Machine intelligence-accelerated discovery of all-natural plastic substitutes.

One possible solution against the accumulation of petrochemical plastics in natural environments is to develop biodegradable plastic substitutes using natural components. However, discovering all-natural alternatives that meet specific properties, such as optical transparency, fire retardancy and mechanical resilience, which have made petrochemical plastics successful, remains challenging. Current approaches still rely on iterative optimization experiments. Here we show an integrated workflow that combines robotics and machine learning to accelerate the discovery of all-natural plastic substitutes with programmable optical, thermal and mechanical properties. First, an automated pipetting robot is commanded to prepare 286 nanocomposite films with various properties to train a support-vector machine classifier. Next, through 14 active learning loops with data augmentation, 135 all-natural nanocomposites are fabricated stagewise, establishing an artificial neural network prediction model. We demonstrate that the prediction model can conduct a two-way design task: (1) predicting the physicochemical properties of an all-natural nanocomposite from its composition and (2) automating the inverse design of biodegradable plastic substitutes that fulfils various user-specific requirements. By harnessing the model's prediction capabilities, we prepare several all-natural substitutes, that could replace non-biodegradable counterparts as exhibiting analogous properties. Our methodology integrates robot-assisted experiments, machine intelligence and simulation tools to accelerate the discovery and design of eco-friendly plastic substitutes starting from building blocks taken from the generally-recognized-as-safe database.

Emerging Engineered Wood for Building Applications.

The building sector, including building operations and materials, was responsible for the emission of ∼11.9 gigatons of global energy-related CO2 in 2020, accounting for 37% of the total CO2 emissions, the largest share among different sectors. Lowering the carbon footprint of buildings requires the development of carbon-storage materials as well as novel designs that could enable multifunctional components to achieve widespread applications. Wood is one of the most abundant biomaterials on Earth and has been used for construction historically. Recent research breakthroughs on advanced engineered wood products epitomize this material's tremendous yet largely untapped potential for addressing global sustainability challenges. In this review, we explore recent developments in chemically modified wood that will produce a new generation of engineered wood products for building applications. Traditionally, engineered wood products have primarily had a structural purpose, but this review broadens the classification to encompass more aspects of building performance. We begin by providing multiscale design principles of wood products from a computational point of view, followed by discussion of the chemical modifications and structural engineering methods used to modify wood in terms of its mechanical, thermal, optical, and energy-related performance. Additionally, we explore life cycle assessment and techno-economic analysis tools for guiding future research toward environmentally friendly and economically feasible directions for engineered wood products. Finally, this review highlights the current challenges and perspectives on future directions in this research field. By leveraging these new wood-based technologies and analysis tools for the fabrication of carbon-storage materials, it is possible to design sustainable and carbon-negative buildings, which could have a significant impact on mitigating climate change.

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.

Damage-tolerant 3D-printed ceramics via conformal coating.

Ceramic materials, despite their high strength and modulus, are limited in many structural applications due to inherent brittleness and low toughness. Nevertheless, ceramic-based structures, in nature, overcome this limitation using bottom-up complex hierarchical assembly of hard ceramic and soft polymer, where ceramics are packaged with tiny fraction of polymers in an internalized fashion. Here, we propose a far simpler approach of entirely externalizing the soft phase via conformal polymer coating over architected ceramic structures, leading to damage tolerance. Architected structures are printed using silica-filled preceramic polymer, pyrolyzed to stabilize the ceramic scaffolds, and then dip-coated conformally with a thin, flexible epoxy polymer. The polymer-coated architected structures show multifold improvement in compressive strength and toughness while resisting catastrophic failure through a considerable delay of the damage propagation. This surface modification approach allows a simple strategy to build complex ceramic parts that are far more damage-tolerant than their traditional counterparts.

Strong, Hydrostable, and Degradable Straws Based on Cellulose-Lignin Reinforced Composites.

The huge consumption of single-use plastic straws has brought a long-lasting environmental problem. Paper straws, the current replacement for plastic straws, suffer from drawbacks, such as a high cost of the water-proof wax layer and poor water stability due to the easy delamination of the wax layer. It is therefore crucial to find a high-performing alternative to mitigate the environmental problems brought by plastic straws. In this paper, all natural, degradable, cellulose-lignin reinforced composite straws, inspired by the reinforcement principle of cellulose and lignin in natural wood are developed. The cellulose-lignin reinforced composite straw is fabricated by rolling up a wet film made of homogeneously mixed cellulose microfibers, cellulose nanofibers, and lignin powders, which is then baked in oven at 150 °C. When baked, lignin melts and infiltrates the micro-nanocellulose network, acting as a polyphenolic binder to improve the mechanical strength and hydrophobicity performance of the resulting straw. The obtained straws demonstrate several advantageous properties over paper straws, including 1) excellent mechanical performance, 2) high hydrostability, and 3) low cost. Moreover, the natural degradability of the cellulose-lignin reinforced composite straws makes them promising candidates to replace plastic straws and suggests possible substitutes for other petroleum-based plastics.

Alignment of Cellulose Nanofibers: Harnessing Nanoscale Properties to Macroscale Benefits.

In nature, cellulose nanofibers form hierarchical structures across multiple length scales to achieve high-performance properties and different functionalities. Cellulose nanofibers, which are separated from plants or synthesized biologically, are being extensively investigated and processed into different materials owing to their good properties. The alignment of cellulose nanofibers is reported to significantly influence the performance of cellulose nanofiber-based materials. The alignment of cellulose nanofibers can bridge the nanoscale and macroscale, bringing enhanced nanoscale properties to high-performance macroscale materials. However, compared with extensive reviews on the alignment of cellulose nanocrystals, reviews focusing on cellulose nanofibers are seldom reported, possibly because of the challenge of aligning cellulose nanofibers. In this review, the alignment of cellulose nanofibers, including cellulose nanofibrils and bacterial cellulose, is extensively discussed from different aspects of the driving force, evaluation, strategies, properties, and applications. Future perspectives on challenges and opportunities in cellulose nanofiber alignment are also briefly highlighted.

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.

Direct observation of the formation and stabilization of metallic nanoparticles on carbon supports.

Direct formation of ultra-small nanoparticles on carbon supports by rapid high temperature synthesis method offers new opportunities for scalable nanomanufacturing and the synthesis of stable multi-elemental nanoparticles. However, the underlying mechanisms affecting the dispersion and stability of nanoparticles on the supports during high temperature processing remain enigmatic. In this work, we report the observation of metallic nanoparticles formation and stabilization on carbon supports through in situ Joule heating method. We find that the formation of metallic nanoparticles is associated with the simultaneous phase transition of amorphous carbon to a highly defective turbostratic graphite (T-graphite). Molecular dynamic (MD) simulations suggest that the defective T-graphite provide numerous nucleation sites for the nanoparticles to form. Furthermore, the nanoparticles partially intercalate and take root on edge planes, leading to high binding energy on support. This interaction between nanoparticles and T-graphite substrate strengthens the anchoring and provides excellent thermal stability to the nanoparticles. These findings provide mechanistic understanding of rapid high temperature synthesis of metal nanoparticles on carbon supports and the origin of their stability.

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.

High temperature shockwave stabilized single atoms.

The stability of single-atom catalysts is critical for their practical applications. Although a high temperature can promote the bond formation between metal atoms and the substrate with an enhanced stability, it often causes atom agglomeration and is incompatible with many temperature-sensitive substrates. Here, we report using controllable high-temperature shockwaves to synthesize and stabilize single atoms at very high temperatures (1,500-2,000 K), achieved by a periodic on-off heating that features a short on state (55 ms) and a ten-times longer off state. The high temperature provides the activation energy for atom dispersion by forming thermodynamically favourable metal-defect bonds and the off-state critically ensures the overall stability, especially for the substrate. The resultant high-temperature single atoms exhibit a superior thermal stability as durable catalysts. The reported shockwave method is facile, ultrafast and universal (for example, Pt, Ru and Co single atoms, and carbon, C3N4 and TiO2 substrates), which opens a general route for single-atom manufacturing that is conventionally challenging.

Fast Growth of Strain-Free AlN on Graphene-Buffered Sapphire.

We study the roles of graphene acting as a buffer layer for growth of an AlN film on a sapphire substrate. Graphene can reduce the density of AlN nuclei but increase the growth rate for an individual nucleus at the initial growth stage. This can lead to the reduction of threading dislocations evolved at the coalescence boundaries. The graphene interlayer also weakens the interaction between AlN and sapphire and accommodates their large mismatch in the lattice and thermal expansion coefficients; thus, the compressive strain in AlN and the tensile strain in sapphire are largely relaxed. The effective relaxation of strain further leads to a low density of defects in the AlN films. These findings reveal the roles of graphene in III-nitride growth and offer valuable insights into the efficient applications of graphene in the light-emitting diode industry.

Wrinkle-Free Single-Crystal Graphene Wafer Grown on Strain-Engineered Substrates.

Wrinkles are ubiquitous for graphene films grown on various substrates by chemical vapor deposition at high temperature due to the strain induced by thermal mismatch between the graphene and substrates, which greatly degrades the extraordinary properties of graphene. Here we show that the wrinkle formation of graphene grown on Cu substrates is strongly dependent on the crystallographic orientations. Wrinkle-free single-crystal graphene was grown on a wafer-scale twin-boundary-free single-crystal Cu(111) thin film fabricated on sapphire substrate through strain engineering. The wrinkle-free feature of graphene originated from the relatively small thermal expansion of the Cu(111) thin film substrate and the relatively strong interfacial coupling between Cu(111) and graphene, based on the strain analyses as well as molecular dynamics simulations. Moreover, we demonstrated the transfer of an ultraflat graphene film onto target substrates from the reusable single-crystal Cu(111)/sapphire growth substrate. The wrinkle-free graphene shows enhanced electrical mobility compared to graphene with wrinkles.

Bottom-up Design of Three-Dimensional Carbon-Honeycomb with Superb Specific Strength and High Thermal Conductivity.

Low-dimensional carbon allotropes, from fullerenes, carbon nanotubes, to graphene, have been broadly explored due to their outstanding and special properties. However, there exist significant challenges in retaining such properties of basic building blocks when scaling them up to three-dimensional materials and structures for many technological applications. Here we show theoretically the atomistic structure of a stable three-dimensional carbon honeycomb (C-honeycomb) structure with superb mechanical and thermal properties. A combination of sp2 bonding in the wall and sp3 bonding in the triple junction of C-honeycomb is the key to retain the stability of C-honeycomb. The specific strength could be the best in structural carbon materials, and this strength remains at a high level but tunable with different cell sizes. C-honeycomb is also found to have a very high thermal conductivity, for example, >100 W/mK along the axis of the hexagonal cell with a density only ∼0.4 g/cm3. Because of the low density and high thermal conductivity, the specific thermal conductivity of C-honeycombs is larger than most engineering materials, including metals and high thermal conductivity semiconductors, as well as lightweight CNT arrays and graphene-based nanocomposites. Such high specific strength, high thermal conductivity, and anomalous Poisson's effect in C-honeycomb render it appealing for the use in various engineering practices.