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RESEARCH PAPER · Macromolecules · 2021

Arresting Elevated-Temperature Creep and Achieving Full Cross-Link Density Recovery in Reprocessable Polymer Networks and Network Composites via Nitroxide-Mediated Dynamic Chemistry

Lingqiao Li, Xi Chen, Kailong Jin, Mohammed A. Bin Rusayyis, John M. Torkelson

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Arresting Elevated-Temperature Creep and Achieving Full Cross-Link Density Recovery in Reprocessable Polymer Networks and Network Composites via Nitroxide-Mediated Dynamic ChemistryOriginalReprocessable covalent adaptable networks with excellent elevated-temperature creep resistance: facilitation by dynamic, dissociative bis(hindered amino) disulfide bonds110Covalent Adaptable Networks Using β-Amino Esters as Thermally Reversible Building Blocks162Vitrimers: Current research trends and their emerging applications480Reprocessing of Covalent Adaptable Polyamide Networks through Internal Catalysis and Ring-Size Effects106Improving creep resistance while maintaining reversibility of covalent adaptive networks via constructing reversibly interlocked polymer networks42A dynamic polyurea network with exceptional creep resistance36Biobased catalyst-free covalent adaptable networks based on CF 3 -activated synergistic aza-Michael exchange and transesterification36Characterising different molecular landscapes in dynamic covalent networks56Closed-loop chemical recycling of thermosetting polymers and their applications: a review276Dynamic covalent exchange induced cyclization in poly(methacrylic anhydride)8Self-healable fiber-reinforced vitrimer composites: overview and future prospects90Simple upcycling of virgin and waste polyethylene into covalent adaptable networks: catalyst-free, radical-based reactive processing with dialkylamino disulfide bonds87Thermally Degradable Poly(n-butyl acrylate) Model Networks Prepared by PhotoATRP and Radical Trap-Assisted Atom Transfer Radical Coupling2Reprocessable and Recyclable Chain-Growth Polymer Networks Based on Dynamic Hindered Urea Bonds76Hydrolytically Stable and Thermo-Mechanically Tunable Poly(Urethane) Thermoset Networks that Selectively Degrade and Generate Reusable Molecules8A highly stable covalent adaptable network through π-π conjugated confinement effect8Creep Mechanics of Epoxy Vitrimer Materials84Reprocessable polyhydroxyurethane networks reinforced with reactive polyhedral oligomeric silsesquioxanes (POSS) and exhibiting excellent elevated temperature creep resistance46Reprocessable Covalent Elastomeric Networks from Functionalized 1,4-cis-Polyisoprene and -Polybutadiene23Covalent Adaptable Networks Based on Dynamic Alkoxyamine Bonds24Healable ablative composites from synergistically crosslinked phenolic resin59A sustainable strategy for reprocessable elastomer based on ground tire rubber4Fabrication of DTC-g-PE-DA@GO@PU chelator for extraction of heavy metals from e-waste0Aero Grade Epoxy Vitrimer towards Commercialization52Recyclability of Vitrimer Materials: Impact of Catalyst and Processing Conditions78Vitrimer Composites: Understanding the Role of Filler in Vitrimer Applicability74Recyclable Sulfur-Cured Rubbers with Enhanced Creep Resistance and Retained Mechanical Properties by Terminal Metal Coordination9A Highly Dynamic Covalent Polymer Network without Creep: Mission Impossible?183A Highly Dynamic Covalent Polymer Network without Creep: Mission Impossible?6Equilibration dynamics of a dynamic covalent network diluted in a metallosupramolecular polymer matrix5Boronic ester-based vitrimeric methylvinyl silicone elastomer with “solid-liquid” feature and rate-dependent mechanical performance34Combining multiple hydrogen bonds and boronic ester chemistry towards mechanically robust and creep resisting elastomer vitrimer43Carbon material/vitrimer composites: Towards sustainable, functional, and high-performance crosslinked polymeric materials43Fabrication of DTC-g-PE-DA@GO@PU Chelator for Extraction of Precious and Toxic Metals from E-Waste4Biobased, Reprocessable, Self-Blown Non-Isocyanate Polyurethane Foams: Influence of Blowing Agent Structure and Functionality39Circularity in polymers: addressing performance and sustainability challenges using dynamic covalent chemistries112Novel covalent adaptable networks (CANs) of ethylene/1-octene copolymers (EOCs) made by free-radical processing: comparison of structure–property relationships of EOC CANs with EOC thermosets27Reprocessable, creep-resistant covalent adaptable networks synthesized using conventional free-radical polymerization conditions with piperidine-based and non-piperidine-based dynamic dialkylamino disulfide chemistry31Catalytic Control of Crystallization in Dynamic Networks21Biobased Transesterification Vitrimers121Rapidly synthesized, self-blowing, non-isocyanate polyurethane network foams with reprocessing to bulk networks via hydroxyurethane dynamic chemistry55Dynamic covalent networks with tunable dynamicity by mixing acylsemicarbazides and thioacylsemicarbazides17Mechanical characterizations, recyclability of thermoplastics through melt grafting a dynamic covalent network onto polyethylene20Biobased, Reprocessable Non-isocyanate Polythiourethane Networks with Thionourethane and Disulfide Cross-Links: Comparison with Polyhydroxyurethane Network Analogues58On the Welding of Vitrimers: Chemistry, Mechanics and Applications104Dynamic covalent exchange in methacrylic anhydride copolymers5Phosphonate‐influenced Diels‐Alder chemistry toward multi‐path recyclable, fire safe thermoset and its carbon fiber composites49One-step reactive processing of vitrimeric thermoplastic polyolefin elastomer with greatly improved thermo-mechanical property33Reprocessable, Bio-Based, Self-Blowing Non-Isocyanate Polyurethane Network Foams from Cashew Nutshell Liquid61Unexpected self-assembly of carbon dots during digital light processing 3D printing of vanillin Schiff-base resin15Multiscale experimental characterisation of mode-I interfacial fracture behaviour of vitrimer composites15Improving the Recyclability of an Epoxy Resin through the Addition of New Biobased Vitrimer11Recent Progress on the 3D Printing of Dynamically Cross‐Linked Polymers37Polybenzoxazine-based covalent adaptable networks: A mini-review45A weak but inert hindered urethane bond for high-performance dynamic polyurethane polymers6Length effect of crosslinkers on the mechanical properties and dimensional stability of vitrimer elastomers with inhomogeneous networks18Covalent adaptable networks and thermosets of multi-block ethylene/1-octene copolymers made by free-radical processing: Effects of melt flow index and crystallinity on thermomechanical properties and reprocessability17Reprocessable Biobased Statistical and Block Copolymer Methacrylic-Based Vitrimers with a Shape Memory Effect24Biobased Vitrimeric Epoxy Networks41Critical effect of exchangeable units distribution on properties of vitrimers: Quantitatively controlling dynamics thus suppressing creep7Increasing the Cross-Link Density in a Dual Dissociative and Associative Polythiourethane Covalent Adaptable Network Improves Both Creep Resistance and Extrudability29Multi-network Systems Including Dynamic and Static Covalent Bonds “Coexistence between Thermoplasticity and Creep Resistance” 3 Ionic Bond・Dynamic Covalent Bond0Rheological and Mechanical Comparison of Di and Tri-Block Copolymer Vitrimers Using Dynamic Imine Exchange0State-of-the-art epoxy vitrimer nanocomposites with graphene, carbon nanotube and silica—fundamentals and applications (radiation shielding, sensing and corrosion resistance)9Multi-network systems in elastomers using dynamic bonds and static covalent bonds “Coexistence between thermoplasticity and heat resistance”12Covalent Adaptable Networks Made by Reactive Processing of Highly Entangled Polymer: Synthesis-Structure-Thermomechanical Property-Reprocessing Relationship in Covalent Adaptable Networks35Investigating Dynamic Changes in 3D‐Printed Covalent Adaptable Polymer Networks3Catalyst‐Free α‐Acetyl Cinnamate/Acetoacetate Exchange to Enable High Creep‐Resistant Vitrimers31Catalyst‐Free α‐Acetyl Cinnamate/Acetoacetate Exchange to Enable High Creep‐Resistant Vitrimers3Investigation on UV-curing Reprocessable Thermosets Bearing Hindered Urea Bonds and Their Composites with Modified Zinc Oxide Nanoparticles4Poly(epoxy-imine) vitrimers. Effect of the structure on the stress relaxation and creep resistance19Reprocessable Polymer Networks Containing Sulfur‐Based, Percolated Dynamic Covalent Cross‐Links and Percolated or Non‐Percolated, Static Cross‐Links8Reprocessable Covalent Adaptable Networks via Free-Radical Polymerization with an Aromatic Disulfide Cross-Linker32Reprocessable, Self-Healing, and Creep-Resistant Covalent Adaptable Network Made from Chain-Growth Monomers with Dynamic Covalent Thionourethane and Disulfide Cross-Links22Rheological and mechanical comparison of di-and tri-block copolymer imine vitrimers18Recent Advances in Vitrimers: A Detailed Study on the Synthesis, Properties and Applications of Bio-Vitrimers24Large‐scale Conformational Changes of Diindole Functional Groups Driven by Cation‐π Interactions and the Toughening Mechanism of Thermosets23D Printing of Strong and Room-Temperature Reprocessable Silicone Vitrimers12Enabling the Reprocessability and Debonding of Epoxy Thermosets Using Dynamic Poly(β‐Amino Amide) Curing Agents27Exploring transamidation and chemical recycling of β-amino amide-derived covalent adaptable networks8Molecular Dynamics Simulation and Theoretical Analysis of Structural Relaxation, Bond Exchange Dynamics, and Glass Transition in Vitrimers32Polypropylene Covalent Adaptable Networks with Full Cross-Link Density Recovery after Reprocessing: Development by Free-Radical Reactive Processing with Resonance-Stabilized, Aromatic Disulfide Cross-Linkers25Reprocessable Polypropylene Covalent Adaptable Networks via Free-Radical Reactive Processing with Vinyl Aromatic Additives15Catalyst-Free Polyhydroxyurethane Covalent Adaptable Networks Exhibiting Full Cross-Link Density Recovery after Reprocessing: Facilitation by Synthesis with Well-Designed Secondary Amines9Covalent Adaptable Networks with Associative Siloxane Exchange Enabled by Amide‐Based Internal Catalysis: Designing for Reprocessability and Extrudability by Increasing the Cross‐Link Density20Dynamic crosslinked elastomers and rubbers25Reprocessable and Highly Creep-Resistant Covalent Adaptable Networks Incorporating Azine Dynamic Cross-Links via Free-Radical Polymerization10Understanding Non-isothermal Crystallization Behaviors of Polyethylene-Derived Vitrimers11Recyclable Ethylene-Vinyl Acetate Covalent Adaptable Networks and Their Structure–Property Relationships13Propylene–Ethylene Copolymer Covalent Adaptable Networks Synthesized by Resonance‐Stabilized, Radical‐Based Reactive Processing with Excellent Elevated‐Temperature Creep Resistance6From β-Dicarbonyl Chemistry to Dynamic Polymers15Reprocessing and degradation capability of biobased epoxy vitrimer composites0A review on the formulation and performance of epoxidized vegetable oil-based vitrimer: stoichiometric calculations, curing agent functionalities and catalyst efficiency6Catalyst Influence on the Crystallization Behaviors and Mechanical Properties of Polyethylene Vitrimers10Creep-resistant, extrudable, and recyclable polyolefin covalent adaptable networks incorporating azine cross-links via reactive processing3Cross-Linker Selection Controls Glass Transition Elevation or Reduction in Dynamic Covalently Bonded Polymer Networks7Covalent Adaptable Networks: Reprocessable Cross-Linked Polymers63Vitrimer-enabled circularity through upcycling mixed polyolefin waste from milk packets into valuable 3D printing feedstock5A tutorial review on designing pluripotent olefinic hybrids via covalent adaptable networks: integrating dynamic chemistry with machine‑learning0Restricting chain mobility in semicrystalline polyethylene and polypropylene via dynamic covalent cross-links: Major effects on elevated-temperature creep, heat distortion temperature, and wear resistance2Chain entanglements enable regeneration of high-performance thermosets3A Dual-Crosslinked Metallo-elastomer Platform for Architecture-Directed Vascular Remodeling0Dynamic covalent strategies and structure–property relationships of reprocessable Polybenzoxazines0Well tunable iminoboronate chemistry for precise activation energy modulation in vitrimers0Large-Strain Viscoelasticity of Partial Vitrimer Silicone Rubber Networks with Stress-Assisted Bond Exchange and Topological Constraints0

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  14. Reprocessable and Recyclable Chain-Growth Polymer Networks Based on Dynamic Hindered Urea Bonds

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  50. Unexpected self-assembly of carbon dots during digital light processing 3D printing of vanillin Schiff-base resin

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