A facile method to fabricate tough and highly stretchable polyacrylamide (PAM) nanocomposite physical hydrogel (NCP gel) was proposed. The hydrogels are dually crosslinked single network with the PAM grafted vinyl...A facile method to fabricate tough and highly stretchable polyacrylamide (PAM) nanocomposite physical hydrogel (NCP gel) was proposed. The hydrogels are dually crosslinked single network with the PAM grafted vinyl hybrid silica nanoparticles (VSNPs) as the analogous covalent crosslinking points and the reversible hydrogen bonds among the PAM chains as the physical crosslinking points. In order to further elucidate the toughening mechanism of the PAM NCP gel, especially to understand the role of the dual crosslinking points, the PAM hybrid hydrogels (H gels) and a series of poly(acrylamide-co-dimethylacrylamide) (P(AM-co-DMAA)) NCP gels were designed and fabricated. Their mechanical properties were compared with those of the PAM NCP gels. The PAM H gels are prepared by simply mixing the PAM chains with bare silica nanoparticles (SNPs). Relative to the poor mechanical properties of the PAM H gel, the PAM NCP gel is remarkably tough and stretchable and also generates large number of micro-cracks to stop notch propagation, indicating the important role of PAM grafted VSNPs in toughening the NCP gel. In the P(AM-co-DMAA) NCP gels, the P(AM-co- DMAA) chains are grafted on VSNPs and the polydimethylacrylamide (PDMAA) only forms very weak hydrogen bonds between themselves. It is found that mechanical properties of the PAM NCP gel, such as the tensile strength and the elongation at break, are enhanced significantly, but those of the P(AM-co-DMAA) NCP gels decreased rapidly with decreasing AM content. This result reveals the role of the hydrogen bonds among the grafted polymer chains as the physical crosslinking points in toughening the NCP gel.展开更多
Mechanochromic hydrogels, a new class of stimuli-responsive soft materials, have potential applications in a number of fields such as damage reporting and stress/strain sensing. We prepared a novel mechanochromic hydr...Mechanochromic hydrogels, a new class of stimuli-responsive soft materials, have potential applications in a number of fields such as damage reporting and stress/strain sensing. We prepared a novel mechanochromic hydrogel using a strategy that has been developed to prepare dual-network(DN) hydrogels. A hydrophobic rhodamine derivative(Rh mechanophore) was covalently incorporated into a first network as a cross-linker. This first network embedded with Rh mechanophore within the DN hydrogel was pre-stretched. This guaranteed that the stress could be transferred extensively to the Rh-crosslinked first network once the hydrogel was under an applied force. Interestingly, we found that the threshold stress required to activate the mechanochromism of the hydrogel was less than 200 kPa, and much less than those in previous reports. Moreover, because of the excellent sensitivity of the hydrogel to stress, the DN hydrogel exhibited reversible freezing-induced mechanochromism. Benefiting from the sensitivity of Rh mechanophore to both p H and force, the DN hydrogel showed p H-regulated mechanochromic behavior. Our experimental results indicate that the preparation strategy we used introduces sensitive mechanochromism into the hydrogel and preserves the advantageous mechanical properties of the DN hydrogel. These results will be beneficial to the design and preparation of mechanochromic hydrogels with high stress sensitivity, and foster their practical applications in a number of fields such as damage reporting and stress/strain sensing.展开更多
本研究以构建高强度、高韧性的自修复水凝胶为目标。利用PVA和淀粉分子之间的氢键作为第一物理交联网络,PVA和硼酸分子之间的动态硼酸脂键作为第二化学交联网络,形成一种双交联结构AR/PVA-B水凝胶。AR/PVA-B水凝胶表现出杰出的机械性能...本研究以构建高强度、高韧性的自修复水凝胶为目标。利用PVA和淀粉分子之间的氢键作为第一物理交联网络,PVA和硼酸分子之间的动态硼酸脂键作为第二化学交联网络,形成一种双交联结构AR/PVA-B水凝胶。AR/PVA-B水凝胶表现出杰出的机械性能(断裂伸长率631.2%,最大应力为24.6 k Pa)和优异的自修复性能(无外界刺激的条件下,室温5 min实现94.5%自修复效率)。此外基于自修复性能水凝胶还表现出优秀的重铸性能。本研究为电子皮肤应用中的高强度和快速自修复性能的PVA水凝胶制备提供理论支持与探索。展开更多
基金financially supported by the National Natural Science Foundation of China(Nos.21474058 and 51633003)State Key Laboratory for Modification of Chemical Fibers and Polymer Materials,Donghua University(No.LK1404)+1 种基金Tsinghua University Scientific Research Project(No.2014Z22069)State Key Laboratory of Organic-Inorganic Composites,Beijing University of Chemical Technology(No.OIC-201601006)
文摘A facile method to fabricate tough and highly stretchable polyacrylamide (PAM) nanocomposite physical hydrogel (NCP gel) was proposed. The hydrogels are dually crosslinked single network with the PAM grafted vinyl hybrid silica nanoparticles (VSNPs) as the analogous covalent crosslinking points and the reversible hydrogen bonds among the PAM chains as the physical crosslinking points. In order to further elucidate the toughening mechanism of the PAM NCP gel, especially to understand the role of the dual crosslinking points, the PAM hybrid hydrogels (H gels) and a series of poly(acrylamide-co-dimethylacrylamide) (P(AM-co-DMAA)) NCP gels were designed and fabricated. Their mechanical properties were compared with those of the PAM NCP gels. The PAM H gels are prepared by simply mixing the PAM chains with bare silica nanoparticles (SNPs). Relative to the poor mechanical properties of the PAM H gel, the PAM NCP gel is remarkably tough and stretchable and also generates large number of micro-cracks to stop notch propagation, indicating the important role of PAM grafted VSNPs in toughening the NCP gel. In the P(AM-co-DMAA) NCP gels, the P(AM-co- DMAA) chains are grafted on VSNPs and the polydimethylacrylamide (PDMAA) only forms very weak hydrogen bonds between themselves. It is found that mechanical properties of the PAM NCP gel, such as the tensile strength and the elongation at break, are enhanced significantly, but those of the P(AM-co-DMAA) NCP gels decreased rapidly with decreasing AM content. This result reveals the role of the hydrogen bonds among the grafted polymer chains as the physical crosslinking points in toughening the NCP gel.
基金financially supported by the National Natural Science Foundation of China (No. 51273189)the National Science and Technology Major Project of the Ministry of Science and Technology of China (No. 2016ZX05016)the National Science and Technology Major Project of the Ministry of Science and Technology of China (No. 2016ZX05046)
文摘Mechanochromic hydrogels, a new class of stimuli-responsive soft materials, have potential applications in a number of fields such as damage reporting and stress/strain sensing. We prepared a novel mechanochromic hydrogel using a strategy that has been developed to prepare dual-network(DN) hydrogels. A hydrophobic rhodamine derivative(Rh mechanophore) was covalently incorporated into a first network as a cross-linker. This first network embedded with Rh mechanophore within the DN hydrogel was pre-stretched. This guaranteed that the stress could be transferred extensively to the Rh-crosslinked first network once the hydrogel was under an applied force. Interestingly, we found that the threshold stress required to activate the mechanochromism of the hydrogel was less than 200 kPa, and much less than those in previous reports. Moreover, because of the excellent sensitivity of the hydrogel to stress, the DN hydrogel exhibited reversible freezing-induced mechanochromism. Benefiting from the sensitivity of Rh mechanophore to both p H and force, the DN hydrogel showed p H-regulated mechanochromic behavior. Our experimental results indicate that the preparation strategy we used introduces sensitive mechanochromism into the hydrogel and preserves the advantageous mechanical properties of the DN hydrogel. These results will be beneficial to the design and preparation of mechanochromic hydrogels with high stress sensitivity, and foster their practical applications in a number of fields such as damage reporting and stress/strain sensing.
文摘本研究以构建高强度、高韧性的自修复水凝胶为目标。利用PVA和淀粉分子之间的氢键作为第一物理交联网络,PVA和硼酸分子之间的动态硼酸脂键作为第二化学交联网络,形成一种双交联结构AR/PVA-B水凝胶。AR/PVA-B水凝胶表现出杰出的机械性能(断裂伸长率631.2%,最大应力为24.6 k Pa)和优异的自修复性能(无外界刺激的条件下,室温5 min实现94.5%自修复效率)。此外基于自修复性能水凝胶还表现出优秀的重铸性能。本研究为电子皮肤应用中的高强度和快速自修复性能的PVA水凝胶制备提供理论支持与探索。