storage devices with adjustable shapes and high flexibility, which is promising for the burgeoning portable and wearable electronics. [7][8][9] Furthermore, the flexibility and elasticity of GPEs are also prone to tolerate the volume change of electrode materials and the dendrites of lithium metal during charge and discharge processes. [10][11][12][13] As a consequence, GPEs have become one of the most desirable alternatives among various electrolytes for the electrochemical energy storage devices, and significant progress has been made in lithium-ion batteries (LIBs), supercapacitors (SCs), lithium-oxygen (Li-O 2 ) batteries as well as the other kinds of electrochemical energy storage devices, such as sodium-ion batteries, lithium-sulfur batteries, fuel cells, and zinc-air batteries. [14][15][16] In order to meet the requirements of wearable devices for flexibility and deformability, more special GPEs with tough, [17] stretchable, [18] and compressible [19] functionalities have been also developed.Typically, a polymeric framework is adopted in GPEs as host material, providing high mechanical integrity. Several criteria for a good polymer host lie in: [20][21][22] (i) fast segmental motion of polymer chain; (ii) special groups promoting the dissolution of salts; (iii) low glass transition temperature (T g ); (iv) high molecular weight; (v) wide electrochemical window; (vi) high degradation temperature. Within the framework, the salts in the GPEs serve as the sources of the charge carriers, which are generally required to have large anions and low dissociation energy for easier dissociating-induced free/mobile ions. According to the types of electrolytes, there are four categories of GPEs based on proton, [23] alkaline, [24] conducting salts, and ionic liquids (ILs). [25] The criteria for an appropriate electrolyte include: [26][27][28] (i) good dissociation without forming ion pairs or ion aggregation; (ii) high thermal, chemical, and electrochemical stability; (iii) high ionic conductivity. In order to dissolve both the polymer hosts and electrolytic salts, the organic/ aqueous solvents are introduced to provide the medium for ionic conduction. A good solvent should simultaneously have high dielectric constant (ɛ > 15), donor number for more dissociation of ion and chemical and electrochemical stability. Organic solvents normally include ethylene carbonate (EC), propylene carbonate (PC), diethyl carbonate (DEC), dimethyl carbonate (DMC), dimethyl formamide (DMF), dimethyl sulphoxide, ethyl methyl carbonate, and tetrahydrofuran.To prepare a high-performance GPE, it is essential to select the species of host polymer, solvent, and electrolytic salt, and then blend them by solution or melt processes, such as casting With the booming development of flexible and wearable electronics, their safety issues and operation stabilities have attracted worldwide attentions. Compared with traditional liquid electrolytes, gel polymer electrolytes (GPEs) are preferred due to their higher safety and adaptability to the design of ...

HIGHLIGHTSFlexible aqueous belt-and fibershaped SIBs with high safety are fabricated Normal saline and cell-culture medium are used directly as electrolytes for SIBs Fiber-shaped SIBs exhibit an electrochemical deoxygenation function

Owing to the high theoretical energy density of metal-air batteries, the aluminum-air battery has been proposed as a promising long-term power supply for electronics. However, the available energy density from the aluminum-air battery is far from that anticipated and is limited by current electrode materials. Herein we described the creation of a new family of all-solid-state fiber-shaped aluminum-air batteries with a specific capacity of 935 mAh g(-1) and an energy density of 1168 Wh kg(-1) . The synthesis of an electrode composed of cross-stacked aligned carbon-nanotube/silver-nanoparticle sheets contributes to the remarkable electrochemical performance. The fiber shape also provides the aluminum-air batteries with unique advantages; for example, they are flexible and stretchable and can be woven into a variety of textiles for large-scale applications.

Flexible lithium-ion batteries are critical for the next-generation electronics. However, during the practical application, they may break under deformations such as twisting and cutting, causing their failure to work or even serious safety problems. A new family of all-solid-state and flexible aqueous lithium ion batteries that can self-heal after breaking has been created by designing aligned carbon nanotube sheets loaded with LiMn O and LiTi (PO ) nanoparticles on a self-healing polymer substrate as electrodes, and a new kind of lithium sulfate/sodium carboxymethylcellulose serves as both gel electrolyte and separator. The specific capacity, rate capability, and cycling performance can be well maintained after repeated cutting and self-healing. These self-healing batteries are demonstrated to be promising for wearable devices.

It is highly desirable to develop flexible and efficient energy-storage systems for widely used wearable electronic products. To this end, fiber-shaped lithium-ion batteries (LIBs) attract increasing interest due to their combined superiorities of miniaturization, adaptability, and weavability, compared with conventional bulky and planar structures. Recent advances in the fabrication, structure, mechanism, and properties of fiber-shaped LIBs are summarized here, with a focus on the electrode material. Remaining challenges and future directions are also highlighted to provide some useful insights from the viewpoint of practical applications.

A fiber-shaped aqueous lithium ion battery is developed with ultrafast charge–discharge rates and high power density in addition to high energy density.

A shape-memory, fiber-shaped supercapacitor is developed by winding aligned carbon nanotube sheets on a shape-memory polyurethane substrate. Despite its flexibility and stretchability, the deformed shapes under bending and stretching can be "frozen" as expected and recovered to the original state when required. Its electrochemical performances are well-maintained during deformation, at the deformed state and after the recovery.

Although lithium-oxygen batteries possess ah igh theoretical energy density and are considered as promising candidates for next-generation power systems,t he enhancement of safety and cycling efficiency of the lithium anodes while maintaining the high energy storage capability remains difficult. Here,w eo vercome this challenge by cross-stacking aligned carbon nanotubes into porous networks for ultrahighcapacity lithium anodes to achieve high-performance lithiumoxygen batteries.T he novel anode shows ar eversible specific capacity of 3656 mAh g À1 ,approaching the theoretical capacity of 3861 mAh g À1 of pure lithium. When this anode is employed in lithium-oxygen full batteries,t he cycling stability is significantly enhanced, owingt ot he dendrite-free morphology and stabilized solid-electrolyte interface.This work presents anew pathway to high performance lithium-oxygen batteries towards practical applications by designing cross-stacked and aligned structures for one-dimensional conducting nanomaterials.