Coupling a Three-Dimensional Nanopillar and Robust Film to Guide Li-Ion Flux for Dendrite-Free Lithium Metal Anodes

Abstract

Lithium metal batteries with high theoretical capacity critically suffer from low cycling stability and safety issues mostly due to lithium dendrites. Regulating the Li-ion conduction and Li deposition is essential to achieve dendritic-free Li metal anodes. Herein, a synergistic strategy that combines a 3D nanocopper layer and a robust polymer protective layer is proposed. The 3D nanocopper layer in situ formed on the Li surface could achieve a uniform electric field distribution and contribute to reducing the nucleation barrier for Li deposition and refining the grain size of Li crystallites. Meanwhile, the Li-Nafion film with high Li-ion conductivity and good flexibility was used as a protective layer to provide homogeneous ion distribution and adapt to the volume change during the Li deposition. Consequently, the NCuLi∥LiCoO 2 full cells exhibited outstanding cycling stability (a capacity retention of 90% over 500 cycles). Our results indicate that the synergistic control of Li-ion conduction and Li deposition is a promising method to achieve dendritic-free Li metal anodes.

Coregulation of Li/Li+ Spatial Distribution by Electric Field Gradient with Homogenized Li‐Ion Flux for Dendrite‐Free Li Metal Anodes

“…This excellent cycling stability surpasses that of the 3D current collectors mentioned in existing studies (Table S1, Supporting Information). [38][39][40][41][42][43][44][45][46] The unique conductor-insulator gradientlayered structure and vertical channels of PrGN aid in creating an even Li-ion flux, reducing the localized current density and hindering the formation of localized "hot spots." Electrochemical impedance spectroscopy (EIS) is used to analyze the resistance of charge transfer.…”

The multicomponent synergistic effect of a hierarchical Li0.485La0.505TiO3 solid-state electrolyte for dendrite-free lithium-metal batteries

“…According to previous reports, LiF with a lower surface transport energy barrier can effectively improve the mechanical strength of the SEI layer, enhance the diffusion rate of Li + , restrain the uncontrolled parasitic reactions. [47][48][49] Moreover, it can also depress the electron transport from the Li metal to the electrolyte and protects the Li metal anode interface. [50][51][52] Based on these advantages, the formation of LiF in the interphase may lead to the dendrite-free operation of the electrode.…”

Stabilization of the Li metal anode through constructing a LiZn alloy/polymer hybrid protective layer towards uniform Li deposition

“…Recently, researchers have incorporated inorganic fillers into the polymer matrix to construct a composite layer for protecting the Li metal anode ideally. [37][38][39][40][41] The high flexibility of the polymer enables the conformal coverage of the Li metal anode and accommodates volume changes during cycling. [42][43][44] Alternatively, inorganic fillers enhance the mechanical properties to block the growth of Li dendrites.…”