Thermally Robust yet Deconstructable and Chemically Recyclable High‐Density Polyethylene (HDPE)‐Like Materials Based on Si−O Bonds DOI Creative Commons
Alayna M. Johnson,

Jeremiah A. Johnson

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(51)

Опубликована: Окт. 30, 2023

Polyethylene (PE) is the most widely produced synthetic polymer. By installing chemically cleavable bonds into backbone of PE, it possible to produce deconstructable PE derivatives; date, however, such designs have primarily relied on carbonyl- and olefin-related functional groups. Bifunctional silyl ethers (BSEs; SiR2 (OR'2 )) could expand scope mimics as they possess strong Si-O facile chemical tunability. Here, we report BSE-containing high-density polyethylene (HDPE)-like materials synthesized through a one-pot catalytic ring-opening metathesis polymerization (ROMP) hydrogenation sequence. The crystallinity these can be adjusted by varying BSE concentration or steric bulk Si-substituents, providing handles control thermomechanical properties. Two methods for recycling HDPE are introduced, including circular approach that leverages acid-catalyzed bond exchange with 1-propanol. Additionally, despite fact starting were chain-growth (ROMP), show recover molar mass dispersity recycled products using step-growth formation exchange, generating high molecular weight mechanical properties similar commercial HDPE.

Язык: Английский

Vitrimer composites: current status and future challenges DOI Creative Commons

Vincent Schenk,

Karine Labastié,

Mathias Destarac

и другие.

Materials Advances, Год журнала: 2022, Номер 3(22), С. 8012 - 8029

Опубликована: Янв. 1, 2022

Vitrimers: one step towards a greener future for the composite industry?

Язык: Английский

Процитировано

127
A Highly Dynamic Covalent Polymer Network without Creep: Mission Impossible? DOI
Filip Van Lijsebetten, Tapas Debsharma, Johan M. Winne

и другие.

Angewandte Chemie International Edition, Год журнала: 2022, Номер 61(48)

Опубликована: Сен. 26, 2022

Dynamic covalent polymer networks provide an interesting solution to the challenging recyclability of thermosets and elastomers. One remaining design constraints, however, is balancing thermal reprocessability in form material flow with dimensional stability during use. As a result, many chemistries are being investigated order improve bond reactivity control robustness. This Minireview highlights number promising concepts, particular emphasis on disconnecting chemical low high temperature regimes obtain creep resistant, yet highly dynamic networks. In addition, we will highlight impact sharp changes when applying extrapolation-based approaches rheological analysis. confident that abandoning myth "permanent" aid development sustainable polymeric materials can truly combine benefits thermoplastic thermoset behaviour.

Язык: Английский

Процитировано

98
Circularity in polymers: addressing performance and sustainability challenges using dynamic covalent chemistries DOI Creative Commons
Tianwei Yan, Alex H. Balzer, Katie M. Herbert

и другие.

Chemical Science, Год журнала: 2023, Номер 14(20), С. 5243 - 5265

Опубликована: Янв. 1, 2023

This review provides a multidisciplinary overview of the challenges and opportunities for dynamic covalent chemistry-based macromolecules towards design new, sustainable, recyclable materials circular economy.

Язык: Английский

Процитировано

48
Strong yet Tough Catalyst‐Free Transesterification Vitrimer with Excellent Fire‐Retardancy, Durability, and Closed‐Loop Recyclability DOI Creative Commons
Guofeng Ye, Siqi Huo, Cheng Wang

и другие.

Small, Год журнала: 2024, Номер 20(45)

Опубликована: Июль 31, 2024

Despite great advances in vitrimer, it remains highly challenging to achieve a property portfolio of excellent mechanical properties, desired durability, and high fire safety. Thus, catalyst-free, closed-loop recyclable transesterification vitrimer (TPN

Язык: Английский

Процитировано

38
Ultrastrong and Thermo‐Remoldable Lignin‐Based Polyurethane Foam Insulation with Active‐Passive Fire Resistance DOI
Lichao Sun,

Yujia Guo,

Rongxian Ou

и другие.

Advanced Functional Materials, Год журнала: 2024, Номер 34(40)

Опубликована: Июнь 19, 2024

Abstract Foam thermal insulators are indispensable for prevailing energy‐saving engineering, however their widespread use brings intractability such as unsustainability, “white pollution”, and fire hazards. The emergence of bio‐based foams is highly appreciated, but the fabrication approaches economically unattractive and/or product properties inferior, making large‐scale implementation unviable. Herein, a versatile, thermally remoldable phosphate‐containing polyurethane composite foam (LPU‐G) constructed from natural lignin expanded graphite flakes via an atmospheric pressure scalable one‐pot strategy. optimal LPU‐G exhibits exceptional mechanical strength, capable supporting over 6000 times its weight without significant deformation. Moreover, demonstrates desired multifunctionality in handling extreme circumstances, including humidity‐tolerant insulation, superb water vapor barrier, withstanding ≈1200 °C flame ignition. Based on “expansion‐conductivity” micro‐mechanism, first material to be sensitive alarm system with ultra‐long time (>1800 s). Surprisingly, can rapidly upcycled into recyclable bulk composites second life through simple thermo‐molding processes rooted multi‐dynamic behavior phosphate, carbamate, hydrogen bonds. easy‐to‐scale represents new generation that address concerns regarding high cost, risk, inferior properties.

Язык: Английский

Процитировано

21
Taking dynamic covalent chemistry out of the lab and into reprocessable industrial thermosets DOI
Stephan Maes, Nezha Badi, Johan M. Winne

и другие.

Nature Reviews Chemistry, Год журнала: 2025, Номер unknown

Опубликована: Янв. 31, 2025

Язык: Английский

Процитировано

5
Remolding and Deconstruction of Industrial Thermosets via Carboxylic Acid-Catalyzed Bifunctional Silyl Ether Exchange DOI
Keith E. L. Husted, Christopher M. Brown, Peyton Shieh

и другие.

Journal of the American Chemical Society, Год журнала: 2023, Номер 145(3), С. 1916 - 1923

Опубликована: Янв. 13, 2023

Convenient strategies for the deconstruction and reprocessing of thermosets could improve circularity these materials, but most approaches developed to date do not involve established, high-performance engineering materials. Here, we show that bifunctional silyl ether, i.e., R'O-SiR2-OR'', (BSE)-based comonomers generate covalent adaptable network analogues industrial thermoset polydicyclopentadiene (pDCPD) through a novel BSE exchange process facilitated by low-cost food-safe catalyst octanoic acid. Experimental studies density functional theory calculations suggest an mechanism involving ester intermediates with formation rates strongly depend on Si-R2 substituents. As result, pDCPD manufactured display temperature- time-dependent stress relaxation as function their Moreover, bulk remolding is enabled first time. Altogether, this work presents new approach toward installation exchangeable bonds into commercial establishes acid-catalyzed versatile addition toolbox dynamic chemistry.

Язык: Английский

Процитировано

40
Fluoride‐Catalyzed Siloxane Exchange as a Robust Dynamic Chemistry for High‐Performance Vitrimers DOI Creative Commons

Chase A. Tretbar,

Jordan Castro,

Kosuke Yokoyama

и другие.

Advanced Materials, Год журнала: 2023, Номер 35(28)

Опубликована: Май 16, 2023

Sustainable development of new technologies requires materials having advanced physical and chemical properties while maintaining reprocessability recyclability. Vitrimers are designed for this purpose; however, their dynamic covalent chemistries often have drawbacks or limited to specialized polymers. Here, fluoride-catalyzed siloxane exchange is reported as an exceptionally robust chemistry scalable production high-performance vitrimers through industrial processing commodity polymers such poly(methyl methacrylate), polyethylene, polypropylene. The show improved resistance creep, heat, oxidation, hydrolysis, excellent melt flow recycling. Furthermore, the between different during mechanical blending results in self-compatibilized blends without any compatibilizers. This offers a general, method producing sustainable strategy recycling mixed plastic wastes.

Язык: Английский

Процитировано

39
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

и другие.

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(43)

Опубликована: Сен. 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.

Язык: Английский

Процитировано

35
Reprocessible Triketoenamine‐Based Vitrimers with Closed‐Loop Recyclability DOI

Z. G. Hu,

Fan Hu,

Lifeng Deng

и другие.

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(34)

Опубликована: Июнь 14, 2023

Development of thermosets that can be repeatedly recycled via both chemical route (closed-loop) and thermo-mechanical process is attractive remains an imperative task. In this work, we reported a triketoenamine based dynamic covalent network derived from 2,4,6-triformylphloroglucinol secondary amines. The resulting does not have intramolecular hydrogen bonds, thus reducing its π-electron delocalization, lowering the stability tautomer structure, enabling feature. By virtue highly reversible bond exchange, novel enables easy construction crosslinked chemically reprocessable networks commercially available monomers. as-made polymer monoliths exhibit high mechanical properties (tensile strength 79.4 MPa Young's modulus 571.4 MPa) undergo monomer-network-monomer (yields up to 90 %) recycling mediated by aqueous solution, with new-generation capable restoring material original state. addition, owing nature, catalyst-free low-temperature reprogrammable adaptable (vitrimer) was achieved. design concept herein applied development other vitrimers repressibility recyclability, sheds light on future sustainable polymers minimal environmental impact.

Язык: Английский

Процитировано

23