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Supporting Information Strong and Tough Fully Physically Crosslinked Double Network Hydrogels with Tunable Mechanics and High Self-Healing Performance Xiao-Hui Wang, Fei Song*, Dan Qian, Yao-Dong He, Wu-Cheng Nie, Xiu-Li Wang, Yu-Zhong Wang* Center for Degradable and Flame-Retardant Polymeric Materials (ERCPM- MoE), College of Chemistry, State Key Laboratory of Polymer Materials Engineering, National Engineering Laboratory of Eco-Friendly Polymeric Materials (Sichuan), Sichuan University, 29 Wangjiang Road, Chengdu 610064, China. * Corresponding authors: [email protected]; [email protected] 1

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Supporting Information

Strong and Tough Fully Physically Crosslinked

Double Network Hydrogels with Tunable

Mechanics and High Self-Healing PerformanceXiao-Hui Wang, Fei Song*, Dan Qian, Yao-Dong He, Wu-Cheng Nie, Xiu-Li Wang,

Yu-Zhong Wang*

Center for Degradable and Flame-Retardant Polymeric Materials (ERCPM-MoE), College of Chemistry, State Key Laboratory of Polymer Materials Engineering, National Engineering Laboratory of Eco-Friendly Polymeric Materials (Sichuan), Sichuan University, 29 Wangjiang Road, Chengdu 610064, China.* Corresponding authors: [email protected]; [email protected]

Figure S1. UV−Vis spectra of different samples to clarify the interaction between Fe3+ and PAA

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(pH 1.5).

Figure S2. UV−Vis spectra of the solutions containing CS and Fe3+ at different pH values.

Figure S3. SEM images of (a) the PAA-Fe3+/CS SN hydrogel and (b) DN hydrogel.

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Figure S4. (a) Frequency dependence of the storage modulus G′, loss modulus G″, and tanδ of the PAA-Fe3+/CS DN hydrogel at a controlled strain of 0.5% at different temperatures, and (b) Arrhenius plot for the temperature-dependent shift factors

Figure S5. Effects of immersion time and Fe3+ amount on the storage moduli of PAA-Fe3+/CS hydrogels collected within sweep frequency from 0.01 Hz to 100 Hz.

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Figure S6. Compressive stress-strain curves of (a) the PAA-Fe3+/CS SN hydrogel and (b) DN hydrogel.

Figure S7. Effect of recovery time on the recovery rate of (a) the PAA-Fe3+/CS SN hydrogel and (b) DN, in terms of tensile stress at the fixed strain of 200%.

Figure S8. Dissipated energy of (a) the PAA-Fe3+/CS SN hydrogel and (b) DN hydrogel during the first and second ten successive loading-unloading measurements.

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Figure S9. Salt and acid resistance of hydrogels. The photos of (a) SN and (b) DN hydrogels after incubation in saline solution with different NaCl concentrations (0.25 g/ml, 0.38 g/ml, and 0.50 g/ml); the photos of (c) SN and (d) DN hydrogels after incubation in acidic solutions (0.38 g/ml NaCl) with different pH values of 1.5, 3.0, and 4.5, respectively (Incubation time: 60 h).

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