Direct Ink Writing of Recyclable Supramolecular Soft Actuators

Lugger, Sean J. D.; Verbroekken, Ruth M C; Mulder, Dirk J.; Schenning, Albert P. H. J.

doi:10.1021/acsmacrolett.2c00359

Cited by 21 publications

(21 citation statements)

References 48 publications

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“…These chemistries, such as thiourea exchange, disulfide exchange, and transesterification reactions, can form stable networks, break under stimulus, and then reform to reinstate the integrity of the network . Recent works have demonstrated the advantages of dynamic and supramolecular bonds in LCEs to facilitate programmable shapes, − healable materials, − and additive manufacturing . The inclusion of hydrogen bonds as exchangeable bonds within liquid crystalline networks (LCNs) and some LCE systems has been studied previously .…”

Section: Introductionmentioning

confidence: 99%

“…29 Recent works have demonstrated the advantages of dynamic and supramolecular bonds in LCEs to facilitate programmable shapes, 33−35 healable materials, 36−38 and additive manufacturing. 39 The inclusion of hydrogen bonds as exchangeable bonds within liquid crystalline networks (LCNs) and some LCE systems has been studied previously. 40 These reports have emphasized chemical responsiveness and the dynamic response of hydrogen bonds to heat or light.…”

Section: ■ Introductionmentioning

confidence: 99%

“…The inclusion of hydrogen bonds as exchangeable bonds within liquid crystalline networks (LCNs) and some LCE systems has been studied previously . These reports have emphasized chemical responsiveness and the dynamic response of hydrogen bonds to heat or light. ,,,− …”

Section: Introductionmentioning

confidence: 99%

See 2 more Smart Citations

Programming Orientation in Liquid Crystalline Elastomers Prepared with Intra-Mesogenic Supramolecular Bonds

Lewis

Herbert

Matavulj

et al. 2023

ACS Appl. Mater. Interfaces

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The large, directional stimuli-response of aligned liquid crystalline elastomers (LCEs) could enable functional utility in robotics, medicine, consumer goods, and photonics. The alignment of LCEs has historically been realized via mechanical alignment of a two-stage reaction. Recent reports widely utilize chain extension reactions of liquid crystal monomers (LCM) to form LCEs that are subject to either surface-enforced or mechanical alignment. Here, we prepare LCEs that contain intra-mesogenic supramolecular bonds synthesized via direct free-radical chain transfer photopolymerization processible by a distinctive mechanical alignment mechanism. The LCEs were prepared by the polymerization of a benzoic acid monomer (11OBA), which dimerized to form a liquid crystal monomer, with a diacrylate LCM (C6M). The incorporation of the intra-mesogenic hydrogen bonds increases the achievable nematic order from mechanical programming. Accordingly, LCEs prepared with larger 11OBA concentration exhibit higher magnitude thermomechanical strain values when compared to a LCE containing only covalent bonds. These LCEs can be reprogrammed with heat to return the aligned film to the polydomain state. The LCE can then be subsequently programmed to orient in a different direction. The facile preparation of (re)programmable LCEs with supramolecular bonds opens new avenues for the implementation of these materials as shape deployable elements.

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Section: Introductionmentioning

confidence: 99%

Section: ■ Introductionmentioning

confidence: 99%

See 1 more Smart Citation

Programming Orientation in Liquid Crystalline Elastomers Prepared with Intra-Mesogenic Supramolecular Bonds

Lewis

Herbert

Matavulj

et al. 2023

ACS Appl. Mater. Interfaces

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“…Only recently, we exploited the DIW of a temperature-responsive supramolecular ink for the facile fabrication of more sustainable soft actuators. [41] In this work, we present a light-triggered, printable supramolecular ink based on a melt-processable polythiourethane (PTU) consisting of responsive LC and dynamic hydrogenbonding segments. This thermoplastic material combines the thermoreversible nature of the supramolecular cross-links with the light-responsivity of the incorporated azobenzene photoswitches.…”

Section: Introductionmentioning

confidence: 99%

“…Only recently, we exploited the DIW of a temperature‐responsive supramolecular ink for the facile fabrication of more sustainable soft actuators. [ 41 ]…”

Section: Introductionmentioning

confidence: 99%

4D Printing of Supramolecular Liquid Crystal Elastomer Actuators Fueled by Light

Lugger

Ceamanos

Mulder

et al. 2022

Adv Materials Technologies

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Recent years have seen major advances in the additive manufacturing of stimuli‐responsive materials, also known as “4D printing,” among which liquid crystal elastomers (LCEs) play an important role. However, during fabrication photo‐crosslinking of the LCEs is required, but this step is time‐consuming and efficient polymerization is challenging, especially in the case of light‐responsive materials. In this work, the first light‐fueled supramolecular LCEs suitable for the direct ink writing (DIW) of soft actuators are synthesized in which a photopolymerization step is not needed. With the responsive supramolecular material, 3D‐printed objects are fabricated by exploiting the thermoreversible interplay of the hydrogen‐bonding physical cross‐links. After printing, the supramolecular LCE shows reversible shape changes in response to light and is capable of bending and lifting a load. Through the combined photothermal and photochemical contributions of the incorporated azobenzene, the actuators can be triggered both in air and water. The freedom provided by DIW allows for the printing of complex responsive objects, as demonstrated by fabricating re‐entrant honeycomb and spiral director structures. This approach of printing light‐responsive supramolecular soft actuators opens avenues toward the application of “smart” and sustainable materials for additive manufacturing without the requirement of photo‐crosslinking.

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Melt‐Extruded Thermoplastic Liquid Crystal Elastomer Rotating Fiber Actuators

Lugger

Engels

Cardinaels

et al. 2023

Adv Funct Materials

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Untethered soft fiber actuators are advancing toward next‐generation artificial muscles, with rotating polymer fibers allowing controlled rotational deformations and contractions accompanied by torque and longitudinal forces. Current approaches, however, are based either on non‐recyclable and non‐reprogrammable thermosets, exhibit rotational deformations and torques with inadequate actuation performance, or involve intricate multistep processing and photopolymerization impeding scalable fabrication and manufacturing of millimeter‐thick fibers. Here, the melt‐extrusion and drawing of a 50 m long thermoplastic liquid crystal elastomer fiber with a ≈1.3 mm diameter on a large scale is reported. With the responsive thermoplastic material, rotating actuators are fabricated via easily exploited programming freedom resulting in large, reversible rotational deformations and torques. The actuation performance of the twisted fibers may be controlled by the programmed twisting density without complicated preparation steps or photocuring being required. The thermoplastic behavior enables fabrication of plied fibers, demonstrated as a triple helical twisted rope constructed from individual rotating fibers delivering up to three times as great rotational and longitudinal forces capable of reversibly opening and lifting a screw cap vial. Besides the programmability, the thermoplastic material employed lends itself to be completely reprocessed into other configurations with self‐healing properties in contrast to thermosets.

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Direct Ink Writing of Recyclable Supramolecular Soft Actuators

Cited by 21 publications

References 48 publications

Programming Orientation in Liquid Crystalline Elastomers Prepared with Intra-Mesogenic Supramolecular Bonds

Programming Orientation in Liquid Crystalline Elastomers Prepared with Intra-Mesogenic Supramolecular Bonds

4D Printing of Supramolecular Liquid Crystal Elastomer Actuators Fueled by Light

Melt‐Extruded Thermoplastic Liquid Crystal Elastomer Rotating Fiber Actuators

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