Ben-Lin Hu

The adaptation of capacitors to wearable electronics requires dielectric materials that combine high permittivity with well resilience. Fully organic stretchable capacitive strain sensors are particularly attractive, but their performance is often limited by the lack of suitable elastic high‐k dielectrics. Relaxor ferroelectric polymers offer intrinsically high dielectric constants; however, conventional elastification approaches, such as thermal and photo‐crosslinking, are constrained by harsh processing conditions and residual chemical species. Here, we present a simple and effective radiation‐crosslinking strategy to convert a relaxor ferroelectric polymer into an elastic dielectric without the need for initiators or elevated temperatures. By employing poly(vinylidene fluoride–trifluoroethylene–chlorofluoroethylene) (P(VDF‐TrFE‐CFE)) in combination with poly(ethylene glycol) diacrylate (PEGDA) as a crosslinking sensitizer, a stable crosslinked network is formed under mild irradiation conditions. The resulting material exhibits a high dielectric constant (∼37 at 25°C and 1 kHz) together with excellent elastic recovery (∼80%), thereby achieving a desirable balance between dielectric performance and resilience. When integrated with stretchable electrodes, the resulting fully organic capacitive device exhibits reproducible capacitance variation to tensile strain, demonstrating its potential for fully organic stretchable capacitive strain sensing. This work establishes a practical strategy for developing high‐permittivity dielectric elastomers and advances the design of stretchable electronic devices.

Polyethylene‐like polyesters, which incorporate chemically cleavable ester linkages into long methylene sequences while retaining characteristic polyethylene‐like chain packing and semicrystalline mechanical behavior, are promising alternatives to persistent polyethylene because they combine comparable mechanical performance with the potential for chemical recycling and biodegradation. However, the ordered crystalline structures required for mechanical performance often sequester ester bonds within crystalline domains, creating an accessibility barrier that hinders chemical recycling and biodegradation. Herein, we decouple this trade‐off through a crystallization modulation strategy by incorporating sterically hindered asymmetric pyrrolidone units into the polyester backbone. This molecular engineering approach relocates cleavable ester bonds from crystalline to amorphous domains while preserving semi‐crystalline reinforcement, confirmed by x‐ray structural analysis. The polymers exhibit tunable mechanical robustness, with tensile strength exceeding 18.7 MPa and lap‐shear adhesion up to 15.3 MPa. They undergo complete depolymerization to easily separable soluble oligomers via methanolysis under ambient pressure, even within mixed‐plastic streams, enabling closed‐loop recycling. Furthermore, the amorphous enrichment of polar units accelerates biodegradation, achieving a mineralization rate 2.3 times that of conventional analogues. This work demonstrates a viable molecular design pathway to reconcile mechanical robustness, mild chemical recyclability, and enhanced environmental degradability in polyethylene‐like materials, offering a route to mitigate long‐term plastic persistence.

Organic ferroelectrics offer solution processability, mechanical flexibility and promising applications in sensing, energy storage and actuation. However, their polarization and Curie temperatures are typically lower than those of inorganic ferroelectrics because weak intermolecular interactions hinder efficient dipole alignment. The development of organic materials that integrate dipole units, long-range dipole ordering and switchable polarization may enable the design of high-performance organic ferroelectrics. Here we report a donor-acceptor cocrystal in which V-shaped donor molecules pack into a gear-like arrangement, enabled by supramolecular interactions. Within this binary confined lattice, a cooperative in-plane rotation of 42° by the donor molecules-triggered by an external electric field-enables reversible polarization switching. This rotational mechanism yields a remanent polarization of 58 μC cm^-2, stable ferroelectricity up to 479 K and a low coercive field of 0.022 MV m^-1, exhibiting superior performance compared with previously reported organic ferroelectrics. These findings provide a pathway towards the design of high-performance organic ferroelectrics.

Piezoelectric elastomers, combining flexibility, resilience, and piezoelectric properties, are promising for wearable devices. Blending ceramic fillers into elastomers is common for fabricating piezoelectric elastomers, but electrical and mechanical mismatches hinder synergistic fusion for a high piezoelectric output. Here, we develop a high-performance piezoelectric elastomer by co-dissolving and evaporating an aqueous solution of a molecular ferroelectric material TMCM-CdCl₃ (TMCM, trimethylchloromethylammonium) and a waterborne polyurethane elastomer. Slightly increasing the TMCM-Cl proportion modulates piezoelectric properties, while adjusting the TMCM-CdCl₃/WPU ratio achieves an optimal balance between piezoelectricity and elasticity. The resulting material exhibits low elastic modulus, large elongation, high elastic recovery, and superior piezoelectric coefficient d₃₃ (42 pC/N) and piezoelectric voltage coefficient (543 × 10^-3 Vm/N) compared to PVDF, enabling a remarkable voltage output up to 7 V. This piezoelectric elastomer not only exhibits outstanding resilience but also excellent electrical output performance, making it a highly suitable energy material for flexible wearable devices.

Elastic ferroelectrics, distinguished by their softness, stretchability, and ferroelectric and piezoelectric responses, are promising candidates in next‐generation wearable electronics. Currently, the intrinsic elastification of ferroelectric polymers has been achieved through a “slight crosslinking” strategy, which relies on costly poly(vinylidene fluoride) (PVDF)‐based copolymers with low Curie temperatures, thereby limiting their operation at high temperatures. In contrast, PVDF homopolymers are low‐cost and possess an inherently high Curie temperature, while their high modulus has long hindered elasticity. Here, we overcome these limitations by introducing highly reactive, soft long‐chain crosslinkers into PVDF homopolymers, enabling simultaneous low cost, high thermal stability, and intrinsic elasticity. By tuning the crosslinking density, intrinsically elastic ferroelectrics based on PVDF homopolymer were obtained with over 80% elastic recovery under 60% strain. Remarkably, the materials retain a high remanent polarization ( P _r ) of 7.00 µC/cm ² at 110°C. The materials maintain stable ferroelectric responses even under strains up to 70%. This study resolves the long‐standing challenge of elastifying high‐modulus PVDF homopolymers and develops a low‐cost, thermally robust, intrinsically elastic ferroelectric. These advances outline a promising pathway toward next‐generation wearable electronics that demand both high elasticity and high‐temperature operation.

Elastic ferroelectrics, distinguished by their softness, stretchability, and ferroelectric and piezoelectric responses, are promising candidates in next‐generation wearable electronics. Currently, the intrinsic elastification of ferroelectric polymers has been achieved through a “slight crosslinking” strategy, which relies on costly poly(vinylidene fluoride) (PVDF)‐based copolymers with low Curie temperatures, thereby limiting their operation at high temperatures. In contrast, PVDF homopolymers are low‐cost and possess an inherently high Curie temperature, while their high modulus has long hindered elasticity. Here, we overcome these limitations by introducing highly reactive, soft long‐chain crosslinkers into PVDF homopolymers, enabling simultaneous low cost, high thermal stability, and intrinsic elasticity. By tuning the crosslinking density, intrinsically elastic ferroelectrics based on PVDF homopolymer were obtained with over 80% elastic recovery under 60% strain. Remarkably, the materials retain a high remanent polarization ( P _r ) of 7.00 µC/cm ² at 110°C. The materials maintain stable ferroelectric responses even under strains up to 70%. This study resolves the long‐standing challenge of elastifying high‐modulus PVDF homopolymers and develops a low‐cost, thermally robust, intrinsically elastic ferroelectric. These advances outline a promising pathway toward next‐generation wearable electronics that demand both high elasticity and high‐temperature operation.

With the rapid advancement of wearable electronics, elastic ferroelectrics, which have been prepared by thermal and photochemical crosslinking, possess tremendous potential applications in wearable devices. However, challenges arose from these crosslinking reactions, such as high crosslinking temperature, long processing time, initiator residues, limited penetration depths. In contrast, radiation crosslinking, triggered by high‐energy particles at room temperature, yields materials with enhanced properties by offering advantages like the absence of active end‐groups and initiators, fast crosslinking speed, deep penetration, and environmental friendliness. In this study, the elastification of ferroelectric polymers, with normal ferroelectric poly(vinylidene fluoride‐co‐trifluoroethylene) (P(VDF‐TrFE)) as the matrix and a crosslinking sensitizer with unsaturated double bonds, was realized via electron beam radiation crosslinking. By adjusting the absorbed doses and the feed ratios of P(VDF‐TrFE) and the crosslinking sensitizer, the crystallinity of the elastic ferroelectrics was controlled, effectively balancing ferroelectricity and resilience. The resulting elastic ferroelectrics maintain stable ferroelectric response under tensile strains up to 55%, exhibiting excellent elasticity and ferroelectric properties. This study presents a simple but efficient approach for preparing intrinsically elastic ferroelectric without high‐temperature reaction, and eliminating the need for heating and cooling steps, providing a potential universal platform for constructing various elastic ferroelectrics.

This work presents an innovative strategy for demethoxylation-free valorization of lignin into bio-based epoxy resins with reduced dielectric constant.

Flexible composites-based piezoelectric nanogenerator (PENG) with low cost, stable properties and sensitivity to mechanical deformation is highly suitable to construct self-powered sensing layer for distributed electrical transmission power lines. However, the lower output performance of the PENG resulting from inadequate effective polarization, hinders its integration with energy management circuits and signal recognition systems. Herein, we propose a high-performance PENG by designing a new piezoelectric ceramic fiber, where BCZT@Ag nanoparticles are grown on the surface of BCZT fibers to form a branch-heterostructure, leading to enhanced charge transport mechanisms and induced polarization in the PENG. The branch-heterostructure ceramic fibers-based PENG exhibits significantly enhanced outputs of 96.4 V and 15.52 µA, which are about 3.2 and 6.5 times higher than those of PENG without specific design. Moreover, an intelligent Power Internet of Things (Power IoTs) system through the synergistic integration of this high-performance PENG and learning-assisted data analytics has been constructed, which enables accurate self-powered real-time monitoring of abnormal vibration states in transmission power lines to prevent rupture-related failures with approximately 96% identification accuracy. This work not only provides an effective strategy to enhance the performance of PENG, but also broadens the application prospects of lead-free piezoelectric ceramics in Power IoTs.

Elastomers are key components of structural and functional materials used in daily life and in the industry because of their resilience under large strains. However, resolving the biodegradability‐reprocessability‐elasticity trilemma remains a major challenge, highlighting the urgent need for effective design strategies in the synthesis of biodegradable thermoplastic elastomers. In this study, an “unchaining intrinsic entropic elasticity” strategy is proposed in the design and synthesis of poly(ethylene‐cyclohexanedimethylene succinate) (PECS) of variable repeat unit compositions. This copolyester has a single chain acting simultaneously as a reversible network and physical cross‐linking point, and can be readily synthesized via a simple one‐pot melt polycondensation using 1,4‐cyclohexanedimethanol, ethylene glycol, and succinic acid, which is applicable to both gram and kg scales. The mechanical properties of PECS copolyesters change from plastic to elastic deformation as the ethylene glycol content increases, along with a gradual disappearance of the yielding phenomenon, thus unchaining its intrinsic entropic elasticity. The elastic recovery of the copolyesters reaches up to ≈90% under a strain of 200%, which indicates outstanding fatigue performance. PECS copolyesters can be multiple melt‐reprocessable, and have excellent blood compatibility based on a hemolysis assay, along with outstanding biodegradability. This work has the potential to reduce nonbiodegradable elastomers that lead to plastic pollution.