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During the past decade, cellulose nanofibrils (CNFs) have shown tremendous potential as a building block to fabricate new advanced materials that are both biocompatible and biodegradable. The excellent mechanical properties of the individual CNF can be transferred to macroscale fibers through careful control in hydrodynamic alignment and assembly processes. The optimization of such processes relies on the understanding of nanofibril dynamics during the process, which in turn requires in situ characterization. Here, we use a shear-free mixing experiment combined with scanning small-angle X-ray scattering (scanning-SAXS) to provide time-resolved nanoscale kinetics during the in situ assembly of dispersed cellulose nanofibrils (CNFs) upon mixing with a sodium chloride solution. The addition of monovalent ions led to the transition to a volume-spanning arrested (gel) state. The transition of CNFs is associated with segmental aggregation of the particles, leading to a connected network and reduced Brownian motion, whereby an aligned structure can be preserved. Furthermore, we find that the extensional flow seems to enhance the formation of these segmental aggregates, which in turn provides a comprehensible explanation for the superior material properties obtained in shear-free processes used for spinning filaments from CNFs. This observation clearly highlights the need for different assembly strategies depending on morphology and interactions of the dispersed nanoparticles, where this work can be used as a guide for improved nanomaterial processes. 

Time-resolved in situ characterization of well-defined mixing processes using small-angle X-ray scattering (SAXS) is usually challenging, especially if the process involves changes of material viscoelasticity. In specific, it can be difficult to create a continuous mixing experiment without shearing the material of interest; a desirable situation since shear flow both affects nanoscale structures and flow stability as well as resulting in unreliable time-resolved data. Here, we demonstrate a flow-focusing mixing device for in situ nanostructural characterization using scanning-SAXS. Given the interfacial tension and viscosity ratio between core and sheath fluids, the core material confined by sheath flows is completely detached from the walls and forms a zero-shear plug flow at the channel center, allowing for a trivial conversion of spatial coordinates to mixing times. With this technique, the time-resolved gel formation of dispersed cellulose nanocrystals (CNCs) was studied by mixing with a sodium chloride solution. It is observed how locally ordered regions, so called tactoids, are disrupted when the added monovalent ions affect the electrostatic interactions, which in turn leads to a loss of CNC alignment through enhanced rotary diffusion. The demonstrated flow-focusing scanning-SAXS technique can be used to unveil important kinetics during structural formation of nanocellulosic materials. However, the same technique is also applicable in many soft matter systems to provide new insights into the nanoscale dynamics during mixing. 

Rice husks are an agricultural residue of great annual production and have a high cellulose content. In this study, we have prepared highly charged carboxyl cellulose nanofibers (CNFs) from rice husks using the TEMPO-oxidation method and the extracted CNFs were evaluated as an adsorbent for the removal of lead( ii ) and lanthanum( iii ) (Pb( ii ) and La( iii )) ions from contaminated water. Three different forms of nanocellulose adsorbents were prepared: suspension, freeze-dried, and nanocomposite containing magnetic nanoparticles, where their adsorption performance was tested against the removal of the two chosen heavy metal ions. The maximum adsorption capacity of rice husk based CNFs was found to be the highest in the nanocellulose suspension, i.e. , 193.2 mg g −1 for Pb( ii ) and 100.7 mg g −1 for La( iii ). The separation of the used adsorbent in the suspension was further facilitated by the gelation of the CNFs and metal cations, where the resulting floc could be removed by gravity-driven filtration. The absorption mechanism of the investigated CNF system is mainly due to electrostatic interactions between negatively charged carboxylate groups and multivalent metal ions. It was found that 90% lanthanum content in the form of lanthanum oxychloride (determined by X-ray powder diffraction) could be obtained by incinerating the CNF/LaCl 3 gel. This study demonstrates a viable and sustainable solution to upcycle agricultural residues into remediation nanomaterials for the removal and recovery of toxic heavy metal ions from contaminated water. 

Synthetic rubber produced from nonrenewable fossil fuel requires high energy costs and is dependent on the presumed unstable petroleum price. Natural rubber latex (NRL) is one of the major alternative sustainable rubber sources since it is derived from the plant ‘Hevea brasiliensis’. Our study focuses on integrating sustainably processed carboxycellulose nanofibers from untreated jute biomass into NRL to enhance the mechanical strength of the material for various applications. The carboxycellulose nanofibers (NOCNF) having carboxyl content of 0.94 mmol/g was prepared and integrated into its nonionic form (–COONa) for its higher dispersion in water to increase the interfacial interaction between NRL and NOCNF. Transmission electron microscopy (TEM) and atomic force microscopy (AFM) analyses of NOCNF showed the average dimensions of nanofibers were length (L) = 524 ± 203 nm, diameter (D) 7 ± 2 nm and thickness 2.9 nm. Furthermore, fourier transform infra-red spectrometry (FTIR) analysis of NOCNF depicted the presence of carboxyl group. However, the dynamic light scattering (DLS) measurement of NRL demonstrated an effective diameter in the range of 643 nm with polydispersity of 0.005. Tensile mechanical strengths were tested to observe the enhancement effects at various concentrations of NOCNF in the NRL. Mechanical properties of NRL/NOCNF films were determined by tensile testing, where the results showed an increasing trend of enhancement. With the increasing NOCNF concentration, the film modulus was found to increase quite substantially, but the elongation-to-break ratio decreased drastically. The presence of NOCNF changed the NRL film from elastic to brittle. However, at the NOCNF overlap concentration (0.2 wt. %), the film modulus seemed to be the highest. 

Nanocellulose, which can be derived from any cellulosic biomass, has emerged as an appealing nanoscale scaffold to develop inorganic–organic nanocomposites for a wide range of applications. In this study, titanium dioxide (TiO 2 ) nanocrystals were synthesized in the cellulose nanocrystal (CNC) scaffold using a simple approach, i.e. , hydrolysis of a titanium oxysulfate precursor in a CNC suspension at low temperature. The resulting TiO 2 nanoparticles exhibited a narrow size range between 3 and 5 nm, uniformly distributed on and strongly adhered to the CNC surface. The structure of the resulting nanocomposite was evaluated by transmission electron microscopy (TEM) and X-ray diffraction (XRD) methods. The growth mechanism of TiO 2 nanocrystals in the CNC scaffold was also investigated by solution small-angle X-ray scattering (SAXS), where the results suggested the mineralization process could be described by the Lifshitz–Slyozov–Wagner theory for Ostwald ripening. The demonstrated TiO 2 /CNC nanocomposite system exhibited excellent performance in dye degradation and antibacterial activity, suitable for a wide range of environmental remediation applications.