Aerogels with both high elastic strain and fast shape recovery after compression have broad application potentials as thermal regulation, absorbents, and electrical devices. However, creating such aerogels from cellulosic materials requires complicated preparation processes. Herein, a simple strategy for scalable production of hemp microfibers using a top‐down method is reported, which can further be assembled into aerogels with interconnected porous structures via ice‐templating technique. With density as low as 2.1 mg cm−3, these aerogels demonstrate isotropic superelasticity, as exhibited by their fast shape restoration from over 80% compressive strain. Due to the high porosity (99.87%) and structural tortuosity, these aerogels show a low thermal conductivity of 0.0215 ± 0.0002 W m−1 K−1, suggesting their potential in thermal insulation application. Certain hydrophobic modification using silane derivative further endows these aerogels with reduced water affinity. Overall, the proposed strategy to prepare bio‐based microfibers using scalable technology, as well as the assembled aerogels, provides new insights into the design and fabrication of multifunctional bio‐based aerogels for value‐added applications.

https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/adfm.202300893

Superelastic and Ultralight Aerogel Assembled from Hemp Microfibers

Abstract The rapid development of wearable electronics has placed higher demands on the design strategies of triboelectric materials. Aerogels have the potential to become advanced triboelectric materials, however, traditional design strategies often require complex processes and additional chemical cross‐linking agents to improve the stability of the gel structure, which limits its practical application. In this work, a scalable and sustainable self‐assembly drive strategy is proposed for the design of bio‐based triboelectric aerogels with multi‐scale winding structures. Interestingly, the autoacceleration effect, which is regarded as “unfavorable” during the autocatalytic polymerization of supramolecules, is rationally exploited to provide the supramolecules within the matrix with an abundance of multiple hydrogen bonds at the same time as their rapid gelation occurs. Thanks to this, the aerogel film exhibits ultra‐high tensile strength (104 MPa) and remains undeformed after resisting an impact of 8000 times its own weight. Highly robust triboelectric aerogel films are used to build wearable self‐powered sensors with ultra‐fast response in complex environments (48 ms), while enabling real‐time interaction between the wearer and the information network. The design idea of “ turning a detriment into an asset ” in this work provides a new idea for the material construction of highly robust wearable sensors. 

Multiscale Structural Triboelectric Aerogels Enabled by Self‐Assembly Driven Supramolecular Winding

Hierarchical Porous Triboelectric Aerogels Enabled by Heterointerface Engineering

Thermally insulating materials from renewable and readily available resources are in high demand for ecologically beneficial applications. Cellulose aerogels made from lignocellulosic waste have various advantages. However, they are fragile and breakable when bent or compressed. In addition, cellulose aerogels are flammable and weather-sensitive. Hence, to overcome these problems, this work included the preparation of polyurethane (PU)-based cellulose nanofiber (CNF) aerogels that had flexibility, flame retardancy, and thermal insulation. Methyl trimethoxysilane (MTMS) and water-soluble ammonium polyphosphate (APP) were added to improve the cross-linking, hydrophobicity, and flame-retardant properties of aerogels. The flexibility of chemically cross-linked CNF aerogels is enhanced through the incorporation of polyurethane via the wet coagulating process. The aerogels obtained during this study have exhibited low weight (density: 35.3-91.96 kg/m3) together with enhanced hydrophobic properties, flame retardancy, and decreased thermal conductivity (26.7-36.7 mW/m K at 25 °C). Additionally, the flame-retardant properties were comprehensively examined and the underlying mechanism was deduced. The aerogels prepared in this study are considered unique in the nanocellulose aerogel category due to their integrated structural and performance benefits. The invention is considered to substantially contribute to the large-scale manufacture and use of insulation in construction, automobiles, and aerospace.

Harnessing the Flexibility of Lightweight Cellulose Nanofiber Composite Aerogels for Superior Thermal Insulation and Fire Protection.

A low temperature environment poses significant challenges to the global economy and public health. However, the existing cold-protective materials still struggle with the trade-off between thickness and thermal resistance, resulting in poor thermal-wet comfort and limited personal cold protection performance. Here, a scalable strategy, based on electrospinning and solution casting, is developed to create aerogel micro/nanofiber membranes with a hierarchical cellular architecture by manipulating the phase separation of the charged jets and of the spreading casting solution. The integration of interconnected nanopores (30-60 nm), ultrafine fiber diameter, and high porosity, enables the aerogel micro/nanofiber membranes with lightweight, ultrathin thickness (∼0.5 mm), and superior warmth retention performance with ultralow thermal conductivity of 14.01 mW m-1 K-1. And the resultant membrane with customized semiclosed walls exhibits both striking wind resistance and satisfactory thermal-wet comfort (3.4 °C warmer than the cutting-edge thermal underwear). This work will inspire the design and development of high-performance fibrous materials for thermal management applications.

Ultrathin Aerogel Micro/Nanofiber Membranes with Hierarchical Cellular Architecture for High-Performance Warmth Retention.

Cellulose aerogels are plagued by intermolecular hydrogen bond-induced structural plasticity, otherwise rely on chemicals modification to extend service life. Here, we demonstrate a petrochemical-free strategy to fabricate superelastic cellulose aerogels by designing hierarchical structures at multi scales. Oriented channels consolidate the whole architecture. Porous walls of dehydrated cellulose derived from thermal etching not only exhibit decreased rigidity and stickiness, but also guide the microscopic deformation and mitigate localized large strain, preventing structural collapse. The aerogels show exceptional stability, including temperature-invariant elasticity, fatigue resistance (~5% plastic deformation after 105 cycles), high angular recovery speed (1475.4° s-1), outperforming most cellulose-based aerogels. This benign strategy retains the biosafety of biomass and provides an alternative filter material for health-related applications, such as face masks and air purification.

A Petrochemical-Free Route to Superelastic Hierarchical Cellulose Aerogel.

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A Petrochemical-Free Route to Superelastic Hierarchical Cellulose Aerogel.