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As an important part of artificial intelligence, electronic skin has received more and more attention recently. However, two serious issues, slow self-healing and lack of direction recognition, have limited the burgeoning of electronic skin largely. Herein, for the first time we report a dual network flexible hydrogel, which was synthesized via cross-linking polyvinyl alcohol (PVA) and polyethylenimine (PEI) with 4-formylbenzoboric acid (Bn) to form a polymer network and then incorporating MXene into the polymer network. Due to the synergy of multiple reversible dynamic covalent bonds and supramolecular interactions, the PVA/Bn/PEI/MXene (PBPM) hydrogel exhibits direction-aware and ultrafast self-healing abilities (self-healing time ∼0.06 s) as well as rapid response performance (signal response time ∼0.12 s). Furthermore, an electronic skin strain sensor assembled by using the PBPM hydrogel can not only efficiently detect the movements in different parts of the prosthetic person body but also specifically identify the directions of the movements including head-down/up and wrist-down/up. The flexible PBPM hydrogel in this work has shown great potential in the applications of artificial skin, soft robots, health monitoring and human-machine exchange interfaces.

Layered double hydroxides (LDHs) have shown remarkable potentials in supercapacitors for their highly-redox capacitance. However, the poor contact with substrate, slow charge transfer and ion diffusion, and low electrical conductivity limit their capacitor performance. In this work, a flexible free-standing supercapacitor was designed, with in-situ grown hollow-structured NiCo layered double hydroxide (H–NiCo LDH) as the active material based on a partial Ni ion substitution of Co ion in ZIF-67, and flexible carbon material as the substrate. Systematical investigation has been conducted in terms of nanostructures of the active material NiCo LDH (hollow or laminar structure) and flexible carbon substrates (acidified carbon cloth or acidified carbon fibers). A hollow-structured NiCo LDH@acidified carbon cloth (H–NiCo LDH@ACC) sample showed a promising capacity of 1377 mC/cm2 (3060 mF/cm2) at 1 mA/cm2, a low charge transfer resistance of 0.15 Ω, a capacity retention of 70% and a coulombic efficiency retention of 99% upon 10,000 cycles at 80 mA/cm2. PDMS-sealed solid-state H–NiCo LDH@ACC//AC devices were fabricated with an energy density of 0.0708 mWh/cm2 at a power density of 0.7 mW/cm2, with no obvious capacity decrease upon bending angles from 0° to 180°. SEM, EDS, XPS, and XRD analyses indicated the H–NiCo LDH has been in-situ grown on flexible carbon substrates. Hollow-structured LDH accelerated charge transfer and ion diffusion compared with a laminar-structured LDH. Acidified carbon cloth (ACC) showed better electrical conductivity compared with the biomass-derived acidified carbon fibers. Thus, a H–NiCo LDH@ACC is proposed as a promising candidate of a flexible supercapacitor.