Lithiophilic‐Gradient, Li<sup>+</sup> Supplementary Interphase Design for Lean Lithium Metal Batteries
Cheng Lü, Jiacheng Liu, Yingche Wang, Helin Wang, Ahu Shao, Chunwei Li, Zhiqiao Wang, Yaxin Zhang, Yunsong Li, Jiawen Tang, Yuxiang Guo, Ting Liu, Xiaodong Zhao, Yue Ma
Abstract
Abstract The practicability of anode‐less/free lithiummetal batteries (LMBs) is impeded by unregulated dendrite formation on thedeposition substrate. Herein, this study presents a lithiophilic‐gradient, layer‐stacked interfacial design for the lean lithium metal battery (LLMB) model. Engineered via a facile wet‐chemistry approach, the high entropy metalphosphide (HEMP) particles with tunable lithiophilic species are dispersedwithin reduced graphene oxide (RGO). Moreover, a poly (vinylidene fluoride co‐hexafluoropropylenepolymer) (PVDF‐HFP), blended with molten Li at the tailorable amounts, forms aLi supplementary top layer through a layer‐transfer printing technique. Theintegrated layer (HEMP@RGO‐MTL@PH) not only regulates the dendrite‐free lithiumdeposition towards the Cu substrate up to 10 mAh cm −2 , but also maintains robust cyclability of the symmetric cell at 5 mA cm −2 even under 83% depth of discharge. As pairing the modified Cu foil with the LiNi 0.8 Mn 0.1 Co 0.1 O 2 cathode (NCM811, 16.9 mg cm −2 , double sided, N/P ratio of 0.21) in the 200 mAh pouch cell, achieves gravimetric energy densities of 414.7 Wh kg −1 , power output of 977.1 W kg −1 , as well as highly reversible phasic evolutionmonitored in operando. This gradient interfacial strategy can promotethe commercialization of energy/power‐dense energy storage solutions.