Fabrication of Cellulose-Graphite Foam via Ion Cross-linking and Ambient-Drying.

Conventional plastic foams are usually produced by fossil-fuel-derived polymers, which are difficult to degrade in nature. As an alternative, cellulose is a promising biodegradable polymer that can be used to fabricate greener foams, yet such a process typically relies on methods (e.g., freeze-drying and supercritical-drying) that are hardly scalable and time-consuming. Here, we develop a fast and scalable approach to prepare cellulose-graphite foams via rapidly cross-linking the cellulose fibrils in metal ions-containing solution followed by ambient drying. The prepared foams exhibit low density, high compressive strength, and excellent water stability. Moreover, the cross-linking of the cellulose fibrils can be triggered by various metal ions, indicating good universality. We further use density functional theory to reveal the cross-linking effect of different ions, which shows good agreement with our experimental observation. Our approach presents a sustainable route toward low-cost, environmentally friendly, and scalable foam production for a range of applications.

Mechanics Design in Cellulose-Enabled High-Performance Functional Materials.

The abundance of cellulose found in natural resources such as wood, and the wide spectrum of structural diversity of cellulose nanomaterials in the form of micro-nano-sized particles and fibers, have sparked a tremendous interest to utilize cellulose's intriguing mechanical properties in designing high-performance functional materials, where cellulose's structure-mechanics relationships are pivotal. In this progress report, multiscale mechanics understanding of cellulose, including the key role of hydrogen bonding, the dependence of structural interfaces on the spatial hydrogen bond density, the effect of nanofiber size and orientation on the fracture toughness, are discussed along with recent development on enabling experimental design techniques such as structural alteration, manipulation of anisotropy, interface and topology engineering. Progress in these fronts renders cellulose a prospect of being effectuated in an array of emerging sustainable applications and being fabricated into high-performance structural materials that are both strong and tough.

Highly Elastic Hydrated Cellulosic Materials with Durable Compressibility and Tunable Conductivity.

Anisotropic cellular materials with direction-dependent structure and durable mechanical properties enable various applications (e.g., nanofluidics, biomedical devices, tissue engineering, and water purification), but their widespread use is often hindered by complex and scale-limited fabrication and unsatisfactory mechanical performance. Here, inspired by the anisotropic and hierarchical material structure of tendons, we demonstrate a facile, scalable top-down approach for fabricating a highly elastic, ionically conductive, anisotropic cellulosic material (named elastic wood) directly from natural wood via chemical treatment. The resulting elastic wood demonstrates good elasticity and durable compressibility, showing no sign of fatigue after 10 000 compression cycles. The chemical treatment not only softens the wood cell walls by partially removing lignin and hemicellulose but introduces an interconnected cellulose fibril network into the wood channels. Atomistic and continuum modeling further reveals that the absorbed water can freely and reversibly move inside the elastic wood and therefore helps the elastic wood accommodate large compressive deformation and recover to its original shape upon compression release. In addition, the elastic wood showed a high ionic conductivity of up to 0.5 mS cm-1 at a low KCl concentration of 10-4 M, which can be tuned by changing the compression ratio of the material. The demonstrated elastic, mechanically robust, and ionically conductive cellulosic material combining inherited anisotropic cellular structure from natural wood and a self-formed internal gel may find a variety of potential applications in ionic nanofluidics, sensors, soft robots, artificial muscle, environmental remediation, and energy storage.

Processing bulk natural wood into a high-performance structural material.

Synthetic structural materials with exceptional mechanical performance suffer from either large weight and adverse environmental impact (for example, steels and alloys) or complex manufacturing processes and thus high cost (for example, polymer-based and biomimetic composites). Natural wood is a low-cost and abundant material and has been used for millennia as a structural material for building and furniture construction. However, the mechanical performance of natural wood (its strength and toughness) is unsatisfactory for many advanced engineering structures and applications. Pre-treatment with steam, heat, ammonia or cold rolling followed by densification has led to the enhanced mechanical performance of natural wood. However, the existing methods result in incomplete densification and lack dimensional stability, particularly in response to humid environments, and wood treated in these ways can expand and weaken. Here we report a simple and effective strategy to transform bulk natural wood directly into a high-performance structural material with a more than tenfold increase in strength, toughness and ballistic resistance and with greater dimensional stability. Our two-step process involves the partial removal of lignin and hemicellulose from the natural wood via a boiling process in an aqueous mixture of NaOH and Na2SO3 followed by hot-pressing, leading to the total collapse of cell walls and the complete densification of the natural wood with highly aligned cellulose nanofibres. This strategy is shown to be universally effective for various species of wood. Our processed wood has a specific strength higher than that of most structural metals and alloys, making it a low-cost, high-performance, lightweight alternative.