to the screening of the surface charge of the fibrils.

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Multivalent ion-induced re-entrant transition of carboxylated cellulose nanofibrils and its influence on nanomaterials’ properties

Abstract: In this work, we demonstrate a re-entrant transition of carboxylated cellulose nanofibrils hydrogel where the gel-strength abruptly increases and then decreases back upon monotonic increase in multivalent salt concentration.

Cited by 34 publications

References 54 publications

Cellulose Nanomaterials as a Future, Sustainable and Renewable Material

Cellulose Nanomaterials as a Future, Sustainable and Renewable Material

Bioactive Hydrogels: Design and Characterization of Cellulose-Derived Injectable Composites

Monovalent Salt and pH-Induced Gelation of Oxidised Cellulose Nanofibrils and Starch Networks: Combining Rheology and Small-Angle X-ray Scattering

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