Carboxylated cellulose nanofibers, prepared by TEMPO-mediated oxidation (TOCN), were processed into asymmetric mesoporous membranes using a facile paper-making approach and investigated as lithium ion battery separators. Membranes made of TOCN with sodium carboxylate groups (TOCN-COO-Na+) showed capacity fading after a few cycles of charging and discharging. On the other hand, its protonated counterpart (TOCN-COOH) showed highly improved electrochemical and cycling stability, displaying 94.5% of discharge capacity maintained after 100 cycles at 1 C rate of charging and discharging. The asymmetric surface porosity of the membranes must be considered when assembling a battery cell as it influences the rate capabilities of the battery. The wood-based TOCN-membranes have a good potential as an ecofriendly alternative to conventional fossil fuel-derived separators without adverse side effects.

Carboxylated cellulose nanofibers (CNF) prepared using the TEMPO-route are good binders of electrode components in flexible lithium-ion batteries (LIB). However, the different parameters employed for the defibrillation of CNF such as charge density and degree of homogenization affect its properties when used as binder. This work presents a systematic study of CNF prepared with different surface charge densities and varying degrees of homogenization and their performance as binder for flexible LiFePO4 electrodes. The results show that the CNF with high charge density had shorter fiber lengths compared with those of CNF with low charge density, as observed with atomic force microscopy. Also, CNF processed with a large number of passes in the homogenizer showed a better fiber dispersibility, as observed from rheological measurements. The electrodes fabricated with highly charged CNF exhibited the best mechanical and electrochemical properties. The CNF at the highest charge density (ISSO mu mol g(-1)) and lowest degree of homogenization (3 + 3 passes in the homogenizer) achieved the overall best performance, including a high Young's modulus of approximately 311 MPa and a good rate capability with a stable specific capacity of 116 mAh g(-1) even up to 1 C. This work allows a better understanding of the influence of the processing parameters of CNF on their performance as binder for flexible electrodes. The results also contribute to the understanding of the optimal processing parameters of CNF to fabricate other materials, e.g., membranes or separators.

Silicon is a good alternative to conventional graphite anode but it has bad cycling and rate performance. To overcome these severe problems, extensively interconnected silicon nanoparticles using carbon network derived from ultrathin cellulose nanofibers were synthesized. Ultrathin cellulose nanofibers, an abundant and sustainable material, entangle each silicon nanoparticle and become extensively interconnected carbon network after pyrolysis. This wide range interconnection provides an efficient electron path by decreasing the likelihood that electrons experience contact resistivity and also suppresses the volume expansion of silicon during lithiation. In addition, Ultrathin cellulose nanofibers are carboxylated and therefore adhesive to silicon nanoparticles through hydrogen bonding. This property makes ultrathin cellulose the perfect carbon source when making silicon composites. As a consequence, it exhibits 808 mAh g(-1) of the reversible capacity after 500 cycles at high current density of 2 A g(-1) with a coulombic efficiency of 99.8%. Even at high current density of 8 A g(-1), it shows a high reversible discharge capacity of 464 mAh g(-1). Moreover, extensively interconnected carbon network prevents the formation of a brittle electrode with a water-based binder. Therefore, this remarkable material has a huge potential for LIBs applications.

The formation of nematically-ordered cellulose nanofiber (CNF) suspensions with an order parameter f(max) approximate to 0.8 is studied by polarized optical microscopy, small-angle X-ray scattering (SAXS), and rheological measurements as a function of CNF concentration. The wide range of CNF concentrations, from 0.5 wt% to 4.9 wt%, is obtained using osmotic dehydration. The rheological measurements show a strong entangled network over all the concentration range whereas SAXS measurements indicate that at concentrations >1.05 wt% the CNF suspension crosses an isotropic-anisotropic transition that is accompanied by a dramatic increase of the optical birefringence. The resulting nanostructures are modelled as mass fractal structures that converge into co-existing nematically-ordered regions and network-like regions where the correlation distances decrease with concentration. The use of rapid, upscalable osmotic dehydration is an effective method to increase the concentration of CNF suspensions while partly circumventing the gel/glass formation. The facile formation of highly ordered fibers can result in materials with interesting macroscopic properties.