Abstract:Twisted structures are ubiquitous in plants and animals. Cellulose and chitin are natural polymers that form the structural skeleton of various twisted systems observed across different length scales, ranging from the molecular to the nano, micro, and macro scale. In addition, cellulose and chitin helicoidal structures are found to be responsible for structural coloration, enhanced mechanical properties, and motion. This review first addresses cellulose and chitin‐based chiral molecular systems and nanoscale h… Show more
“…Chiral nematic structures are known for their exceptional mechanical robustness, possessing multiple toughening mechanisms that enhance their mechanical properties. Chiral nematic structures are complex three-dimensional structures arranged in torsional layers . This structure is maintained by noncovalent bonding interactions, enabling the material to absorb external forces and dissipate energy efficiently through intermolecular motions and rearrangements .…”
Section: Resultsmentioning
confidence: 99%
“…Chiral nematic structures are complex three- dimensional structures arranged in torsional layers. 64 This structure is maintained by noncovalent bonding interactions, enabling the material to absorb external forces and dissipate energy efficiently through intermolecular motions and rearrangements. 65 At the same time, the angular differences between the layers create barriers to crack extension and increase toughness by deflecting crack paths.…”
Iridescent cellulose nanocrystal (CNC) films with chiral nematic nanostructures exhibit great potential in optical devices, sensors, painting, and anticounterfeiting applications. CNCs can assemble into a chiral nematic liquid crystal structure by evaporationassisted self-assembly (EISA) and vacuum-assisted self-assembly (VASA) techniques. However, there is a lack of comprehensive examinations of their structure−property correlations, which are essential for fabricating materials with unique properties. In this work, we gained insights into the optical, mechanical, and structural differences of CNC films engineered using the two techniques. In contrast to the random self-assembly at the liquid−air interface in EISA, the continuous external pressure in the VASA process forces CNCs to assemble at the filter−liquid interface. This results in fewer defects in the interfaces between tactoids and highly ordered cholesteric phases. Owing to the distinct CNC assembly behaviors, the films prepared by these two methods show great differences in the nanostructure, microstructure, and macroscopic morphology. Consequently, the highly ordered cholesteric structure gives VASA-CNC films a more uniform structural color and enhanced mechanical performance. These fundamental understandings of the relationship of structure−property nanoengineering through various assembly techniques are essential for designing and constructing high-performance chiral iridescent CNC materials.
“…Chiral nematic structures are known for their exceptional mechanical robustness, possessing multiple toughening mechanisms that enhance their mechanical properties. Chiral nematic structures are complex three-dimensional structures arranged in torsional layers . This structure is maintained by noncovalent bonding interactions, enabling the material to absorb external forces and dissipate energy efficiently through intermolecular motions and rearrangements .…”
Section: Resultsmentioning
confidence: 99%
“…Chiral nematic structures are complex three- dimensional structures arranged in torsional layers. 64 This structure is maintained by noncovalent bonding interactions, enabling the material to absorb external forces and dissipate energy efficiently through intermolecular motions and rearrangements. 65 At the same time, the angular differences between the layers create barriers to crack extension and increase toughness by deflecting crack paths.…”
Iridescent cellulose nanocrystal (CNC) films with chiral nematic nanostructures exhibit great potential in optical devices, sensors, painting, and anticounterfeiting applications. CNCs can assemble into a chiral nematic liquid crystal structure by evaporationassisted self-assembly (EISA) and vacuum-assisted self-assembly (VASA) techniques. However, there is a lack of comprehensive examinations of their structure−property correlations, which are essential for fabricating materials with unique properties. In this work, we gained insights into the optical, mechanical, and structural differences of CNC films engineered using the two techniques. In contrast to the random self-assembly at the liquid−air interface in EISA, the continuous external pressure in the VASA process forces CNCs to assemble at the filter−liquid interface. This results in fewer defects in the interfaces between tactoids and highly ordered cholesteric phases. Owing to the distinct CNC assembly behaviors, the films prepared by these two methods show great differences in the nanostructure, microstructure, and macroscopic morphology. Consequently, the highly ordered cholesteric structure gives VASA-CNC films a more uniform structural color and enhanced mechanical performance. These fundamental understandings of the relationship of structure−property nanoengineering through various assembly techniques are essential for designing and constructing high-performance chiral iridescent CNC materials.
“…This goes beyond the linear dependence of the modulus on the cross-link concentration, suggesting a more complex network configuration compared to that schematized in Figure B,C. Indeed, various authors − report that cellulose chains in solution, in the presence of water, form heterogeneous bundles or ordered mesophases, depending on the grade of cellulose used. Also, Tharmann et al reported that the modulus of cross-linked actin gels varies with the power of 3.5 of the cross-linker concentration, and this was ascribed to the formation of actin chain bundles.…”
The addition of water to native cellulose/1-ethyl-3methylimidazolium acetate solutions catalyzes the formation of gels, where polymer chain−chain intermolecular associations act as cross-links. However, the relationship between water content (W c ), polymer concentration (C p ), and gel strength is still missing. This study provides the fundamentals to design water-induced gels. First, the sol−gel transition occurs exclusively in entangled solutions, while in unentangled ones, intramolecular associations hamper interchain cross-linking, preventing the gel formation. In entangled systems, the addition of water has a dual impact: at low water concentrations, the gel modulus is water-independent and controlled by entanglements. As water increases, more cross-links per chain than entanglements emerge, causing the modulus of the gel to scale as. Immersing the solutions in water yields hydrogels with noncrystalline, aggregate-rich structures. Such water−ionic liquid exchange is examined via Raman, FTIR, and WAXS. Our findings provide avenues for designing biogels with desired rheological properties.
Bioinspired and biomimetic materials have revolutionized many aspects in the engineering sciences, ranging from basic technologies to advanced applications such as the Gecko's nanostructure for sticky tapes or the sharkskin for swimming suits. Research in these subjects in Germany has been supported by several national priority research programs since 2009 (SPP 1420: Biomimetic Materials Research: Functionality by Hierarchical Structuring of Materials, [1] SPP 1569: Generation of Multifunctional Inorganic Materials by Molecular Bionics, 2012-2019 [2] ), which strongly accelerated developments and investigations in the field. Recently, also photonic applications of bioinspired strategies have come within reach, demonstrating the huge potential of the approach nature has chosen in many directions (SPP 1839: Tailored Disorder -A science-and engineering-based approach to materials design for advanced photonic applications, 2015-2024 [3] ). These developments have been accompanied by a biennial DGM Bioinspired Materials conference series, which was launched in 2012. [4] The present Advanced Functional Materials feature issue now proudly presents accompanying papers from the 6 th DGM "Bioinspired Materials [5] " together with additional most recent and advanced research work pushing the limits of our exciting interdisciplinary research field. The collected perspectives, reviews and research articles represent the current state-of-the-art in the design of functional and structural materials and systems inspired by principles found in living nature. Main topics of this include the study and formation of hierarchical structures and the properties of complex-shaped biological materials. The transfer of biological principles into functional materials and systems made of organic and/or inorganic components represents a further main area. Beside synthesis and
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