Disulfide-Mediated Reversible Polymerization toward Intrinsically Dynamic Smart Materials

Journal of the American Chemical Society, Год журнала: 2022, Номер 144(5), С. 2022 - 2033

Опубликована: Янв. 6, 2022

The development of a dynamic chemistry toolbox to endow materials behavior has been key the rational design future smart materials. rise supramolecular and covalent offers many approaches construction polymers that can adapt, respond, repair, recycle. Within this toolbox, building blocks based on 1,2-dithiolanes have become an important scaffold, featuring their reversible polymerization mediated by disulfide bonds, which enables unique class at intersection adaptable networks. This Perspective aims explore as versatile structural unit for summarizing state art well providing overview fundamental challenges involved in research area its potential directions.

Язык: Английский

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Room-temperature self-healing supramolecular polyurethanes based on the synergistic strengthening of biomimetic hierarchical hydrogen-bonding interactions and coordination bonds

Chemical Engineering Journal, Год журнала: 2022, Номер 451, С. 138673 - 138673

Опубликована: Авг. 18, 2022

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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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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Photoinduced Dithiolane Crosslinking for Multiresponsive Dynamic Hydrogels

Advanced Materials, Год журнала: 2023, Номер unknown

Опубликована: Янв. 30, 2023

While many hydrogels are elastic networks crosslinked by covalent bonds, viscoelastic with adaptable crosslinks increasingly being developed to better recapitulate time and position-dependent processes found in tissues. In this work, 1,2-dithiolanes presented as dynamic photocrosslinkers of hydrogels, resulting disulfide bonds throughout the hydrogel that respond multiple stimuli. Using lipoic acid a model dithiolane, formed under physiological conditions, enabling cell encapsulation via an initiator-free light-induced dithiolane ring-opening photopolymerization. The allow for photoinduced responses including stress relaxation, stiffening, softening, network functionalization using single chemistry, which can be supplemented permanent reaction alkenes further control properties connectivity irreversible thioether crosslinks. Moreover, complementary photochemical approaches used achieve rapid complete sample degradation radical scission post-gelation stiffening when irradiated presence reactive gel precursor. results herein demonstrate versatility material chemistry study direct 2D 3D cell-material interactions. This work highlights dithiolane-based photocrosslinking robust method generating range biologically relevant mechanical chemical varied on demand.

Язык: Английский

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Acid‐catalyzed Disulfide‐mediated Reversible Polymerization for Recyclable Dynamic Covalent Materials

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(11)

Опубликована: Янв. 5, 2023

Poly(1,2-dithiolane)s are a family of intrinsically recyclable polymers due to their dynamic covalent disulfide linkages. Despite the common use thiolate-initiated anionic ring-opening polymerization (ROP) under basic condition, cationic ROP is still not exploited. Here we report that bond can act as proton acceptor, being protonated by acids form sulfonium cations, which efficiently initiate 1,2-dithiolanes and result in high-molecular-weight (over 1000 kDa) poly(disulfide)s. The reaction be triggered adding catalytic amounts non-coordinating anion salts, completed few minutes at room temperature. acidic conditions allow applicability for monomers. Importantly, condition open air without inert protection, enabling nearly quantitative chemical recycling from bulk materials original

Язык: Английский

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Transparent High‐Performance Supramolecular Plastics Operating in All‐Weather Environments

Advanced Functional Materials, Год журнала: 2023, Номер 33(11)

Опубликована: Янв. 3, 2023

Abstract Supramolecular plastics (SMPs) can be made mechanically robust, repairable, and recyclable, rendering themselves promising alternatives to their conventional predecessors address environmental concerns. However, dense accumulations of noncovalent bonds generally lead mechanical brittleness as well intolerance toward heat moisture. To resolve this issue, a simple strategy preparing high‐performance SMP by constructing highly dense, but irregular hydrogen‐bond networks with hierarchical structures is proposed. The resultant exhibits an outstanding combination good comprehensive properties (high stiffness, strength, toughness ductile failure when fracturing), excellent dynamic behaviors (repairability recyclability), high tolerances moisture temperatures (as 90 °C). Additionally, the also shows dielectric constant, exhibiting great potential for applications such healable flexible touch screens energy storage. Last, through structure characterizations molecular simulation, study provides fundamental insight into mechanism behind high‐performances from nano‐ micro‐scales, which expected inspire design wide range other SMPs that use different chemistries.

Язык: Английский

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A renewably sourced, circular photopolymer resin for additive manufacturing

Nature, Год журнала: 2024, Номер 629(8014), С. 1069 - 1074

Опубликована: Май 15, 2024

The additive manufacturing of photopolymer resins by means vat photopolymerization enables the rapid fabrication bespoke 3D-printed parts. Advances in methodology have continually improved resolution and speed, yet both process design resin technology remained largely consistent since its inception 1980s

Язык: Английский

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Emerging Hydrogen-Bond Design for High-Performance Dynamic Polymeric Materials

ACS Materials Letters, Год журнала: 2023, Номер 5(2), С. 480 - 490

Опубликована: Янв. 13, 2023

The hydrogen bond, one of the simplest and most versatile noncovalent interactions, is essential for many dynamic functions in living systems. After long-term fundamental development, H-bond chemistry has been well established, with a large family molecular moieties tunable binding affinities available. In past several years, growing interest polymeric materials aroused series emerging applications material design. This Perspective aims at discussing design principles H-bond-based by summarizing state art recently emerged materials. Opportunities challenges are proposed to provide an overview this research topic, possible future directions, potential applications.

Язык: Английский

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