Reversible Deposition of Lithium Particles Enabled by Ultraconformal and Stretchable Graphene Film for Lithium Metal Batteries

Abstract

Originating from inhomogeneous Li deposition and dissolution, the formation of dendritic and/or dead Li lies as a fundamental barrier to the practical implementation of Li metal anodes for high‐energy Li‐ion batteries. Here, an ultraconformal and stretchable solid‐electrolyte interphase (SEI) composed of parallelly stacked few‐layer defect‐free graphene nanosheets, which can deform to remain ultraconformal during the expansion and shrinkage of micro‐sized Li metal particles is reported. The shape‐adaptive graphene protective skin is prepared via a facile mechanical method followed by Li stripping, which enables fast Li‐ion diffusion, and inhibits Li dendrites and Li pulverization. The interlayer slips and wrinkles of the graphene film endow the robust protective skin with high stretchability. This work represents a unique strategy of building ultraconformal and stretchable 2D‐materials‐based protective skins on the surface of Li metal toward high‐energy, long‐life, and safe Li metal batteries.

Self‐Healing Properties of Alkali Metals under “High‐Energy Conditions” in Batteries

“…[14] All the abovementioned limitations can be overcome or reduced if dendrite growth/breakage can be prevented during the deposition/ dissolution process. Many studies have been reported on the construction of dendrite-free metal anodes: a) fabrication of modified electrodes or metal substrate surfaces, [15][16][17][18][19][20][21][22][23][24] b) synthesis of new electrolytes, [25][26][27][28][29] c) use of solid electrolytes, [22,[30][31][32] and d) improvement of the electrode-electrolyte interface. [9,15,33,34] However, these studies have rarely focused on the properties, such as the stability of dendrites during charging and discharging, of dendrites.…”

Commercialization‐Driven Electrodes Design for Lithium Batteries: Basic Guidance, Opportunities, and Perspectives

“…Similarly, stacked graphene layers were reported to protect Li metal anode by a facile and low-cost strategy (Figure 16e). [280] The graphene was from mechanical shear-induced exfoliation of graphite, and then incorporated into Li foil by parallel alignment. The dense graphene layers not only acted as ultra-conformal SEI layer on Li anode, but also functioned as a shape-adaptive protective skin for Li deposition beneath it.…”

“…e) Schematic illustration of Li deposition behavior with nondeformable SEI and deformable SEI with graphene coating. Reproduced with permission [280]. Copyright 2019, Wiley-VCH.…”

Characterizing Batteries by In Situ Electrochemical Atomic Force Microscopy: A Critical Review

“…To date, various methods aiming to engineer the electrode—electrolyte interface have been shown to be effective in optimizing the SEI layer and suppressing lithium dendrite growth. Strategies include optimizing electrolyte composition, [ 151 ] using additives, [ 152 ] constructing an artificial SEI, [ 153,154 ] use of graphene, [ 155 , 156 ] or covalent organic framework protection layers, [ 157 ] and lowering anode roughness and stress. [ 158,159 ]…”