Entropy-Driven Design of Highly Impact-Stiffening Supramolecular Polymer Networks with Salt-Bridge Hydrogen Bonds

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(11), P. 7533 - 7542

Published: March 7, 2024

Impact-stiffening materials that undergo a strain rate-induced soft-to-rigid transition hold great promise as soft armors in the protection of human body and equipment. However, current impact-stiffening materials, such polyborosiloxanes shear-thickening fluids, often exhibit limited response. Herein, we propose design strategy for fabricating highly supramolecular polymer networks by leveraging high-entropy-penalty physical interactions. We synthesized fully biobased comprising poly(α-thioctic acid) arginine clusters, whose chain dynamics are governed specific guanidinium-carboxylate salt-bridge hydrogen bonds. The resulting material exhibits an exceptional response ∼2100 times, transitioning from dissipating state (21 kPa, 0.1 Hz) to stiffened glassy (45.3 MPa, 100 with increasing rates. Moreover, material's high energy-dissipating hot-melting properties bring excellent damping performance easy hybridization other scaffolds. This entropy-driven approach paves way development next-generation soft, sustainable, impact-resistant materials.

Language: Английский

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Neural Network‐Inspired Polyurea Ionogel with Mechanical Robustness, Low Hysteresis, and High Transparency for Soft Iontronics

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(37)

Published: March 7, 2024

Abstract Concurrently achieving mechanical robustness, low hysteresis, and high transparency are essential for ionogels to enhance their reliability satisfy the requirements in soft electronics. Fabricating comprising these characteristics presents a considerable challenge. Herein, inspired by structure of neural networks, new strategy situ formation dense urea moieties aggregated domains is proposed achieve topology‐tailoring polyurea ionogels. Initially, leveraging pronounced disparity reactivity isocyanate (─NCO) groups between isophorone diisocyanate (IPDI) NCO‐terminated prepolymer (PPGTD), IPDI preferentially reacts with deblocked trifunctional latent curing agents, resulting domains. Thereafter, interconnected via PPGTD establish polymer networks which ionic liquid uniformly dispersed, forming like Attributed this unique design strategy, ionogel demonstrates remarkable properties, including strength (0.6–2.4 MPa), excellent toughness (0.9–4.3 MJ m −3 ), hysteresis (6.6–11.6%), (>92%), along enhanced fatigue puncture resistance. Furthermore, exhibit outstanding versatility, enabling strain sensors, flexible electroluminescence devices, nanogenerators. This contributes unparalleled combinatory catering diverse demands iontronics.

Language: Английский

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Bamboo-inspired ultra-strong nanofiber-reinforced composite hydrogels

Nature Communications, Journal Year: 2025, Volume and Issue: 16(1)

Published: Jan. 24, 2025

Biological materials, such as bamboo, are naturally optimized composites with exceptional mechanical properties. Inspired by natural composites, traditional methods involve extracting nanofibers from sources and applying them in composite which, however, often results less ideal To address this, this study develops a bottom-up nanofiber assembly strategy to create strong fiber-reinforced hydrogels inspired the hierarchical of bamboo. Self-assembled chitosan-sodium alginate (CSNFs) combined tannic acid (TA) poly(vinyl alcohol) (PVA) interfacial crosslinker hydrogel matrix, respectively, emulate fundamental cellulose-lignin-hemicellulose composition unit Strong electrostatic interactions hydrogen bonding form between functional groups these components. These molecular can be further reinforced constructing higher-order structure through stretch-induced orientation. The resulting achieves good performance, including high tensile strength up 60.2 MPa simultaneous 48.0 ultimate strain 470%. This approach demonstrates construct robust effectively leveraging interactions. By mimicking bamboo's highly integrated structural composition, it offers promising solution for creating advanced bioinspired materials excellent There is interest properties biological artificial but structures challenging replicate. Here, authors report development bamboo-inspired favourable performance.

Language: Английский

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A self-damping triboelectric tactile patch for self-powered wearable electronics

eScience, Journal Year: 2024, Volume and Issue: unknown, P. 100324 - 100324

Published: Oct. 1, 2024

Language: Английский

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Mechanically Adaptive Polymers Constructed from Dynamic Coordination Equilibria

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(17)

Published: March 7, 2024

Abstract Designing materials capable of adapting their mechanical properties in response to external stimuli is the key preventing failure and extending service life. However, existing mechanically adaptive polymers are hindered by limitations such as inadequate load‐bearing capacity, difficulty achieving reversible changes, high cost, a lack multiple responsiveness. Herein, we address these challenges using dynamic coordination bonds. A new type material with both rate‐ temperature‐responsiveness was developed. Owing stimuli‐responsiveness equilibria, prepared polymers, PBMBD‐Fe PBMBD‐Co, exhibit properties, including temperature‐sensitive strength modulation rate‐dependent impact hardening. Benefitting from nature bonds, exhibited impressive energy dissipation, damping capacity (loss factors 1.15 2.09 at 1.0 Hz), self‐healing, 3D printing abilities, offering durable customizable resistance protective performance. The development impact‐resistant comprehensive has potential applications sustainable intelligent protection fields.

Language: Английский

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Sterically Hindered Oleogel‐Based Underwater Adhesive Enabled by Mesh‐Tailoring Strategy

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(29)

Published: April 29, 2024

Underwater adhesives hold significant relevance in daily life and numerous industrial applications. Despite considerable efforts, developing scalable, high-performance underwater through a simple effective method remains formidable challenge. This study presents novel mesh-tailoring strategy for situ, rapid, ultrastrong oleogel-based (OUA), which comprises highly crosslinked polyurethane network with matching mesh size (≈2.22 nm) that precisely entraps bio-based epoxidized soybean oil (ESO) molecules (≈2.31 by steric hindrance effect. oleogel exhibits unprecedented robust mechanical properties (≈35 MPa) maintains stability under extreme conditions, including high temperatures (100 °C), pressures (30 MPa), immersion various solvents (water, ethanol, or ESO). In particular, this displays hydrophobicity, rapid curing, strong interface affinity, resulting ultrahigh adhesion strength (up to 2.13 exceptional substrate universality. Moreover, the remarkable environmental adaptability of OUA enable its use harsh aqueous environments, acidic/alkaline, saline, temperature solutions. The comprehensive capabilities underscore potential building structures, repairing leaky containers, sealing broken submarine pipelines. research establishes foundation designing next-generation offers fresh perspectives exploring materials.

Language: Английский

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Recyclable and mechanically tough nanocellulose reinforced natural rubber composite conductive elastomers for flexible multifunctional sensor

International Journal of Biological Macromolecules, Journal Year: 2024, Volume and Issue: 268, P. 131946 - 131946

Published: April 29, 2024

Language: Английский

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Intelligent anti-impact elastomers by precisely tailoring the topology of modular polymer networks

Materials Horizons, Journal Year: 2024, Volume and Issue: 11(13), P. 3143 - 3156

Published: Jan. 1, 2024

Utilizing the modular construction strategy, intelligent anti-impact elastomers with varying topology network structures have been prepared by tailoring stereoscopic and linear building blocks as independent modules.

Language: Английский

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Sterically Hindered Organogels with Self‐Healing, Impact Response, and High Damping Properties

Advanced Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 3, 2024

Abstract Organogel materials are vital for impact or shock resistance because of their highly tailored dynamic properties. However, concurrently achieving excellent anti‐impact and damping performances, high stability, self‐healing properties is challenging. Herein, a novel intelligent protective organogel (IPO) comprising boronic ester containing poly(urethane–urea) as the network skeleton with matching mesh size synthesized, precisely entraps hyperbranched fluid used bulky solvent via steric hindrance. The IPO exhibits ability, responsiveness (a 1950‐fold increase in flow stress under various speeds), energy dissipation (the loss factor >0.8 from 10 −4 to 4 Hz). maintains its mechanical during hot pressing hydrolysis, exhibiting stability. Furthermore, omnibearing protection. When coating, dissipates force by 87% 89% control upon passive active impact, respectively. pad, it attenuates 91% amplitude high‐frequency vibrations. This study offers perspective on synthesis sterically hindered provides valuable insights into development next‐generation that exhibit vibration resistance.

Language: Английский

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Insertion of Urea Moieties for One‐Component Strong yet Tough, Self‐Healing Polyurea Protective Materials

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 34(4)

Published: Oct. 15, 2023

Abstract Polyurea has gained increasing attention in civil engineering, flexible electronics, and other emerging fields. However, owing to the rapid polymerization, tailoring their mechanical properties of polyurea for different applications remains challenging. Herein, a novel strategy is proposed insertion urea moieties prepare one‐component robust, mechanically tunable, healable polyurea. First, prepared latent curing agent, isophorone diisocyanate (IPDI), NCO‐terminated prepolymer (PPGTD) are mixed. Due large difference reactivity ─NCO groups IPDI PPGTD, first reacts with deblocked amino form continuous moieties. The resulting inserted into This provides tremendous improvement strength (500% increase), storage modulus (532% toughness (281% increase). Additionally, as‐prepared exhibits excellent self‐healing, impact resistance, high transparency (>90%), dielectric constant (≈4.5). Thus, it can be used as protective film substrate electronic devices. Furthermore, good versatility, which laminated alumina ceramic sheets composites. work opens up promising avenue design fabrication material electronics new insights engineering anti‐impact materials.

Language: Английский

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