Macromolecules, Год журнала: 2025, Номер unknown
Опубликована: Май 19, 2025
Язык: Английский
Macromolecules, Год журнала: 2025, Номер unknown
Опубликована: Май 19, 2025
Язык: Английский
Nature Reviews Materials, Год журнала: 2024, Номер 9(12), С. 866 - 886
Опубликована: Авг. 19, 2024
Язык: Английский
Процитировано
34Green Chemistry, Год журнала: 2024, Номер 26(5), С. 2384 - 2420
Опубликована: Янв. 1, 2024
While our society is facing the challenge of accumulating plastic waste, this review discusses recent advances towards polymer circularity with an emphasis on manipulations monomer–polymer equilibrium to create chemically recyclable polymers.
Язык: Английский
Процитировано
16Macromolecules, Год журнала: 2024, Номер 57(3), С. 869 - 879
Опубликована: Янв. 24, 2024
The design of cyclic monomers is crucial for the development polymers with ideal thermal and mechanical properties by ring-opening polymerization. Herein, we provide a systematic investigation into thio-modification effects on polymerization behavior ether–ester final corresponding poly(ether-alt-ester)s. position significantly affected thermodynamics thus could regulate ceiling temperature (Tc). O-to-S substitutions in monomer′s ether/ester sites would increase α-H acidity, catalytic system strictly determined chain initiation process as well chain-end groups. Density functional theory calculations experimental studies revealed that at ester site accelerate under same conditions, thanks to high reactivity thioester group strong nucleophilicity end. resulting poly(ether-alt-ester)s exhibited crystallinity, precisely tunable physicochemical properties, recyclability, high-density polyethylene-like which exemplifies potential heteroatom modification modulating poly(ether-alt-ester)′s properties. This detailed structure–(de)polymerizability structure–property relationships will inspire future monomer toward performance.
Язык: Английский
Процитировано
13Angewandte Chemie, Год журнала: 2024, Номер 136(24)
Опубликована: Апрель 8, 2024
Abstract Environmentally friendly crosslinked polymer networks feature degradable covalent or non‐covalent bonds, with many of them manifesting dynamic characteristics. These attributes enable convenient degradation, facile reprocessibility, and self‐healing capabilities. However, the inherent instability these crosslinking bonds often compromises mechanical properties networks, limiting their practical applications. In this context, environmentally dual‐crosslinking (denoted EF‐DCPNs) have emerged as promising alternatives to address challenge. materials effectively balance need for high ability degrade, recycle, and/or self‐heal. Despite potential, investigations into EF‐DCPNs remain in nascent stages, several gaps limitations persist. This Review provides a comprehensive overview synthesis, properties, applications recent progress EF‐DCPNs. Firstly, synthetic routes rich variety possessing two distinct types (i.e., imine, disulfide, ester, hydrogen bond, coordination other bonds) are introduced. Subsequently, complex structure‐ nature‐dependent mechanical, thermal, electrical discussed, followed by exemplary electronics biotechnology. Finally, future research directions rapidly evolving field outlined.
Язык: Английский
Процитировано
13Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(13)
Опубликована: Фев. 15, 2024
Abstract The development of new chemically recyclable polymers via monomer design would provide a transformative strategy to address the energy crisis and plastic pollution problem. Biaryl‐fused cyclic esters were targeted generate axially chiral polymers, which impart material performance. To overcome non‐polymerizability biaryl‐fused DBO, ester Me‐DBO installed with dimethyl substitution was prepared enable its polymerizability enhancing torsional strain. Impressively, readily went through well‐controlled ring‐opening polymerization, producing polymer P(Me‐DBO) high glass transition temperature ( T g >100 °C). Intriguingly, mixing these complementary enantiopure containing axial chirality promoted transformation from amorphous crystalline material, affording semicrystalline stereocomplex melting more than 300 °C. capable depolymerizing back in efficiency, highlighting an excellent recyclability.
Язык: Английский
Процитировано
11Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(24)
Опубликована: Апрель 8, 2024
Environmentally friendly crosslinked polymer networks feature degradable covalent or non-covalent bonds, with many of them manifesting dynamic characteristics. These attributes enable convenient degradation, facile reprocessibility, and self-healing capabilities. However, the inherent instability these crosslinking bonds often compromises mechanical properties networks, limiting their practical applications. In this context, environmentally dual-crosslinking (denoted EF-DCPNs) have emerged as promising alternatives to address challenge. materials effectively balance need for high ability degrade, recycle, and/or self-heal. Despite potential, investigations into EF-DCPNs remain in nascent stages, several gaps limitations persist. This Review provides a comprehensive overview synthesis, properties, applications recent progress EF-DCPNs. Firstly, synthetic routes rich variety possessing two distinct types (i.e., imine, disulfide, ester, hydrogen bond, coordination other bonds) are introduced. Subsequently, complex structure- nature-dependent mechanical, thermal, electrical discussed, followed by exemplary electronics biotechnology. Finally, future research directions rapidly evolving field outlined.
Язык: Английский
Процитировано
10Journal of the American Chemical Society, Год журнала: 2023, Номер 145(50), С. 27788 - 27799
Опубликована: Ноя. 21, 2023
Poly(disulfide)s are an emerging class of sulfur-containing polymers with applications in medicine, energy, and functional materials. However, the constituent dynamic covalent S-S bond is highly reactive presence sulfide (RS-) anion, imposing a persistent challenge to control polymerization. Here, we report anion-binding approach arrest high reactivity RS- chain end synthesis linear poly(disulfide)s, realizing rapid, living ring-opening polymerization 1,2-dithiolanes narrow dispersity regioselectivity (Mw/Mn ∼ 1.1, Ps 0.85). Mechanistic studies support formation thiourea-base-sulfide ternary complex as catalytically active species during propagation. Theoretical analyses reveal synergistic catalytic model where catalyst preorganizes protonated base anionic establish spatial confinement over bound monomer, effecting observed regioselectivity. The system amenable monomers various groups, semicrystalline also obtained from lipoic acid derivatives by enhancing
Язык: Английский
Процитировано
18Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(17)
Опубликована: Фев. 29, 2024
Abstract Elemental sulfur, a waste product of the oil refinement process, represents promising raw material for synthesis degradable polymers. We show that simple lithium alkoxides facilitate polymerisation elemental sulfur S 8 with industrially relevant propylene oxide (PO) and CS 2 (a base chemical sourced from itself) to give poly(monothiocarbonate‐alt‐S x ) in which can be controlled by amount supplied sulfur. The situ generation thiolate intermediates obtained rearrangement, follows PO incorporation, allows combine epoxides into one polymer sequence would otherwise not possible. Mechanistic investigations reveal alkyl oligosulfide ring opening chain length equilibration represent better nucleophiles inserting next if compared trithiocarbonates competing addition, causes selectivity. polymers crosslinked multifunctional thiols yield reprocessable networks. Our report demonstrates how mechanistic understanding intrinsically incompatible building blocks utilisation.
Язык: Английский
Процитировано
9Polymer Chemistry, Год журнала: 2024, Номер 15(11), С. 1070 - 1076
Опубликована: Янв. 1, 2024
A seven-membered cyclic carbonate bearing a cis -fused cyclohexane structure enabled the chemical recycling of polycarbonate to high-ring-strain monomer.
Язык: Английский
Процитировано
7Journal of the American Chemical Society, Год журнала: 2024, Номер 146(26), С. 18074 - 18082
Опубликована: Июнь 21, 2024
A cyclic thioenone system capable of controlled ring-opening polymerization (ROP) is presented that leverages a reversible Michael addition-elimination (MAE) mechanism. The monomers are easy to access and modify for the first time incorporate dynamic reversibility MAE with chain-growth polymerization. This strategy features mild conditions, tunable functionalities, molecular weights (
Язык: Английский
Процитировано
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