MACROMOLECULES
·
2021
·
IF 5.985
Cong Du,Xin Ning Zhang,Tao Lin Sun,Miao Du,Qiang Zheng,Zi Liang Wu
Forming robust associative interactions has been an effective strategy for the design of tough hydrogels. However, the role of associative interactions in the dynamics of hydrogels still remains elusive. Here, we report a series of poly(acrylamide-co-methacrylic acid) hydrogels with moderate water contents and excellent mechanical properties that are facilely synthesized by free-radical copolymerization. The mechanical properties of these hydrogels vary with the feeding molar fraction of acrylamide (fam). The gels with fam of 0.2–0.35 exhibit high toughness and good stability in water, which is related to the dense hydrogen bonds and relatively high segment rigidity of the matrix. Dynamic modulus spectra extended by time-temperature superposition and relaxation measurements indicate that the gels undergo glassy-to-rubbery transition with decreased frequency, and the robust hydrogen bonds, whose density is 1–3 times that of entanglements, retard chain disentanglement and contribute to the plateau modulus of the gels at low frequencies. The activation energy for the dissociation of the robust hydrogen bonds is ∼46 kJ mol–1. Furthermore, a decrease in water content results in the shift of dynamic modulus spectra to low frequencies and an increase in transition temperature due to the reduced segment relaxation. To further examine the structure of gel networks, the tensile behaviors of the gels are analyzed using a viscoelastic model. It is found that each partial chain includes 20–30 Kuhn segments, which are stretched after the fracture of intrachain hydrogen bonds to release the hidden length, dissipate energy, and thus toughen the gels. This understanding of the dynamics of the network at different timescales and the contribution of associative interactions to the mechanical properties should be informative for the design of other tough hydrogels.
研究领域:
材料科学
·
高分子化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMISTRY OF MATERIALS
·
2019
·
IF 10.159
Yan Jie Wang,Xin Ning Zhang,Yihu Song,Yiping Zhao,Li Chen,Fengmei Su,Liangbin Li,Zi Liang Wu,Qiang Zheng
Design of tough hydrogels has made great progress in the past two decades. However, the synthetic tough gels are usually much softer than some biotissues (e.g., skins with modulus up to 100 MPa). Here we report a new class of ultrastiff and tough supramolecular hydrogels facilely prepared by copolymerization of methacrylic acid and methacrylamide. The gels with water content of approximately 50–70 wt % possessed remarkable mechanical properties, with Young’s modulus of 2.3–217.3 MPa, tensile breaking stress of 1.2–8.3 MPa, breaking strain of 200–620%, and tearing fracture energy of 2.9–23.5 kJ/m2, superior to most existing hydrogels, especially in terms of modulus. Typical yielding and crazing were observed in the gel under tensile loading, indicating the forced elastic deformation of these hydrogels in a glassy state, as confirmed by dynamic mechanical analysis. The ultrahigh stiffness was attributed to the dense cross-linking and reduced segmental mobility caused by the robust intra- and interchain hydrogen bonds. Because of the dynamic nature of noncovalent bonds, these supramolecular gels also showed rate-dependent mechanical performances along with good shape memory and recyclability. This strategy should be applicable for other systems toward robust mechanical properties, versatile functionalities, and promising applications of hydrogel materials as structural elements.
研究领域:
材料科学
·
生物医学工程
✓ 已验证
产品关联
DOI
高影响因子
Soft Matter
·
2025
·
IF 2.8
Yun-song Zhou,Yang Sheng,Peng Zhang,Rong Zhang,Mark Bradley,Yi-xin Sun
The self-assembly of small molecules into supramolecular hydrogels is of great significance in mimicking biological systems. In this study, we investigated the formation and structure change of supramolecular hydrogels based on the self-assembly behavior of an achiral coumarin derivative (G1) and a chiral phenylalanine derivative (ALP). It was observed that G1 and ALP can self-assemble at various molar ratios, resulting in distinct nanostructured morphologies. Specifically, at a molar ratio of G1/ALP (4 : 1), the achiral G1 molecules initially bifurcate and diverge, ultimately forming a dendritic microstructure at the G1 termini. When the G1/ALP ratio was adjusted to 2 : 1, a chrysanthemum-like microstructure emerged. UV-light can destroy the self-assembled gel structure of different G1/ALP ratios, changing it from gel to sol. The emergence of these higher-order chiral structures during self-assembly was attributed to hydrogen bonding and π–π stacking interactions between the molecules. This research offers valuable insights into the understanding of biological self-assembly processes and the design of artificial biomedical materials.
研究领域:
材料科学
·
生物化学
·
纳米技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Advanced Science
·
2025
·
IF 14.1
Shuhang Deng,Shijia He,Guilong Yan,Li Wang,Zhenyu Li,Jingyu Chen,Jingjuan Lai,Dong Li,Dong Xiang,Chunxia Zhao,Hui Li,Xuezhong Zhang,Han Li,Xungai Wang,Yuanpeng Wu
Existing polymer materials often lack the ability to dynamically adjust lubrication in response to external stimuli. This gap in adaptable lubrication technology limits their application in advanced systems such as intelligent motion devices and soft robotics. To address this challenge, a dual-responsive lubricating hydrogel is introduced designed with a thermal and shear-responsive supramolecular network integrated into a stable polymer framework. The hydrogel exhibits a partial gel-sol transition under thermal or shear stress, mimicking the mucus secretion behavior of hagfish. As a result, the hydrogel′s surface secretes a liquid supramolecular layer that significantly alters its coefficient of friction (COF), achieving up to a 20-fold reduction in friction due to the reversible supramolecular transition. This hydrogel demonstrates significant potential as an intelligent lubrication material capable of dynamically responding to varying stimuli, paving the way for more adaptive and efficient lubrication technologies.
研究领域:
材料科学
·
生物仿生学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2024
·
IF 7.7
Ruonan Jiang,Xiaohu Zhai,Yang Liu,Juan Chen,Shuang-Ying Gui,Huanhuan Liu
Extracted from Platycodon grandiflorum , platycodon grandiflorum polysaccharides (PGPs) with diverse biological functions have been extensively employed for modification and fabrication of hydrogels for biomedical applications, such as wound dressings. However, since the lack of effective structural design, the reported polysaccharide-based hydrogel dressings are still suffered from structural failures and limited bio-functionality. Herein, we demonstrate a facile and general strategy to fabricate a supramolecular hydrogel composed of PGP-based polymer brush as building blocks combined with a Ca 2+ -mediated self-assembly process. The specific polymer brush with high branch functionality was achieved with polyacrylamide arms evenly grown on the PGP (grafting efficiency as high as 80 %) with series of chemical modifications. With above structural merits, the resulting hydrogel with densely crosslinked polymer brush featured enhanced mechanical strength as well as self-healing, and shear-thinning behaviors. Further biocompatible investigation indicated the as-prepared hydrogels with admirable performances in self-adhesion (adhesive strength of 16.7–79.5 kPa), a pH-responsive swelling ratio as high as 44 at pH 5.4, and pH-responsive degradation. They also showed antioxidant capacity by scavenging DPPH activity of nearly 80 % in 20 min, hemocompatibility, cell viability and cell migration. Impressively, the PGP-based polymer brush hydrogel served as a wound dressing revealed significant acceleration on wound closure.
研究领域:
生物材料
·
医学工程
·
高分子化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Scientific Reports
·
2015
·Vol. 5
·期 1
·1-6
·
IF 5.578
Xue Qiang,Ren He,Xu Chao,Wang Gang,Ren Chunhua,Hao Jihui,Ding Dan
In this study, we synthesized a peptide of Nap-GFFYGRGD, which could self-assemble into supramolecular nanofibers. The peptide itself could only form nanofibers but not hydrogels due to the relative weak inter-fiber interactions. The resulting nanofibers were then utilized as the vehicles for anticancer drug doxorubicin. It was found that the nanofibers of Nap-GFFYGRGD could not encapsulate doxorubicin, whereas the drug formed nanospheres, which were located at the surface of the nanofibers. Due to the electrostatic interactions between the negatively charged nanofibers and the positively charged doxorubicin nanospheres, the doxorubicin nanospheres were able to serve as a cross-linker to increase the inter-fiber interactions, leading to the formation of stable three-dimentional fiber networks and hydrogels. The resulting doxorubicin-peptide hydrogels were capable of releasing the drug in a sustained manner, which also showed comparable cytotoxicity as compared to free doxorubicin against a variety of cancer cell lines including HeLa and MCF-7 cancer cells. Therefore, this successful example using drug as the peptide nanofiber cross-linkers provided a new strategy for fabricating supramolecular hydrogelation for controlled delivery of anticancer drugs.
研究领域:
生物材料
·
药理学
·
肿瘤学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2022
·
IF 6.76
Jia Yang,Qiong Kang,Bin Zhang,Xiyu Tian,Shuzheng Liu,Gang Qin,Qiang Chen
Ionic conductive hydrogel-based sensors have been capturing growing attention in various areas, but still cannot satisfy the operating requirements of next generation wearable electronics. Herein, inspired by biosystems, we demonstrate ionic conductive supramolecular hydrogels with simple one-step method based on salting-out effect and multiple hydrogen bond interactions. The supramolecular hydrogels exhibit high toughness and strength, quick self-recovery, high sensitive sensing performance as well as good self-healing, fatigue and frost resistances in mechanical and sensing properties, and can monitor large and subtle movements and physiological activities of the human body sensitively, quickly and stably. Thus, it provides a convenient and promising way to obtain stretchable sensors of excellent comprehensive properties, which have tremendous application potential as wearable electronic devices in harsh environments.
研究领域:
材料科学
·
生物医学工程
✓ 已验证
产品关联
DOI
高影响因子
MACROMOLECULAR RAPID COMMUNICATIONS
·
2022
·Vol. 43
·期 15
·2200103
·
IF 5.006
Zhiwen Zeng,Shan Yu,Cuiping Guo,Daohuan Lu,Zhijie Geng,Dating Pei
Conductive hydrogels used as electronics have received much attention due to their great flexibility and stretchability. However, the fabrication of ideal conductive hydrogels fulfilling the excellent mechanical properties and outstanding sensitivity remains a great challenge until now. Moreover, high sensitivity and broad linearity range are pivotal for the feasibility and accuracy of hydrogel sensors. In this study, a conductive supramolecular hydrogel is engineered by directly mixing the aqueous dispersion of MXene with the precursor of N -acryloyl glycinamide (NAGA) monomer and then rapidly photo cross-linked by UV irradiation. The resultant PNAGA/MXene hydrogel-sensors exhibit high mechanical strength (4.8 MPa), great stretchability (630%), and excellent durability. The conductive hydrogel-based sensor presents excellent conductivity (17.3 S m −1 ) and a wide scope of linear dependence of sensitivity on strain (0%–125%, gauge factor = 2.05). It displays reliable detection of various motions, including repeated subtle movements and large strain. It also shows good degradation in vitro and antifouling capability. This work may provide a simple and promising platform for engineering conductive supramolecular hydrogels with integrated high performance aiming for smart wearable electronics, electronic skin, soft robots, and human–machine interfacing.
研究领域:
材料科学
·
生物医学工程
·
柔性电子
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF POLYMER SCIENCE
·
2022
·Vol. 60
·期 15
·2280-2288
·
IF 3.046
Lingtao Fang,Jian Hu,Chuan Wei Zhang,Jialun Wei,Hai Chao Yu,Si Yu Zheng,Zi Liang Wu,Qiang Zheng
Forming carboxyl-Fe 3+ coordination bonds as physical crosslinks is an effective strategy to develop tough hydrogels. Considering the inhibition of ferric ions on free-radical polymerization, these coordination bonds cannot be formed during the reaction, and a soaking process of preformed hydrogels is usually required for mechanical enhancement, resulting in uncontrollable gradient structure, long preparation time, and unnecessary waste of metallic ions. A facile strategy is reported here to prepare tough metallosupramolecular hydrogels by polymerization and in situ formation of coordination bonds with phosphates as the temporal ligands of Fe 3+ ions. The phosphate ligands in the precursor solution form coordination complexes with the Fe 3+ ions, which avoids the inhibition and ensures the polymerization. After swelling the resultant hydrogel in water, the ligands are substituted by carboxyl groups of the gel matrix due to the variation of local pH. The equilibrated hydrogel with carboxyl-Fe 3+ coordination bonds as the physical crosslinks possesses excellent mechanical properties that can be tuned over a wide range by adjusting the polymer compositions and the concentrations of phosphate ligands and Fe 3+ ions. This strategy should be applicable to other systems to enable synthesis of functional hydrogels with Fe 3+ ions as the additive toward specific applications in engineering and biomedical fields. Graphical
研究领域:
材料科学
·
化学工程
·
生物医学工程
✓ 已验证
产品关联
DOI
高影响因子
MACROMOLECULAR CHEMISTRY AND PHYSICS
·
2017
·Vol. 219
·期 2
·1700398
·
IF 2.5
Wei Ji,Minggao Qin,Chuanliang Feng
Recently, photoresponsive hydrogels have attracted increasing interest due to their ability to provide precise spatial and temporal control of drug release. Herein, a new kind of coumarin-based photoresponsive supramolecular hydrogelator without conventional gelation motif is designed and synthesized through a facile one-pot method. The gelation process, photoresponsiveness, self-assembly morphology, self-assembly mechanism, and release kinetics are fully investigated by various characterization methods (e.g., scanning electron microscopy, single crystal X-ray diffraction, high pressure liquid chromatography, UV–vis spectroscopy). Furthermore, encapsulated methyl violet dye molecules can be precisely released from the hydrogel by manipulating photoirradiation time. The study reveals that the coumarin-based photoresponsive hydrogel holds great potential as soft materials for controllable drug release.
研究领域:
材料科学
·
药物递送
·
化学
✓ 已验证
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2024
·
IF 18.5
Jing Guo,Ruihui Liu,Yuezi Lv,Hui Xie,Shaobing Zhou
Shape-morphing hydrogels can mimic the dynamism of living creatures and are popular for designing soft machines, such as actuators and robots. However, most existing shape-morphing hydrogels present a single morphing pathway between two shapes, sequential and multistage shape-morphing in real scenarios has rarely been captured. Although a strategy that assembles functional hydrogel components has been reported, it is likely to simultaneously increase the complexity and weaken the versatility of hydrogel machines. Here, a light-encoding strategy based on the dynamic coordination between the ferric iron and carboxyl group (Fe 3+ ─COO − ) to integrate the frame and actuating units into a single hydrogel without assembly is proposed. The spatiotemporal control of light irradiation is expected to make the light-encoding process sequential and reprogrammable. Results demonstrate that the light-encoded patterns determine the morphing route and further activate shape-morphing owing to swelling mismatch. The actuating units can be successively created by localized irradiation or elaborately turned by re-coordinating and light-encoding. This endows the encoded hydrogel with sequential and multistage shape-morphing behavior, similar to the living creatures. This strategy allows the design of assembly-free soft machines with sequential and multistage shape-morphing performance, which will benefit the design of more types of hydrogel machines.
研究领域:
材料科学
·
生物工程
✓ 已验证
产品关联
DOI
高影响因子
Chemistry-An Asian Journal
·
2016
·Vol. 11
·期 23
·3430-3435
·
IF 4.592
Lei Gao,Yuxia Gao,Yuan Lin,Yong Ju,Song Yang,Jun Hu
Graphical Time to heal : A dual-component charge-transfer (CT)-induced supramolecular hydrogel was fabricated by using pyrene-tailored pyridinium (PYP) and 2,4,7-trinitrofluorenone (TNF) as the electron donor and acceptor, respectively (see scheme). This hydrogel exhibited a distinct injectable self-healing property that could be utilized to create desired patterns on substrates, which holds potential in fields like three-dimensional printing and surface coating. In this study, a dual-component charge-transfer (CT)-induced supramolecular hydrogel was fabricated using pyrene-tailored pyridinium (PYP) and 2,4,7-trinitrofluorenone (TNF) as the electron donor and acceptor, respectively. Its thermal stability and mechanical property have been modulated effectively by altering the concentration or molar ratio of PYP and TNF. Moreover, this CT hydrogel exhibited a distinct injectable self-healing property that could be utilized to create desired patterns on substrates. Such property holds potential for this CT hydrogel in fields like three-dimensional printing and surface coating.
研究领域:
材料科学
·
化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）