Bombyx mori silk with a nanoscale porous architecture significantly deforms in response to changes in relative humidity. Despite the increasing amount of water adsorption and water-responsive strain with increasing porosity of the silk, there is a range of porosities that result in silk's optimal water-responsive energy density at 3.1 MJ m −3 . Our findings show the possibility of controlling water-responsive materials’ swelling pressure by controlling their nanoporosities.
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β‐Sheet Nanocrystals Dictate Water Responsiveness of Bombyx Mori Silk
Water‐responsive (WR) materials that strongly swell and shrink in response to changes in relative humidity (RH) have shown a great potential to serve as high‐energy actuators for soft robotics and new energy‐harvesting systems. However, the design criteria governing the scalable and high‐efficiency WR actuation remain unclear, and thus inhibit further development of WR materials for practical applications. Nature has provided excellent examples of WR materials that contain stiff nanocrystalline structures that can be crucial to understand the fundamentals of WR behavior. This work reports that regenerated
- PAR ID:
- 10458577
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Macromolecular Rapid Communications
- Volume:
- 41
- Issue:
- 7
- ISSN:
- 1022-1336
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Abstract Biological water-responsive materials that deform with changes in relative humidity have recently demonstrated record-high actuation energy densities, showing promise as high-performance actuators for various engineering applications. However, there is a lack of theories capable of explaining or predicting the stress generated during water-responsiveness. Here, we show that the nanoscale confinement of water dominates the macroscopic dehydration-induced stress of the regenerated silk fibroin. We modified silk fibroin’s secondary structure, which leads to various distributions of bulk-like mobile and tightly bound water populations. Interestingly, despite these structure variations, all silk samples start to exert force when the bound-to-mobile (B/M) ratio of confined water reaches the same level. This critical B/M water ratio suggests a common threshold above which the chemical potential of water instigates the actuation. Our findings serve as guidelines for predicting and engineering silk’s WR behavior and suggest the potential of describing the WR behavior of biopolymers through confined water.
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null (Ed.)The spider major ampullate (MA) silk exhibits high tensile strength and extensibility and is typically a blend of MaSp1 and MaSp2 proteins with the latter comprising glycine–proline–glycine–glycine-X repeating motifs that promote extensibility and supercontraction. The MA silk from Darwin's bark spider ( Caerostris darwini ) is estimated to be two to three times tougher than the MA silk from other spider species. Previous research suggests that a unique MaSp4 protein incorporates proline into a novel glycine–proline–glycine–proline motif and may explain C. darwini MA silk's extraordinary toughness. However, no direct correlation has been made between the silk's molecular structure and its mechanical properties for C. darwini . Here, we correlate the relative protein secondary structure composition of MA silk from C. darwini and four other spider species with mechanical properties before and after supercontraction to understand the effect of the additional MaSp4 protein. Our results demonstrate that C. darwini MA silk possesses a unique protein composition with a lower ratio of helices (31%) and β-sheets (20%) than other species. Before supercontraction, toughness, modulus and tensile strength correlate with percentages of β-sheets, unordered or random coiled regions and β-turns. However, after supercontraction, only modulus and strain at break correlate with percentages of β-sheets and β-turns. Our study highlights that additional information including crystal size and crystal and chain orientation is necessary to build a complete structure–property correlation model.more » « less
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Abstract Sponge‐like materials made from regenerated silk fibroin biopolymers are a tunable and advantageous platform for in vitro engineered tissue culture and in vivo tissue regeneration. Anisotropic, three‐dimensional (3D) silk fibroin sponge‐like scaffolds can mimic the architecture of contractile muscle. Herein, we use silk fibroin solution isolated from the cocoons of
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Abstract Smart textiles that sense, interact, and adapt to environmental stimuli have provided exciting new opportunities for a variety of applications. However, current advances have largely remained at the research stage due to the high cost, complexity of manufacturing, and uncomfortableness of environment‐sensitive materials. In contrast, natural textile materials are more attractive for smart textiles due to their merits in terms of low cost and comfortability. Here, water fog and humidity‐driven torsional and tensile actuation of thermally set twisted, coiled, plied silk fibers, and weave textiles from these silk fibers are reported. When exposed to water fog, the torsional silk fiber provides a fully reversible torsional stroke of 547° mm−1. Coiled‐and‐thermoset silk yarns provide a 70% contraction when the relative humidity is changed from 20% to 80%. Such an excellent actuation behavior originates from water absorption‐induced loss of hydrogen bonds within the silk proteins and the associated structural transformation, which are corroborated by atomistic and macroscopic characterization of silk and molecular dynamics simulations. With its large abundance, cost‐effectiveness, and comfortability for wearing, the silk muscles will open up additional possibilities in industrial applications, such as smart textiles and soft robotics.
