Supramolecular Organic Nanofiller: A New Reinforcement Strategy for Dynamic Covalent Polymer Networks Toward Upcycling of Carbon Fiber Composites DOI Open Access
Zhipeng Zhang, Qian Lu,

Dandan Hu

et al.

Advanced Materials, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 22, 2025

Abstract Dynamic covalent polymer networks (DCPN) provide an important solution to the challenging recyclability of thermoset elastomers. However, dynamic bonds exhibit relatively weak bond energies, considerably decreasing mechanical properties DCPN. Herein, a novel reinforcement strategy for DCPN involving in situ formation supramolecular organic nanofillers through asynchronous polymerization is proposed. Owing difference reactivity isocyanate groups and gradual deblocking aldimine, cross‐linking hexamethylene diisocyanate isocyanate‐terminated prepolymer containing oxime–urethane with deblocked tris(2‐aminoethyl)amine facilitates transition from molecular interpenetration chains into immiscible polymerization. This results thermodynamic incompatibility between hyperbranched clusters long chains, inducing spontaneous nanofillers. Compared traditional strategies, improve Furthermore, interactions enable network excellent recyclability. The unique prepared allow their combination carbon fibers (CF) form CF composites outstanding personal‐protection applications, achieving composite upcycling. study offers on upcycling high‐performance composites.

Language: Английский

Circular 3D printing of high-performance photopolymers through dissociative network design DOI

Bo Yang,

Tiantian Ni,

Jingjun Wu

et al.

Science, Journal Year: 2025, Volume and Issue: 388(6743), P. 170 - 175

Published: April 10, 2025

One approach for closed-loop plastics recycling relies on reverting polymers back into monomers because one can then make new without loss of properties. This depolymerization requirement restricts the molecular design to making with high mechanical performance. We report a three-dimensional (3D) printing chemistry through stepwise photopolymerization by forming dithioacetal bonds. The polymerized network be transformed photoreactive oligomer dissociation network-oligomer transformation is reversible, therefore allowing circular 3D using same material. Our offers flexibility modular adjustments in backbone polymer. allows access fully recyclable elastomers, crystalline polymers, and rigid glassy toughness, them potentially suitable diverse applications.

Language: Английский

Citations

2
Mechanically Robust, Recyclable, and Self‐Healing Polyimine Networks DOI Creative Commons

Ping Yu,

Haiyue Wang, Ting Li

et al.

Advanced Science, Journal Year: 2023, Volume and Issue: 10(19)

Published: April 23, 2023

To achieve energy saving and emission reduction goals, recyclable healable thermoset materials are highly attractive. Polymer copolymerization has been proven to be a critical strategy for preparing high-performance polymeric materials. However, it remains huge challenge develop Here, polyimine dynamic networks based on two monomers with bulky pendant groups, which not only displayed mechanical properties higher than the strong tough polymers, e.g., polycarbonate, but also excellent self-repairing capability recyclability as thermosets developed. Owing stability of conjugation effect by aromatic benzene rings, final far more stable reported counterparts, exhibiting hydrolysis resistance under both alkaline condition most organic solvents. These structure can completely depolymerized into recovery in an acidic aqueous solution at ambient temperature. Resulting from units, this method allows exchange reactions vitrimer easily within minutes self-healing function. Moreover, introduction trifluoromethyl diphenoxybenzene backbones significantly increases tensile This work provides effective fabricating polymer multiple functions.

Language: Английский

Citations

42
Reversible Amidation Chemistry Enables Closed‐Loop Chemical Recycling of Carbon Fiber Reinforced Polymer Composites to Monomers and Fibers DOI Open Access
Bo Qin, Siyuan Liu, Jiang‐Fei Xu

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(43)

Published: Sept. 7, 2023

Highly efficient recycling of carbon fiber reinforced polymer composites into monomers and fibers is a formidable challenge. Herein, we present closed-loop approach for using reversible amidation chemistry, which enables the complete recovery intact pure monomers. The network, synthesized by between macromonomer linear polyethyleneimine bifunctional maleic anhydride cross-linker, serves as matrix construction with exceptional mechanical properties, thermal stability solvent resistance. matrices can be fully depolymerized under acidic condition at ambient temperature, allowing effective separation both two reclaimed retain nearly identical properties to pristine ones, while are recycled high yields (>93 %). They reused in multiple cycles manufacture new composites, whose recover over 95 % their original properties. This line research presents promising design high-performance sustainable thermoset offering significant environmental economic benefits.

Language: Английский

Citations

35
Hyperbranched Dynamic Crosslinking Networks Enable Degradable, Reconfigurable, and Multifunctional Epoxy Vitrimer DOI Creative Commons
Yuanbo Zhang, Hongxia Yan, Ruizhi Yu

et al.

Advanced Science, Journal Year: 2023, Volume and Issue: 11(2)

Published: Nov. 7, 2023

Abstract Degradation and reprocessing of thermoset polymers have long been intractable challenges to meet a sustainable future. Star strategies via dynamic cross‐linking hydrogen bonds and/or covalent can afford reprocessable thermosets, but often at the cost properties or even their functions. Herein, simple strategy coined as hyperbranched crosslinking networks (HDCNs) toward in‐practice engineering petroleum‐based epoxy into degradable, reconfigurable, multifunctional vitrimer is provided. The special characteristics HDCNs involve spatially topological crosslinks for solvent adaption multi‐dynamic linkages reversible behaviors. resulting displays mild room‐temperature degradation dimethylacetamide realize cycling carbon fiber powder from composite. Besides, they supra toughness high flexural modulus, transparency well fire‐retardancy surpassing original thermoset. Notably, it noted in chance‐following that ethanol molecule induce reconstruction network by ester‐exchange, converting stiff elastomeric feature, such material records an ultrahigh modulus (5.45 GPa) −150 °C ultralow‐temperature condition uses. This shaping up be potentially advanced address post‐consumer waste, also provide newly crosslinked mode designs high‐performance polymer.

Language: Английский

Citations

35
Acid‐Cleavable Aromatic Polymers for the Fabrication of Closed‐Loop Recyclable Plastics with High Mechanical Strength and Excellent Chemical Resistance DOI
Xingyuan Lu, Peng Xie, Xiang Li

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 63(7)

Published: Dec. 22, 2023

Although closed-loop recycling of dynamic covalent bond-based plastics does not require catalysts, their mechanical strength and chemical stability remain a major concern. In this study, recyclable poly(aryl imine) (PAI) with high excellent resistance are fabricated by copolymerizing aromatic amines aldehydes through imine bonds. The resulting PAI plastic tensile 58.2 MPa exhibits in acidic basic aqueous solutions various organic solvents. can be depolymerized mixed solvent tetrahydrofuran (THF)/HCl solution the dissociation bonds, monomers facilely recovered purity isolated yields due to solubility difference between selective efficient also realized monomer conversion because hydrolysis generates amines. used re-fabricate original plastics. This selectively from complicated polymer waste streams mild depolymerization conditions its most

Language: Английский

Citations

32
Biorenewable and circular polydiketoenamine plastics DOI
Jérémy Demarteau, Benjamin Cousineau, Zilong Wang

et al.

Nature Sustainability, Journal Year: 2023, Volume and Issue: 6(11), P. 1426 - 1435

Published: July 27, 2023

Language: Английский

Citations

30
Dynamic Covalent Adaptable Polyimide Hybrid Dielectric Films with Superior Recyclability DOI
Baoquan Wan, Mengyu Xiao,

Xiaodi Dong

et al.

Advanced Materials, Journal Year: 2023, Volume and Issue: unknown

Published: June 29, 2023

Abstract Polyimides (PIs) used in advanced electrical and electronic devices can be electrically/mechanically damaged, resulting a significant waste of resources. Closed‐loop chemical recycling may prolong the service life synthetic polymers. However, design dynamic covalent bonds for preparing chemically recyclable crosslinked PIs remains challenging task. Herein, new PI films containing oligomer, chain extender, crosslinker are reported. They exhibit superior recyclability excellent self‐healable ability owing to synergistic effect extender crosslinker. The produced completely depolymerized an acidic solution at ambient temperature, leading efficient monomer recovery. recovered monomers remanufacture without deteriorating their original performance. In particular, designed serve as corona‐resistant with recovery rate approximately 100%. Furthermore, carbon fiber reinforced composites (CFRCs) matrices suitable harsh environments recycled multiple times non‐destructive up preparation high‐strength adaptable hybrid from simple oligomers, extenders, crosslinkers provide solid basis sustainable development fields.

Language: Английский

Citations

29
Direct and Catalyst-Free Ester Metathesis Reaction for Covalent Adaptable Networks DOI

Shijia Yang,

Wenxing Liu, Jing Guo

et al.

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(38), P. 20927 - 20935

Published: Sept. 15, 2023

Thermosetting polymers possess excellent environmental resistance and mechanical properties but cannot be reprocessed due to their covalently cross-linked structures. Recycling of thermosets via the implantation dynamic covalent bonds offers a promising solution. Here, we report direct catalyst-free ester metathesis N-acyloxyphthalimide (NAPI) at about 100 °C without requirement hydroxyl groups its utilization for fabrication adaptable networks (CANs). NAPI has interesting sigmoid kinetics with fast exchange rate, which proceeds free radical chain mechanism, guaranteeing associative under rather low dissociation. The bifunctional molecule as both precursor substrate is key dissociatively initiated (DAssociative) mechanism kinetic behavior. Based on efficient metathesis, polyester networks, poly(N-acyloxyphthalimides) (PNAPIs), show malleability. Notably, PNAPIs exhibit exceptional solvent stability elevated temperatures owing unique DAssociative suggesting exciting opportunities designing recyclable thermosetting polymers.

Language: Английский

Citations

24
Chemically Recyclable Supramolecular Thermosets toward Strong and Reusable Hot-Melt Adhesives DOI
Chunyang Bao, Yanlong Yin, Yuhan Ding

et al.

Macromolecules, Journal Year: 2023, Volume and Issue: 56(17), P. 6633 - 6643

Published: Aug. 25, 2023

Chemically recyclable thermosets are an ideal substitute for traditional in the development of a circular economy and sustainable environment. However, efficient easy-to-achieve chemical recycling strategies remains challenging. Herein, series supramolecular that can be chemically recycled under mild acid conditions at room temperature fabricated by cross-linking polyimine polymers with dynamic boroxines (PIx-Boroxine). By tailoring molar content boroxines, PI1.2-boroxine exhibit tensile strength ∼30.6 MPa, yield 33.0 elongation break ∼111.6%, Young's modulus ∼679.6 MPa. Because nature imine bonds, PIx-boroxine thermoset exhibits fast stress relaxation behavior, which enables them to have good reprocessing ability. These unique features also guarantee high-performance reusable hot-melt adhesive. The maximum lap shear PIx-Boroxine-based adhesives stainless steel bonding adhesive reach ∼18.6 is comparable commercial adhesives. Meanwhile, reused least 10 times only small amount reduction strength. More importantly, easily depolymerized 0.1 M HCl/H2O solution temperature. Further, monomers efficiently separated simple separation procedure. recovered fabricate new without losing their mechanical properties. This work provides design strategy develop recyclability, will contribute modern society.

Language: Английский

Citations

23
Photothermal-responsive lignin-based polyurethane with mechanically robust, fast self-healing, solid-state plasticity and shape-memory performance DOI
Xiaochun Liu, Zhiyi Huang,

Jianxin Wu

et al.

International Journal of Biological Macromolecules, Journal Year: 2024, Volume and Issue: 271, P. 132499 - 132499

Published: May 20, 2024

Language: Английский

Citations

15