Role of a Solid–Electrolyte Interphase in the Dendritic Electrodeposition of Lithium: A Brownian Dynamics Simulation Study

Abstract

A robust, flexible, and uniform layer of solid-electrolyte interphase (SEI) is known to regulate the dendritic growth of a lithium metal anode during electrodeposition. The underlying mechanism and extent of such regulation are largely unknown. The present Brownian dynamics simulation elucidates the suppressive role of a SEI layer in the dendritic electrodeposition. By thinning out a SEI layer to a subnanometer scale, a dendrite with long arms becomes dense and mossy, and it grows much slower in time. The radial diffusion of lithium ions through a thin SEI layer gives an isotropic growth of a round tip, instead of a dendritic ramification along a particular direction.

Stabilizing metal battery anodes through the design of solid electrolyte interphases

“…Brownian dynamics simulation shows that through thinning the SEI layer into a sub-nanometer scale, the radial diffusion of Li + results in an isotropic growth and suppresses the dendritic electrodeposition. 127 Linear analysis indicates that morphological instabilities of metal deposition can be suppressed by increasing the surface tension through controlling the SEI. Meanwhile, ASEI with high elastic stresses as well as fixed anions can also enhance the interfacial stability.…”

Effects of Adsorbate Diffusion and Edges in a Transition from Particle to Dendritic Morphology during Silver Electrodeposition

“…The modeling also advances in the quantitative description of the process, as we argue that the characteristic sizes of the deposited structures are set by the diffusion lengths of silver atoms and we use those lengths to estimate diffusion coefficients. For comparison, although several studies have already highlighted the importance of adsorbate relaxation in the initial stages of metal electrodeposition − and in the formation of dendritic films, − previous models − did not show the organized morphology of nanotrees or nanofeathers.…”

Designing Advanced Liquid Electrolytes for Alkali Metal Batteries: Principles, Progress, and Perspectives

“…Brownian dynamics simulations showed that the radial diffusion of Li + results in an anisotropic growth and suppresses the dendritic electrodeposition by thinning the SEI layer to a sub-nanometer scale (Figure 3e). [67] Nagaoka et al [68] confirmed that the reduction products of Li salts constitute the main body of the SEI using the Red Moon method, a hybrid Monte Carlo (MC)/MD reaction method, to simulate the formation mechanism of SEI at the atomic level. [59] Reproduced with permission.…”

“…e) Schematic for the electrodeposition of lithium dendrites enabled by Brownian dynamics simulation. [ 67] Reproduced with permission. Copyright 2020, American Chemical Society.…”

“…Copyright 2019, Springer Nature. e) Schematic for the electrodeposition of lithium dendrites enabled by Brownian dynamics simulation [67]. Reproduced with permission.…”