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ACS Nano · 2021 · IF 15.881

Tough and Degradable Self-Healing Elastomer from Synergistic Soft–Hard Segments Design for Biomechano-Robust Artificial Skin

Xiaochen Xun,Xuan Zhao,Qi Li,Bin Zhao,Tian Ouyang,Zheng Zhang,Zhuo Kang,Qingliang Liao,Yue Zhang

Increasing biomechanical applications of skin-inspired devices raise higher requirements for the skin-bionic robustness and environmental compatibility of elastomers. Here, a tough and degradable self-healing elastomer (TDSE) is developed by a synergistic soft–hard segments design. The polyester/polyether copolymer is introduced in soft segments to endow TDSE with flexibility and degradability. The two isomeric diamines are regulated in hard segments for elevating the toughness and fracture energy to 82.38 MJ/m3 and 43299 J/m2 and autonomous self-healing ability with 93% efficiency in 7 h for the TDSE. Employing TDSE and ionic liquid, a biomechano-robust artificial skin (BA-skin) is constructed with a stretch-insensitive mechanosensation capability during 50% cyclic stretching. The BA-skin has high biomechano-robustness to bear tear damage and good environmental compatibility with total decomposability in a lipase solution. This work provides a molecular design guideline for high-performance skin-bionic elastomers for applications in skin-inspired devices.

CAS / MDL: 68-12-2 109-99-9
研究领域: 材料科学 · 生物医学工程 · 高分子化学
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Journal of Materials Chemistry C · 2024 ·Vol. 12 ·期 26 ·9685-9692 · IF 5.7

A self-healing elastomer with outstanding mechanical properties was designed based on urea bonds

Yanpeng Cao,Rui Yan,Xiaoye Wo,Jinlong Ma,Xiao Yu,Aijun Li,Jian Huang,Fenghua Li,Qixian Zhang

Owing to the demand for high sensitivity and lightweight flexible electronic devices, researchers have made efforts to develop wearable devices by integrating flexible electronic devices onto flexible and self-healing substrates. Developing self-healing materials with excellent self-healing efficiency and ultra-high mechanical performance at room temperature is very important. A new self-healing material was successfully synthesized as a high-strength polyurethane elastomer by introducing functional segments with different structural rigidities, including thiourea and oxime–urethane bonds. It was named 2,5-dithiobiurea–dimethylglyoxime–urethane complex-based polyurethane elastomer (DBTU–DOU–PU, hereinafter referred to as DDPU). The mechanical strength of DDPU can be restored to 5 MPa after repairing for 10 min at room temperature (25 ± 2 °C). After 72 h recovery, the tensile strength of DDPU is 65.4% of its initial value. The colorless and transparent DDPU material may have broad application prospects such as in electronic skin, human-computer intelligent interaction, and flexible self-healing sensors.

研究领域: 材料科学 · 生物医学工程 · 高分子化学
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LANGMUIR · 2020 · IF 3.557

Constructing Electrically and Mechanically Self-Healing Elastomers by Hydrogen Bonded Intermolecular Network

Ruiyu Yang,Yujin Yao,Zaihua Duan,Zhen Yuan,Huiling Tai,Yadong Jiang,Yonghao Zheng,Dongsheng Wang

One key limitation of artificial skin-like materials is the shortened service life caused by mechanical damages during practical applications. The ability to self-heal can effectively extend the material service life, reduce the maintenance cost, and ensure safety. Therefore, it is important and necessary to fabricate materials with simultaneously mechanical and electrical self-healing behavior in a facile and convenient way. Herein, we report a stretchable and conductive self-healing elastomer based on intermolecular networks between poly(acrylic acid) (PAA) and reduced graphene oxide (rGO) through a facile and convenient postreduction and one-pot method. The introduction of rGO provides the PAA-GO elastomers with good mechanical stability and electrical properties. Moreover, this material exhibited both electrical and mechanical self-healing properties. After cutting, the elastomers self-healed quickly (∼30 s) and efficiently (∼95%) at room temperature. The elastomers were accurate and reliable in detecting external strain even after healing. The elastomers were further applied for strain sensors, which were attached directly to human skin to monitor external movements, including finger bending and wrist twisting.

CAS / MDL: 109-99-9
研究领域: 材料科学 · 生物医学工程
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ADVANCED FUNCTIONAL MATERIALS · 2021 ·Vol. 31 ·期 11 ·2008328 · IF 18.808

A New Strategy of Discretionarily Reconfigurable Actuators Based on Self-Healing Elastomers for Diverse Soft Robots

Jiaming Lou,Zenghe Liu,Lei Yang,Yifan Guo,Dong Lei,Zhengwei You

Actuators have shown great promise in many fields including soft robotics. Since reconfiguration allows actuators to change their actuation mode, it is considered a key characteristic for new-generation adaptive actuators. However, it remains a challenge to design simple and universal methods to fabricate actuators that can be reconfigured to allow diverse actuation modes. Here, a macroscopically discretionary healing-assembly strategy to fabricate reconfigurable soft actuators based on intrinsic self-healing poly(dimethylglyoxime-urethane) (PDOU) elastomers is developed. The PDOU elastomers with different degrees of crosslinking show different responsiveness to solvents, and are seamlessly healed. Crosslinked and non-crosslinked PDOU elastomers as building units are healing-assembled into actuators/robots with diverse actuation behaviors. Notably, the assembled actuators/robots are readily reprogrammed to exhibit multiple actuation modes by simply tailoring and reassembling without any external stimuli. This work paves a new, simple, powerful, and universal method to construct sophisticated soft robots.

研究领域: 材料科学 · 软体机器人学
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RSC Advances · 2022 ·Vol. 12 ·期 33 ·21512-21519 · IF 4.036

A stretchable and healable elastomer with shape memory capability based on multiple hydrogen bonds

Jiacheng Ma,Shifeng Wen,Zhufeng Yue

Although a wide range of self-healing materials have been reported by researchers, it is still a challenge to endow exceptional mechanical properties and shape memory characteristics simultaneously in a single material. Inspired by the structure of natural silk, herein, we have adopted a simple synthetic method to prepare a kind of elastomer (HM-PUs) with stiff, healable and shape memory capabilities assisted by multiple hydrogen bonds. The self-healing elastomer exhibits a maximum tensile strength of 39 MPa, toughness of 111.65 MJ m−3 and self-healing efficiency of 96%. Moreover, the recuperative efficiency of shape memory could reach 100%. The fundamental study of HM-PUs will facilitate the development of flexible electronics and medical materials.

研究领域: 材料科学 · 生物医学工程
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Polymer Chemistry · 2021 ·Vol. 12 ·期 42 ·6145-6153 · IF 5.582

Application of a super-stretched self-healing elastomer based on methyl vinyl silicone rubber for wearable electronic sensors

Tianwen Yu,Yifei Shan,Zhixi Li,Xiaoxiao Wang,Huanan Cui,Kun Yang,Yongyan Cui

Wearable electronic devices, represented by wearable sensors with self-healing properties, are key to the development of the relevant research studies. However, problems of sensors such as low sensitivity, low flexibility, low durability and poor self-healing ability remain to be solved. Herein, we designed and prepared a new type of silicone-based self-healing elastomer MVSR-UPY in which methyl vinyl silicone rubber was modified by an olefin decomposition reaction, and then constructed a quadruple hydrogen bonding network by introducing 2-ureido-4[1H]-pyrimidinones (UPY). The prepared elastomer that can be recycled and reprocessed was endowed with excellent self-healing and super-stretching properties of up to 2000%. A three-layer (LBL) strain sensor with high sensitivity and durability was fabricated using the elastomer as the substrate, which was able to monitor various activities of the human body accurately. It is notable that writing different letters on the sensor produces different resistance signals and makes it possible for us to distinguish between the written letters. Therefore, the sensor we designed can meet the various needs of wearable electronic devices and provide more possibilities for its development.

CAS / MDL: 67-68-5 109-99-9
研究领域: 材料科学 · 生物医学工程 · 柔性电子
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Mechanically robust, highly adhesive and autonomously low-temperature self-healing elastomer fabricated based on dynamic metal − ligand interactions tailored for functional energetic composites

Yana Zhang,Jiaoyang Chen,Guangpu Zhang,Jianqiang Xv,Jianhua Xv,Yubing Hu,Hu Guo,Fan guo,JiaJun Fu,Wei Jiang

Self-healing materials are used in various applications because of their capacity to prolong the material’s longevity and durability. Several important properties, including high adhesion force to various surfaces and mechanical robustness have the potential to further expand their application in various fields. In this study, we designed an energy-containing and high-adhesion elastomer (3,5-BTP-PDMS-4), which was fabricated via the click polymerization, that could self-heal at −20 °C. The prepared polymer adhesive exhibited prominent mechanical strength with a high Young’s modulus of up to 17.91 MPa. The material also showed that it could autonomously and completely self-heal and restore its mechanical properties within 6 h at room temperature when the 3,5-BTP-PDMS-4 sample was cut into two separate pieces. Moreover, this material was found to possess a high adhesion force of up to 1.65 MPa on steel, which increased when the temperature was reduced. Furthermore, we prepared TATB-based PBXs using 3,5-BTP-PDMS-4 as a binder because of its energy-containing property and excellent self-healing properties to heal cracks generated during fabrication, transportation and storage. Surprisingly, the TATB-based PBXs achieved complete self-healing at 0 °C and partial self-healing at −20 °C, although the low plastic explosive crystals were detrimental to the material’s self-healing properties. The successful development of a polymer adhesive that has a high-Young’s modulus and can autonomously and completely self-heal could help expand its applications with enhanced versatility in several fields, including military and civil applications.

研究领域: 材料科学 · 化学工程 · 聚合物科学 · 能量材料
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Petroleum Science · 2021 · IF 4.09

Self-healing elastomer modified proppants for proppant flowback control in hydraulic fracturing

Jian-Da Li,Gui-Cai Zhang,Ji-Jiang Ge,Wen-Li Qiao,Ping Jiang,Hai-Hua Pei

To address proppant flowback issues during post-fracturing treatments and production, self-healing elastomer modified proppants (SMPs) are proposed. Owing to their inherent self-aggregation behavior, the SMPs can aggregate together spontaneously to prevent proppant flowback and increase the pack porosity. It is noteworthy that the SMPs have a firm and dry self-healing elastomer (SE) coating, making their storage, transport and use as conventional proppants possible. The SE synthesized through polymerization is rich in amidogens and carbonyl groups as characterized by Fourier transform infrared spectroscopy and the proton nuclear magnetic resonance. Thermal and thermomechanical properties of the SE coating are revealed by the thermogravimetric analysis, the differential scanning calorimetry and the rheological tests. The self-aggregation behavior of the SMPs is demonstrated by the adhesion force tests. The reversible hydrogen bonding interactions in SE coating contribute to the self-aggregation behavior of the SMPs, which is revealed by the thixotropy test and the FTIR analysis at different temperatures. With the self-aggregation behavior, the crushed proppants can aggregate in situ to form a stable structure again and therefore reduce the threat of narrowing down the fracture and proppant flowback, which has an important practical significance during oil and gas production.

CAS / MDL: 7447-40-7 497-19-8
研究领域: 石油工程 · 材料科学 · 化学工程
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EUROPEAN POLYMER JOURNAL · 2021 · IF 4.598

Preparation of mechanically robust and autonomous self-healable elastomer based on multiple dynamic interactions

Minhui Wang,Jiahui Zhou,Xiaolin Jiang,Yeming Sheng,Min Xu,Xun Lu

Self-healing materials have attracted considerable attention because of their sustainable property of prolonging service life and reducing resource consumption. However, as plenty of room-temperature self-healable materials have been studied, it still remains a great challenge to equip these materials with admirable mechanical strength since there is a compromise between intermolecular interactions and chain mobility. Herein, a novel strategy of integrating self-healing ability with robustness in polymeric elastomer at ambient condition was developed. The synthesized polyurethane was equipped with multiple reversible interactions including disulfide bonds, oxime urethane bonds, H-bonds and coordination interactions, and formed triple cross-linking network. What’s important is that Cu 2+ could not only act as the coordination center, but also serve as the catalyst to accelerate disulfide exchange and oxime urethane exchange reaction. XPS and stress relaxation tests revealed that the introduction of CuCl 2 reduced the relaxation activation energy of both the disulfide metathesis and oxime urethane exchange reaction. Thanks to the multiple interactions design and the effects of Cu 2+ , the elastomer was endowed with excellent mechanical strength of 19.5 MPa and self-healing efficiency of 83% at room temperature.

研究领域: 材料科学 · 聚合物化学 · 机械工程
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Nature Communications · 2023 ·Vol. 14 ·期 1 ·1-8 · IF 16.6

3D printing of self-healing personalized liver models for surgical training and preoperative planning

Lu Yahui,Chen Xing,Han Fang,Zhao Qian,Xie Tao,Wu Jingjun,Zhang Yuhua

3D printing can produce intuitive, precise, and personalized anatomical models, providing invaluable support for precision medicine, particularly in areas like surgical training and preoperative planning. However, conventional 3D printed models are often significantly more rigid than human organs and cannot undergo repetitive resection, which severely restricts their clinical value. Here we report the stereolithographic 3D printing of personalized liver models based on physically crosslinked self-healing elastomers with liver-like softness. Benefiting from the short printing time, the highly individualized models can be fabricated immediately following enhanced CT examination. Leveraging the high-efficiency self-healing performance, these models support repetitive resection for optimal trace through a trial-and-error approach. At the preliminary explorative clinical trial (NCT06006338), a total of 5 participants are included for preoperative planning. The primary outcomes indicate that the negative surgery margins are achieved and the unforeseen injuries of vital vascular structures are avoided. The 3D printing of liver models can enhance the safety of hepatic surgery, demonstrating promising application value in clinical practice.

CAS / MDL: 114235-67-5
研究领域: 生物医学工程 · 外科技术 · 材料科学 · 医学影像
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Healable, highly thermal conductive, flexible polymer composite with excellent mechanical properties and multiple functionalities

Dong Wang,Shangyang Ren,Jiaoyang Chen,Yukun Li,Zhifeng Wang,Jianhua Xu,Xu Jia,Jiajun Fu

Flexible and electrically insulating polymers are ideal heat dissipation packaging materials for flexible electronic devices, but their inherent low thermal conductivity has gradually become a bottleneck for their application in high-performance flexible electronics. Here, we report a high thermal conductive polymer composite, which was synthesized by an effective and feasible method of implanting hydroxylated boron nitride nanosheets (hy-BNNSs) into self-healable elastomer material (SM). The introduction of hy-BNNSs endowed the composite with an ultrahigh in-plane thermal conductivity of 12.6 ± 0.71 W m −1 K −1 and excellent mechanical properties including superior flexibility, remarkable recovery ability and humidity stability. Moreover, the composite demonstrated the deformation recovery ability and dimensional stability at 70 °C, which are indispensable in flexible electronic applications, and are fairly rare in healable composites. Benefiting from dynamic characteristics of non-covalent hydrogen bonds and disulfide bonds within polymeric materials, the composite can restore the mechanical properties, heat dissipation properties, and dielectric properties. All the results demonstrate it an ideal candidate for thermal management in flexible electronic devices.

CAS / MDL: 4098-71-9
研究领域: 材料科学 · 聚合物科学 · 纳米技术 · 柔性电子 · 热管理
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