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Entanglement significantly enhances the mechanical performance and functionality of both natural and synthetic materials. However, developing straightforward, versatile strategies for creating high-performance entangled polymer materials remains a challenge. Here, a co-initiating-system dual-mechanism strategy is designed for fabricating printable entangled polymer multinetworks. This thermal-light dual-initiation process benefits the synthesis of high-molecular-weight polymers and promotes the rapid formation of multinetworks within hydrogels. The resulting long polymer chains enable hydrogels with higher mechanical performance, lower stress relaxation, and activation energy compared to short polymer chain-contained samples. Such a method proves more effective than traditional self-thickening and strengthening techniques for enhancing hydrogel entanglements and is also compatible with additive manufacturing, enabling the design of complex 2D webs with adaptive mechanical performance and capable of detecting and sensing applications. This work provides an effective strategy for designing high-performance entangled polymer materials, which are set to impact numerous fields, from advanced sensing to material science and beyond.
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http://dx.doi.org/10.1038/s41467-025-59669-3 | DOI Listing |
Adv Mater
September 2025
School of Chemistry and Biochemistry, School of Materials Science and Engineering, Center for Organic Photonics and Electronics, Georgia Institute of Technology, Atlanta, GA, 30332, USA.
Molecular spin systems that can be chemically tuned, coherently controlled, and readily integrated within devices remain central to the realization of emerging quantum technologies. Organic high-spin materials are prime candidates owing to their similarity in electronic structure to leading solid-state defect-based systems, light element composition, and the potential for entanglement and qubit operations mediated through spin-spin exchange. However, the inherent instability of these species precludes their rational design, development, and application.
View Article and Find Full Text PDFACS Appl Mater Interfaces
September 2025
School of Integrative Engineering, Chung-Ang University, 84 Heukseok-ro, Dongjak-gu, Seoul 06974, Republic of Korea.
This paper presents a strategy for noise suppression and stability enhancement of organic photodetectors (OPDs) by introducing pH-neutralized and transfer-laminated poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) as the hole-transporting layer (HTL). Although PEDOT:PSS is widely used as an HTL material, its intrinsic acidity and structural instability hinder the performance of the OPD. Here, imidazole-induced neutralization promotes a linear entangled structure, while transfer lamination enables controlled PSS domain distribution.
View Article and Find Full Text PDFJ Colloid Interface Sci
August 2025
State Key Lab of Metal Matrix Composites, School of Materials Science and Engineering and Zhangjiang Institute for Advanced Study, Shanghai Jiao Tong University, 200240 Shanghai, China; School of Physical Science and Technology, ShanghaiTech University, Shanghai 200031, China. Electronic address: hu
Physical hydrogels, hydrophilic polymer networks with reversible crosslinks, have drawn attention in cutting-edge applications due to high tunability and biocompatibility. The self-healing capability and elasticity are crucial to ensure the robustness and lifespan of the hydrogel, but achieving these exclusive properties remains challenging. Herein, fully self-healable and elastic hydrogel is achieved through long-chain polyacrylic acid (PAA) scaffold and follow-up polymerization of polyacrylamide (PAM).
View Article and Find Full Text PDFChemphyschem
September 2025
Key Laboratory of Advanced Structural Materials, Ministry of Education, School of Materials Science and Engineering, Changchun University of Technology, Changchun, Jilin, 130012, China.
Polymer resistive random-access memory (RRAM) holds great promise for flexible wearable electronics and artificial intelligence, yet its development is hindered by chain entanglement and intermolecular interactions, leading to processing challenges, high operating voltages, and unstable switching parameters. Herein, metal-porphyrin-terminated hyperbranched polyimides (ATPP@HBPI, (Zn)ATPP@HBPI, and (Cu)ATPP@HBPI) were synthesized. The hyperbranched structure mitigates intermolecular interactions, while ionic doping modulates conductivity, and the synergistic effect of ions and electrons optimizes resistive switching behavior.
View Article and Find Full Text PDFInt J Biol Macromol
August 2025
Jiangsu Co-Innovation Center of Efficient Processing and Utilization of Forest Resources, College of Materials Science and Engineering, Nanjing Forestry University, Nanjing, Jiangsu 210037, China. Electronic address:
Current shielding technologies predominantly focus on performance optimization while neglecting fire safety considerations especially in construction building. To address the vulnerability of electromagnetic interference (EMI) shielding materials to accidental fires, we develop sustainable biocarbon/cellulose composites with integrated EMI shielding and flame-retardant capabilities. This approach employs porous biocarbon particles as functional units combined with three-dimensional cellulose networks through hydrogen bonding, van der Waals forces, and physical entanglements.
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