Fig. 4: Structural evolution and internal interactions of hyperhysteresis-mediated mechanical training strategy.

A Schematic illustration of the hyperhysteresis-mediated mechanical training strategy ranging from isotropous nanofibrils to hierarchically aligned nanofibrillar network via mechanical training, to hierarchical fibrillar network interpenetrated by chemically cross-linked network via UV light-initiated radical polymerization. SEM images and corresponding 2D WAXS patterns of (B) SN–H, C SN–E before and after mechanical training and (D) mechanically trained DN–E (n = 3 independent samples). E The 1D WAXS profiles of SN–H, SN–E and DN–E. The WAXS intensity profiles develop remarkable crystalline peaks of PVA after solvent substituting and mechanical training. F The 1D SAXS profiles of corrected scattering intensity Iq2 versus vector q for SN–H, SN–E with mechanical training and mechanically trained DN–E. The scattering peak emerged in the low q region gradually increases, indicating that the intercrystal spacing between neighboring nanocrystalline domains decreases after solvent substituting and mechanical training. G Schematic diagram of the structural arrangement of water cluster-PVA, DES ball-PVA, PAAc-PVA and PVA-PVA obtained by DFT optimizations. H Comparison of interaction energy of water cluster and DES ball, water cluster-PVA, DES ball-PVA, PAAc-PVA and PVA-PVA obtained by DFT calculations. I Structure and electrostatic potential distribution of water cluster and DES ball obtained by DFT optimizations. J Representative DSC thermographs of SN–H, SN–E with mechanical training and mechanically trained DN–E to measure the crystallinities. Compared with SN–H, SN–E and DN–E show significant endothermic peaks of PVA nanocrystalline domains. K Measured average crystallinities of SN–H in the dry states, SN–E without mechanical training and mechanically trained DN–E. L Schematics indicate the structural evolution and enhanced nanocrystalline domains in the process of carrying out hyperhysteresis-mediated mechanical training strategy.