Using 2-methyl-2-acrylamidopropanesulfonic acid sodium salt (NaAMPS),polyvinyl alcohol (PVA),and carboxymethyl cellulose (CMC) as raw materials,N,N′-methylene bisacrylamide as the cross-linking agent and 2-oxoglutaric acid as the initiator,the first network of the gel was formed by UV light triggered chemical cross-linking of NaAMPS.Cyclic freezing-thawing method was used to form the second network of the gel by hydrogen bonding between PVA chains.The third gel network was formed by ionic complexation between Al3+ and carboxyl groups of CMC,and the PNaAMPS/PVA/CMC-Al3+ composite hydrogel was successfully prepared.The microscopic morphologies of the gels were characterized and the mechanical properties of the gels were tested.The results showed that the internal network of the hydrogels became denser after the formation of the first and second networks,and the formation of hydrogen bonds between PVA chains increased the fracture strength from 14kPa to 53kPa.The formation of the third network of CMC-Al3+ increased the fracture strength to be 127kPa.In addition,N-isopropyl acrylamide (NIPAM) was added to the gel as a pre-polymerization monomer,and the gel exhibited a self-enhancement of fracture strength after mechanical training,with an enhancement of fracture strength of 23% at the mechanical training strain of 40%,and the fracture strength enhancement of 56% as the mechanical training strain increased from 40% to 160%.This hydrogel achieved the self-reinforcement of mechanical properties through the mechanical training-induced structural damage and reconstruction process,which broadened the practical applications in various fields and could lay the foundation for self-reinforced materials used in applications such as soft robots and smart devices.
[1] Liu H,Li M X,Ouyang C,et al.Biofriendly,stretchable,and reusable hydrogel electronics as wearable force sensors[J].Small,2018,14(36):1801711.
[2] Liao M H,Liao H,Ye J J,et al.Polyvinyl alcohol-stabilized liquid metal hydrogel for wearable transient epidermal sensors[J].ACS Applied Materials & Interfaces,2019,11(50):47358-47364.
[3] Wang Y J,Liu J Y,Zhu D L,et al.Active tube-shaped actuator with embedded square rod-shaped ionic polymer-metal composites for robotic-assisted manipulation[J].Applied Bionics and Biomechanics,2018,2018:4031705.
[4] Lu C,Zhao L,Hu Y M,et al.A molecular-regulation strategy towards low-voltage driven,multi degree of freedom IPMC catheters[J].Chemical Communications,2018,54(63):8733-8736.
[5] Duan X Y,Yu J Y,Zhu Y X,et al.Large-scale spinning paproach to engineering knittable hydrogel fiber for soft robots[J].ACS Nano,2020,14(11):14929-14938.
[6] Zhu Q L,Du C,Dai Y H,et al.Light-steered locomotion of muscle-like hydrogel by self-coordinated shape change and friction modulation[J].Nature Communications,2020,11(1):5166.
[7] Matsuda T,Kawakami R,Namba R,et al.Revisiting the origins of the fracture energy of tough double-network hydrogels with quantitative mechanochemical characterization of the damage zone[J].Macromolecules,2021,54(22):10331-10339.
[8] Xu B,Zheng P B,Gao F,et al.A mineralized high strength and tough hydrogel for skull bone regeneration[J].Advanced Functional Materials,2017,27(4):1604327.
[9] Wang Z,Zheng X J,Ouchi T.Toughening hydrogels through force-triggered chemical reactions that lengthen polymer strands[J].Science,2021,374(6564):193-196.
[10] Gan D L,Xing W S,Jiang L L,et al.Plant-inspired adhesive and tough hydrogel based on Ag-lignin nanoparticles-triggered dynamic redox catechol chemistry[J].Nature Communications,2019,10(1):1487.
[11] Han L,Lu X,Liu K Z,et al.Mussel-inspired adhesive and tough hydrogel based on nanoclay confined dopamine polymerization[J].ACS Nano,2017,11(3):2561-2574.
[12] Long R,Hui C Y.Fracture toughness of hydrogels:measurement and interpretation[J].Soft Matter,2016,12(39):8069-8086.
[13] Brown H R.A model of the fracture of double network gels[J].Macromolecules,2007,40(10):3815-3818.
[14] Tanaka Y.A local damage model for anomalous high toughness of double-network gels[J].Europhysics Letters (EPL),2007,78(5),DOI:10.1209/0295-5075/78/56005.
[15] Rehman H U,Chen Y J,Guo Y L,et al.Stretchable,strong and self-healing hydrogel by oxidized CNT-polymer composite[J].Composites Part A:Applied Science and Manufacturing,2016,90:250-260.
[16] Cao J L,He G H,Ning X Q,et al.Hydroxypropyl chitosan-based dual self-healing hydrogel for adsorption of chromium ions[J].International Journal of Biological Macromolecules,2021,174:89-100.
[17] Wei Z,Yang J H,Liu Z Q,et al.Novel biocompatible polysaccharide-based self-healing hydrogel[J].Advanced Functional Materials,2015,25(9):1352-1359.
[18] Wang Y X,Niu J Y,Hou J,et al.A novel design strategy for triple-network structure hydrogels with high-strength,tough and self-healing properties[J].Polymer,2018,135:16-24.
[19] Matsuda T,Kawakami R,Namba R,et al.Mechanoresponsive self-growing hydrogels inspired by muscle training[J].Science,2019,363(6426):504-508.
[20] Zheng W J,Liu Z Q,Xu F,et al.In vitro platelet adhesion of PNaAMPS/PAAm and PNaAMPS/PDMAAm double-network hydrogels[J].Macromolecular Chemistry and Physics,2015,216(6):641-649.
[21] Gong Z Y,Zhang G P,Zeng X L,et al.High-strength,tough,fatigue resistant,and self-healing hydrogel based on dual physically cross-linked network[J].ACS Applied Materials & Interfaces,2016,8(36):24030-24037.
[22] Sinha V,Chakma S.Synthesis and evaluation of CMC-g-AMPS/Fe/Al/AC composite hydrogel and their use in fluoride removal from aqueous solution[J].Environmental Technology & Innovation,2020,17:100620.
[23] Wang Y Q,Liao J W,Wu X G,et al.Thermal and NIR controlled flexible switching devices using a smart conductive composite hydrogel approach[J].Composites Science and Technology,2022,222:109371.
基金资助
山西省自然科学基金项目(2021-0302123158);山西浙大新材料与化工研究院技术开发项目(2022SX-TD023)