“…To address the Li dendrite issues associated with Li metal anodes, researchers have investigated various approaches, − including introducing stable hosts, − modifying structures of current collectors, − constructing artificial solid electrolyte interphase (SEI), − separator modification, − and optimizing electrolyte composition. − As an important component in batteries, separator plays a critical role in determining the diffusion of Li ions and safety issues of Li-ion batteries. − Due to its chemical stability, relatively low price, no requirement to change either electrode or electrolyte systems, commercial polyolefin separator modification is a convenient alternative to regulate the Li deposition behavior . Also recently, a growing number of works have demonstrated that surface modification of separator is a promising route to avoid Li dendritic growth, , their schemes including improving separator wettability, regulating Li ionic flux, − and lithiophilic modifications. , However, due to huge Young’s modulus difference between the coating layer and the substrate, the intrinsic low surface energy of polyolefin separator, and continuous immersion in the polar electrolyte during charge/discharge cycles, the drop-dregs phenomenon of the coating layer desquamated from polyolefin separator extensively exists in traditional separator modification methods. − Unfortunately, these detached points would act as defects that cause a nonuniform Li ionic flux and increase in separator impedance, finally resulting in the generation of Li dendrite, significantly diminished practical performance, and even serious safety concerns of Li metal batteries. − Hence, the drop-dregs issue is still a big hurdle for separator modification methods toward long-term stable Li metal anodes because of potential failure at interface connection, especially between the soft separator and the rigid inorganic coating layer.…”