a.Engineering Research Center of Energy Storage Materials and Devices, Ministry of Education, School of Chemistry, Xi’an Jiaotong University, Xi’an 710049, China
b.Polymer Materials & Engineering Department School of Materials Science & Engineering Chang’an University, Xi’an 710064, China
c.School of Electrical Engineering, Xi’an Jiaotong University, Xi’an 710049, China
d.Department of Nuclear Medicine, the First Affiliated Hospital of China, Xi’an Jiaotong University, Xi’an 710049, China
yilongcheng@mail.xjtu.edu.cn
纸质出版日期:2024-10-01,
网络出版日期:2024-08-28,
收稿日期:2024-05-11,
修回日期:2024-06-02,
录用日期:2024-06-03
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Li, M.; Zhang, M. Y.; Lei, W. X.; Lv, Z. T.; Shang, Q. H.; Zhao, Z.; Li, J. T.; Cheng, Y. L. Tough polymeric hydrogels based on amino acid derivative mediated dynamic metal coordination bonds. Chinese J. Polym. Sci. 2024, 42, 1578–1588
Meng Li, Meng-Yuan Zhang, Wu-Xuan Lei, et al. Tough Polymeric Hydrogels Based on Amino Acid Derivative Mediated Dynamic Metal Coordination Bonds[J]. Chinese Journal of Polymer Science, 2024,42(10):1578-1588.
Li, M.; Zhang, M. Y.; Lei, W. X.; Lv, Z. T.; Shang, Q. H.; Zhao, Z.; Li, J. T.; Cheng, Y. L. Tough polymeric hydrogels based on amino acid derivative mediated dynamic metal coordination bonds. Chinese J. Polym. Sci. 2024, 42, 1578–1588 DOI: 10.1007/s10118-024-3177-6.
Meng Li, Meng-Yuan Zhang, Wu-Xuan Lei, et al. Tough Polymeric Hydrogels Based on Amino Acid Derivative Mediated Dynamic Metal Coordination Bonds[J]. Chinese Journal of Polymer Science, 2024,42(10):1578-1588. DOI: 10.1007/s10118-024-3177-6.
This study reported the preparation of tough polymer hydrogels through Zr
4+
coordination. Compared to AAla without hydroxyl groups
copolymerization of ASer with AM in water followed by incubation with ZrOCl
2
solution significantly improved the comprehensive mechanical properties of the hydrogels and demonstrated great potential for applications in flexible sensors.
The development of physically crosslinked hydrogels with excellent mechanical and sensing properties is of importance for expanding the practical applications of intelligent soft hydrogel materials. Herein
after copolymerization of hydroxyl-containing amino acid derivative N-acryloyl serine (ASer) with acrylamide (AM)
we introduce Zr
4+
through an immersion strategy to construct metal ion-toughened non-covalent crosslinked hydrogels (with tensile strength of up to 5.73 MPa). It is found that the synergistic coordination of hydroxyl and carboxyl groups with Zr
4+
substantially increases the crosslinking density of the hydrogels
thereby imparting markedly superior mechanical properties compared to hydroxyl-free Zr
4+
-crosslinked hydrogels
such as N-acryloyl alanine (AAla) copolymerized with AM hydrogels (with tensile strength of 2.98 MPa). Through the adjustment of the composition of the copolymer and
the density of coordination bonds
the mechanical properties of the hydrogels can be modulated over a wide range. Additionally
due to the introduction of metal ions and the dynamic nature of coordination bonds
the hydrogels also exhibit excellent sensing performance and good self-recovery properties
paving the way for the development of flexible electronic substrates with outstanding comprehensive performances.
HydrogelAmino acidMetal coordinationMechanical performanceFlexible sensor
Zhang, Y. S.; Khademhosseini, A. Advances in engineering hydrogels.Science2017,356, eaaf3627..
Wegst, U. G. K.; Ashby, M. F. The mechanical efficiency of natural materials.Philos. Mag.2004,84, 2167−2186..
Huang, H.; Dong, Z.; Ren, X.; Jia, B.; Li, G.; Zhou, S.; Zhao, X.; Wang, W. High-strength hydrogels: fabrication, reinforcement mechanisms, and applications.Nano Res.2023,16, 3475−3515..
Gong, J. P.; Katsuyama, Y.; Kurokawa, T.; Osada, Y. Double-network hydrogels with extremely high mechanical strength.Adv. Mater.2003,15, 1155−1158..
Liu, J.; Tan, C. S. Y.; Yu, Z.; Li, N.; Abell, C.; Scherman, O. A. Tough supramolecular polymer networks with extreme stretchability and fast room-temperature self-healing.Adv. Mater.2017,29, 1605325..
Wang, J.; Lin, L.; Cheng, Q.; Jiang, L. A strong bio-inspired layered PNIPAM–clay nanocomposite hydrogel.Angew. Chem. Int. Ed.2012,51, 4676−4680..
Okumura, Y.; Ito, K. The Polyrotaxane Gel: A Topological Gel by Figure-of-Eight Cross-links.Adv. Mater.2001,13, 485−487..
Hu, J. Y.; Jiao, D.; Hao, X. P.; Kong, X.; Zhang, X. N.; Du, M.; Zheng, Q.; Wu, Z. L. A facile strategy to fabricate tough and adhesive elastomers byin situformation of coordination complexes as physical crosslinks.Adv. Funct. Mater.2023,33, 2307402..
Sun, T. L.; Kurokawa, T.; Kuroda, S.; Ihsan, A. B.; Akasaki, T.; Sato, K.; Haque, M. A.; Nakajima, T.; Gong, J. P. Physical hydrogels composed of polyampholytes demonstrate high toughness and viscoelasticity.Nat. Mater.2013,12, 932−937..
Zhang, M.; Yu, J.; Shen, K.; Wang, R.; Du, J.; Zhao, X.; Yang, Y.; Xu, K.; Zhang, Q.; Zhang, Y.; Cheng, Y. Highly stretchable nanocomposite hydrogels with outstanding antifatigue fracture based on robust noncovalent interactions for wound healing.Chem. Mater.2021,33, 6453−6463..
Lai, J. C.; Jia, X. Y.; Wang, D. P.; Deng, Y. B.; Zheng, P.; Li, C. H.; Zuo, J. L.; Bao, Z. Thermodynamically stable whilst kinetically labile coordination bonds lead to strong and tough self-healing polymers.Nat. Commun.2019,10, 1164..
Zhang, Z.; Zhao, J.; Guo, Z.; Zhang, H.; Pan, H.; Wu, Q.; You, W.; Yu, W.; Yan, X. Mechanically interlocked networks cross-linked by a molecular necklace.Nat. Commun.2022,13, 1393..
Nie, F. M.; An, C. H.; Cao, D. F.; Liu, J.; Zhou, Y. F.; Lu, Y. G.; Ma, Z.; Pan, L.; Li, Y. S. Ru(II) catalyst enables dynamic dual-cross-linked elastomers with near-infrared self-healing toward flexible electronics.Adv. Funct. Mater.2021,32, 2110616..
Li, C. H.; Zuo, J. L. Self-healing polymers based on coordination bonds.Adv. Mater.2019,32, 1903762..
Lai, J. C.; Li, L.; Wang, D. P.; Zhang, M. H.; Mo, S. R.; Wang, X.; Zeng, K. Y.; Li, C. H.; Jiang, Q.; You, X. Z.; Zuo, J. L. A rigid and healable polymer cross-linked by weak but abundant Zn(II)-carboxylate interactions.Nat. Commun.2018,9, 2725..
Tang, Z.; Huang, J.; Guo, B.; Zhang, L.; Liu, F. Bioinspired engineering of sacrificial metal-ligand bonds into elastomers with supramechanical performance and adaptive recovery.Macromolecules2016,49, 1781−1789..
Li, M.; Lyu, Q.; Sun, L.; Peng, B.; Zhang, L.; Zhu, J. Fluorescent metallosupramolecular elastomers for fast and ultrasensitive humidity sensing.ACS Appl. Mater. Interfaces2020,12, 39665−39673..
Rao, Y. L.; Chortos, A.; Pfattner, R.; Lissel, F.; Chiu, Y. C.; Feig, V.; Xu, J.; Kurosawa, T.; Gu, X.; Wang, C.; He, M.; Chung, J. W.; Bao, Z. Stretchable self-healing polymeric dielectrics cross-linked through metal-ligand coordination.J. Am. Chem. Soc.2016,138, 6020−6027..
Yang, C. H.; Wang, M. X.; Haider, H.; Yang, J. H.; Sun, J.-Y.; Chen, Y. M.; Zhou, J.; Suo, Z. Strengthening alginate/polyacrylamide hydrogels using various multivalent cations.ACS Appl. Mater. Interfaces2013,5, 10418−10422..
Yu, H. C.; Li, C. Y.; Du, M.; Song, Y.; Wu, Z. L.; Zheng, Q. Improved toughness and stability ofκ-carrageenan/polyacrylamide double-network hydrogels by dual cross-linking of the first network.Macromolecules2019,52, 629−638..
Yu, H. C.; Hao, X. P.; Zhang, C. W.; Zheng, S. Y.; Du, M.; Liang, S.; Wu, Z. L.; Zheng, Q. Engineering tough metallosupramolecular hydrogel films with Kirigami structures for compliant soft electronics.Small2021,17, 2103836..
Zheng, S. Y.; Shen, Y.; Zhu, F.; Yin, J.; Qian, J.; Fu, J.; Wu, Z. L.; Zheng, Q. Programmed deformations of 3D-printed tough physical hydrogels with high response speed and large output force.Adv. Funct. Mater.2018,28, 1803366..
Yu, H. C.; Zheng, S. Y.; Fang, L.; Ying, Z.; Du, M.; Wang, J.; Ren, K. F.; Wu, Z. L.; Zheng, Q. Reversibly transforming a highly swollen polyelectrolyte hydrogel to an extremely tough one and its application as a tubular grasper.Adv. Mater.2020,32, 2005171..
Dou, X. Q.; Feng, C. L. Amino acids and peptide-based supramolecular hydrogels for three-dimensional cell culture.Adv. Mater.2017,29, 1604062..
Li, M.; Zhang, M.; Liu, Z.; Xie, R.; Yang, Y.; Shen, K.; Yang, A.; Cheng, Y. Injectable and self-fused hydrogels with antifouling capability based on amino acid derivatives for postoperative anti-adhesion application.Sci. China Mater.2024,67, 1521−1532..
Yu, J.; Xu, K.; Chen, X.; Zhao, X.; Yang, Y.; Chu, D.; Xu, Y.; Zhang, Q.; Zhang, Y.; Cheng, Y. Highly stretchable, tough, resilient, and antifatigue hydrogels based on multiple hydrogen bonding interactions formed by phenylalanine derivatives.Biomacromolecules2021,22, 1297−1304..
Yu, J.; Qin, Y.; Yang, Y.; Zhao, X.; Zhang, Z.; Zhang, Q.; Su, Y.; Zhang, Y.; Cheng, Y. Robust hydrogel adhesives for emergency rescue and gastric perforation repair.Bioact. Mater.2023,19, 703−716..
Filippidi, E.; Cristiani, T. R.; Eisenbach, C. D.; Waite, J. H.; Israelachvili, J. N.; Ahn, B. K.; Valentine, M. T. Toughening elastomers using mussel-inspired iron-catechol complexes.Science2017,358, 502−505..
Huang, Y.; Xiao, L.; Zhou, J.; Liu, T.; Yan, Y.; Long, S.; Li, X. Strong tough polyampholyte hydrogelsviathe synergistic effect of ionic and metal-ligand bonds.Adv. Funct. Mater.2021,31, 2103917..
Zheng, S. Y.; Ding, H.; Qian, J.; Yin, J.; Wu, Z. L.; Song, Y.; Zheng, Q. Metal-coordination complexes mediated physical hydrogels with high toughness, stick-slip tearing behavior, and good processability.Macromolecules2016,49, 9637−9646..
Dou, X.; Wang, H.; Yang, F.; Shen, H.; Wang, X.; Wu, D. One-step soaking strategy toward anti-swelling hydrogels with a stiff “armor”.Adv. Sci.2023,10, 2206242..
Chen, B.; Chen, Q.; Xiao, S.; Feng, J.; Zhang, X.; Wang, T. Giant negative thermopower of ionic hydrogel by synergistic coordination and hydration interactions.Sci. Adv.2021,7, eabi7233..
Song, P.; Xu, Z.; Dargusch, M. S.; Chen, Z. G.; Wang, H.; Guo, Q. Granular nanostructure: a facile biomimetic strategy for the design of supertough polymeric materials with high ductility and strength.Adv. Mater.2017,29, 1704661..
Zhao, Z.; Fan, X.; Wang, S.; Jin, X.; Li, J.; Wei, Y.; Wang, Y. Natural polymers-enhanced double-network hydrogel as wearable flexible sensor with high mechanical strength and strain sensitivity.Chinese Chem. Lett.2023,34, 107892..
Murugan, D.; Arumugam, H.; Arumugam, S.; Mani, M.; Kannan, S. Superparamagnetic freeze-thawed PVA hydrogel for applications in tissue engineering, drug delivery and bioimaging.Colloids Surf. A: Physicochem. Eng. Asp.2024,690, 133790..
Sormani, G.; Korde, A.; Rodriguez, A.; Denecke, M.; Hassanali, A. Zirconium coordination chemistry and its role in optimizing hydroxymate chelation: insights from molecular dynamics.ACS Omega2023,8, 36032−36042..
Liu, D.; Jiang, P.; Wang, Y.; Lu, Y.; Wu, J.; Xu, X.; Ji, Z.; Sun, C.; Wang, X.; Liu, W. Engineering tridimensional hydrogel tissue and organ phantoms with tunable springiness.Adv. Funct. Mater.2023,33, 2214885..
Tan, Z.; Li, S.; Wang, F.; Qian, D.; Lin, J.; Hou, J.; Li, Y. High performance polymer solar cells with as-prepared zirconium acetylacetonate film as cathode buffer layer.Sci. Rep.2014,4, 4691..
Ju, H.; Zhu, Q. L.; Zuo, M.; Liang, S.; Du, M.; Zheng, Q.; Wu, Z. L. Toughening hydrogels by forming robust hydrazide-transition metal coordination complexes.Chem. Eur. J.2023,29, e202300969..
Chen, J.; Gao, Y.; Shi, L.; Yu, W.; Sun, Z.; Zhou, Y.; Liu, S.; Mao, H.; Zhang, D.; Lu, T.; Chen, Q.; Yu, D.; Ding, S. Phase-locked constructing dynamic supramolecular ionic conductive elastomers with superior toughness, autonomous self-healing and recyclability.Nat. Commun.2022,13, 4868..
Jiang, Y.; Zhan, D.; Zhang, M.; Zhu, Y.; Zhong, H.; Wu, Y.; Tan, Q.; Dong, X.; Zhang, D.; Hadjichristidis, N. Strong and ultra-tough ionic hydrogel based on hyperbranched macro-cross-linker: influence of topological structure on properties.Angew. Chem. Int. Ed.2023,62, e202310832..
Zhang, M.; Yang, Y.; Li, M.; Shang, Q.; Xie, R.; Yu, J.; Shen, K.; Zhang, Y.; Cheng, Y. Toughening double-network hydrogels by polyelectrolytes.Adv. Mater.2023,35, e2301551..
Hu, L.; Wang, Y.; Liu, Q.; Liu, M.; Yang, F.; Wang, C.; Pan, P.; Wang, L.; Chen,L.; Chen, J. Real-time monitoring flexible hydrogels based on dual physically cross-linked network for promoting wound healing.Chinese Chem. Lett.2023,34, 108262..
Fang, X.; Sun, J. One-step synthesis of healable weak-polyelectrolyte-based hydrogels with high mechanical strength, toughness, and excellent self-recovery.ACS Macro Lett.2019,8, 500−505..
Lin, P.; Ma, S.; Wang, X.; Zhou, F. Molecularly engineered dual-crosslinked hydrogel with ultrahigh mechanical strength, toughness, and good self-recovery.Adv. Mater.2015,27, 2054−2059..
Hu, X.; Vatankhah-Varnoosfaderani, M.; Zhou, J.; Li, Q.; Sheiko, S. S. Weak hydrogen bonding enables hard, strong, tough, and elastic hydrogels.Adv. Mater.2015,27, 6899−905..
Shen, J.; Dai, Y.; Xia, F.; Zhang, X. Role of divalent metal ions in the function and application of hydrogels.Prog. Polym. Sci.2022,135, 101622..
Wang, Y.; Xie, Y.; Xie, X.; Wu, D.; Wu, H.; Luo, X.; Wu, Q.; Zhao, L.; Wu, J. Compliant and robust tissue-like hydrogels via ferric ion-induced of hierarchical structure.Adv. Funct. Mater.2023,33, 2210224..
Lu, X.; Si, Y.; Zhang, S.; Yu, J.; Ding, B.In situsynthesis of mechanically robust, transparent nanofiber-reinforced hydrogels for highly sensitive multiple sensing.Adv. Funct. Mater. 2021, 31, 2103117..
Zheng, S.; Chen, X.; Shen, K.; Cheng, Y.; Ma, L.; Ming, X. Hydrogen bonds reinforced ionogels with high sensitivity and stable autonomous adhesion as versatile ionic skins.ACS Appl. Mater. Interfaces2024,16, 4035−4044..
Shen, K.; Liu, Z.; Xie, R.; Zhang, Y.; Yang, Y.; Zhao, X.; Zhang, Y.; Yang, A.; Cheng, Y. Nanocomposite conductive hydrogels with Robust elasticity and multifunctional responsiveness for flexible sensing and wound monitoring.Mater. Horiz.2023,10, 2096−2108..
Yuan, W.; Qu, X.; Lu, Y.; Zhao, W.; Ren, Y.; Wang, Q.; Wang, W.; Dong, X. MXene-composited highly stretchable, sensitive and durable hydrogel for flexible strain sensors.Chinese Chem. Lett.2021,32, 2021−2026..
Liu, Y.; Tian, G.; Du, Y.; Shi, P.; Li, N.; Li, Y.; Qin, Z.; Jiao, T.; He, X. Highly stretchable, low-hysteresis, and adhesive ta@mxene-composited organohydrogels for durable wearable sensors.Adv. Funct. Mater.2024, 2315813..
Wang, W.; Zhou, H.; Xu, Z.; Li, Z.; Zhang, L.; Wan, P. Flexible conformally bioadhesive mxene hydrogel electronics for machine learning-facilitated human-interactive sensing.Adv. Mater.2024, 2401035..
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