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Journal of Energy Chemistry · 2023 · IF 13.1

An intrinsically self-healing and anti-freezing molecular chains induced polyacrylamide-based hydrogel electrolytes for zinc manganese dioxide batteries

Haiyang Liao,Wenzhao Zhong,Chen Li,Jieling Han,Xiao Sun,Xinhui Xia,Ting Li,Abolhassan Noori,Mir F. Mousavi,Xin Liu,Yongqi Zhang

The anti-freezing strategy of hydrogels and their self-healing structure are often contradictory, it is vital to break through the molecular structure to design and construct hydrogels with intrinsic anti-freezing/self-healing for meeting the rapid development of flexible and wearable devices in diverse service conditions. Herein, we design a new hydrogel electrolyte (AF/SH-Hydrogel) with intrinsic anti-freezing/self-healing capabilities by introducing ethylene glycol molecules, dynamic chemical bonding (disulfide bond), and supramolecular interaction (multi-hydrogen bond) into the polyacrylamide molecular chain. Thanks to the exceptional freeze resistance (84% capacity retention at −20 °C) and intrinsic self-healing capabilities (95% capacity retention after 5 cutting/self-healing cycles), the obtained AF/SH-Hydrogel makes the zinc||manganese dioxide cell an economically feasible battery for the state-of-the-art applications. The Zn||AF/SH-Hydrogel||MnO 2 device offers a near-theoretical specific capacity of 285 mA h g −1 at 0.1 A g −1 (Coulombic efficiency ≈100%), as well as good self-healing capability and mechanical flexibility in an ice bath. This work provides insight that can be utilized to develop multifunctional hydrogel electrolytes for application in next generation of self-healable and freeze-resistance smart aqueous energy storage devices.

研究领域: 材料科学 · 能源存储 · 化学工程
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Materials Today Communications · 2024 · IF 3.7

Effect of aging on structure and properties of self-healing-enhanced SBS modified asphalt with dual dynamic chemical bonds

Tianwei Zhang,Shanjun Gao,Yanheng He,Quantao Liu,Shi Xu,Ronghua Zhuang,Shangheng Zeng,Jianying Yu

The introduction of dynamic chemical bonds (disulfide bonds, hydrogen bonds, etc.) into the network structure of SBS modified asphalt (SMA) can notably improve its healing properties. However, aging may break the dynamic chemical bonds in self-healing SMA, thereby deteriorating its healing ability. Therefore, it is crucial to investigate the effects of aging on the structure and properties of self-healing SMA with dynamic chemical bonds. Herein, self-healing SBS modified asphalts (SD/SMA and DDH/SMA) containing single disulfide bonds (SD) and dual disulfide bonds and hydrogen bonds (DDH) were prepared by free radical reaction, respectively. The SD/SMA and DDH/SMA were subjected to Thin Film Oven Test (TFOT) aging and Pressurized Aging Vessel (PAV) aging. Chemical structure analysis showed that the disulfide bonds underwent partial break after PAV aging. Nevertheless, the results of the healing tests indicated that compared to SMA, SD/SMA and DDH/SMA maintained superior healing properties after aging under the break-reorganization effect of dynamic chemical bonds. The fatigue healing indices of SD/SMA and DDH/SMA were 51.9 % and 95.8 % higher than those of SMA after PAV aging. The rheology tests revealed that SD/SMA and DDH/SMA had higher recovery rates and low-temperature cracking resistance than SMA before and after aging. Compared with SMA, SD/SMA and DDH/SMA had superior anti-aging performance. After PAV aging, the ductility retention rate of SD/SMA and DDH/SMA was 72.9 % and 98.9 % higher than that of SMA. Furthermore, compared to SD/SMA, DDH/SMA containing dual disulfide and hydrogen bonds had better healing capability, rheological properties and anti-aging performance.

研究领域: 材料科学 · 化学工程
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NEW JOURNAL OF CHEMISTRY · 2020 ·Vol. 44 ·期 25 ·10586-10591 · IF 3.288

Rapidly self-healing, magnetically controllable, stretchable, smart, moldable nanoparticle composite gel

Wenhui Zheng,Yangyang Li,Huawei Wei,Guolin Gao,Dawei Zhang,Zaixing Jiang

Rational design of a magnetic and fast self-healing gel is significant in the field of shape construction. Magnetic gels with rapid self-healing ability constructed using nanoparticles and dynamic chemical bonds have so far been elusive. Here, an ultrafast self-healing magnetic gel based on thioctic acid (TA), ferric chloride (FeCl3) and ferric oxide (Fe3O4) has been successfully synthesized. The reversible interactions of the S–S bond, hydrogen bond and iron(III)–carboxylate coordinate bonds endow a 100% self-healing efficiency for the magnetic gel after healing in air for only 10 min, and a saturation magnetization of the gel of 0.27 emu g−1 can be achieved. The intelligent in situ healing ability of the as-obtained magnetic gel guarantees the same function and shape as the original gel. This combination of high-efficiency repaired performance and magnetic properties can broaden the range of applications for shape construction through the “building blocks” consisting of magnetic gels.

研究领域: 材料科学 · 化学工程
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Manipulate dynamic chemical interactions in renewable polymers for 3D printing tunable, healable, and recyclable metamaterials

Yuchao Wu,Cheng Qiu,Karla J. Silva,Jaeho Shin,Shaoyun Wang,Bujingda Zheng,Zhenru Chen,Guoliang Huang,James M. Tour,Jian Lin

Mechanical metamaterials have garnered significant interests due to their unique properties, which arise from the periodic structures of their constituent units. However, traditional mechanical metamaterials suffer from limitations of fixed properties of the constituent units or irreversibility if they are damaged or little-to-no recyclability. Addressing this challenge, herein, a photoresin consisting of a monomer synthesized from a renewable biomass—epoxidized soybean oil (ESO)—citric acid (CA) and other components was developed for light-based 3D printing. It is discovered that the UV irradiation initiates photopolymerized of the highly photoactive epoxidized soybean oil-ethyl acrylamide (ESO-EA) monomer while enabling the epoxy-acid reaction (EAR) of the epoxy groups in ESO-EA with carboxyl groups in CA to create dynamic chemical bonds (DCBs). This formed dynamic crosslinking network endows the printed material with tunable tensile strengths (0.3–10.4 MPa) and shape memory behaviors (transition temperature: 22–48 °C) while maintaining high stretchability (fractural strain: 81 %–205 %). Thermal annealing facilitates dynamic transesterification reactions (DTER) to further improve the mechanical properties while making the printed materials healable and recyclable. By integrating these innovations into liquid crystal display (LCD) based 3D printing, we demonstrate origami metamaterials with tunable, multi-stable mechanical behaviors as well as property recovery after self-healing of the damaged structures by both simulations and experiments. Finally, the printed metamaterials can be recycled with the well-preserved properties.

CAS / MDL: 8013-07-8
研究领域: 材料科学 · 化学工程
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ACS Applied Materials & Interfaces · 2025 · IF 8.2

Boosting the Actuation Performance of a Dynamic Supramolecular Polyurethane–Urea Elastomer via Kinetic Control

Run-Pan Nie,Hua-Dong Huang,Ding-Xiang Yan,Li-Chuan Jia,Jun Lei,Zhong-Ming Li

The ongoing soft actuation has accentuated the demand for dielectric elastomers (DEs) capable of large deformation to replace the traditional rigid mechanical apparatus. However, the low actuation strain of DEs considerably limits their practical applications. This work developed high-performance polyurethane–urea (PUU) elastomers featuring large actuation strains utilizing an approach of kinetic control over the microphase separation structure during the fabrication process. Additionally, disulfide (DS) bonds were incorporated as dynamic chemical linkages to effectively heal the mechanical damage in the resulting elastomer (PUUDS). Alteration in processing conditions creates notable differences in the rate of phase separation among the multiphase materials. A faster phase separation rate is associated with a reduced degree of microphase separation, increased spacing within hard domains, a higher proportion of disordered hydrogen bonds, and hydrogen bonding index. These changes synergistically improved the electromechanical properties of the PUUDS elastomers, thereby enhancing their actuation performance. The sample processed under the fastest phase separation condition showed the lowest Young’s modulus and a pronounced dielectric response at low frequencies. The electrostriction effect accounts for 89% of the total electromechanical coupling, achieving a significant reduction in the driving voltage during actuation. The maximum actuation strain recorded was 21.6% at an electric field of 45 MV/m. Benefiting from the fully reversible dynamic network, the damaged PUUDS elastomer can be healed and restored to its original elongation at break after 3 h at room temperature. Practical application was demonstrated through the development of a miniature butterfly model constructed from a single-layer PUUDS elastomer, showcasing potential applications in soft robotics. These findings highlight the critical role of kinetic control in optimizing the performance of advanced DEs.

CAS / MDL: 4098-71-9 25190-06-1
研究领域: 材料科学 · 软体机器人 · 高分子化学
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ACS Applied Nano Materials · 2025 · IF 5.5

Development of a Graphene Oxide-Enhanced Thermoresponsive Self-Healing Waterborne Polyurethane Elastomer for Abdominal Wall Defect Repair

He Gan,Lin Wang,Ran Sun,Junchen Li,Zhirong Zhao,Yuan Chen,Weiliang Tian,Fan Yang,Qian Huang

Polyurethane has been widely utilized in medical devices, owing to its excellent biocompatibility, mechanical properties, and processability. This study presents a thermoresponsive self-healing waterborne polyurethane elastomer (WPU) incorporating graphene oxide (GO), designed to enhance the repair of abdominal wall defects. This material integrates multiple functionalities including antimicrobial activity, tissue regeneration, and self-healing capabilities, offering a safer and more effective solution. The WPU matrix provides excellent biocompatibility and controllable degradability, contributing to reduced tissue adhesion and promoted abdominal wall regeneration. The incorporation of GO endows the material with photothermal properties, enabling localized thermal effects under near-infrared irradiation to achieve synergistic antimicrobial effects. Furthermore, the dynamic chemical bonds in the cross-linked network confer thermoresponsive self-healing ability. In infected skin and abdominal wall defect rat models, the WPU-GO elastomer exhibited potent antimicrobial activity, promoted wound closure, reduced inflammation, and demonstrated excellent antiadhesion and tissue regeneration capabilities. This multifunctional material shows remarkable potential in abdominal wall defect treatment.

研究领域: 生物材料 · 高分子科学 · 生物医学工程 · 纳米技术 · 再生医学 · 伤口愈合
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Self-healing polyurethane coatings based on dynamic chemical bond synergy under conditions of photothermal response

Kang Chen,Haoxin Zhu,Zhiyi Zhang,Yingqing Shao,Qianhui Yu,Xinlei Cao,Siyan Pan,Xin Mu,Zhenhua Gao,Di Wang,Shuangying Wei,Shuaiyuan Han

Self-healing coatings represent a promising advancement in intelligent materials, as they possess the ability to autonomously heal damage through a self-regeneration mechanism. However, a significant challenge is to strike a balance between the self-healing capability and mechanical performance under specific healing conditions, such as heat or light. This limitation hinders the application of self-healing coatings. This study describes a series of syntheses of a waterborne polyurethane (WPU) based on a vanillin-derived aromatic Schiff base (VASB). The VASB-WPU was created by incorporating dynamic reversible covalent bonds into the backbone chain and introducing supramolecular interactions (hydrogen bonds and ionic bonds) into the side chain. The VASB-WPU exhibits self-healing properties and vitrimer characteristics. By implementing a healing process that involves light and heat stimulation, the VASB-WPU exhibits an impressive healing efficiency of 92.43% in thin films while maintaining exceptional mechanical performance, with a tensile stress of 10.59 MPa and a toughness of 16.56 MJ/m 3 . Furthermore, the VASB-WPU coatings exhibit exceptional multiple shape memory capabilities and self-healing effects. When applied to wooden surfaces, the VASB-WPU coatings can achieve 100% self-healing of a 5 μm scratch at the interface in just 3 min of irradiation. A new method has been introduced for developing intelligent self-healing coatings for wood.

研究领域: 材料科学 · 聚合物化学 · 涂层技术
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CHEMISTRY OF MATERIALS · 2019 · IF 10.159

Smart Hydrogels with Antibacterial Properties Built from All Natural Building Blocks

Mengyu Li,Hui Wang,Junfei Hu,Jingjing Hu,Song Zhang,Zhen Yang,Yiwen Li,Yiyun Cheng

Smart hydrogels with multistimuli responsiveness have been increasingly exploited as soft matters for biomedical applications in drug delivery, tissue engineering, and bioactuators. While many of the effects have been well documented, the facile fabrication of multiresponsive hydrogels with specific functionality is met with profound challenges, particularly in the redundant synthesis of macromolecular building blocks and the integration of multiple dynamic linkages to construct hydrogel networks. To address this issue, herein, we report a simple and rapid fabrication of smart hydrogels by direct gelation of all naturally occurring building blocks including aminoglycosides, protocatechualdehyde, and Fe(III) via two types of dynamic chemical bonds. The resulting smart hydrogels could perform excellent dynamic features and promising multiresponsiveness to different stimuli including temperature, light, pH, redox, and electricity, and also exhibited high antibacterial activities. This study offers new opportunities in the facile preparation of smart hydrogels for a wide range of applications.

研究领域: 材料科学 · 生物医学工程 · 化学 · 药学
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POLYMER · 2023 · IF 4.6

Highly sensitive, super high stretchable hydrogel strain sensor with underwater repeated adhesion and rapid healing

Liang Liu,Yunxin Chen,Chunxia Zhao,Min Guo,Yuanpeng Wu,Yuntao Li,Dong Xiang,Hui Li,Li Wang,Xiaoyan Zhang

Traditional hydrogel-based strain sensors do not work well under water due to extreme swelling and poor adhesion to substrates in water-rich conditions. Inspired by the jellyfish tentacles, a super stretchable dual crosslinked hydrogel was prepared as a motion sensor underwater. The hydrogel contained a cationic surfactant , hexadecyl trimethyl ammonium bromide (CTAB), that crosslinked with hydrophobic lauryl methacrylate (LMA) units in an AA-LMA copolymer . Al 3+ ions also coordinated with carboxyl groups in PAA chains and amino groups on chitosan (CS) to form ionic crosslink points. The formed hydrogel exhibited excellent anti-swelling characteristics, superior tensile properties (≈3000%), and rapid self-healing performance. Due to the complementary effects of electrostatic interactions and dynamic chemical bond formation, the hydrogel efficiently and repeatably adhered to various biological tissues, such as hogskin and shrimp, in aquatic environments. Moreover, the hydrogel-based strain sensor showed high sensitivity (GF = 2.04) over a wide sensing range from 0 to 1000% strain with high stability in air and water. The prepared materials' unique performance further expands their application prospects in flexible wearable devices , anti-counterfeiting recognition, and other fields in environmental conditions.

CAS / MDL: 7727-54-0
研究领域: 材料科学 · 生物医学工程 · 可穿戴技术 · 传感技术
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