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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2024 · IF 7.7

Facile fabrication of temperature/pH dual sensitive hydrogels based on cellulose and polysuccinimide through aqueous amino-succinimide reaction

Chunwang Hu,Hongliang Wei,Hongli Chen,Bing Zhang,Wenjing Zhang,Gang Wang,Tao Guo

A temperature/pH dual sensitive hydrogel with a semi-interpenetrating network (semi-IPN) structure was synthesized through an aqueous amino-succinimide reaction between water-soluble polysuccinimide and polyethyleneimine in the presence of thermosensitive cellulose derivatives. Single-factor experiments were carried out to optimize the preparation conditions of the semi-IPN hydrogel. The swelling behavior and cytotoxicity assay of the hydrogel were tested. Finally, taking 5- fluorouracil (5-Fu) as a model drug, the release performance of the 5-Fu-loaded hydrogel was investigated. The results indicated that the swelling ratio (SR) first decreased and then increased when the pH of the solutions ascended from 2 to 10. The SR decreased with the increase in temperature. In addition, the swelling behavior of the hydrogel was reversible and reproducible under different pH values and temperatures. The prepared hydrogels had good cytocompatibility. The release behavior of 5-Fu was most consistent with the Korsmeyer-Peppas model and followed the case II diffusion. The acidic environment was beneficial for the release of 5-Fu. The preparation process of the semi-IPN hydrogel is simple and the reaction can proceed quickly in water. The strategy introduced here has great potential for application in the preparation of drug carriers.

CAS / MDL: 9004-65-3
研究领域: 材料科学 · 高分子化学 · 药学
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ACS Applied Bio Materials · 2019 · IF 0

Super Hydrophilic Semi-IPN Fluorescent Poly(N-(2-hydroxyethyl)acrylamide) Hydrogel for Ultrafast, Selective, and Long-Term Effective Mercury(II) Detection in a Bacteria-Laden System

Dong Zhang,Yingchun Yao,Jiahui Wu,Iryna Protsak,Wei Lu,Xiaomin He,Shengwei Xiao,Mingqiang Zhong,Tao Chen,Jintao Yang

Convenient, low-cost chemosensors for hazardous mercury ion detection have been receiving more and more attention in recent studies. However, most of these practical studies are based on an ideal sterile detecting atmosphere and ignore the role of bacteria in actual Hg(II) analytes. Herein, we demonstrate a new type of hydrophilic semi-IPN fluorescent polyHEAA hydrogel chemosensors fabricated by UV polymerization in situ interpenetrating fluorescent polymer PA-NDBCB with a polyHEAA network. Because of specific intermolecular interaction, i.e., hydrogen bonding between hydrophilic fluorescent polymer and polyHEAA matrix comprising a distinct semi-IPN structure, the mechanical property of bulk fluorescent hydrogels can be greatly improved over that of pure polyHEAA hydrogels. Moreover, the design of the hydrogel chemosensors rely on the highly efficient cyclization reaction between Hg(II) ions and the thiourea moieties that induce a visible “green-to-blue” fluorescence color change. On account of the hydrophilic porous structures, these hydrogel chemosensors achieve ultrafast, sensitive, selective Hg(II) detection (detection limit of 0.067 μM) and enable facile ratiometric actual detection in real-world aqueous system. Notably, they maintain fluorescence emission and detection property even under long-term coculture in a complex E. coli bacteria-laden environment. This novel strategy could inspire future construction of soft interfaces/fluorescent apparatus for hazardous Hg(II) detection in a complex real-world system.

研究领域: 材料科学 · 环境科学 · 化学
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PROGRESS IN ORGANIC COATINGS · 2023 · IF 6.6

Free-standing interpenetrating PVA-PEGDA films with excellent antifogging performance and mechanical robustness

Xiuxian Gu,Junhui He,Xiaochun Hu

Robust antifogging films have significant potential for a wide range of applications on the surfaces of transparent materials. Nevertheless, currently either their preparation methods are complex or their mechanical properties such as hardness, wear, scrub and water resistance are yet to be improved before they can be applied in practical applications. In this work, we have developed a facile room temperature approach to fabricating free-standing films of excellent antifogging properties and mechanical robustness. Glutaraldehyde (GA) was used to cross-link polyvinyl alcohol (PVA) and ultraviolet (UV) light was applied to initiate polymerization of poly (ethylene glycol) diacrylate (PEGDA), leading to robust interpenetrating networks (IPN). The films also had excellent mechanical properties with pencil hardness up to 8H, Taber wear-resistance up to 10,000 cycles, and sponge scrub resistance up to 300 cycles. The tensile strength and tearing strength of films reached as high as 100 MPa and 700 kN/m, respectively, much higher than those of free-standing films reported so far. This approach may hold great potential for broad application on various substrates, particularly those with low glass transition temperatures (e.g., transparent plastic films). It may expand the possibilities for future applications of free-standing antifogging films for screens, optical lenses and so on.

CAS / MDL: 9002-89-5
研究领域: 材料科学 · 聚合物化学 · 表面工程
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JOURNAL OF APPLIED POLYMER SCIENCE · 2023 ·Vol. 140 ·期 21 ·e53868 · IF 3

Enhancing anti-thermal hysteresis ability, response stability and sensitivity of polymer humidity sensor by in-situ crosslinking curing method

Xuqi Hu,Xueting Yu,Xiaoyan Xiong,Siyi Li,Tao Jin,Yufang Chen

Compared with room temperature, the responsive curve of polymer humidity sensor usually presents a nonlinear shift and distortion at higher temperature conditions, this will sharply decrease the accuracy and working stability of polymer humidity sensor. In this paper, an organic–inorganic cross-linked interpenetrating network (c-IPN) between silocane compounds and acrylic prepolymer resin has been constructed to prepare a c-IPN humidity-sensitive material by in-situ crosslinking reaction. The results shows that the prepared c-IPN polymer humidity sensor shows more sensitive in range of 30–90% RH, with higher linearity coefficient of 0.9996 and lower hysteresis coefficient of 1.25% RH. And the c-IPN polymer humidity sensor exhibits more higher stability at higher temperature than that at room temperature. Meanwhile, the temperature coefficient of the c-IPN polymer humidity sensor can decrease to 0.53% RH/°C, along with temperature hysteresis curve linear coefficient increase to (R 2 = −0.999), when (3-aminopropyl) triethoxysilane is used at dosage of 10 wt.% druing crosslinking reaction. This study presents a feasible practical technical solution for developing novel high-performance polymer humidity-sensitive materials and its humidity sensors at wider temperature range.

CAS / MDL: 1122-58-3
研究领域: 材料科学 · 传感器技术 · 聚合物化学 · 湿度传感技术
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ADVANCED FUNCTIONAL MATERIALS · 2023 ·Vol. 33 ·期 26 ·2300710 · IF 19

Double Cross-Linked Biomimetic Hyaluronic Acid-Based Hydrogels with Thermo-Stimulated Self-Contraction and Tissue Adhesiveness for Accelerating Post-Wound Closure and Wound Healing

Yaodong Zhao,Bingcheng Yi,Jilin Hu,Dongjie Zhang,Guotai Li,Yun Lu,Qihui Zhou

When skin trauma occurs, rapid achievement of the post-wound closure is required to prevent microbial invasion, inhibit scar formation and promote wound healing. To develop a wound dressing for accelerating post-wound-closure and wound healing, a thermo-responsive and tissue-adhesive hydrogel with interpenetrating polymer networks (IPN) is fabricated based on N -dimethylbisacrylamide (NIPAM) and glutaraldehyde (GTA) cross-linked hyaluronic acid (HA). Results not only confirm the thermo-stimulated self-contraction and tissue adhesiveness of the HA-based IPN (PNI-HA), which effectively aids wound closure via mechanical stretch, but also verify the hemocompatibility and cytocompatibility of PNI-HA that tend to accelerate wound healing. In vivo, a mouse model of total skin defect demonstrates that PNI-HA acting as hydrogel sealant significantly achieves the sutureless post-wound-closure at the early stage of wound healing, and then promotes wound healing by reducing inflammatory cells infiltration, promoting angiogenesis as well as reducing collagen deposition. These results indicate that the developed thermo-responsive and tissue-adhesive hydrogel dressing offers a candidate to serve as a tissue sealant for wound healing.

研究领域: 生物材料 · 组织工程 · 伤口愈合 · 生物医学工程
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CHEMICAL ENGINEERING JOURNAL · 2020 · IF 10.652

Fabrication of bio-based amphiphilic hydrogel coating with excellent antifouling and mechanical properties

Guangming Lu,Shu Tian,Jingyu Li,Yongjian Xu,Shuan Liu,Jibin Pu

Antifouling coatings are crucial to protect marine facilities and aquacultures from the damage of microorganisms for long-term serves. However, it is still a challenge to fabricate coating with excellent antifouling performance and superior mechanical stability. Here, we report a bio-based amphiphilic hydrogel coating with excellent antifouling and mechanical properties. The coating was achieved by the in-situ formation of hydrophobic and hydrophilic interpenetrating polymer network (IPN). The hydrophobic part from a synthesized silicon-containing epoxy resin contributes to superior mechanical properties including high tensile strength and excellent adhesion of 5B. While the hydrophilic hydrogel part from the cross-linking of a hydrophilic polymer with AgNPs gives excellent antifouling properties, resist to proteins, bacteria, algae, and other marine organisms. The antifouling performance of the coating was evaluated by the attachment of proteins (BSA-FITC), bacteria ( Escherichia coli and Bacillus subtilis ), and Algae ( Navicula torguatum and Phaeodactylum tricornutum ). The results show that the bio-based amphiphilic hydrogel coating (e.g. SA-1-5) endows surface with excellent resistance to the fouling of proteins, bacteria and microorganisms. The overall antifouling and mechanical properties of the amphiphilic coating was also evaluated by field test in East China Sea from June 3rd 2020 to July 17th 2020 that the bio-based amphiphilic hydrogel coating was intact and almost no marine organisms attached. This work provides a new strategy for the fabrication of bio-based and high-performance antifouling coatings.

研究领域: 材料科学 · 海洋生物学 · 化学工程 · 生物技术
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Acta Biomaterialia · 2023 · IF 9.7

A hydrogel reservoir as a self-contained nucleus pulposus cell delivery vehicle for immunoregulation and repair of degenerated intervertebral disc

Yulin Jiang,Juehan Wang,Dan Sun,Zheng Liu,Lin Qi,Meixuan Du,Jing Wang,Yubao Li,Ce Zhu,Yong Huang,Yueming Song,Limin Liu,Ganjun Feng,Li Zhang

The strategies for modulating the local inflammatory microenvironment to inhibit intervertebral disc degeneration (IVDD) have garnered significant interest in recent years. In this study, we developed a "self-contained" injectable hydrogel capable of storing Mg 2+ while carrying nucleus pulposus (NP) cells, with the aim of inhibiting IVDD through immunoregulation . The hydrogel consists of sodium alginate (SA), poly(N-isopropylacrylamide) (PNIPAAm), silicate ceramics (SC), and NP cells. When injected into the NP site, PNIPAAm gelates instantly under body temperature, forming an interpenetrating network (IPN) hydrogel with SA. Ca 2+ released from the SC can crosslink the SA in situ , forming a SA/PNIPAAm hydrogel with an interpenetrating network (IPN) encapsulating the NP cells. Moreover, inside the hydrogel, Mg 2+ released from SC are effectively encapsulated and maintained at a desirable concentration. These Mg 2+ facilitates the local cell matrix synthesis and promotes immunomodulation (upregulating M2 / downregulating M1 macrophage polarization), thus inhibiting the IVDD progression. The proposed hydrogel has biocompatibility and is shown to enhance the expression of collagen II (COL II) and aggrecan . The potential of the injectable hydrogel in IVD repair has also been successfully demonstrated by in vivo studies. Statement of significance • A unique injectable hydrogel consisting of sodium alginate (SA), poly(N-isopropylacrylamide) (PNIPAAm), silicate ceramics (SC) and nucleus pulposus cells, has been created for intervertebral disc repair applications. • This is the first “self-contained” cell delivery system capable of releasing and subsequently storing Mg 2+ in the hydrogel reservoir for localized treatment. • The role of Mg 2+ in regulating the macrophage polarity transformation (from pro-inflammatory M1 to anti-inflammatory M2 phenotype) has been unveiled in the context of intervertebral disc repair.

研究领域: 生物材料 · 组织工程 · 再生医学 · 生物医学工程 · 骨科
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EUROPEAN POLYMER JOURNAL · 2023 · IF 6

Strong, self-healing, shape memory PAA-PANI/PVA/PDA/AOP conductive hydrogels with interpenetrating network and hydrogen bond interaction

Liying Wan,Peijie Li,Meiling Yan,Jianhong Wang,Xibao Li

Conductive hydrogels have attracted much attention in soft electronic devices. However, it is still a challenging to be integrated with outstanding mechanical performance, self-healing, shape memory and conductive capability. Herein, we developed a multifunctional conductive hydrogel via interpenetrating network (IPN) and multiple hydrogen bond interaction. Poly (acrylic acid)-polyaniline (PAA-PANI) and polyvinyl alcohol (PVA) form bones of IPN through chemical and physical double cross-linking. Chemically crosslinking of IPN was obtained by in situ polymerization of acrylic acid and aniline. Physical crosslinking is realized by more multiple hydrogen bonds (N–H···O, O–H···O, O–H···N, N–H···N) interaction among PVA, polydopamine and PF127 diamino oxygen derivatives. PANI forms a conductive path in the IPN to ensure its conductivity. IPN hydrogels with multiple hydrogen bonds has excellent mechanical strength, which is much higher than conventional conductive hydrogels. Moreover, the structure endowed the hydrogel low swelling property, good self-healing and thermal-responsive shape memory effect. The multifunctional IPN conductive hydrogel have potential applications in smart devices including self-healing electronic devices, soft robot, and sensors.

CAS / MDL: 547-58-0
研究领域: 材料科学 · 电化学 · 软体机器人 · 传感器 · 智能材料
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

One-pot interpenetrating epoxy thermosets from renewable dual biomass to high performance

Jingjing Meng,Hao Guan,Chunyu Li,Zhiyong Li,Zheng Fang,Kai Guo

The 5-hydroxymethylfurfural, honokiol, and magnolol are converted into sustainable epoxy monomers, i.e. , 5,5′-(((3′,5-diallyl-[1,1′-biphenyl]-2,4′-diyl)bis(oxy))bis- (methyl-ene))bis(2-((oxiran-2-ylmethoxy)methyl)furan) (MGHF) and 5,5′-(((5,5′-diallyl-[1,1′-biphenyl]-2,2′-diyl)bis(oxy))bis(methylene))bis(2-((oxiran-2-ylmethoxy)- methyl)furan) (MGMF), and they are finally cured by 3,3′-diamino diphenylsulfone (33DDS) and 4,4′-diamino diphenylsulfone (44DDS), thus affording novel interpenetrating polymer networks (IPN). Interestingly, 33DDS induces a twist-stacked structure, whereas 44DDS provides a planar weave matrix. As to the twist-stacked layout MGMF/33DDS, it behaves a superhigh storage modulus (∼5.04 GPa), a high phase transition temperature ( T g , 222.7 °C), and an elevated onset temperature ( T d5 , 362.8 °C). For planar weave arrays, MGHF/44DDS shows the highest values in T g (224.9 °C), lap shear strength (∼20.4 MPa), hardness (∼508 MPa), and reduced Young’s modulus (∼6.06 GPa). Furthermore, MGMF/44DDS shows an excellent dielectric property (11.15, 0.02) (∼1 kHz, 25 °C) and a moderate thermal conductivity (0.355 W (m·K) −1 ) alonging with increased flame retardancy. Besides, those biobased epoxy resin wastes are reclaimable through aerobic or anaerobic pyrolysis. Anaerobic pyrolysis of planar weave networks selectively yields more doped graphene, whereas similar event readily happens to the aerobic pyrolysis of the twist-stacked polymers. In view of these reported advantages, this novel strategy opens new avenues for multifunctional epoxy resins.

研究领域: 材料科学 · 化学工程 · 可持续化学 · 高分子科学
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