Covalent Adaptable Liquid Crystal Networks Enabled by Reversible Ring-Opening Cascades of Cyclic Disulfides

Journal of the American Chemical Society, Год журнала: 2021, Номер 143(32), С. 12543 - 12551

Опубликована: Июль 19, 2021

The development of covalent adaptable liquid crystal networks (LCNs) enabled by introducing dynamic bonds has endowed actuators with self-healing properties and reversible shape programmability, broadening their applications in diverse soft robotic devices. However, the finite molecular design strategy limits recyclability architectural diversity these materials. Here, a is first reported for fabricating photoresponsive polydisulfide-based LCNs ring-opening polymerization cyclic dithiolane groups. Based on disulfide metathesis, resulting materials are self-healable, reshapable, reprogrammable. Importantly, equilibrium between polymer backbones dithiolane-functionalized monomers enables catalytic depolymerization to recycle monomers, which could significantly weaken disadvantage subtractive manufacturing photomechanical This work rooted chemistry would provide an economical environmentally friendly fabrication functional robotics excellent programmability renewability beyond.

Язык: Английский

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Self-Healing Ti₃C₂ MXene/PDMS Supramolecular Elastomers Based on Small Biomolecules Modification for Wearable Sensors

ACS Applied Materials & Interfaces, Год журнала: 2020, Номер 12(40), С. 45306 - 45314

Опубликована: Сен. 14, 2020

Flexible conductive composites can be used as wearable strain sensors, which are widely in the fields of new-generation robotics, electronic skin, and human detection. However, how to make that simultaneously possess flexibility, stretchability, self-healing, sensing capability is challenging research. In this work, we innovatively designed prepared a silicone polymer composite. MXenes amino poly(dimethylsiloxane) were modified by small biomolecules via an esterification reaction Schiff base reaction, respectively. The uniformly dispersed, endows composite with good electrical conductivity. reversibility multiple hydrogen bonds imine system makes it have ideal tensile properties high-efficiency self-healing ability without external stimulation. containing 10 wt % A-MXenes showed elongation 81%, its mechanical strength could reach 1.81 MPa. After repair, conductivity restored 98.4 97.6%, addition, further evaluated for value sensors. Even after cut-healed processes, still accurately detect tiny movements (including speaking, swallowing, pressing). This kind MXene/PDMS elastomers based on modification has great potential simple preparation method provides guidance future multifunctional flexible materials.

Язык: Английский

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Thiol-Mediated Uptake

JACS Au, Год журнала: 2021, Номер 1(6), С. 710 - 728

Опубликована: Май 3, 2021

This Perspective focuses on thiol-mediated uptake, that is, the entry of substrates into cells enabled by oligochalcogenides or mimics, often disulfides, and inhibited thiol-reactive agents. A short chronology from initial observations in 1990 until today is followed a summary cell-penetrating poly(disulfide)s (CPDs) cyclic (COCs) as privileged scaffolds uptake inhibitors potential antivirals. In spirit Perspective, main part brings together topics possibly could help to explain how really works. Extreme sulfur chemistry mostly related COCs their thiosulfinates/-onates, diselenolanes, benzopolysulfanes, but also arsenics Michael acceptors, viewed context acidity, ring tension, exchange cascades, adaptive networks, affinity columns, molecular walkers, ring-opening polymerizations, templated polymerizations. Micellar pores (or lipid ion channels) are considered, peptides natural antibiotics voltage sensors, concise gallery membrane proteins, possible targets provided, including CLIC1, chloride channel; TMEM16F, Ca-activated scramblase; EGFR, epithelial growth factor receptor; protein-disulfide isomerase, known HIV transferrin receptor, top hit proteomics recently identified cellular SARS-CoV-2.

Язык: Английский

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Acylhydrazine-based reticular hydrogen bonds enable robust, tough, and dynamic supramolecular materials

Science Advances, Год журнала: 2022, Номер 8(4)

Опубликована: Янв. 28, 2022

Supramolecular materials are widely recognized among the most promising candidates for future generations of sustainable plastics because their dynamic functions. However, weak noncovalent cross-links that endow properties usually trade off materials' mechanical robustness. Here, we present discovery a simple and robust supramolecular cross-linking strategy based on acylhydrazine units, which can hierarchically cross-link solvent-free network poly(disulfides) by forming unique reticular hydrogen bonds, enabling conversion soft into stiff material. The resulting exhibit increase in stiffness exceeding two to three orders magnitude compared those hydrogen-bonding analogous carboxylic acids, simultaneously preserving repairability, malleability, recyclability materials. also show high adhesion strength various surfaces while allowing multiple surface attachment cycles without fatigue, illustrating viable approach how robustness dynamics be merged material design.

Язык: Английский

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Deep Eutectic Solvents‐Based Ionogels with Ultrafast Gelation and High Adhesion in Harsh Environments

Advanced Functional Materials, Год журнала: 2023, Номер 33(9)

Опубликована: Фев. 1, 2023

Adhesive materials have recently drawn intensive attention due to their excellent sealing ability, thereby stimulating advances in science and industrial usage. However, reported adhesives usually exhibit weak adhesion strength, require high pressure for strong bonding, display severe deterioration various harsh environments. In this work, instead of water or organic solvents, a deep eutectic solution (DES) was used as the medium photopolymerization zwitterionic polarized monomers, thus generating novel ionogel with tunable mechanical properties. Multiple hydrogen bonds electrostatic interactions between DES monomers facilitated ultrafast gelation instant bonding without any external pressure, which rarely previously. Furthermore, different environments (e.g., water, acidic basic buffers, saline solutions) onto hydrophilic glass tissues) hydrophobic polymethyl methacrylate, polystyrene, polypropylene) adherends demonstrated. Also, stretchability at extreme temperatures (-80 80 °C) indicated its widespread applications. biocompatible showed burst stomach intestine tissues prevent liquid leakage, highlighting potential an adhesive patch. This provides unprecedented opportunities fields packaging industry, marine engineering, medical adhesives, electronic assembly.

Язык: Английский

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A Chemically Recyclable Crosslinked Polymer Network Enabled by Orthogonal Dynamic Covalent Chemistry

Angewandte Chemie International Edition, Год журнала: 2022, Номер 61(39)

Опубликована: Авг. 4, 2022

Chemical recycling of synthetic polymers offers a solution for developing sustainable plastics and materials. Here we show that two types dynamic covalent chemistry can be orthogonalized in solvent-free polymer network thus enable chemically recyclable crosslinked material. Using simple acylhydrazine-based 1,2-dithiolane as the starting material, disulfide-mediated reversible polymerization acylhydrazone-based crosslinking combined one-pot reaction, resulting mechanically robust, tough, processable The bonds both backbones crosslinkers endow with depolymerization capability under mild conditions and, importantly, virgin-quality monomers recovered separated. This proof-of-concept study opportunities to design materials based on toolbox.

Язык: Английский

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Reversible Wet‐Adhesive and Self‐Healing Conductive Composite Elastomer of Liquid Metal

Advanced Functional Materials, Год журнала: 2022, Номер 32(35)

Опубликована: Июнь 22, 2022

Abstract Stretchable conductors with the combination of high elasticity and electric conductivity have long been pursued in soft electronics. Liquid metals (LMs), whose mechanical properties match well elastomeric matrix, successfully applied robotics, electronic skins wearable devices. But it remains challenging to develop conductive composite elastomers LMs reversible adhesion self‐healing. Herein, EGaIn droplets are uniformly dispersed into elastomer, which contain dynamic disulfide endow elastomer thermal processability, recyclability, wet adhesion, With content ≥40 vol.%, resultant shows 1.3 × 104 S m −1 , self‐healing 8.0 h, strength up 670 kPa after curing for 2.0 h. When serving as adhesive, can easily adhere metal electrode light LED even when stretched 50%. self‐adhesive bioelectrode, also detect human electromyography signals. Thus, not only may this study provide a new platform designing self‐adhesive, self‐healing, liquid metals, but their promise facileness building damage‐endurable electronics applying human–machine interfaces.

Язык: Английский

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Self-healing, self-adhesive, and stretchable conductive hydrogel for multifunctional sensor prepared by catechol modified nanocellulose stabilized poly(α-thioctic acid)

Carbohydrate Polymers, Год журнала: 2023, Номер 313, С. 120813 - 120813

Опубликована: Март 16, 2023

Язык: Английский

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Robust and dynamic underwater adhesives enabled by catechol-functionalized poly(disulfides) network

National Science Review, Год журнала: 2022, Номер 10(2)

Опубликована: Июль 25, 2022

Developing molecular approaches to the creation of robust and water-resistant adhesive materials promotes a fundamental understanding interfacial adhesion mechanisms as well future applications biomedical materials. Here, we present simple strategy that combines natural thioctic acid mussel-inspired iron-catechol complexes enable ultra-strong can be used underwater simultaneously exhibit unprecedentedly high strength on diverse surfaces. Our experimental results show crosslinking interaction complexes, high-density hydrogen bonding, are responsible for ultra-high strength. The embedding effect hydrophobic solvent-free network poly(disulfides) further enhances water-resistance. dynamic covalent also makes resulting reconfigurable, thus enabling reusability via repeated heating cooling. This molecule-engineering offers general versatile solution design construction supramolecular

Язык: Английский

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New Advances in Covalent Network Polymers via Dynamic Covalent Chemistry

Chemical Reviews, Год журнала: 2024, Номер 124(12), С. 7829 - 7906

Опубликована: Июнь 3, 2024

Covalent network polymers, as materials composed of atoms interconnected by covalent bonds in a continuous network, are known for their thermal and chemical stability. Over the past two decades, these have undergone significant transformations, gaining properties such malleability, environmental responsiveness, recyclability, crystallinity, customizable porosity, enabled development integration dynamic chemistry (DCvC). In this review, we explore innovative realm polymers focusing on recent advances achieved through application DCvC. We start examining history fundamental principles DCvC, detailing its inception core concepts noting key role reversible bond formation. Then reprocessability DCvC is thoroughly discussed, starting from milestones that marked evolution progressing to current trends applications. The influence crystallinity then reviewed, covering diversity, synthesis techniques, functionalities. concluding section, address challenges faced field speculates potential future directions.

Язык: Английский

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