A Diffusion‐‐Reaction Competition Mechanism to Tailor Lithium Deposition for Lithium‐Metal Batteries

Abstract

Lithium metal is recognized as one of the most promising anode materials owing to its ultrahigh theoretical specific capacity and low electrochemical potential. Nonetheless, dendritic Li growth has dramatically hindered the practical applications of Li metal anodes. Realizing spherical Li deposition is an effective approach to avoid Li dendrite growth, but the mechanism of spherical deposition is unknown. Herein, a diffusion-reaction competition mechanism is proposed to reveal the rationale of different Li deposition morphologies. By controlling the rate-determining step (diffusion or reaction) of Li deposition, various Li deposition scenarios are realized, in which the diffusion-controlled process tends to lead to dendritic Li deposition while the reaction-controlled process leads to spherical Li deposition. This study sheds fresh light on the dendrite-free Li metal anode and guides to achieve safe batteries to benefit future wireless and fossil-fuel-free world.Supporting information and the ORCID identification number(s) for the author(s) of this article can be found under: https://doi.

Constructing multifunctional solid electrolyte interface via in-situ polymerization for dendrite-free and low N/P ratio lithium metal batteries

“…This well-defined unique nanosized Li deposition with isotropic spherical features ensures the smooth surface formation without any sharp tip, thus avoiding serious safety hazards caused by dendritic Li growth. Besides, spherical Li exhibits minimum surface-to-volume ratio, which signifies higher CE and longer cycle life by exhibiting less side reactions between fresh Li and electrolyte 48 . Mechanical properties are quantitatively described by the Young's modulus obtained from force indentation curves (Fig.…”

“…The severe Li particle aggregation and non-uniform Li deposition can be ascribed to the slow diffusion and fast consumption of Li + upon deposition and the rapid decline of ion concentration in the SEI layer. The slowly diffused Li + in the SEI layer induced inhomogeneous Li plating and the dendritic Li growth under the diffusion-controlled condition 52 . The BE of PVDF with Li was further calculated, which shows very low adsorbability on Li, rendering an unstable film formed on the surface of Li and limited capability to homogenize Li deposition and inhibit dendrite growth ( Supplementary Fig.…”

Stabilizing metal battery anodes through the design of solid electrolyte interphases

“…[44][45][46] In addition, the SEI (LiN x O y and Li 3 N) generated by NO 3 À has been argued to possess a high ionic conductivity, which can regulate the lithium morphology to be more spherical and compact rather than needle-like with a high surface area. 47 A B…”

Boosting the Optimization of Lithium Metal Batteries by Molecular Dynamics Simulations: A Perspective

“…To achieve successful Li metal anodes, we need to obtain a deep understanding of Li deposition behavior. [80] Both internal and external The color scheme used is as follows: Li: purple, O: red, C: gray, H: white, F: cyan, and S: yellow. Reproduced with permission.…”

“…To achieve successful Li metal anodes, we need to obtain a deep understanding of Li deposition behavior. [ 80 ] Both internal and external factors can affect the behavior of Li deposition. The external elements usually include temperature, pressure, and fold and the internal elements are containing current density, electrolyte components, the surface properties and morphology of electrode.…”