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ADVANCED FUNCTIONAL MATERIALS · 2019 ·Vol. 29 ·期 27 ·1901721 · IF 15.621

Printing Hydrogels and Elastomers in Arbitrary Sequence with Strong Adhesion

Hang Yang,Chenghai Li,Meng Yang,Yudong Pan,Qianfeng Yin,Jingda Tang,Hang Jerry Qi,Zhigang Suo

Many recently demonstrated devices require the integration of hydrogels and hydrophobic elastomers. Extrusion print is a promising method for rapid prototyping but existing approaches do not fulfill a basic requirement: print integrated structures of a hydrogel and an elastomer, in arbitrary sequence, with strong adhesion. This paper demonstrates an approach to fulfill this requirement. During print, the ink of each material flows through a nozzle under a pressure gradient but retains the shape against gravity and capillarity. During cure, covalent bonds form to link monomer units into polymer chains, crosslink the polymer chains into the polymer networks of the hydrogel and the elastomer, as well as interlink the two polymer networks into an integrated structure. The approach covalently interlinks the hydrogel network and the elastomer network by adding an interlink initiator in one of the inks. An adhesion energy above 5000 J m −2 is demonstrated. Printed morphing structures survive swelling and printed artificial axons survive repeated hits of a hammer. This approach opens a road to the development of soft devices for broad applications in medicine and engineering.

研究领域: 生物医学工程 · 材料科学
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COLLOIDS AND SURFACES B-BIOINTERFACES · 2021 · IF 5.268

Adhesive, self-healing, conductive Janus gel with oil-water responsiveness

Jinling Liu,Jie Ai,Jiawen Chen,Ying Guo,Jianrong Lin,Qinhui Chen

The anisotropic Janus gel shows more diverse characteristic and responsiveness due to its asymmetric chemical structure. Herein, the water/oil PDA-PAA/PBMA-PEHMA Janus gel was prepared by one-step polymerization of incompatible monomers. In this Janus gel, PDA-PAA layer possesses good adhesion effect and self-healing property attributing to the chemical bonds and the hydrogen bonds among DA, AA, or each other, and the π-π stacking of DA. The IPN structure of the water phase and the oil phase makes Janus gel have good mechanical properties. The above chemical and physical effects dissipate a large amount of energy when PDA-PAA/PBMA-PEHMA Janus gel is subjected to external forces, so it has excellent fatigue resistance. The hydrophilic PDA-PAA side and the lipophilic PBMA-PEHMA side show different swelling responses in the oil-water medium. The internal stress difference caused by this different swelling makes the Janus gel show curl toward different directions in different media. Then, conductivity media of NaCl added in PDA-PAA layer endows Janus gel with anisotropic conductivity. It is possible to judge the hydrophilic and hydrophobic properties of solution by monitoring the current change of conductive Janus gel. Conductive Janus gel can also be used to monitor human body motion and micro motion. This conductive/insulating Janus gel is suitable for flexible sensor used in harsh environment.

研究领域: 材料科学 · 生物医学工程
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JOURNAL OF BIOMATERIALS SCIENCE-POLYMER EDITION · 2020 · IF 2.69

The preparation of multifunction chitosan adhesive hydrogel by “one- step” method

Ruixue Liu,Yingbo Li,Jichao Chen,Xiaojing Zhang,Zhibin Niu,Yadong Sun

Chitosan adhesive hydrogels have attracted interest because of their unique properties. However, it is still a challenge to use simple and unmodified chitosan to synthesize multifunctional hydrogels with adhesive, self-healing and strain sensing properties. Here, a multifunctional hydrogel of Ca2+-chitosan/polyacrylamide(Ca2+- CS/PAAm)with adhesive self-healing and strain sensing properties was carried out by one-step preparation method. The hydrogel has the ability to adhere to a variety of materials, wherein the adhesion strength to rubber surface is 48.4 kPa. The hydrogel has excellent strain sensing capability on finger bending or cyclic stretching, the sensitivity factor is 0.41 ± 0.015. The cut hydrogel healed completely at room temperature within 4 h, and the healing hydrogel can be stretched to 5 times of its original length. This makes Ca2+-CS/PAAm hydrogel to be great potential in the application of strain sensors, wound dressing and skin adhesives.

研究领域: 生物材料 · 医学工程 · 高分子化学
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS · 2020 · IF 3.99

A multi-functional reversible hydrogel adhesive

Yonggan Yan,Shulei Xu,Huanxi Liu,Xin Cui,Jinlong Shao,Peng Yao,Jun Huang,Xiaoyong Qiu,Chuanzhen Huang

Designing and fabricating self-healing hydrogel adhesive is essential in many physical and biological applications such as wound closure and cartilage repair. In this work, a new type of hydrogel adhesive has been developed through ultraviolet (UV) curing acrylamide (AM) monomer and hyper-branched polyethylenimine (PEI) polymer. The synthesized PAM-PEI hydrogel (weight ratio for PEI: PAM = 1: 9) shows high stretchability (1D extension ratio > 5500 %) and good plasticity (it can be extended into 2D hydrogel film), quick self-healing property (within 30 s) at ambient enviornment and good adhesiveness to both inorganic (23 kPa ∼ 90 kPa for metal and glass) and organic substrates (∼ 8 kPa for polytetrafluoroethylene , 1 ∼ 7 kPa for skin and liver). More importantly, the adhesion-strip-cycle test suggested that the adhesion measured was reversible and did not attenuate for at least 5 cycles on various surfaces. Rheology tests have demonstrated the repeatability of self-healing behavior of the hydrogel between small (1%) and large (1000 %) strain. In addition, the self-healed hydrogel fragments show good injectability, which can be potentially used for 3D-printing. This work provides a facile way of preparing multifunctional hydrogel adhesive with potential engineering applications.

CAS / MDL: 9002-98-6 110-26-9
研究领域: 生物材料学 · 组织工程 · 再生医学
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CELLULOSE · 2022 ·Vol. 30 ·期 1 ·397-411 · IF 6.123

Bioinspired adhesive and self-healing bacterial cellulose hydrogels formed by a multiple dynamic crosslinking strategy for sealing hemostasis

Yi Xiaotong,Cheng Feng,Wei Xinjing,Li Hongbin,Qian Jingting,He Jinmei

Abstract Hydrogels have attracted widespread attention in controlling bleeding due to their superiority in matching irregular defects. However, inadequate mechanical performance, insufficient adhesion and long gelation times still hinder their application for hemostasis. In this study, a novel hydrogel with self-healing and adhesive properties was designed and synthesized by introducing reversible borate ester bonds of polyvinyl alcohol-borax into tannic acid-modified bacterial cellulose (TA@BC). As demonstrated by tensile stress‒strain tests and rheological measurements, the hydrogels have excellent mechanical performance owing to the synergistic multiple crosslinked bonds among tannic acid-modified bacterial cellulose (TA@BC), polyvinyl alcohol polymer chains and borax in a covalent polymer network. The hydrogels show good self-healing properties and adhesion to different substrates. Moreover, blood loss from a wound treated with the designed hydrogel was approximately 1/5th that from an untreated wound, demonstrating the excellent hemostatic capacity of the hydrogels. Therefore, the designed hydrogels have potential applications in hemostasis and wound dressing. Graphical abstract

CAS / MDL: 56-17-7 9002-89-5
研究领域: 生物医学工程 · 材料科学
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MACROMOLECULAR RAPID COMMUNICATIONS · 2024 · IF 4.2

Amyloid Proteins Adhesive for Slippery Liquid-Infused Porous Surfaces

Na Feng,Shuting Miao,Xin Guo,Ziyi Yang,Luke Yan,Peng Yang,Jia Kong

Biomimetic slippery liquid-infused porous surfaces (SLIPS) have emerged as a promising solution to solve the limitations of superhydrophobic surfaces, such as inadequate durability in corrosion protection and a propensity for frosting. However, the challenge of ensuring strong, lasting adhesion on diverse materials to enhance the durability of the lubricant layer remains. The research addresses this by leveraging amyloid phase-transitioned lysozyme (PTL) as an adhesive interlayer, conferring stable attachment of SLIPS across a variety of substrates, including metals, inorganics, and polymers. The silica-textured interface robustly secures the lubricant with a notably low sliding angle of 1.15°. PTL-mediated adhesion fortifies the silicone oil attachment to the substrate, ensuring the retention of its repellent efficacy amidst mechanical stressors like ultrasonication, water scrubbing, and centrifugation. The integration of robust adhesion, cross-substrate compatibility, and durability under stress affords the PTL-modified SLIPS exceptional anti-fouling, anti-icing, and anti-corrosion properties, marking it as a leading solution for advanced protective applications.

研究领域: 材料科学 · 生物化学 · 表面工程
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LANGMUIR · 2021 · IF 3.882

Self-Healing Silicone Elastomer with Stable and High Adhesion in Harsh Environments

Shengping Dai,Meng Li,Hao Yan,Hao Zhu,Hongwei Hu,Yixing Zhang,Guanggui Cheng,Ningyi Yuan,Jianning Ding

Adhesive and self-healing elastomers are urgently needed for their convenience and intelligence in biological medicine, flexible electronics, intelligent residential systems, etc. However, their inevitable use in harsh environments results in further enhancement requirements of the structure and performance of adhesive and self-healing elastomers. Herein, a novel self-healing and high-adhesion silicone elastomer was designed by the synergistic effect of multiple dynamic bonds. It revealed excellent stretchability (368%) and self-healing properties at room temperature (98.1%, 5 h) and in a water environment (96.4% for 5 h). Meanwhile, the resultant silicone elastomer exhibited high adhesion to metal and nonmetal and showed stable adhesion in harsh environments, such as under acidic (pH 1) and alkaline (pH 12) environments, salt water, petroleum ether, water, etc. Furthermore, it was applied as a shatter-proof protective layer and a rust-proof coating, proving its significant potential in intelligent residential system applications.

研究领域: 材料科学 · 生物医学工程 · 柔性电子
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Journal of the Australian Ceramic Society · 2023 ·Vol. 59 ·期 4 ·915-922 · IF 1.9

Achieving high stability and anti-adherence performance of ZrO2 ceramic product via hydrophobic modified surface

Zhang Jianxiong

ZrO 2 is widely used. However, surface hydrophilicity is harmful to waterproof devices. In this work, epoxy-based polyhedral oligomeric silsesquioxane (POSS) was chemically bonded to ZrO 2 sheet surface for weather-resistant hydrophobicity and anti-adherence property. First, ZrO 2 sheet was modified with hydroxyls, followed by amino modification. Then, surface POSS modification was performed via ring-opening addition. Next, composition and micro-morphology of POSS-treated sheet were clarified. Ultimately, the dependence of water contact angle of POSS-modified sheet on POSS solution treating time was researched, and the highest contact angle of 132.6° was gained by 24-h treating. Acid corrosion, alkali corrosion, and ultraviolet radiation for 48 h were employed to verify good weather resistance with contact angles over 120°. POSS-modified sheet had good anti-adherence capacity. Cooperation of POSS and ZrO 2 was utilized to obtain low surface energy and high surface roughness. This work might help to obtain hydrophobic ceramics as catalyst supports for oil-phase reactions.

研究领域: 材料科学 · 表面化学
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ACS Applied Materials & Interfaces · 2021 · IF 9.229

Folic Acid-Based Coacervate Leading to a Double-Sided Tape for Adhesion of Diverse Wet and Dry Substrates

Shuitao Gao,Wenkai Wang,Tongyue Wu,Shasha Jiang,Jinwan Qi,Zhiyang Zhu,Bin Zhang,Jianbin Huang,Yun Yan

Adhesives are crucial both in nature and in diversified artificial fields, and developing environment-friendly adhesives with economic procedures remains a great challenge. We report that folic acid-based coacervates can be a new category of excellent adhesives for all kinds of surfaces with long-lasting adhesiveness. Aided by the electrostatic interaction between the π–π stacked folic acid quartets and polycations, the resultant coacervates are able to interact with diversified substrates via a polyvalent hydrogen bond, coordination, and electrostatic interactions. The adhesivity to wood is superior to the strong commercial glues, but without releasing any toxic components. Upon evaporating water, the coacervate can be casted into a non-adhesive flexible self-supporting film, which restores the adhesive coacervate immediately on contacting water with original adhesive ability. In this way, the coacervate can be facilely tailored into a double-sided tape (DST), which is convenient for storage and application under ambient conditions. Given its excellent adhesive performance, release of nontoxic gases, and convenience in storage and application, the folic acid-based DST is very promising as a new adhesive material.

CAS / MDL: 26062-79-3
研究领域: 材料科学 · 生物化学
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ACS Applied Materials & Interfaces · 2019 · IF 8.456

Adhesive Tough Magnetic Hydrogels with High Fe3O4 Content

Xiaocheng Hu,Guodong Nian,Xueya Liang,Lei Wu,Tenghao Yin,Haotian Lu,Shaoxing Qu,Wei Yang

Magnetic hydrogels have promising applications in flexible electronics, biomedical devices, and soft robotics. However, most existing magnetic hydrogels are fragile and suffer insufficient magnetic response. In this paper, we present a new approach to fabricate a strong, tough, and adhesive magnetic hydrogel with nontoxic polyacrylamide (PAAm) hydrogel as the matrix and the functional additive [3-(trimethoxysilyl)propyl methacrylate coated Fe3O4] as the inclusions. This magnetic hydrogel not only offers a relatively high modulus and toughness compared to the pure hydrogel but also responds to the magnetic field rapidly because of high magnetic particle content (up to 60%, with respect to the total weight of the polymers and water). The hydrogel can be bonded to hydroxyl-rich hard and soft surfaces. Magnetic hydrogel with polydimethylsiloxane (PDMS) coating exhibits excellent underwater performance. The bonding between magnetic hydrogel and PDMS is very stable even under cyclic loading. An artificial muscle and its magnetomechanical coupling performance are demonstrated using this hydrogel. The adhesive tough magnetic hydrogel will open up extensive applications in many fields, such as controlled drug delivery systems, coating of soft devices, and microfluidics. The strategy is applicable to other functional soft materials.

CAS / MDL: 79-06-1
研究领域: 材料科学 · 生物医学工程 · 软体机器人技术
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CHEMISTRY OF MATERIALS · 2023 · IF 8.6

Graphene/Polyolefin Elastomer Films as Thermal Interface Materials with High Thermal Conductivity, Flexibility, and Good Adhesion

Xin Sun,Zheng-Yi Wang,Yang Wang,Xiang-Yun Du,Ji-Dong Liu,Cheng Zhang,Weili Li,Zheng-Bai Zhao

Heat dissipation has become a central issue for the development of the microelectronic industry. Thermal interface materials (TIMs) have been widely applied to electron component cooling, which is used to bond the heat spreader and the chip together. Most research on TIMs has only dealt with thermal conductivity enhancement. However, the mechanical properties and adhesion of TIMs are indispensable for practical applications, as well as postcleaning to remove TIMs. A graphene nanosheet/polyolefin elastomer (GNP/POE) film was designed and prepared by a facile method, in which the heat conduction paths were efficiently constructed, and the good mechanical properties of POE were reserved. The thermal conductivity of as-prepared GNP/POE film can reach 1.07 W m–1 K–1 at an extremely low filler loading of 0.62 wt %. Furthermore, the tensile strength, elongation at break, and adhesion of the prepared GNP/POE film are as good as those of commercial TIM productions. The prepared GNP/POE film can be used as TIMs for chip cooling and exhibits a good heat dissipation effect. Additionally, the prepared GNP/POE film can be peeled off from the chip without residue, after the chip has finished running, which is significant for practical production. This work provides valuable information and insight into the design and fabrication of TIMs in the future.

研究领域: 材料科学 · 热管理技术
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2022 · IF 8.025

Robust and adhesive lignin hybrid hydrogel as an ultrasensitive sensor

Huijuan Xiu,Haizhi Zhao,Lei Dai,Jingyu Li,Zhi Wang,Yuxin Cui,Yurou Bai,Xinyi Zheng,Jinbao Li

The fabrication of hydrogel for sensing purposes remains to be a challenge since the hydrogel needs to have both good mechanical strength and adhesiveness. This work reports a robust and adhesive hydrogel mainly constructed with AgNPs@lignin, polyacrylamide (PAM) and sodium alginate (SA). The silver nanoparticles (AgNPs) were in-situ generated via the reaction between lignin and silver ammonia ([Ag(NH 3 ) 2 ] + ). The resultant lignin hybrid hydrogel exhibited a stress, strain and tearing energy up to 0.055 MPa, 1000% and 250 J·m −2 , respectively. Furthermore, the hydrogel adhered to different materials with an adhesion energy of higher than 230 J·m −2 . This hydrogel was demonstrated to be an ideal sensing material since it could detect both large-scale motions and tiny physiological signals including breathing and pulse. The hydrogel also exhibited good antibacterial performance and biocompatibility. This work provides a good example to design a lignin-based high-performance hydrogel material for sensing purposes.

研究领域: 材料科学 · 生物医学工程
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