Lithium ion batteries (LIBs) are one of the most potential energy storage devices among various rechargeable batteries due to their high energy/power density, long cycle life, and low self‐discharge properties. However, current LIBs fail to meet the ever‐increasing safety and fast charge/discharge demands. As one of the main components in LIBs, separator is of paramount importance for safety and rate performance of LIBs. Among the various separators, composite separators have been widely investigated for improving their thermal stability, mechanical strength, electrolyte uptake, and ionic conductivity. Herein, the challenges and limitations of commercial separators for LIBs are reviewed, and a systematic overview of the state‐of‐the‐art research progress in composite separators is provided for safe and high rate LIBs. Various combination types of composite separators including blending, layer, core–shell, and grafting types are covered. In addition, models and simulations based on the various types of composite separators are discussed to comprehend the composite mechanism for robust performances. At the end, future directions and perspectives for further advances in composite separators are presented to boost safety and rate capacity of LIBs.

Although sodium-ion batteries (SIBs) and potassiumion batteries (PIBs) are promising prospects for next-generation energy storage devices, their low capacities and inferior kinetics hinder their further application. Among various phosphate-based polyanion materials, titanium pyrophosphate (TiP 2 O 7 ) possesses outstanding ion transferability and electrochemical stability. However, it has rarely been adopted as an anode for SIBs/PIBs due to its poor electronic conductivity and nonreversible phase transitions. Herein, an ultrastable TiP 2 O 7 with enriched oxygen vacancies is prepared as a SIB/PIB anode through P-containing polymer mediation carbonization, which avoids harsh reduction atmospheres or expensive facilities. The introduction of oxygen vacancies effectively increases the pseudocapacitance and diffusivity coefficient and lowers the Na insertion energy barrier. As a result, the TiP 2 O 7 anode with enriched oxygen vacancies exhibits ultrastable Na/K ion storage and superior rate capability. The synthetic protocol proposed here may offer a simple pathway to explore advanced oxygen vacancy-type anode materials for SIBs/PIBs.

Lithium metal batteries (LMBs) have aroused extensive interest in the field of energy storage owing to the ultrahigh anode capacity. However, strong solvation of Li + and slow interfacial ion transfer associated with conventional electrolytes limit their long-cycle and high-rate capabilities. Herein an electrolyte system based on fluoroalkyl ether 2,2,2-trifluoroethyl-1,1,2,3,3,3-hexafluoropropyl ether (THE) and ether electrolytes is designed to effectively upgrade the long-cycle and high-rate performances of LMBs. THE owns large adsorption energy with ether-based solvents, thus reducing Li + interaction and solvation in ether electrolytes. With THE rich in fluoroalkyl groups adjacent to oxygen atoms, the electrolyte owns ultrahigh polarity, enabling solvation-free Li + transfer with a substantially decreased energy barrier and ten times enhancement in Li + transference at the electrolyte/anode interface. In addition, the uniform adsorption of fluorine-rich THE on the anode and subsequent LiF formation suppress dendrite formation and stabilize the solid electrolyte interphase layer. With the electrolyte, the lithium metal battery with a LiFePO 4 cathode delivers unprecedented cyclic performances with only 0.0012% capacity loss per cycle over 5000 cycles at 10 C. Such enhancement is consistently observed for LMBs with other mainstream electrodes including LiCoO 2 and LiNi 0.5 Mn 0.3 Co 0.2 O 2 , suggesting the generality of the electrolyte design for battery applications.

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