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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.

Natural plant fiber-reinforced polymer composites (PFRP) have emerged as an environmental-friendly material in the construction industry, but their creep behavior is a critical concern for load-bearing structures. This study investigates the creep behavior of flax fiber-reinforced polymer composites (FFRP) using the time-temperature superposition principle (TTSP). Due to the application of TTSP on the tensile creep behavior of FFRP is not fully understood, three potential methods for calculating the critical parameters during TTSP are compared to obtain an efficient application method to build the creep master curve. A 2,000-h long-term creep test is conducted parallelly on the same sample to validate the accuracy of the creep analysis results. The study proposes an ideal method to determine the key parameters in TTSP, providing valuable insights for the practical application of PFRP in the construction industry. Meanwhile, the research results in this study would be helpful in better understanding the creep behavior of FFRP via short-term accelerated tests.

Charge transfer complexes (CTCs) based on self-assembled donor and acceptor molecules allow light absorption of significantly redshifted wavelengths to either the donor or acceptor. In this work, we demonstrate a CTC embedded in a hydrogen-bonded liquid crystal elastomer (LCE), which in itself is fully reformable and reprocessable. The LCE host acts as a gate, directing the self-assembly of the CTC. When hydrogen bonding is present, the CTC behaves as a near-infrared (NIR) dye allowing photothermal actuation of the LCE. The CTC can be disassembled in specific regions of the LCE film by disrupting the hydrogen bond interactions, allowing selective NIR heating and localized actuation of the films. The metastable non-CTC state may persist for weeks or can be recovered on demand by heat treatment. Besides the CTC variability, the capability of completely reforming the shape, color, and actuation mode of the LCE provides an interactive material with unprecedented application versatility.

Flax fiber-reinforced polymer (FFRP) composites are emerging popular environmental-friendly construction materials. However, their significant creep properties have been a major concern for using FFRP in load-bearing structures. This article presents an investigation of the effect of environmental humidity on the creep behavior of the FFRP. Samples with flax fiber in 0°, 90°, and ± 45° were manufactured, respectively, by the vacuum infusion method. Accelerated creep tests were conducted on samples in different relative humidities (RH), and the results were analyzed by the time–temperature superposition principle (TTSP). It is found the creep development of samples with 0° and 90° fiber increases with the RH, and their 30-year total strain in 97% RH is about 10 times higher than that in 11% RH. The samples with ±45° fiber are found not obviously sensitive to the humidity change. The scanning electron microscope (SEM) check indicates the change in the fiber–matrix interface and cracks between microfibrils in a fiber bundle is the main reason for the change of creep behavior in high humidity. This study may benefit the design of structures made of natural fiber-reinforced polymer composites, especially for load-bearing structures working in high-humidity environments.

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.

The application of reprocessable and reprogrammable soft actuators is limited by the synthetic strategies, 3D-shaping capabilities, and small deformations. In this work, melt-processable supramolecular soft actuators based on segmented copolymers containing thiourethane and liquid crystal segments have been prepared via sequential thiol addition reactions in a one-pot approach using commercially available building blocks. The actuators demonstrated immediate, reversible response and weightlifting capabilities with large deformations up to 32%. Through exploiting the supramolecular cross-links, the material could be recycled and reprogrammed into 3D actuators and welded into an actuator assembly with different deformation modes. Our work offers a one-pot synthesis and straightforward melt-processable approach to prepare supramolecular soft actuators with large deformations that can be reprocessed and reprogrammed into arbitrary 3D shapes.

Soft polymer actuators have myriad applications and have therefore gained considerable attention in recent years. However, it remains challenging to prepare soft actuators with predefined shapes. Here, a bilayer polymer actuator with a (re)programmable shape is prepared from a microporous anisotropic polypropylene scaffold and a thin, pH-responsive liquid crystalline network (LCN) layer. The hydrogen bonds between dimerized benzoic acid derivatives in the LCN can be disrupted by an alkaline treatment, resulting in a pH-responsive LCN hydrogel layer. The pH-responsive actuation is governed by both the anisotropic mechanical properties of the scaffold and the cross-link density of the LCN hydrogel. Ca2+ ions can be used to chemically cross-link the actuator resulting in an initial programmed shape. The shape fixing can be reversed by removing the Ca2+ ions with an ethylenediaminetetraacetic acid (EDTA) solution. The shape fixing can be performed locally, resulting in pH-responsive actuators with three-dimensional initial configurations of choice., Soft polymer actuators have myriad applications and have therefore gained considerable attention in recent years. However, it remains challenging to prepare soft actuators with predefined shapes. Here, a bilayer polymer actuator with a (re)programmable shape is prepared from a microporous anisotropic polypropylene scaffold and a thin, pH-responsive liquid crystalline network (LCN) layer. The hydrogen bonds between dimerized benzoic acid derivatives in the LCN can be disrupted by an alkaline treatment, resulting in a pH-responsive LCN hydrogel layer. The pH-responsive actuation is governed by both the anisotropic mechanical properties of the scaffold and the cross-link density of the LCN hydrogel. Ca2+ ions can be used to chemically cross-link the actuator resulting in an initial programmed shape. The shape fixing can be reversed by removing the Ca2+ ions with an ethylenediaminetetraacetic acid (EDTA) solution. The shape fixing can be performed locally, resulting in pH-responsive actuators with three-dimensional initial configurations of choice.

Hydrogen-bonded liquid crystalline polymers have emerged as promising “smart” supramolecular functional materials with stimuli-responsive, self-healing, and recyclable properties. The hydrogen bonds can either be used as chemically responsive (i.e., pH-responsive) or as dynamic structural (i.e., temperature-responsive) moieties. Responsiveness can be manifested as changes in shape, color, or porosity and as selective binding. The liquid crystalline self-organization gives the materials their unique responsive nanostructures. Typically, the materials used for actuators or optical materials are constructed using linear calamitic (rod-shaped) hydrogen-bonded complexes, while nanoporous materials are constructed from either calamitic or discotic (disk-shaped) complexes. The dynamic structural character of the hydrogen bond moieties can be used to construct self-healing and recyclable supramolecular materials. In this review, recent findings are summarized, and potential future applications are discussed.

Direct ink writing (DIW) of liquid crystal elastomers (LCEs) has rapidly paved its way into the field of soft actuators and other stimuli-responsive devices. However, currently used LCE systems for DIW require postprinting (photo)polymerization, thereby forming a covalent network, making the process time-consuming and the material nonrecyclable. In this work, a DIW approach is developed for printing a supramolecular poly(thio)urethane LCE to overcome these drawbacks of permanent cross-linking. The thermo-reversible nature of the supramolecular cross-links enables the interplay between melt-processable behavior required for extrusion and formation of the network to fix the alignment. After printing, the actuators demonstrated a reversible contraction of 12.7% or bending and curling motions when printed on a passive substrate. The thermoplastic ink enables recyclability, as shown by cutting and printing the actuators five times. However, the actuation performance diminishes. This work highlights the potential of supramolecular LCE inks for DIW soft circular actuators and other devices.

Soft actuators allowing multifunctional, multishape deformations based on single polymer films or bilayers remain challenging to produce. In this contribution, direct ink writing is used for generating patterned actuators, which are in between single- and bilayer films, with multifunctionality and a plurality of possible shape changes in a single object. The key is to use the controlled deposition of a light-responsive liquid crystal ink with direct ink writing to partially cover a foil at strategic locations. We found patterned films with 40% coverage of the passive substrate by an active material outperformed “standard” fully covered bilayers. By patterning the film as two stripes, a range of motions, including left- and right-handed twisting and bending in orthogonal directions, could be controllably induced in the same actuator. The partial coverage also left space for applying liquid crystal inks with other functionalities, exemplified by fabricating a light-responsive green reflective actuator whose reflection can be switched “on” and “off”. The results presented here serve as a toolbox for the design and fabrication of patterned actuators with dramatically expanded shape deformation and functionality capabilities.