Thermoswitchable catalysis to inhibit and promote plastic flow in vitrimers

Van Lijsebetten, Filip; Maes, Stephan; Winne, Johan M.; Du Prez, Filip E.

doi:10.1039/d4sc00417e

Chem. Sci.

2024

DOI: 10.1039/d4sc00417e

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Thermoswitchable catalysis to inhibit and promote plastic flow in vitrimers

Filip Van Lijsebetten,

Stephan Maes,

Johan M. Winne

et al.

Abstract: Acid-base catalysis is a common strategy to induce covalent bond exchanges in dynamic polymer networks. Strong acids or strong bases can promote rapid network rearrangements, and are simultaneously preferred catalysts...

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Cited by 4 publications

References 74 publications

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Enabling the Reprocessability and Debonding of Epoxy Thermosets Using Dynamic Poly(β‐Amino Amide) Curing Agents

Nguyen,

Maes,

Du Prez

2024

Adv Funct Materials

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Epoxy resins, by showing outstanding performances, stand out as the most applied materials in thermoset products. However, their excellent properties, associated with covalently cross‐linked structures, come at the expense of recyclability, thus posing environmental and regulatory challenges. Herein, starting from the recently explored reversibility of robust poly(β‐amino amide)s, dynamic curing agents are synthesized in a one‐pot procedure for their use in the preparation of epoxy‐derived dynamic networks. The obtained materials retain desirable properties while being fully (re)processable, with high temperature‐dependent viscoelasticity (activation energy (Ea) of ≈230 to 270 kJ mol−1). Moreover, this new generation of epoxy materials shows excellent resistance to hydrolysis and creep at elevated temperatures (up to 120 °C). As an entry point to further applications, the reversible curing agents are implemented in adhesive formulations, showcasing lap shear strengths that are comparable to commercial hardeners (up to 9 MPa). The β‐amino amide groups provide the obtained adhesives with the additional functionality of heat‐triggered deconstruction at elevated temperatures (130 to 150 °C), and re‐bonding capacity with up to 80% recovery in lap‐shear strength. To encourage industrial adoption, a cost‐effective, drop‐in synthesis protocol is developed using only bulk chemicals, hence facilitating practical implementation.

show abstract

Enabling the Reprocessability and Debonding of Epoxy Thermosets Using Dynamic Poly(β‐Amino Amide) Curing Agents

Nguyen,

Maes,

Du Prez

2024

Adv Funct Materials

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Controlling the Relaxation Dynamics of Polymer Networks by Combining Associative and Dissociative Dynamic Covalent Bonds

Cornellà,

Furia,

Van Assche

et al. 2024

Advanced Materials

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Dynamic polymer networks offer a promising solution to key challenges in polymers such as recyclability, processability, and damage repair. However, the trade‐off between combining facile processability, fast self‐healing, and high creep resistance remains a major obstacle to implementation. To overcome this, two very distinct dynamic covalent chemistries, Diels–Alder and transesterification, is combined in a single network. The resulting dual dynamic networks offer an unprecedented set of properties and control over the relaxation times. The system decouples the relaxation dynamics of the network from the spatial motifs, and the tuning of the ratio between chemistries enables to control of the relaxation dynamics over six orders of magnitude. Taking advantage of this control, the composition and rheological behavior is optimized to drastically improve the resolution for extrusion‐based additive manufacturing of dynamic covalent networks. Additionally, two well‐defined and separated stress relaxation peaks are observed at compositions close to 50% of each dynamic chemistry, accentuating the double character of the system's relaxation dynamics. This atypical situation, enables to preparation of self‐healing materials with negligible creep, and with shape‐memory properties solely leveraging the two distinct relaxation dynamics, instead of the glass transition temperature or the melting point.

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Repairable 3D printable photopolymer resins based on low-activation-energy adaptable covalent bonding

Ye,

Janssen,

Schnelting

et al. 2024

Polymer

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Thermoswitchable catalysis to inhibit and promote plastic flow in vitrimers

Abstract: Acid-base catalysis is a common strategy to induce covalent bond exchanges in dynamic polymer networks. Strong acids or strong bases can promote rapid network rearrangements, and are simultaneously preferred catalysts...

Cited by 4 publications

References 74 publications

Enabling the Reprocessability and Debonding of Epoxy Thermosets Using Dynamic Poly(β‐Amino Amide) Curing Agents

Enabling the Reprocessability and Debonding of Epoxy Thermosets Using Dynamic Poly(β‐Amino Amide) Curing Agents

Controlling the Relaxation Dynamics of Polymer Networks by Combining Associative and Dissociative Dynamic Covalent Bonds

Repairable 3D printable photopolymer resins based on low-activation-energy adaptable covalent bonding

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