Detection, Analysis, and Behavior of Soft-Shorts in Solid-State Batteries

Abstract

Lithium metal batteries face numerous challenges before being employed in practical energy storage systems. Chief among these is the suppression of lithium dendrites, which lead to cell shorting and thermal runaway. In the field of solid-state batteries, there is often talk of “soft-shorts”, where small lithium dendrites form, short, then disappear. However, there is no clear consensus on the definition of soft-shorts, how they behave, and what their presence means for solid electrolyte development. Here, we use composite polymer electrolytes as exemplary solid electrolytes to detect, analyze, and thoroughly describe the varied behavior of soft-shorts. We define soft-shorts and show quantitatively that both ionic and electronic current flow simultaneously in a soft-shorted cell. The amount of each current depends on dendrite size, which dictates the resistance to the electronic pathway as well as Joule heating of the thin metal filaments. This heating leads to the “burning out” of the dendrites, which is responsible for the rapid un-shorting of soft-shorted cells. We use computational modeling to quantify the dendrite properties and explain how this leads to the observed transient behavior. More persistent soft-shorts are analyzed with temperature-dependent, quantitative electrochemical impedance fitting, where it is shown that parallel ionic and electronic current paths present impedance data that can be misinterpreted without rigorous analysis. The advantages and disadvantages of several soft-short characterization techniques are discussed. In the end, we show that soft-shorts are diverse in nature and thus require diverse tools and keen eyes from researchers to avoid the over-selling of flawed materials for lithium metal batteries.