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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2024 · IF 7.7

Sustainable chitin-derived elastomers via grafting strategy with tunable mechanical and adhesion properties

Yuxian Xing,Yi Wei,Chongxiao Ge,Rui Hu,Yaqiong Zhang,Baoxia Wang,Zhiqiang Wang,Feng Jiang

With increasing environmental awareness and the pursuit of sustainable development goals, environmentally friendly sustainable thermoplastic elastomers (TPEs) derived from natural resources are highly desired to replace traditional TPEs. However, preparing sustainable TPEs with high mechanical properties and multifunctionality from biobased feedstocks remains a significant challenge. In this work, a series of chitin- graft -poly(acrylamide- co -2-ethylhexyl acrylate) (Chitin- g -P(AM- co -EHA)) copolymers were synthesized through reversible addition-fragmentation chain transfer (RAFT) polymerization. The tensile strength of Chitin- g -P(AM- co -EHA) copolymers can be tuned over a wide range from 1.0 to 7.3 MPa by adjusting the chitin and PAM contents. Benefiting from the brush-like architecture, Chitin- g -P(AM- co -EHA) copolymer exhibits improved mechanical properties over its linear counterparts. Moreover, these Chitin- g -P(AM- co -EHA) copolymers show good adhesion performance on different substrates. The shear strength can achieve 7.5 MPa for Chitin0.8-PAM50, which is high enough for commercial applications. The combination of chitin and grafting strategy can promote the development of strong chitin-based sustainable elastomers. This approach can be further utilized to design novel high-performance biobased elastomers and adhesives derived from natural resources.

研究领域: 材料科学 · 生物化学
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JOURNAL OF APPLIED POLYMER SCIENCE · 2025 · IF 2.8

Colorimetric Dye-Loaded, Adhesive, and Stretchable Hydrogel Sensor: A Sensitive and Visible H2S Gas Sensing Platform

Leixin Liu,Shanshan Yuan,Chenxi Guan,Jian Zhou,Yi Yao,Qiliang Zhang,Fangli Gang

Hydrogen sulfide (H 2 S), as a toxic gas, is one of the occupational hazards to workers' health. Traditional H 2 S sensors often suffer from external circuits, measurement systems, liquid-phase reactions, or high detection limits. Herein, a colorimetric sensor for H 2 S detection was developed by incorporating colorimetric dye [lead acetate, Pb(OAc) 2 ] into polyacrylamide (PAM)/polyvinyl alcohol (PVA) hydrogel. Benefitting from the interpenetrating polymer network, non-covalent interactions such as hydrogen bonds and dense internal structure, the hydrogel exhibited excellent adhesion to different substances (adhesion strength up to 14.11 kPa) and mechanical properties (tensile strength up to 116.92 kPa, elongation rate up to 576%). Furthermore, due to the liquid-phase reaction system and excellent [Pb(OAc) 2 ] loading capacity provided by the hydrogel, the prepared sensors exhibited excellent sensing performance response time, sensitivity, and simplicity. The theoretical detection limit of the sensor was 0.69 ppm, and the minimum exposure time required for detection was 14 s. The colorimetric effect of the hydrogels was positively correlated with the addition of Pb(OAc) 2 and the extension of time. The results showed that the color change of PAM/PVA/Pb(OAc) 2 hydrogel can be visible to the naked eye even if the concentration of H 2 S is only 1 ppm. It is expected that this hands-free, arbitrarily adhesive, stretchable hydrogel colorimetric sensor strategy for visual detection of H 2 S will extend toxic gas alarm systems to a new level.

研究领域: 材料科学 · 环境科学 · 生物医学工程
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CARBOHYDRATE POLYMERS · 2022 · IF 10.723

Ultrastretchable and adhesive agarose/Ti3C2Tx-crosslinked-polyacrylamide double-network hydrogel for strain sensor

Tingrui Lin,Shuangxiao Li,Yang Hu,Lang Sheng,Xibang Chen,Xueyan Que,Jing Peng,Huiling Ma,Jiuqiang Li,Maolin Zhai

A novel agarose/Ti 3 C 2 T x -crosslinked-polyacrylamide (AG/T-PAM) double-network (DN) hydrogel is synthesized by combining heating-cooling and γ-ray radiation-induced polymerization. The AG/T-PAM DN hydrogel possesses excellent mechanical properties with 4250% stretchability, and good adhesion to different substrates, such as an adhesive strength of 1148 kPa to copper at 30 °C. The resultant hydrogel also exhibits excellent tensile and compression sensing properties due to the variation of conductive network within hydrogel. The flexible and wearable strain sensor composed of the AG/T-PAM DN hydrogel presents rapid response to strain withstand 1000 cycles, and can monitor various movements of human body with a high sensibility. The AG/T-PAM DN hydrogel-based strain sensor will have broad application in large-scale strain detection scenarios requiring high sensitivity and adhesion.

研究领域: 材料科学 · 生物医学工程
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ACS Applied Bio Materials · 2024 · IF 4.6

Mucoadhesive Thiolated Hyaluronic Acid/Pluronic F127 Nanogel Formation via Thiol–Maleimide Click Reaction for Intravesical Drug Delivery

Fayang Li,Xianhuang Chen,Yuanqiao He,Zhiping Peng

The development of nanocarriers to prolong the residence time and enhance the permeability of chemotherapeutic drugs on bladder mucosa is important in the postsurgery treatment of superficial bladder cancers (BCs). Here, the mucoadhesive HA-SH/PF127 nanogels composed of a temperature-sensitive Pluronic F127 (PF127) core and thiolated hyaluronic acid (HA-SH) shell were prepared by the emulsification/solvent evaporation method. The nanogels were constructed through the thiol-maleimide click reaction in the HA-SH aqueous side of the oil–water interface and self-oxidized cross-linking thiols between HA-SH. The HA-SH/PF127 nanogels prepared at different thiol-to-maleimide group molar ratios, water-to-oil volume ratios, and cross-linking reaction times were characterized regarding hydrodynamic diameter (Dh) and zeta potential (ζ), and the optimal formulation was obtained. The excellent mucoadhesive properties of the HA-SH/PF127 nanogels were evaluated by using the mucin particle method. Doxorubicin (DOX) was encapsulated in the PF127 core of DOX@HA-SH/PF127 nanogels with a high loading efficiency (87.5%) and sustained release from the nanogels in artificial urine. Ex vivo studies on porcine bladder mucosa showed that the DOX@HA-SH/PF127 nanogels enhanced the penetration of the DOX into the bladder mucosa without disrupting the mucus structure or the bladder tissue. A significant dose-dependent cytotoxic effect of DOX@HA-SH/PF127 nanogels on both T24 and MB49 cells was observed. The present study demonstrates that the mucoadhesive HA-SH/PF127 nanogels are a promising intravesical drug delivery system for superficial BC therapy.

研究领域: 药剂学 · 肿瘤学 · 生物材料
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JOURNAL OF APPLIED POLYMER SCIENCE · 2025 · IF 2.8

Preparation and Performance Evaluation of Nucleobase-Mediated Hydrogels Based on Hybrid Crosslinking

Qihai Wang,Zhifeng Luo,Xiaoli Ren,Haoran Fu,Quan Zhou,Keyou Chen,Shenwen Fang

Adhesive hydrogels frequently demonstrate poor mechanical properties; therefore, it is still challenging to integrate excellent adhesiveness and self-healing properties in one hydrogel. In this work, adenine and thymine were modified by grafting double bonds and then introduced into the structure of the polyacrylamide gel together with N, N′-methylene bisacrylamide (MBA) using a hybrid crosslinking strategy, and then a series of hybrid cross-linked hydrogels with adhesiveness and self-healing properties were successfully prepared. The hybrid crosslinking hydrogel exhibited a tunable adhesive performance and strength, by varying the content of base pairs, monomer concentration, cross-linker concentration, and initiator concentration. The recommended synthesis conditions for the P(AM-mAT) hydrogel were as follows: mA-mT concentration of the total monomer weight 5 wt%, total monomer concentration of 25 wt%, crosslinker (MBA) concentration of 0.5 wt%, and initiator APS concentration of 1.25 wt%. Under optimal conditions, the gel synthesized showed a hardness of 282 g and an adhesive force of 154.5 g. This hydrogel material exhibited excellent adhesion properties to materials such as plastics, glass, metals, and wood, with the best adhesion observed on glass.

研究领域: 材料科学 · 生物化学
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ACS Applied Polymer Materials · 2024 · IF 4.4

Polyethylene Glycol-Based Conductive Hydrogels with Anti-Freezing, Water Retention and Self-Adhesion for Flexible Sensors

Yangengchen Zhong,Mingjie Liu,Chuyang Xiang,Yeying Lin,Youjun Guan,Kunyu Ren,Chengyun Ning,Lei Zhou,Limin Lu,Rumin Fu,Guoxin Tan

Conductive hydrogels are characterized by their extraordinary stretchability, flexibility, and biocompatibility, making them ideal materials for flexible wearable sensors. However, they often encounter challenges such as freezing and water loss, which can adversely affect their conductivity and stretching performance. In this study, we introduce a conductive hydrogel incorporating polyethylene glycol (PEG), acrylic acid (AA), acrylamide (AM), and lithium chloride (LiCl), which exhibits low-temperature tolerance, resistance to drying, self-adhesion, and mechanical robustness. The hydrogel’s excellent mechanical properties, including an elongation at break of 1120% and a toughness of 2.9 MJ m–3, are attributed to the formation of a tight polymer network between P(AA-AM) and PEG through hydrogen bonding. The multiple hydrogen bonding system between PEG and the polymer networks, combined with the hydration of LiCl and electrostatic interactions between the carboxyl group and Li+, significantly enhances the hydrogel’s freezing resistance (down to −60 °C), water retention (with only 20% water loss after 15 days), and self-adhesion (with an adhesion strength to pig skin of up to 55.08 kPa). When employed as a flexible sensor, the P(AA–AM)/PEG/LiCl hydrogel exhibited excellent sensing properties for monitoring various human motions, with an impressive gauge factor of 1.91 and electrical conductivity of 4.50 S m–1 Moreover, it maintained a high electrical conductivity (3.82 S m–1) even at −20 °C. The conductive hydrogel consistently produced stable and reliable electrical signals in response to external mechanical stimuli, making it a preferred material for human motion monitoring.

研究领域: 材料科学 · 生物医学工程
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Advanced Healthcare Materials · 2024 · IF 10

Injectable Bioadhesive Photocrosslinkable Hydrogels with Sustained Release of Kartogenin to Promote Chondrogenic Differentiation and Partial-Thickness Cartilage Defects Repair

Qian Han,Jiahui He,Lang Bai,Ying Huang,Baojun Chen,Zhenlong Li,Meiguang Xu,Qiaonan Liu,Shuai Wang,Nuanyang Wen,Jing Zhang,Baolin Guo,Zhanhai Yin

Partial-thickness cartilage defect (PTCD) is a common and formidable clinical challenge without effective therapeutic approaches. The inherent anti-adhesive characteristics of the extracellular matrix within cartilage pose a significant impediment to the integration of cells or biomaterials with the native cartilage during cartilage repair. Here, an injectable photocrosslinked bioadhesive hydrogel, consisting of gelatin methacryloyl (GM), acryloyl-6-aminocaproic acid- g -N-hydroxysuccinimide (AN), and poly(lactic- co -glycolic acid) microspheres loaded with kartogenin (KGN) (abbreviated as GM/AN/KGN hydrogel), is designed to enhance interfacial integration and repair of PTCD. After injected in situ at the irregular defect, a stable and robust hydrogel network is rapidly formed by ultraviolet irradiation, and it can be quickly and tightly adhered to native cartilage through amide bonds. The hydrogel exhibits good adhesion strength up to 27.25 ± 1.22 kPa by lap shear strength experiments. The GM/AN/KGN hydrogel demonstrates good adhesion, low swelling, resistance to fatigue, biocompatibility, and chondrogenesis properties in vitro. A rat model with PTCD exhibits restoration of a smoother surface, stable seamless integration, and abundant aggrecan and type II collagen production. The injectable stable adhesive hydrogel with long-term chondrogenic differentiation capacity shows great potential to facilitate repair of PTCD.

CAS / MDL: 60-32-2
研究领域: 生物医学工程 · 组织工程 · 再生医学
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Advanced Healthcare Materials · 2024 ·Vol. 13 ·期 19 ·2304444 · IF 10

Nature-Inspired Gelatin-Based Adhesive Hydrogel: A Rapid and User-Friendly Solution for Hemostatic Applications

Haihua Wang,Mengxi Wang,Jingheng Wu,Shilei Zhu,Yanan Ye,Yushan Liu,Ke Li,Ruyue Li,Yuhang Zhang,Meng Wei,Xin Yang,Leixin Meng

Conventional hemostatic agents face challenges in achieving rapid hemostasis and effective tissue repair due to limited hemostatic scenarios, suboptimal efficacy, and inadequate adhesion to wet tissues. Drawing inspiration from nature-sourced materials, a gelatin-based adhesive hydrogel (AOT)  is designed, easily prepared and quick to form, driven by Schiff base and multiple hydrogen bonds for applications in arterial and liver bleeding models. AOT exhibits exceptional adhesion to wet tissues (48.67 ± 0.16 kPa) and displays superior hemostatic properties with reduced blood loss and hemostatic time compared to other hydrogels and conventional hemostatic materials. Moreover, AOT exhibits good biocompatibility and biodegradability. In summary, this easily prepared adhesive hydrogel has the potential to supplant traditional hemostatic agents, offering a novel approach to achieve swift sealing of hemostasis and facilitate wound healing and repair in broader application scenarios, owing to its unique advantages.

CAS / MDL: 9004-61-9 7790-28-5
研究领域: 生物材料学 · 医学工程 · 创伤修复
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Journal of Materials Chemistry A · 2025 · IF 9.5

Mussel-inspired Strong and Tough Hydrogel with Self-adhesive based on Dynamic Interactions for Flexible Wearable Electronics

Xiaoyong Zhang,Fan Li,Zhaozhao Li,Yongping Bai

Emerging conductive hydrogels showcase profound potential for sophisticated manipulation and various sensing applications. However, it is still challenging to prepare conductive hydrogel materials with the integration of mechanically tough, reliable healability, and high adhesion strength for skin comfort. Inspired by the robust adhesive mechanisms of mussel proteins, we present an innovative adhesive hydrogel (PVA-DBA) with exceptional adhesive properties, elasticity, and self-healing capability, achieved through the integration of PVA-DOPA copolymer and Fe³⁺ ions within a PAM-PAA hydrogel. The DOPA groups confer strong interfacial adhesion, yielding an adhesion strength of 63.0 kPa on porcine skin (simulate human skin) under ambient conditions, with repeatable use across 6 cycles without residual interfacial traces. The catechol-carboxyl interactions, enhanced by Fe³⁺ coordination, impart the hydrogel with high tensile strength, stretchability, and toughness while accelerating gelation kinetics. The unique structural composition provides multiple functional groups (-NH₂, -COOH, and catechol), collectively reinforcing mechanical stability and self-healing performance, achieving an impressive strain self-repair rate of 81.2%. The resultant PVA-DBA hydrogel demonstrates both mechanical robustness and adhesive functionality, along with sensitive conductivity, making it highly suitable for integration into sensing devices that detect bodily motions such as finger, elbow, and knee bending, with a response time of 400 ms. Furthermore, this hydrogel shows potential in sports applications, effectively recording stretching and bending movements, marking a significant advancement in the development of intelligent and responsive material systems.

研究领域: 材料科学 · 生物医学工程 · 化学工程
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CARBOHYDRATE POLYMERS · 2025 · IF 12.5

Ultrafast self-gelling, superabsorbent, and adhesive chitosan-based hemostatic powders for rapid hemostasis and wound healing

Ashuang Liu,Shengyong Cui,Lei Song,Xiangshu Guo,Zhimao Huang,Shancan Wang,Kai Cheng,Ying Xiao,Youfen Fan,Rong Wang

Hemostatic powders are widely used for managing bleeding from wounds with various irregular shapes. However, their limited liquid absorption capacity and difficulty in removal after application remain significant clinical challenges. Herein, we introduce a multifunctional hemostatic powder composed of dually crosslinked poly([2-(methacryloyloxy)ethyl]trimethylammonium chloride- co -acrylic acid) (pMATC- co -AA) and N -[(2-hydroxy-3-trimethylammonium)propyl] chitosan chloride (HTCC), which are integrated via electrostatic interactions and hydrogen bonding. This hemostatic powder exhibits superb liquid-absorbing capacity (94.5 times its own weight in water and 9.1 times in blood), sufficient adhesive properties (5.9 kPa on pig skin), and on-demand removability. It significantly reduces the number of viable Escherichia coli and Staphylococcus aureus by 4.61 and 4.04 orders of magnitude, respectively, thus providing an effective microbiological barrier for the wound. Furthermore, a series of in vivo and in vitro experiments confirm the powder's excellent hemostatic properties. The hydrogel formed on the wound after hemostasis can be removed by saline rinsing on demand, due to its superb liquid-absorbing capacity. Notably, the powder demonstrates good in vivo biocompatibility, with minimal risk of impeding wound healing, and it facilitates the healing process during the later stages. In sum, the hemostatic powder offers a promising solution for trauma bleeding control and acute wound treatment.

研究领域: 生物医学工程 · 材料科学 · 创伤治疗
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APPLIED SURFACE SCIENCE · 2024 · IF 6.3

Fluorosilane emulsifying chlortrifluoroethylene ternary copolymerization design towards strong adhesion, anti-corrosion, fluorescent waterborne fluorocarbon coatings for tinplate substrate

Yi Wu,Shuqi Qiao,Jiawei Wu,Chen Zhou,Cheng Zhao,Zhicheng Pan,Jinfeng Yuan,Kai Han,Mingwang Pan

Waterborne fluorinated ethylene and vinyl ether copolymer (FEVE) coatings are progressively replacing solvent-based FEVE coatings because of their environmental friendliness. However, their practical application is limited due to the poor adhesion, waterproofing, and corrosion resistance, as well as the environmentally unfriendly nature of the small emulsifiers used. Here, a novel waterborne FEVE coating with excellent adhesion, anti-corrosion, and fluorescent properties was developed using amphiphilic fluorosilane oligomer (PFSQ) as microreactors and chlorotrifluoroethylene (CTFE), isobutyl vinyl ether (IBVE), and glycidyl methacrylate (GMA) as copolymer monomers. The introduction of fluorosilane significantly enhances the hydrophobicity of the coating (the water contact angle increased from 69.3 ± 2.4° to 131.4 ± 1.1°). The epoxy groups in the GMA units of terpolymer facilitate bonding of the coating to the substrate, enhancing the adhesion of the coating to the tinplate substrate (the lap shear strength increased from 0.47 ± 0.04 to 0.92 ± 0.01 MPa). Moreover, the interaction between the epoxy groups of GMA and the silicon hydroxyl groups of PFSQ in the synergistic network leads to the intrinsic luminescence of the coating. In addition, the coating exhibits superior corrosion resistance. The molecular structure design provides a new idea for the development of multifunctional waterborne FEVE coating.

研究领域: 材料科学 · 表面工程 · 化学工程
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POLYMER INTERNATIONAL · 2024 · IF 2.9

Silicone-containing polyurea elastomer possessing main-chain boron–oxygen bonds with delayed stress relaxation and improved adhesive properties

Shilong Zhang,Youhao Xiong,Yangwei Wang,Yuqi Ma,Jialiang Li,Chaobo Jiang,Ce Wang,Yanling Zhu,Yongsheng Zhao,Guangcheng Zhang

Polyurea (PU) elastomers have attracted considerable attention in the field of protective polymeric coatings. In this work, a dithiol-terminated boronic ester was synthesized and used to incorporate dynamic boron–oxygen (B–O) bonds in the PU main chain based on thiol isocyanate while amino-terminated polydimethylsiloxane (PDMS) was introduced to retain good chain flexibility. The modified PU elastomer was found to have a microphase-separated structure in which the hard blocks served as physical crosslinks. The glass transition temperature ( T g ) slightly increases when dynamic B–O bonds exist while further introduction of PDMS soft segment can lower T g to −55.63 °C. The introduction of dynamic B–O bonds and diminished hydrogen bonding led to a decrease in mechanical strength and elongation at break. Interestingly, the simultaneous incorporation of PDMS and dynamic B–O bonds is favorable for strain rate dependence and suppressing stress relaxation. The potential for bond-exchange interactions between the dynamic B–O bonds and hydroxyl groups on metal surfaces substantially improved the adhesion of the PU elastomer to metal substrates. Therefore, our work can offer valuable insights for the structural design of functional PU coatings tailored for anti-impact applications. © 2024 Society of Chemical Industry.

研究领域: 材料科学 · 聚合物化学
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