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Tunable dynamic networks of cellulose nanofibrils (CNFs) are utilized to prepare high‐performance polymer gel electrolytes. By swelling an anisotropically dewatered, but never dried, CNF gel in acidic salt solutions, a highly sparse network is constructed with a fraction of CNFs as low as 0.9%, taking advantage of the very high aspect ratio and the ultra‐thin thickness of the CNFs (micrometers long and 2–4 nm thick). These CNF networks expose high interfacial areas and can accommodate massive amounts of the ionic conductive liquid polyethylene glycol‐based electrolyte into strong homogeneous gel electrolytes. In addition to the reinforced mechanical properties, the presence of the CNFs simultaneously enhances the ionic conductivity due to their excellent strong water‐binding capacity according to computational simulations. This strategy renders the electrolyte a room‐temperature ionic conductivity of 0.61 ± 0.12 mS cm−1 which is one of the highest among polymer gel electrolytes. The electrolyte shows superior performances as a separator for lithium iron phosphate half‐cells in high specific capacity (161 mAh g−1 at 0.1C), excellent rate capability (5C), and cycling stability (94% capacity retention after 300 cycles at 1C) at 60 °C, as well as stable room temperature cycling performance and considerably improved safety compared with commercial liquid electrolyte systems. [ABSTRACT FROM AUTHOR]

Abstract: Composites based on interpenetrating networks (IPNs) of cellulose nanofibril (CNF) aerogels and polyacrylamide are prepared and exhibit robust mechanical, water retaining, and re‐swelling capacities. Furthermore, their swelling behavior is not affected by an increased ionic strength of the aqueous phase. These unprecedented IPNs combine the water retaining capacity of the polyacrylamide with the mechanical strength provided by the CNF aerogel template. The CNF aerogel/polyacrylamide composites exhibit a compressive stress at break greater than 250% compared with a neat polyacrylamide hydrogel. Furthermore, the composites retain their wet compression properties after drying and re‐swelling, whereas the neat polyacrylamide hydrogels fail at a significantly lower stress and strain after drying and re‐swelling. These composite materials highlight the potential of CNF aerogels to strengthen the mechanical properties and reduce the number of fracture defects during the drying and re‐swelling of a hydrogel. These composites show the potential of being optimized for a plethora of applications, especially in the hygiene field and for biomedical devices. [ABSTRACT FROM AUTHOR]

We show that water-based porosimetry ( WBP), a facile, simple, and nondestructive porosimetry technique, accurately evaluates both the pore size distribution and throat size distribution of sacrificially templated macroporous alumina. The pore size distribution and throat size distribution derived from the WBP evaluation in uptake (imbibition) and release (drainage) mode, respectively, were corroborated by mercury porosimetry and X-ray micro-computed tomography (μ-CT). In contrast with mercury porosimetry, the WBP also provided information on the presence of 'dead-end pores' in the macroporous alumina. [ABSTRACT FROM AUTHOR]

This study presents a novel, green, and efficient way of preparing crosslinked aerogels from cellulose nanofibers (CNFs) and alginate using non‐covalent chemistry. This new process can ultimately facilitate the fast, continuous, and large‐scale production of porous, light‐weight materials as it does not require freeze‐drying, supercritical CO2 drying, or any environmentally harmful crosslinking chemistries. The reported preparation procedure relies solely on the successive freezing, solvent‐exchange, and ambient drying of composite CNF‐alginate gels. The presented findings suggest that a highly‐porous structure can be preserved throughout the process by simply controlling the ionic strength of the gel. Aerogels with tunable densities (23–38 kg m−3) and compressive moduli (97–275 kPa) can be prepared by using different CNF concentrations. These low‐density networks have a unique combination of formability (using molding or 3D‐printing) and wet‐stability (when ion exchanged to calcium ions). To demonstrate their use in advanced wet applications, the printed aerogels are functionalized with very high loadings of conducting poly(3,4‐ethylenedioxythiophene):tosylate (PEDOT:TOS) polymer by using a novel in situ polymerization approach. In‐depth material characterization reveals that these aerogels have the potential to be used in not only energy storage applications (specific capacitance of 78 F g−1), but also as mechanical‐strain and humidity sensors. [ABSTRACT FROM AUTHOR]

Designing engineering materials with high stiffness and high toughness is challenging as stiff materials tend to be brittle. Many biological materials realize this objective through multiscale (i.e. atomic‐ to macroscale) mechanisms that are extremely difficult to replicate in synthetic materials. Inspired from the architecture of such biological structures, we here present flow‐assisted organization and assembly of renewable native cellulose nanofibrils (CNFs), which yields highly anisotropic biofibers characterized by a unique combination of high strength (1010 MPa), high toughness (62 MJ m−3) and high stiffness (57 GPa). We observed that properties of the fibers are primarily governed by specific ion characteristics such as hydration enthalpy and polarizability. A fundamental facet of this study is thus to elucidate the role of specific anion binding following the Hofmeister series on the mechanical properties of wet fibrillar networks, and link this to the differences in properties of dry nanostructured fibers. This knowledge is useful for rational design of nanomaterials and is critical for validation of specific ion effect theories. The bioinspired assembly demonstrated here is relevant example for designing high‐performance materials with absolute structural control. [ABSTRACT FROM AUTHOR]

Designing engineering materials with high stiffness and high toughness is challenging as stiff materials tend to be brittle. Many biological materials realize this objective through multiscale (i.e. atomic‐ to macroscale) mechanisms that are extremely difficult to replicate in synthetic materials. Inspired from the architecture of such biological structures, we here present flow‐assisted organization and assembly of renewable native cellulose nanofibrils (CNFs), which yields highly anisotropic biofibers characterized by a unique combination of high strength (1010 MPa), high toughness (62 MJ m−3) and high stiffness (57 GPa). We observed that properties of the fibers are primarily governed by specific ion characteristics such as hydration enthalpy and polarizability. A fundamental facet of this study is thus to elucidate the role of specific anion binding following the Hofmeister series on the mechanical properties of wet fibrillar networks, and link this to the differences in properties of dry nanostructured fibers. This knowledge is useful for rational design of nanomaterials and is critical for validation of specific ion effect theories. The bioinspired assembly demonstrated here is relevant example for designing high‐performance materials with absolute structural control. [ABSTRACT FROM AUTHOR]

Abstract: The heterogeneous nature of non‐cellulosic polysaccharides, such as arabinoxylan, makes it difficult to correlate molecular structure with macroscopic properties. To study the impact of specific structural features of the polysaccharides on crystallinity or affinity to other cell wall components, collections of polysaccharides with defined repeating units are required. Herein, a chemoenzymatic approach to artificial arabinoxylan polysaccharides with systematically altered branching patterns is described. The polysaccharides were obtained by glycosynthase‐catalyzed polymerization of glycosyl fluorides derived from arabinoxylan oligosaccharides. X‐ray diffraction and adsorption experiments on cellulosic surfaces revealed that the physicochemical properties of the synthetic polysaccharides strongly depend on the specific nature of their substitution patterns. The artificial polysaccharides allow structure–property relationship studies that are not accessible by other means. [ABSTRACT FROM AUTHOR]

Abstract: The heterogeneous nature of non‐cellulosic polysaccharides, such as arabinoxylan, makes it difficult to correlate molecular structure with macroscopic properties. To study the impact of specific structural features of the polysaccharides on crystallinity or affinity to other cell wall components, collections of polysaccharides with defined repeating units are required. Herein, a chemoenzymatic approach to artificial arabinoxylan polysaccharides with systematically altered branching patterns is described. The polysaccharides were obtained by glycosynthase‐catalyzed polymerization of glycosyl fluorides derived from arabinoxylan oligosaccharides. X‐ray diffraction and adsorption experiments on cellulosic surfaces revealed that the physicochemical properties of the synthetic polysaccharides strongly depend on the specific nature of their substitution patterns. The artificial polysaccharides allow structure–property relationship studies that are not accessible by other means. [ABSTRACT FROM AUTHOR]

Step by step: A robust and rapid method for the layer‐by‐layer assembly of polymers and nanoparticles on strong and elastic aerogels has been developed. Thin films of biomolecules, conducting polymers, and carbon nanotubes were assembled, which resulted in aerogels with a number of functions, including a high charge‐storage capacity. [ABSTRACT FROM AUTHOR]

Schritt für Schritt: Eine schnelle Methode zur schichtweisen Abscheidung von Polymeren und Nanopartikeln auf starken und elastischen Aerogelen wurde entwickelt. Dünne Filme aus Biomolekülen, leitenden Polymeren oder Kohlenstoffnanoröhren wurden auf diese Weise abgeschieden, wodurch funktionelle Aerogele mit verbesserten Eigenschaften, einschließlich hoher Ladungsspeicherkapazitäten zugänglich waren. [ABSTRACT FROM AUTHOR]