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3D printing of unique structures with tunable properties offers significant advantages in the fabrication of complex and customized electronic devices. This study introduces a process-microstructure–property-guided manufacturing route to fabricate PVDF-2D MoS2 piezoelectric nanocomposites with tunable piezoelectric properties without having a postprocess. We control PVDF's microstructure through direct ink writing (DIW) 3D printing while tuning PVDF-MoS2 interfacial strain by controlling rheology and 3D printing parameters, such as nozzle size and printing speed. Our approach demonstrates tunable piezoelectricity in PVDF-MoS2, achieving a 15-fold increase in the piezoelectric coefficient (d33) at a printing-induced shear stress of 6685 Pa. This enhancement arises from the electrostatic interactions between PVDF and MoS2 and the filler distribution and alignment caused by the in situ shear stress in 3D printing, as confirmed by XPS and Raman mapping analyses. Our findings advance the understanding of piezoelectric mechanisms in PVDF-based nanocomposites, laying the foundation for 3D printing of piezoelectric sensors in wearable device applications with enhanced performance and customization capabilities. [ABSTRACT FROM AUTHOR]

Supramolecular adhesives are attracting considerable attentions owing to their dynamic and reversible bonding, while the complex curing conditions and poor performance under extreme conditions severely restrict their applicability. Herein, a series of tetra‐crown ether‐terminated polyethylene glycol (TCE‐PEG) adhesives are presented in which plenty of supramolecular interactions, including Van der Waals, hydrogen bonding, π–π staking, metal coordination, and electrostatic ones, provide strong adhesion on multiple types of substrates. Highly relevant for practical applications, ultra‐strong adhesivity of TCE‐PEG can be achieved without requiring additional ultraviolet radiation, heat, or chemical treatment at ambient temperature. It also exhibits durable adhesive behavior, excellent underwater stability, and low‐temperature tolerance. Especially, by incorporating ionic polymer fragments of polyethyleneimine hydrochloride, additional hydrogen bonding between secondary amines and crown ether rings can be induced to enhance the lap‐shear strength to 7.21 MPa due to the formation of supramolecular cross‐linked network. This work pioneers a rather unique supramolecular approach for easily formed, ultra‐strong crown‐ether‐based adhesives bearing great potential for applications in critical environments of limited heat source and unallowed solvent usage. [ABSTRACT FROM AUTHOR]

Cross-linked polymers with covalent adaptable networks (CANs) can be reprocessed under external stimuli owing to the exchangeability of dynamic covalent bonds. Optimization of reprocessing conditions is critical since increasing the reprocessing temperature costs more energy and even deteriorates the materials, while reducing the reprocessing temperature via molecular design usually narrows the service temperature range. Exploiting CO2 gas as an external trigger for lowering the reprocessing barrier shows great promise in low sample contamination and environmental friendliness. Herein, we develop a type of CANs incorporated with ionic clusters that achieve CO2-facilitated recyclability without sacrificing performance. The presence of CO2 can facilitate the rearrangement of ionic clusters, thus promoting the exchange of dynamic bonds. The effective stress relaxation and network rearrangement enable the system with rapid recycling under CO2 while retaining excellent mechanical performance in working conditions. This work opens avenues to design recyclable polymer materials with tunable dynamics and responsive recyclability. Cross-linked polymers with covalent adaptable networks are reprocessed under external stimuli at high temperatures which might deteriorate their performance. Here, the authors introduce carbon dioxide responsive ionic clusters into covalent adaptable polymer networks to facilitate the exchange of dynamic bonds providing materials with a rapid recycling and good mechanical performance. [ABSTRACT FROM AUTHOR]

Additively manufactured flexible and high‐performance piezoelectric devices are highly desirable for sensing and energy harvesting of 3D conformal structures. Herein, the study reports a significantly enhanced piezoelectricity in polyvinylidene fluoride (PVDF) achieved through the in situ dipole alignment of PVDF within PVDF‐2D molybdenum disulfide (2D MoS2) composite by 3D printing. The shear stress‐induced dipole poling of PVDF and 2D MoS2 alignment are harnessed during 3D printing to boost piezoelectricity without requiring a post‐poling process. The results show a remarkable, more than the eight‐fold increment in the piezoelectric coefficient (d33) for 3D printed PVDF‐8wt.% MoS2 composite over cast neat PVDF. The underlying mechanism of piezoelectric property enhancement is attributed to the increased volume fraction of β phase in PVDF, filler fraction, heterogeneous strain distribution around PVDF‐MoS2 interfaces, and strain transfer to the nanofillers as confirmed by microstructural analysis and finite element simulation. These results provide a promising route to design and fabricate high‐performance 3D piezoelectric devices via 3D printing for next‐generation sensors and mechanical–electronic conformal devices. [ABSTRACT FROM AUTHOR]

Despite intensive research on sustainable elastomers, achieving elastic vitrimers with significantly improved mechanical properties and recyclability remains a scientific challenge. Herein, inspired by the classical elasticity theory, we present a design principle for ultra-tough and highly recyclable elastic vitrimers with a defined network constructed by chemically crosslinking the pre-synthesized disulfide-containing polydimethylsiloxane (PDMS) chains with tetra-arm polyethylene glycol (PEG). The defined network is achieved by the reduced dangling short chains and the relatively uniform molecular weight of network strands. Such elastic vitrimers with the defined network, i.e., PDMS-disulfide-D, exhibit significantly improved mechanical performance than random analogous, previously reported PDMS vitrimers, and even commercial silicone-based thermosets. Moreover, unlike the vitrimers with random network that show obvious loss in mechanical properties after recycling, those with the defined network enable excellent thermal recyclability. The PDMS-disulfide-D also deliver comparable electrochemical signals if utilized as substrates for electromyography sensors after the recycling. The multiple relaxation processes are revealed via a unique physical approach. Multiple techniques are also applied to unravel the microscopic mechanism of the excellent mechanical performance and recyclability of such defined network., (© 2023 Wiley-VCH GmbH.)