Electrically activated soft actuators with large deformability are important for soft robotics but enhancing durability and efficiency of electrochemical actuators is challenging. Herein, we demonstrate that the actuation performance of an ionic two-dimensional covalent-organic framework based electrochemical actuator is improved through the ordered pore structure of opening up efficient ion transport routes. Specifically, the actuator shows a large peak to peak displacement (9.3 mm, ±0.5 V, 1 Hz), a fast-response time to reach equilibrium-bending (~1 s), a correspondingly high bending strain difference (0.38%), a broad response frequency (0.1–20 Hz) and excellent durability (>99%) after 23,000 cycles. The present study ascertains the functionality of soft electrolyte as bionic artificial actuators while providing ideas for expanding the limits in applications for robots.

We rationally synthesized the thermoplastic and hydrophilic poly(urethane-acrylate) (HPUA) binder for a type of printable and stretchable Ag flakes–HPUA (Ag-HPUA) electrodes in which the conductivity can be enhanced by human sweat. In the presence of human sweat, the synergistic effect of Cl− and lactic acid enables the partial removal of insulating surfactant on silver flakes and facilitates sintering of the exposed silver flakes, thus the resistance of Ag-HPUA electrodes can be notably reduced in both relaxed and stretched state. The on-body data show that the resistance of one electrode has been decreased from 3.02 to 0.62 ohm during the subject’s 27-min sweating activity. A stretchable textile sweat-activated battery using Ag-HPUA electrodes as current collectors and human sweat as the electrolyte was constructed for wearable electronics. The enhanced conductivity of the wearable wiring electrode from the reaction with sweat would provide meritorious insight into the design of wearable devices.

Biological ion channels rely on ions as charge carriers and unidirectional ion flow to produce and transmit signals. To realize artificial biological inspired circuitry and seamless human-machine communication, ion-transport-based rectification devices should be developed. In this research, poly(methyl methacrylate) (PMMA) and poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) gel polymer electrolytes (GPEs) are assembled to construct a novel ionic diode, enabling ion rectification through ion-diffusion/migration that emulates biological systems. This ion rectification results from the different diffusion/migration behaviors of mobile ions transporting in the GPE heterojunction. The electrical tests of the GPE heterojunction reveal outstanding rectifying ratio of 23.11. The GPE ionic diode operates in wide temperature window, from −20 °C (anti-freezing) to 125 °C (thermal tolerance). The absence of redox reactions is verified in the cyclic voltammogram. The GPE ionic diodes are used to construct ionic logic gates for signal communication. Furthermore, rectification of a triboelectric nanogenerator and potential for synaptic devices are demonstrated.

An electrochromic device (ECD), which can switch between black and transmissive states under electrical bias, is a promising candidate for smart windows due to its color neutrality and excellent durability. Most of the black ECDs are achieved through a reversible electrodeposition and dissolution mechanism; however, they typically suffer from relatively poor cycling stability and a slow coloration/ bleaching time. Herein, we present a heat-insulating black ECD with a gel electrolyte that operates via reversible Ni−Cu electrodeposition and dissolution. With the adoption of a Cu alloying strategy and a compatible gel electrolyte, this two-electrode ECD (5.0 cm × 2.5 cm) can achieve a cycling stability of 1500 cycles with transmittance modulation up to 55.2% in short coloration (6.2 s) and bleaching times (13.2 s) at a wavelength of 550 nm. Additionally, the ECD can be switched from the transparent state (visible light transmittance: 0.566) to the opaque state (visible light transmittance: 0.003) within 1 min, reaching transmittance less than 5% across the visible−near-infrared spectrum (400−2000 nm) to efficiently block solar heat. Besides, in the voltage-off state, the black Ni−Cu alloy film can be sustained for more than 60 min (at room temperature, λ = 550 nm). Under infrared irradiation (170 W/m 2 ) for 30 min, the black ECD blocks up to 35.0% of infrared radiation, which not only effectively prevents the heat transmission for energy management but also finds potential applications for promoting indoor human health and indoor farming.

Formation of ionogels through in situ polymerization can effectively improve electrolyte processability; however, the curing process has been slow and oxygen‐sensitive. Considering the low oxygen solubility of poly(ionic liquid)s (PILs), in situ polymerized ionogels are designed to realize excellent electrolytes. Herein, two in situ polymerized ionogels (PIL A & PIL B) are formulated, and they can be rapidly photocured within a minute. The ionogels are highly transparent, stretchable, and exhibit excellent physicochemical stability, including thermal, electrochemical, and air stability, allowing them to perform in various conditions. Benefitting from these properties, two high‐performance electrochromic devices (ECDs) are assembled, with iron‐centered coordination polymer (FeCP) and tungsten oxide (P‐WO3) electrochromic materials, achieving high color contrast (45.2% and 56.4%), fast response time (1.5/1.9 and 1.7/6.4 s), and excellent cycling endurance (>90% retention over 3000 cycles). Attributed to the thermal robustness of the ionogels, the ECDs can also be operated over a wide temperature range (−20 to 100 °C). With the use of deformable substrates (e.g., ultrathin ITO glass), curved electrochromic eye protector and flexible electrochromic displays are realized, highlighting their potential use in futuristic wearables.