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BIOMACROMOLECULES · 2019 · IF 5.667

Injectable and Near-Infrared-Responsive Hydrogels Encapsulating Dopamine-Stabilized Gold Nanorods with Long Photothermal Activity Controlled for Tumor Therapy

Jinfeng Zeng,Dongjian Shi,Yanglin Gu,Tatsuo Kaneko,Li Zhang,Hongji Zhang,Daisaku Kaneko,Mingqing Chen

Gold nanorods (AuNRs) are confirmed to have excellent and repeated photothermal properties under near-infrared (NIR)-light irradiation above 780 nm. However, AuNRs easily leaked out from local pathological tissues and circulated in the body, reducing photothermal therapy (PTT) efficacy. By complexing AuNRs with a scaffold via interactions, AuNRs might be dispersed in the scaffold and fixed in the tumor site. Thus, based on the mussel-mimetic adhesion concept, AuNRs were designed to be coated with polydopamine (PDA), and then the prepared polydopamine-coated AuNRs (AuNR-PDA) were incorporated into a thermosensitive injectable hydrogel composed of β-glycerophosphate-bound chitosan (CGP) and dopamine-modified alginate (Alg-DA) efficiently. Due to the strong interactions between PDA and polymers, AuNR-PDA could be immobilized stably and evenly into the obtained CGP/Alg-DA/AuNR composite hydrogel, which can avoid overheating locally or leaking out. The sol–gel transition temperature of the composite hydrogel was adjusted to the body temperature at around 37 °C to be conveniently injectable in vivo. With NIR irradiation at 808 nm of wavelength, the composite hydrogel was locally heated quickly to over 50 °C depending on controlling the irradiation powers and times. Moreover, the in vitro cytotoxicity test of the composite hydrogel showed good biocompatibility to normal cells but obvious suppression to tumor cells’ growth under multiple times of photothermal therapy. Furthermore, the in vivo antitumor test demonstrated the obvious suppression to tumor growth of the CGP/Alg-DA/AuNR composite hydrogel under multiple PTTs. Therefore, the injectable CGP/Alg-DA/AuNR hydrogel could be a promising candidate for the long-term repeated photothermal treatment of tumors.

研究领域: 生物材料 · 纳米技术 · 癌症治疗 · 生物医学工程 · 药学
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Frontiers in Robotics and AI · 2021 · IF 0

Fatigue Damage–Resistant Physical Hydrogel Adhesion

Li Qi,Wang Luochang,Liu Qihan,Hong Wei,Yang Canhui

Strong adhesion between hydrogels and various engineering surfaces has been achieved; yet, achieving fatigue-resistant hydrogel adhesion remains challenging. Here, we examine the fatigue of a specific type of hydrogel adhesion enabled by hydrogen bonds and wrinkling and show that the physical interactions–based hydrogel adhesion can resist fatigue damage. We synthesize polyacrylamide hydrogel as the adherend and poly(acrylic acid-co-acrylamide) hydrogel as the adhesive. The adherend and the adhesive interact via hydrogen bonds. We further introduce wrinkles at the interface by biaxially prestretching and then releasing the adherends and perform butt-joint tests to probe the adhesion performance. Experimental results reveal that the samples with a wrinkled interface resist fatigue damage, while the samples with a flat interface fail in ~9,000 cycles at stress levels of 70 and 63% peak stresses in static failure. The endurance limit of the wrinkled-interface samples is comparable to the peak stress of the flat-interface samples. Moreover, we find that the nearly perfectly elastic polyacrylamide hydrogel also suffers fatigue damage, which limits the fatigue life of the wrinkled-interface samples. When cohesive failure ensues, the evolutions of the elastic modulus of wrinkled-interface samples and hydrogel bulk, both in satisfactory agreements with the predictions of damage accumulation theory, are alike. We observe similar behaviors in different material systems with polyacrylamide hydrogels with different water contents. This work proves that physical interactions can be engaged in engineering fatigue-resistant adhesion between soft materials such as hydrogels.

研究领域: 材料科学 · 生物医学工程
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JOURNAL OF MATERIALS RESEARCH · 2015 ·Vol. 30 ·期 11 ·1797-1807 · IF 1.647

Responsiveness, swelling, and mechanical properties of PNIPA nanocomposite hydrogels reinforced by nanocellulose

Yi Chen,Weijian Xu,Wenyong Liu,Guangsheng Zeng

Nanocrystalline cellulose (NCC) whisker obtained from acid hydrolysis of cotton was incorporated into the freezing polymerized PNIPA/clay hydrogels to prepare inorganic–organic hybrid nanocomposite hydrogels (named as C-NC gels). The influence of NCC on the properties of C-NC gels was investigated systematically. It was found that all C-NC gels exhibit similar lower critical solution temperature as that of NCC-free gels, being independent of the NCC content. However, with the increase of NCC content in C-NC gels, the swelling ability of gels decreases slightly while the response rate of gels increases gradually, the gels with high content of NCC exhibit an ultrarapid deswelling rate due to the amount of interconnected micropores appeared inside the gels. Moreover, the enhancement effect of increased NCC on the gels is significant, which is also determined by the swelling degree of gels directly. Comparably, for the gels with the same content of NCC, higher strength was found when the gels were kept in lower swelling ratio due to the stronger interaction of NCC through hydrogen bond in the gels.

研究领域: 高分子材料 · 生物医学工程 · 软物质物理 · 智能响应材料 · 组织工程
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Materials Express · 2020 ·Vol. 10 ·期 12 ·2122-2129 · IF 1.65

High-strength p(HEMA-co-AA) hydrogels with photoluminescence crosslinked by 2-hydroxyethyl methacrylate modified silica/carbon dots colloids

Wei Lai,Wang Jun,Arshad Naila,Wang Jianying

2-Hydroxyethyl methacrylate (HEMA) improved colloids of silica/carbon dots (SiO2/HMCDs) were used by means of new translucent, nontoxic cross-linking centers comprising two non-toxic components, silica colloids and carbon dots. The direct photopolymerization of a mixture of acrylic acid (AA), HEMA, and SiO2/HMCDs afforded ultrahigh strength and mechanically robust hydrogel. The fabricated fluorescent SiO2/HMCDs-based hydrogels demonstrated stable photoluminescence owing to their outstanding mechanical flexibility. Fluorescent hydrogels exhibited tensile strength of up to ∼ 13.2 MPa by processing with 1 wt% SiO2/HMCDs content. More importantly, the mechanical properties (stress or strain) could be changed by controlling the content of SiO2/HMCDs and H2O. Relative hierarchical structure attributed to high mechanical strength.

CAS / MDL: 64-17-5 25952-53-8
研究领域: 材料科学 · 生物医学工程 · 化学工程
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Soft Matter · 2020 ·Vol. 17 ·期 6 ·1566-1573 · IF 3.14

Tough hybrid microgel-reinforced hydrogels dependent on the size and modulus of the microgels

Chun Li,Xiaohu Zhou,Lifei Zhu,Ziyao Xu,Peng Tan,Haifei Wang,Guokang Chen,Xuechang Zhou

Microgel-reinforced (MR) hydrogels are tough hydrogels with dispersed rigid microgels embedded in a continuous soft matrix. MR gels have the great potential to provide not only mechanical toughness but also the desired functional matrix by incorporation of various functional microgels. Understanding the toughening mechanism of the MR hydrogels is critical for the rational design of the desired functionally tough MR gels. However, our current knowledge of the toughening mechanism of MR gels mainly comes from the MR hydrogels with both chemically crosslinked dispersed microgels and a continuous matrix. Little is known about the hybrid MR gels with physically crosslinked microgels embedded in a chemically crosslinked matrix. Herein, we synthesize such hybrid MR hydrogels with the ionic crosslinked calcium alginate microgels incorporated into the chemically crosslinked polyacrylamide (PAAm) matrix. The alginate microgels show strong size and modulus effects on the toughening enhancement: the larger microgels could toughen the MR gels more than the small ones, and the microgels with medium modulus could maximize the toughness of the MR gels. By comparison of the mechanical performances of the MR and the corresponding double network (DN) hydrogels, we have proposed that the hybrid MR gels may have the same toughening mechanism as the bulk DN gel. This work tries to better understand the structure–property relationships of both MR and DN gels and help in the design of more functionally tough MR gels with the desired properties.

CAS / MDL: 9005-38-3
研究领域: 材料科学 · 生物医学工程
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Polymers · 2019 ·Vol. 11 ·期 10 ·1564 · IF 3.164

Smart Composite Hydrogels with pH-Responsiveness and Electrical Conductivity for Flexible Sensors and Logic Gates

Tong Wang,Xuan Zhang,Zichao Wang,Xiuzhong Zhu,Jie Liu,Xin Min,Tao Cao,Xiaodong Fan

Stimuli-responsive conductive hydrogels have a wide range of applications due to their intelligent sensing of external environmental changes, which are important for smart switches, soft robotics, and flexible sensors. However, designing stimuli-responsive conductive hydrogels with logical operation, such as smart switches, remains a challenge. In this study, we synthesized pH-responsive conductive hydrogels, based on the copolymer network of acrylic acid and hydroxyethyl acrylate doped with graphene oxide. Using the good flexibility and conductivity of these hydrogels, we prepared a flexible sensor that can realize the intelligent analysis of human body motion signals. Moreover, the pH-responsive conductive hydrogels were integrated with temperature-responsive conductive hydrogels to develop logic gates with sensing, analysis, and driving functions, which realized the intellectualization of conductive hydrogels.Keywords:stimuli-responsive conductive hydrogels;pH-responsive;composite hydrogels;flexible sensors;logic gates

CAS / MDL: 62-53-3 868-77-9 83-86-3
研究领域: 材料科学 · 生物医学工程
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ACS Applied Materials & Interfaces · 2016 · IF 7.145

Self-Propelling Hydrogel/Emulsion-Hydrogel Soft Motors for Water Purification

Hui Wang,Xiaoyu Gu,Chaoyang Wang

We fabricate a kind of catalytic self-propelling hydrogel soft motor (H-motor) via a facile injection loading method with low energy consumption. The factors influencing the practicability of H-motors, including locomotive ability and reusability, are investigated. The succession of rapid bubble evolution and propulsion endows the millimeter-sized columnar H-motors with length/diameter of 1 a remarkable speed of 3.84 mm s–1 in 10% (w/w) hydrogen peroxide (H2O2) solution. Moreover, the H-motors maintain undiminished propulsion capability and functionality even after repeated loading for 6 times. Additionally, we also fabricate emulsion-hydrogel soft motors (E-H-motors) templated from the oil/water (O/W) emulsion for the first time, which exhibit a faster speed of 4.33 mm s–1 under the same conditions. It can be ascribed to the additional liberation of low-boiling oil phase stored in the emulsion-hydrogels caused by catalytic reaction heat, which is appropriate for larger propulsive situations. The stabilized, efficient, and reusable H-motors are selected for industrial effluents purification to fit the imperious demands about the disposal of organic pollutants in water. The synergy effect between catalytic degradation and enhanced intermixing of the fluid flow around the miniaturized soft motors gives rise to an effective and exhaustive removal of organic contaminants.

CAS / MDL: 110-18-9
研究领域: 材料科学 · 环境科学 · 化学工程
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2023 · IF 8.2

Oral colon-targeted responsive alginate/hyaluronic acid-based hydrogel propels the application of infliximab in colitis

Manxiu Huai,Mingliang Pei,Jiaxing Pan,Yun Zhu,Yingwen Chen,Peng Du,Yanming Duan,Huixiong Xu,Wensong Ge

Currently, commercialized infliximab (IFX) has rapidly propelled the clinical treatment of IBD, however, its inherent attributes, such as off-target effects and rapid metabolism, severely limit practical applications. Moreover, high doses injection of IFX can result in IBD treatment failure, which may induce other side effects. In this study, an colon microenvironment-responsive hydrogel (AL/HA hydrogel), consisting of acid-resistant sodium alginate and colon-degraded and targeted hyaluronic acid, was constructed by simple Ca 2+ /Zn 2+ cross-linking. The ion-mediated hydrogel exhibited the protective effect of gastrointestinal tract to avoid early drug leakage, while the inflammation environments showed well-controlled drug release and significant biodegradable behaviors. Additionally, oral hydrogel exhibited long-standing enteritis areas compared with normal mice. Therefore, hydrogel-assisted enteritis treatment has great potential in IBD as an oral agent. After that, IFX was packaged in hydrogel to fabricate a facile oral antibody delivery system to treat IBD. IFX-embedded hydrogel showed remarkable therapeutic effect on IBD compared with free IFX. Surprisingly, oral hydrogel below 7 times IFX achieve the same amount of IFX-infused treatment that will further help alleviate the drawbacks of IFX. Our work elaborated on the efficacy of oral AL/ [email protected] in IBD, providing a guarantee for the future of promoted clinical transformation.

CAS / MDL: 9011-18-1 81-88-9
研究领域: 药剂学 · 生物医学工程 · 胃肠病学
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Chiral design of tough spring-shaped hydrogels for smart umbrellas

Mingqi Chen,Guangjie Song,Bin Ren,Lin Cai,Mokarram Hossain,Chunyu Chang

Developing hydrogel artificial muscles to mimic the motion of natural muscles has long attracted scientists from the perspective of materials science for potential applications in soft robotics. However, rational design of hydrogel artificial muscles with large stroke, rapid actuation speed, and high work capacity remains a major challenge. Herein, we reported two kinds of chiral spring-shaped hydrogels that were prepared via consecutive shaping process (e.g., stretching, twisting, folding, coiling, and fixing). By switching the chirality of coil, homochiral muscle and heterochiral muscle were obtained, respectively. Homochiral muscle could rapidly expand to 560% with an average speed of 6.7 % s −1 in response to NIR irradiation, whose maximum work capacity reached 45 J kg −1 . On contrary, heterochiral muscle contracted 69% within 1 min under NIR irradiation with a maximum work capacity of 33 J kg −1 . Interestingly, the parasol containing homochiral muscles opened autonomously during dehydration process, while the umbrellas containing heterochiral muscle could opened rapidly when water was applied. This work provided an innovative strategy for developing tough hydrogel muscles with opposite chiralities.

CAS / MDL: 814-68-6
研究领域: 材料科学 · 软体机器人 · 生物仿生学
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European Physical Journal Plus · 2024 ·Vol. 139 ·期 1 ·1-13 · IF 2.8

Stretchable and tough polystyrene hydrogels by introducing polyacrylamide network

Wang Runda,Jiang Zhongying,Yang Fangyuan,Lei Yiteng,Sheng Jie

This study presents a novel category of tough PS-p(AAm-co-MBAA) double network (DN) hydrogels, synthesized through fully chemically cross-linked methods by introducing polyacrylamide network into hydrophobic polystyrene networks. Herein, we obtain the carboxyl-modified polystyrene (CPS) synthesized by polystyrene (PS) using reversible addition–fragmentation chain transfer (RAFT) polymerization, CPS and 4-arm amine poly(ethylene glycol) (4-arm-PEG-NH 2 ) serve as the first chemical cross-linking, providing a brittle and stiff network that allows energy dissipation. Concurrently, the second chemical cross-linking points, created by acrylamide (AAm) and N,N’-methylenebis(acrylamide) (MBAA), impart a ductile and soft network to enhance stretchability. The optimal tough PS-p(AAm-co-MBAA) DN hydrogel displays remarkable properties, including super stretchability (≈5.9 times), tensile strength (≈0.43 MPa), high toughness (≈1.66 MJ m −3 ), good recoverability property (≈94.6% stiffness recovery and ≈88% toughness recovery without any waiting time), and fatigue resistance. This study introduces a novel approach to design and manufacture tough hydrogels with remarkable overall characteristics by employing the collaborative process of RAFT polymerization. Graphical

研究领域: 材料科学 · 高分子化学 · 软物质物理 · 机械工程
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Polymers · 2022 ·Vol. 14 ·期 23 ·5316 · IF 4.967

High Multi-Environmental Mechanical Stability and Adhesive Transparent Ionic Conductive Hydrogels Used as Smart Wearable Devices

Yuxuan Wu,Jing Liu,Zhen Chen,Yujie Chen,Wenzheng Chen,Hua Li,Hezhou Liu

Ionic conductive hydrogels used as flexible wearable sensor devices have attracted considerable attention because of their easy preparation, biocompatibility, and macro/micro mechanosensitive properties. However, developing an integrated conductive hydrogel that combines high mechanical stability, strong adhesion, and excellent mechanosensitive properties to meet practical requirements remains a great challenge owing to the incompatibility of properties. Herein, we prepare a multifunctional ionic conductive hydrogel by introducing high-modulus bacterial cellulose (BC) to form the skeleton of double networks, which exhibit great mechanical properties in both tensile (83.4 kPa, 1235.9% strain) and compressive (207.2 kPa, 79.9% strain) stress–strain tests. Besides, the fabricated hydrogels containing high-concentration Ca2+show excellent anti-freezing (high ionic conductivities of 1.92 and 0.36 S/m at room temperature and −35 °C, respectively) properties. Furthermore, the sensing mechanism based on the conductive units and applied voltage are investigated to the benefit of the practical applications of prepared hydrogels. Therefore, the designed and fabricated hydrogels provide a novel strategy and can serve as candidates in the fields of sensors, ionic skins, and soft robots.Keywords:smart wearable devices;ionic conductive hydrogels;multi-environmental mechanical stability;multifunctional hydrogels

研究领域: 材料科学 · 生物医学工程
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Journal of Materials Chemistry B · 2019 ·Vol. 7 ·期 8 ·1311-1321 · IF 5.047

Magnetic double-network hydrogels for tissue hyperthermia and drug release

Jingda Tang,Yancheng Qiao,Yanhui Chu,Zongfei Tong,Yifan Zhou,Wenlei Zhang,Shejuan Xie,Jian Hu,Tiejun Wang

Magnetic-field driven soft materials have found extensive applications in fields such as soft robotics, shape morphing and biomedicine. Compared to magnetoactive elastomers (MAEs), magnetic hydrogels have shown significant advantages for in vivo applications, because of their better biocompatibility, as well as their soft and wet nature. However, the poor mechanical properties and ion sensitivity of conventional magnetic hydrogels will severely limit their applications especially under physiological conditions. Double network hydrogels are tough and stable, but do not respond to environmental stimuli. Here magnetic double network (M-DN) hydrogels have been developed with outstanding mechanical performances and ion-resistant stability. M-DN hydrogels show a high modulus of ∼0.4 MPa and a high toughness of ∼1500 J m−2. The volume, magnetic and mechanical properties of M-DN hydrogels show negligible deterioration in ionic solutions. M-DN hydrogels exhibit magnetic responsiveness and have been used for tissue hyperthermia and drug release by magnetic induction heating. The induction heating behavior of M-DN hydrogels can be tuned to meet the clinical requirements, by changing the magnetic field strength or the composition of magnetic hydrogels. M-DN hydrogels may be inspiring to the development of responsive DN hydrogels and expand their more potential applications in load-bearing biomedical engineering.

研究领域: 生物医学工程 · 软体机器人技术 · 响应性材料 · 转化医学 · 肿瘤治疗
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