A jigsaw-structured artificial solid electrolyte interphase for high-voltage lithium metal batteries

Abstract

The practical application of lithium-metal batteries is hindered by insufficient lithium Coulombic efficiency and uncontrolled dendrite growth, bringing a challenge concerning how to create robust solid electrolyte interphases (SEIs) that can regulate Li+ transport and protect reactive lithium-metal. Here, we present the rational construction of a multi-component jigsaw-like artificial SEI by the integration of fluorine-containing silane and polyether-containing silane. The fluorine-donating group prevents the parasitic reaction and yields a dense structure for homogeneous lithium deposition. Additionally, the lithophilicity of ethylene glycol backbone facilitates the rapid transport of Li+ and the cross-linked network increases mechanical robustness of the SEI. With this artificial SEI, we show highly reversible lithium plating and stripping cycling for more than 500 hours. Moreover, we also demonstrate stable operation of high-voltage LiNi0.8Co0.1Mn0.1O2 cathode in both coin and pouch cells under high loading, limiting excess lithium, and lean electrolyte conditions, holding great prospects for the practical application of high-voltage lithium-metal batteries.

Interfacial chemistry regulation using functional frameworks for stable metal batteries

“…This endows an ideal articial SEI with high cation transference number (t x +), high diffusion coefficient (D x +), and high mechanical strength. [75][76][77] Fig. 2a illustrates the relationship among t x + , D x + , and safe capacity, in which higher t x + and D x + can lead to enhanced safe capacity of LMBs at a xed current density.…”

Research Progress on the Structural Design and Optimization of Silicon Anodes for Lithium-Ion Batteries: A Mini-Review

“…Zhou et al [96] directly constructed a multifunctional polypyrrole protective layer on the surface of silicon nanoparticles as artificial SEI. Chen et al [97] constructed a multi-component puzzle-shaped artificial SEI by combining fluoro silane and polyether silane (Figure 8C). The application of fluorinated groups produces a uniform and dense structure for the electrode, and ethylene glycol as the main chain promotes ion transport efficiency.…”

Tandem Design of Functional Separators for Li Metal Batteries with Long‐Term Stability and High‐Rate Capability

“…[11,12] A considerable amount of efforts has been devoted to address the Li dendrite issue in LMBs, such as electrolyte additives, [13,14] employing solid-state electrolytes, [15][16][17][18][19] 3D Li matrix, [20,21] current collector design and artificial solid electrolyte interphase (SEI). [22][23][24][25] These strategies have been shown to impede dendrite growth by 1) increasing the Li-ion transference number (t Li + ), 2) homogenizing Li + flux, 3) reducing local current density, and 4) building a high-quality SEI. Separator as a vital part of LMBs has also been endowed with more meaning in regulating Li plating and solid/liquid interface stability.…”