ACS Applied Polymer Materials, Journal Year: 2024, Volume and Issue: 6(19), P. 11877 - 11888
Published: Sept. 24, 2024
Language: Английский
Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(14), P. 9920 - 9927
Published: April 1, 2024
Plastic recycling is critical for waste management and achieving a circular economy, but it entails difficult trade-offs between performance recyclability. Here, we report thermoset, poly(α-cyanocinnamate) (PCC), synthesized using Knoevenagel condensation terephthalaldehyde (TPA) triarm cyanoacetate star, that tackles this difficulty by harnessing its intrinsically conjugated dynamic chemical characteristics. PCCs exhibit extraordinary thermal mechanical properties with typical Tg of ∼178 °C, Young's modulus 3.8 GPa, tensile strength 102 MPa, along remarkable flexibility dimensional stabilities. Furthermore, end-of-life can be selectively degraded partially recycled back into one starting monomer TPA new production cycle or reprocessed through exchange aided chain-ends. This study lays the scientific groundwork design robust recyclable thermosets, transformative potential in plastic engineering.
Language: Английский
Citations
17
Nature Reviews Chemistry, Journal Year: 2025, Volume and Issue: unknown
Published: Jan. 31, 2025
Language: Английский
Citations
3
Advanced Materials, Journal Year: 2024, Volume and Issue: unknown
Published: Dec. 10, 2024
Skeletal muscles represent a role model in soft robotics featuring agile locomotion and incredible mechanical robustness. However, existing actuators lack an optimal combination of actuation parameters (including modes, work capacity, strength, damage repair) to rival biological tissues. Here, biomimetic structural design strategy via multilevel relaxations (α/β/γ/δ-relaxation) modulation is proposed for robust healable actuator materials with muscle-like diastole contraction abilities by orientational alignment dendritic polyphenol-modified nano-assembles eutectogels. The anisotropic hierarchical micro-nanostructures assembled supramolecular interaction mimic the relative slippage actin filaments myosin muscles, ensuring bistable through rapid thermal α-relaxation expansion. Furthermore, kinetically active secondary β/γ/δ-relaxation at reconfigurable interfaces can conquer limited self-healing ability fixed-orientation polymeric chains. obtained artificial muscle exhibits high output actuation, properties (tensile strength 33.5 MPa), desired functional, efficiency (89.7%), exceeding typical natural living systems. bionic micro-nano achieves bottom-up cooperative relaxation integrate all-round performance which paves way substantial advancements next-generation intelligent robotics.
Language: Английский
Citations
14
Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(23), P. 16112 - 16118
Published: May 28, 2024
Thermosets, characterized by their permanent cross-linked networks, present significant challenges in recyclability and brittleness. In this work, we explore a polarized Knoevenagel C═C metathesis reaction for the development of rigid yet tough malleable thermosets. Initial investigation on small molecule model reactions reveals feasibility conducting base-catalyzed solvent-free environment. Subsequently, thermosetting poly(α-cyanocinnamate)s (PCCs) were synthesized via condensation between triarm cyanoacetate star dialdehyde. The thermal mechanical properties developed PCCs can be easily modulated altering structure Remarkably, introduction ether groups into PCC leads to combination high rigidity toughness with Young's modulus ∼1590 MPa, an elongation at break ∼79%, reaching ∼30 MJ m3. These values are competitive traditional thermosets, but far exceed them ductility toughness. Moreover, facilitates stress relaxation within bulk polymer thus rendering excellent malleability reprocessability. This work overcomes limitations introducing groundbreaking insights design contributing significantly sustainability materials.
Language: Английский
Citations
11
Materials Today, Journal Year: 2025, Volume and Issue: unknown
Published: Jan. 1, 2025
Language: Английский
Citations
1
International Journal of Biological Macromolecules, Journal Year: 2025, Volume and Issue: 295, P. 139567 - 139567
Published: Jan. 6, 2025
Language: Английский
Citations
1
Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: unknown
Published: June 3, 2024
Covalent adaptable networks (CANs), leveraging the dynamic exchange of covalent bonds, emerge as a promising material to address challenge irreversible cross-linking in thermosetting polymers. In this work, we explore introduction catalyst-free and associative C=C/C=N metathesis reaction into polyurethanes, creating CANs with superior stability, solvent resistance, thermal/mechanical properties. By incorporating reaction, stress-relaxation is significantly accelerated compared imine-bond-only networks, rate adjustable by modifying substituents ortho position double bonds. The obtained plasticity enables recycle without altering chemical structure or mechanical properties, also found be vital for achieving shape memory functions complex spatial structures. This new crosslinker polymer has potential accelerate ongoing exploration malleable functional thermoset
Language: Английский
Citations
7
Small, Journal Year: 2024, Volume and Issue: unknown
Published: Oct. 11, 2024
Abstract Reversible and recyclable thermosets have garnered increasing attention for their smart functionality sustainability. However, they still face challenges in balancing comprehensive performance dynamic features. Herein, silicon (Si)─oxygen (O) imidazole units covalent bonds are coupled to generate a new class of bio‐polyimines (Bio‐Si‐PABZs), endow them with high excellent reprocessing capability acid‐degradability. By tailoring the molar content diamines, this Bio‐Si‐PABZs displayed both markedly glass transition temperature (162 °C) char yield at 800 °C an oxygen atmosphere (73.1%). These favorable properties outperformed various previously reported polyimines competed effectively commercial fossil‐based polycarbonate. Moreover, scratch (≈10 µ m) on surface samples can be self‐healing within only 2 min, effective “ Bird Nest ”‐to‐“ Torch ” recycling also achieved through free amines solution. Most importantly, bio‐based siloxane adhesive derived from intermediate Bio‐Si‐PABZ‐1 by acidic degradation demonstrated broad robust adhesion substrates, values reaching up ≈3.5 MPa. For first time, study lays scientific groundwork designing polyimine Si─O units, as well converting plastic wastes into thermal‐reversibility renewable adhesives.
Language: Английский
Citations
6
Advanced Materials, Journal Year: 2024, Volume and Issue: 36(21)
Published: April 5, 2024
Abstract Dynamically crosslinked polymers (DCPs) have gained significant attention owing to their applications in fabricating (re)processable, recyclable, and self‐healable thermosets, which hold great promise addressing ecological issues, such as plastic pollution resource scarcity. However, the current research predominantly focuses on redefining and/or manipulating geometries while replicating bulk properties. Given inherent design flexibility of dynamic covalent networks, DCPs also exhibit a remarkable potential for various novel through postsynthesis reprogramming In this review, recent advancements strategies that enable transform properties after synthesis are presented. The underlying mechanisms associated material overviewed mainly three distinct strategies, namely latent catalysts, material‐growth, topology isomerizable networks. Furthermore, mutual relationship impact these when integrated within one system discussed. Finally, application prospects relevant issues necessitating further investigation, along with solutions analyzed.
Language: Английский
Citations
6
Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(26), P. 18074 - 18082
Published: June 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 (
Language: Английский
Citations
5