It remains challenging to develop stretchable and self‐healable polymer electrolytes with improved ion‐conductive nature for high‐performance multifunctional flexible supercapacitors. Herein, a P(AM‐SBMA‐AMPS)‐SiO₂ zwitterion‐containing polyelectrolyte hydrogel is fabricated via copolymerization of acrylamide (AM), sulfobetaine methacrylate (SBMA) zwitterionic monomer, and 2‐acrylamido‐2‐methyl‐1‐propanesulfonic acid (AMPS) anionic monomer grafted from the surface of vinyl silica nanoparticles (VSNPs). The hydrogen bonding among polymer chains and the high‐density dynamic ionic interactions between SBMA and AMPS work as reversible “sacrificial bonds” to toughen hydrogel, while the VSNPs function as multifunctional crosslinkers and stress transfer centers, which makes these hydrogels tough (fracture energy 2.7 MJ m⁻³), stretchable (fracture strain 4,016%), and self‐healable (fracture strain of healable sample 775%). More importantly, this zwitterion‐containing polyelectrolyte hydrogel exhibits high ionic conductivities (3.4 S m⁻¹) owing to the highly hydration capacity of the zwitterionic polyelectrolyte copolymer which produced efficient ion migration channels for ion transport. Accordingly, a flexible supercapacitor based on this multifunctional hydrogel as electrolyte demonstrates a high electric double‐layer capacitive capacitance of 60.6 F g⁻¹ at 0.5 A g⁻¹ and excellent capacitance retention of ~98% over 1,000 cycles as well as encouraging electrochemical properties at subzero temperature. This work provides new insights into the synthesis of highly conductive and multifunctional polyelectrolyte hydrogels for high‐performance flexible supercapacitors. © 2020 Wiley Periodicals, Inc.

中文翻译：

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具有高离子导电性的可逆性高拉伸性和自愈性两性离子聚电解质水凝胶，用于高性能柔性和耐寒超级电容器

对于高性能多功能柔性超级电容器而言，开发具有改善的离子导电性的可拉伸和自修复聚合物电解质仍然具有挑战性。这里是P（AM‐SBMA‐AMPS）‐SiO ₂含两性离子的聚电解质水凝胶是通过丙烯酰胺（AM），磺基甜菜碱甲基丙烯酸酯（SBMA）两性离子单体和从乙烯基二氧化硅纳米粒子表面接枝的2-丙烯酰胺基-2-甲基-1-丙烷磺酸（AMPS）阴离子单体的共聚反应制得的（ VSNP）。聚合物链之间的氢键以及SBMA和AMPS之间的高密度动态离子相互作用充当可逆的“牺牲键”，以增韧水凝胶，而VSNP则充当多功能交联剂和应力传递中心，使这些水凝胶坚韧（断裂能2.7 MJ m ^-3），可拉伸（断裂应变为4016％）和可自愈（可修复样品的断裂应变为775％）。更重要的是，由于两性离子聚电解质共聚物的高水合能力，该含两性离子的聚电解质水凝胶显示出高的离子电导率（3.4 S m ^-1），从而产生了有效的离子迁移通道以进行离子传输。因此，基于这种多功能水凝胶作为电解质的柔性超级电容器在0.5 A g ^-1下显示出60.6 F g ^-1的高双电层电容在1,000次循环中具有约98％的出色电容保持率，并在零以下温度下具有令人鼓舞的电化学性能。这项工作为合成用于高性能柔性超级电容器的高导电性和多功能聚电解质水凝胶提供了新的见解。©2020 Wiley Periodicals，Inc.