Rapidly Prepared Nanocellulose Hybrids as Gas Barrier, Flame Retardant, and Energy Storage Materials

Abstract

Cellulose nanofibril (CNF) hybrid materials show great promise as sustainable alternatives to oil-based plastics owing to their abundance and renewability. Nonetheless, despite the enormous success achieved in preparing CNF hybrids at the laboratory scale, feasible implementation of these materials remains a major challenge due to the time-consuming and energy-intensive extraction and processing of CNFs. Here, we describe a scalable materials processing platform for rapid preparation (<10 min) of homogeneously distributed functional CNF−gibbsite and CNF−graphite hybrids through a pH-responsive self-assembly mechanism, followed by their application in gas barrier, flame retardancy, and energy storage materials. Incorporation of 5 wt % gibbsite results in strong, transparent, and oxygen barrier CNF−gibbsite hybrid films in 9 min. Increasing the gibbsite content to 20 wt % affords them self-extinguishing properties, while further lowering their dewatering time to 5 min. The strategy described herein also allows for the preparation of freestanding CNF−graphite hybrids (90 wt % graphite) that match the energy storage performance (330 mA h/g at low cycling rates) and processing speed (3 min dewatering) of commercial graphite anodes. Furthermore, these ecofriendly electrodes can be fully recycled, reformed, and reused while maintaining their initial performance. Overall, this versatile concept combines a green outlook with high processing speed and material performance, paving the way toward scalable processing of advanced ecofriendly hybrid materials.

Bio-Based Binder Development for Lithium-Ion Batteries

“…CMC-based Graphite 300 [60] Graphite 141 [37] Graphite 300 [70] Si-based 1153 [23] Si-based 1100 [64] Si-based 1000-1900 [65] Si-based 1544 [28] CNF-based Graphite 330 [77] Graphite 345 [73] Lignin-based Graphite 305 [47] Si-based 1914 [28] Si-based 939 [81] Si/graphite 492 [28] Guar gum-based Graphite 310 [84] Si-based 2222 [82] Si-based 1402 [39] Table 1. Cont.…”

“…In particular, TEMPO–periodate-oxidized cellulose electrodes showed higher specific capacities at high cycling rates (10% increase at 400 mA/g), because of the enhanced chemical compatibility with both graphite and the electrolyte, as well as an ability to form a strong fibrillar network that prevents structural damage upon graphite expansion [ 76 ]. Additionally, a sustainable approach was reported to produce freestanding CNF–graphite hybrids (90 wt% graphite) exhibiting energy storage performance (330 mAh/g) and processing speed on par with commercial graphite anodes [ 77 ]. These eco-friendly electrodes possess the remarkable ability to be completely recycled, reformed, and reused without compromising their original performance.…”

Affine Deformation and Self-Assembly Alignment in Hydrogel Nanocomposites

“…The precise control and prediction of order in nanocomposite materials remain crucial objectives in the design of advanced nanomaterials. In recent years, materials inspired by the hierarchical structures found in nature have gained substantial popularity. − Many methodologies have emerged trying to translate to man-made materials the exceptional property profiles of naturally formed hierarchical structures, such as the ones found in wood, bone, enamel, and nacre. − In particular, the thermal, mechanical, and permeability properties of in-plane-oriented nacre-like materials have been intensively investigated . Nacre is found in the inner shells of mollusks and mussels.…”

“…Ordered nacre-like materials are usually made from suspension/melt mixing or in situ approaches. , For instance, they are produced via casting, , vacuum filtration, and layer-by-layer assembly (L-b-L) , methods to achieve high-performance materials . For some years now, a major development has been the implementation of water-based nanocomposites and large-area fabrication via solvent evaporation, akin to paper-making. ,− After that, building block formation, including cross-linking techniques and drying conditions, has been extensively optimized to realize nano- and mesoscopic assemblies of clay silicates (reduced) graphene oxide, MXenes, boron nitride, dichalcogenides, and so forth. ,− Most reports follow the rationale that a polymeric core–shell formation and subsequent particle alignment by directed or evaporative self-assembly mechanisms preserve the high aspect ratio of platelets or sheet fillers. ,, However, the colloidal ordering principle is seldom explained or explored in any detail. Some point out excluded volume associations, ,, as in an Onsager-like treatment .…”

“… 22 , 24 − 28 Most reports follow the rationale that a polymeric core–shell formation and subsequent particle alignment by directed or evaporative self-assembly mechanisms preserve the high aspect ratio of platelets or sheet fillers. 7 , 8 , 18 However, the colloidal ordering principle is seldom explained or explored in any detail. Some point out excluded volume associations, 18 , 29 , 30 as in an Onsager-like treatment.…”