Revealing the Principles of Confining Electroplated Lithium beneath the CVD Grown Single Layer 2D Materials

Abstract Owing to the nanoscale thickness, excellent mechanical and chemical stabilities, 2D materials including graphene and hexagonal boron nitride have emerged as promising artificial solid electrolyte interphase (SEI) candidates for lithium metal batteries. However, whether the implementation of 2D materials is beneficial to electrochemical performance remains controversial, and the key to confining the electroplated Li beneath the 2D materials remains elusive. Here, a nanocrystalline graphene (NG) film is synthesized on high‐carbon Cu and the Li plating/stripping behavior on Cu grown with different 2D materials is investigated. Interestingly, in contrast to the commonly obtained Li particles on other substrates during nucleation, a smooth Li layer is obtained on NG/Cu, leading to a compact Li layer with more stable electrochemical performance. The finite element method simulations validate that the low electrical conductivity and the high density of defects on NG film drive the fast entry of electrolytes into the NG/Cu interface and promote homogenous Li nucleation. This work reveals the principles of confining electroplated Li beneath the 2D materials, and paves the way for the applications of 2D materials in artificial SEIs and anode‐free lithium metal batteries.