Energy-storage technologies such as lithium-ion batteries and supercapacitors have become fundamental building blocks in modern society. Recently, the emerging direction toward the ever-growing market of flexible and wearable electronics has nourished progress in building multifunctional energy-storage systems that can be bent, folded, crumpled, and stretched while maintaining their electrochemical functions under deformation. Here, recent progress and well-developed strategies in research designed to accomplish flexible and stretchable lithium-ion batteries and supercapacitors are reviewed. The challenges of developing novel materials and configurations with tailored features, and in designing simple and large-scaled manufacturing methods that can be widely utilized are considered. Furthermore, the perspectives and opportunities for this emerging field of materials science and engineering are also discussed.

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The fundamental understandings and technological innovations in lithium-ion batteries are essential for delivering high energy density, stable cyclability, and cost-effective energy storages with the growing demands in the applications of electrical vehicles and smart grid. Solid-state electrolytes (SSEs) are more promising than organic liquid electrolyte in terms of excellent safety in developing lithium-metal anode as well as other high-capacity cathode chemistries, such as sulfur and oxygen. Considerable efforts have been made to give birth to the superionic conductors with ionic conductivities higher than 10 À3 S cm À1 at room temperature. However, the high interfacial impedances from the poor compatibility of SSEs with electrodes limit their practical applications, which are discussed in this review. Furthermore, the recent advances and critical challenges for all-solid-state lithium-metal batteries based on the cathode materials of lithium-intercalation compounds, sulfur, and oxygen are overviewed, and their future developments are also prospected.

The widespread implementation of high-energy-density lithium metal batteries has long been fettered by lithium dendrite-related failure. Here we report a new strategy to address the issue of dendrite growth by a polyimide-coating layer with vertical nanoscale channels of high aspect ratio. Smooth, granular lithium metal was deposited on the modified electrode instead of typical filamentary growths. In a comparison with the bare planar electrode, the modified electrode achieved greatly enhanced Coulombic efficiency and longer cycle life. Homogeneous Li flux distribution above the modified electrode from the nanochannel confinement can account for a uniform Li nucleation and a nondendrite growth. We also demonstrated that the polyimide coating with microscale pores loses the confinement effects and fails to suppress lithium dendrites. This strategy of spatially defined lithium growth in vertical-aligned nanochannels provides a novel approach and a significant step toward stabilizing Li metal anodes.

Modern lithium ion batteries are often desired to operate at a wide electrochemical window to maximize energy densities. While pushing the limit of cutoff potentials allows batteries to provide greater energy densities with enhanced specific capacities and higher voltage outputs, it raises key challenges with thermodynamic and kinetic stability in the battery. This is especially true for layered lithium transition-metal oxides, where capacities can improve but stabilities are compromised as wider electrochemical windows are applied. To overcome the above-mentioned challenges, we used atomic layer deposition to develop a LiAlF solid thin film with robust stability and satisfactory ion conductivity, which is superior to commonly used LiF and AlF. With a predicted stable electrochemical window of approximately 2.0 ± 0.9 to 5.7 ± 0.7 V vs Li/Li for LiAlF, excellent stability was achieved for high Ni content LiNiMnCoO electrodes with LiAlF interfacial layer at a wide electrochemical window of 2.75-4.50 V vs Li/Li.