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Rechargeable batteries have been a profoundly greater part of our lives than we could have ever imagined. The rechargeable Li‐ion batteries (LIBs) that have been developed for transport systems even put fossil fuels in the corner. However, state‐of‐the‐art Li‐ion batteries with graphite anodes are now approaching their theoretical specific energy limits, so they cannot meet the increasing demands of a range of portable electronics and large‐scale energy storage systems. Li metal is one of the most promising anode materials that could break through the energy density bottleneck of Li‐ion batteries due to its ultrahigh specific capacity and very low potential compared to other anode materials. Nonetheless, the direct use of Li metal in commercial battery systems has been hindered due to significant obstacles associated with it such as safety issues, corrosion from chemical reactions that occur inside the battery, or poor cycling performance. The fundamental reason for these problems is the dendritic growth of Li‐ions on the Li metal anode during cycling, as a result of the interfacial phenomena of Li metal and electrolytes. Modification of the Li metal interface with an electrolyte presents an efficient solution to solve these problems. In this review, the current challenges facing the development of Li metal anodes are presented in detail. The most recent advances in Li metal anodes using a controlled interface between the Li metal surface and an electrolyte are highlighted and an introduction on the synthesis and production methods for the application of high‐energy‐density battery systems such as Li‐oxygen (Li−O2), Li‐sulfur (Li−S), and Li metal batteries with high‐energy density cathodes is presented. Furthermore, the recent developments in the in situ/operando analysis tools adopted for the investigation of Li metal anodes such as the structural and chemical changes, dynamic properties, and solid–electrolyte interface (SEI) layer properties are described and summarized. Finally, some suggestions are given in the direction of the development of Li metal with artificial surface layers for use in future high‐energy batteries.

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High-capacity anode materials are promising candidates for increasing the energy density of lithium (Li)-ion batteries due to their high theoretical capacities. However, a rapid capacity fading due to the huge volume changes during charge-discharge cycles limits practical applications. Herein, a layering-charged polymeric binder is introduced that can effectively integrate high-capacity anodes using a strong yet reversible Coulomb interaction and enriched hydrogen bonding. The charged polymeric binder builds a dynamically charge-directed network on the active materials with high versatility and efficiently dissipates the electrode stress with its excellent mechanical properties. In addition, poly(ethylene glycol) (PEG) moieties of the charged binder offer a fast Li-ion conduction pathway that can form an ultra-thick silicon oxide (SiO x )-based electrode (≈10.2 mAh cm −2 ) without compromising the reversible specific capacity and promote effective charge interaction as a mechanical modulator. Such an unprecedented charge-directed binder provides insights into the rational design of a binder for high-capacity anodes.

which can be realized by advancing battery materials and engineering the cell architectures. Particularly, automotive battery technology has been extensively evaluated and provides relatively stringent requirements on key performance indicators such as fast-charging capability and maximum energy density along with other critical factors (battery lifetime (>8 years), robustness to wide temperature, and safety), while non-EV batteries are flexible and tolerable in their design. [1] Putting differently, such practical standards guided for EV batteries assist battery scientists, at least in the academia, in aligning the ultimate goal and initiative for advanced battery developments, despite the recent application of new cell chemistry (typically known as post-lithium (Li) or beyond Li), [2] which have raised emerging challenges that require multiscale material-level understanding, design, and breakthroughs across the cell architecture. [3] Automotive battery technology has made great strides in terms of cost, process, and material perspective, yet advancing the batteries invariably starts with new battery chemistry and consequently new material chemistry in its major (e.g., cathode, anode, electrolyte, separator) and complementary cell components (e.g., current collector, binder, tap, packaging, etc.). Polymeric materials are indispensable to the design of batteries regardless of battery shape, size, chemistry, and manufacturing at the lab or industry scale as processable at every strategic point of battery production with multifunctionalities and cost-effectiveness. [4] From the conventional viewpoint, the role (or function) of polymeric materials has been confined to the structural support of composite electrodes and devices and the physical barrier between the cathode and anode for battery safety. Figure 1a shows the multiscale use of polymeric materials in a single cell and device. The polymeric binder serves as a chemical adhesive capable of maintaining the electrode integrity, ensuring electron/ion diffusion, and uniformly distributing the active material (Figure 1b). [5] A separator commonly fabricated from semicrystalline polyolefin (e.g., polyethylene (PE) and polypropylene (PP)), provides an ionic conduction path through a liquid electrolyte filling pores and electrically separates the two electrodes to prevent a battery short circuit, thereby directly related to safety (Figure 1c). [6] Additionally, a polymer has been used as a matrix for reducing the portion of flammable liquid solvent Riding on the rapid growth in electric vehicles and the stationary energy storage market, high-energy-density lithium-ion batteries and next-generation rechargeable batteries (i.e., advanced batteries) have been long-accepted as essential building blocks for future technology reaching the specific energy density of 400 Wh kg −1 at the cell-level. Such progress, mainly driven by the emerging electrode materials or electrolytes, necessitates the development of polymeric materials with advanced functionalities in the battery t...

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Lithium-based batteries have been attractive as promising energy storage systems in recent decades and they have been widely available since the rechargeable battery is closely related to human life. The...