Bio‐Inspired Multiscale Design for Strong and Tough Biological Ionogels

Structure design provides an effective solution to develop advanced soft materials with desirable mechanical properties. However, creating multiscale structures in ionogels to obtain strong mechanical properties is challenging. Here, an in situ integration strategy for producing a multiscale‐structured ionogel (M‐gel) via ionothermal‐stimulated silk fiber splitting and moderate molecularization in the cellulose‐ions matrix is reported. The produced M‐gel shows a multiscale structural superiority comprised of microfibers, nanofibrils, and supramolecular networks. When this strategy is used to construct a hexactinellid inspired M‐gel, the resultant biomimetic M‐gel shows excellent mechanical properties including elastic modulus of 31.5 MPa, fracture strength of 6.52 MPa, toughness reaching 1540 kJ m−3, and instantaneous impact resistance of 3.07 kJ m−1, which are comparable to those of most previously reported polymeric gels and even hardwood. This strategy is generalizable to other biopolymers, offering a promising in situ design method for biological ionogels that can be expanded to more demanding load‐bearing materials requiring greater impact resistance.

[1]  Penghui Zhu,et al.  Ultrastretchable Ionogel with Extreme Environmental Resilience through Controlled Hydration Interactions , 2022, Advanced Functional Materials.

[2]  Weida Hu,et al.  Poss Hybrid Poly(Ionic Liquid) Ionogel Solid Electrolyte for Flexible Lithium Batteries , 2022, SSRN Electronic Journal.

[3]  D. Kaplan,et al.  Engineered Tough Silk Hydrogels through Assembling β-Sheet Rich Nanofibers Based on a Solvent Replacement Strategy. , 2022, ACS nano.

[4]  Chengyi Hou,et al.  Synergistic Solvation and Interface Regulations of Eco‐Friendly Silk Peptide Additive Enabling Stable Aqueous Zinc‐Ion Batteries , 2022, Advanced Functional Materials.

[5]  Q. Zhang,et al.  3D Printed High‐Strength Supramolecular Polymer Hydrogel‐Cushioned Radially and Circumferentially Oriented Meniscus Substitute , 2022, Advanced Functional Materials.

[6]  M. Dickey,et al.  Tough and stretchable ionogels by in situ phase separation , 2022, Nature Materials.

[7]  Chaoji Chen,et al.  A Stiffness‐Switchable, Biomimetic Smart Material Enabled by Supramolecular Reconfiguration , 2021, Advanced materials.

[8]  Liyun Ma,et al.  From Mesoscopic Functionalization of Silk Fibroin to Smart Fiber Devices for Textile Electronics and Photonics , 2021, Advanced science.

[9]  Yang Li,et al.  Mechanically and Environmentally Stable Triboelectric Nanogenerator Based on High-Strength and Anti-Compression Self-Healing Ionogel , 2021, Nano Energy.

[10]  Yunqi Liu,et al.  Shape‐Engineerable Silk Fibroin Papers for Ideal Substrate Alternatives of Plastic Electronics , 2021, Advanced Functional Materials.

[11]  Yang Shu,et al.  Microwave-Triggered Ionic Liquids-based Hydrogel Dressing with Excellent Hyperthermia and Transdermal Drug Delivery Performance , 2021, Chemical Engineering Journal.

[12]  Grace X. Gu,et al.  Mechanical Training-Driven Structural Remodeling: A Rational Route for Outstanding Highly Hydrated Silk Materials. , 2021, Small.

[13]  Meifang Zhu,et al.  Mechanically Strong and Multifunctional Hybrid Hydrogels with Ultrahigh Electrical Conductivity , 2021, Advanced Functional Materials.

[14]  M. Porfiri,et al.  Extreme flow simulations reveal skeletal adaptations of deep-sea sponges , 2021, Nature.

[15]  Xiulin Fan,et al.  Ambiently and Mechanically Stable Ionogels for Soft Ionotronics , 2021, Advanced Functional Materials.

[16]  R. Xiao,et al.  Editing the Shape Morphing of Monocomponent Natural Polysaccharide Hydrogel Films , 2021, Research.

[17]  Xingcai Zhang,et al.  Bio‐Inspired Ionic Skin for Theranostics , 2020, Advanced Functional Materials.

[18]  J. Aizenberg,et al.  Mechanically robust lattices inspired by deep-sea glass sponges , 2020, Nature Materials.

[19]  Haipeng Yu,et al.  Assembly of silver nanowires and PEDOT:PSS with hydrocellulose toward highly flexible, transparent and conductivity-stable conductors , 2020 .

[20]  D. Kaplan,et al.  Stimuli-responsive composite biopolymer actuators with selective spatial deformation behavior , 2020, Proceedings of the National Academy of Sciences.

[21]  Wenshuai Chen,et al.  Cellulose‐Based Flexible Functional Materials for Emerging Intelligent Electronics , 2020, Advanced materials.

[22]  Zhigang Suo,et al.  Stretchable and fatigue-resistant materials , 2020 .

[23]  Liangbing Hu,et al.  A Dynamic Gel with Reversible and Tunable Topological Networks and Performances , 2020 .

[24]  D. Weitz,et al.  Observations of 3 nm Silk Nanofibrils Exfoliated from Natural Silkworm Silk Fibers , 2020 .

[25]  Yongyuan Ren,et al.  Ionic liquid–based click-ionogels , 2019, Science Advances.

[26]  Peiyi Wu,et al.  A highly transparent and ultra-stretchable conductor with stable conductivity during large deformation , 2019, Nature Communications.

[27]  Lei Jiang,et al.  Preparation of High‐Performance Ionogels with Excellent Transparency, Good Mechanical Strength, and High Conductivity , 2017, Advanced materials.

[28]  Bryan M. Wong,et al.  A Transparent, Self‐Healing, Highly Stretchable Ionic Conductor , 2016, Advanced materials.

[29]  Fei Yang,et al.  A Universal Soaking Strategy to Convert Composite Hydrogels into Extremely Tough and Rapidly Recoverable Double‐Network Hydrogels , 2016, Advanced materials.

[30]  J. Aizenberg,et al.  New functional insights into the internal architecture of the laminated anchor spicules of Euplectella aspergillum , 2015, Proceedings of the National Academy of Sciences.

[31]  Yunbai Luo,et al.  Synthesis and thermophysical properties of imidazolate-based ionic liquids: Influences of different cations and anions , 2014 .

[32]  Jie Ding,et al.  Mechanically Robust, Electrically Conductive and Stimuli‐Responsive Binary Network Hydrogels Enabled by Superelastic Graphene Aerogels , 2014, Advanced materials.

[33]  Diwakar Z. Shende,et al.  Synthesis, Characterization and Application of 1-Butyl-3 Methylimidazolium Chloride as Green Material for Extractive Desulfurization of Liquid Fuel , 2013, TheScientificWorldJournal.

[34]  J. Aizenberg,et al.  Skeleton of Euplectella sp.: Structural Hierarchy from the Nanoscale to the Macroscale , 2005, Science.

[35]  Dawei Zhao,et al.  Rapid Microwave-Assisted Ionothermal Dissolution of Cellulose and Its Regeneration Properties , 2019, Journal of Renewable Materials.