PNNL

Abstract

Lithium (Li) dendrite formation is one of the critical challenges for rechargeable Li metal batteries. The traditional method to suppress Li dendrites by using high-quality solid electrolyte interface (SEI) films cannot effectively solve this problem. Recently, we proposed a novel self-healing electrostatic shield (SHES) mechanism to change the Li deposition behavior. The SHES mechanism forces Li to be deposited in the region away from protuberant tips by using non-Li cations as additives that preferentially accumulate but not deposit on the active sites of Li electrode. In this paper, the electrochemical behavior of cesium cation (Cs+) as the typical non-Li cation suitable for the SHES mechanism was further investigated in detail to reveal its effects on preventing Li dendrites and interactions with Li electrode. It is found that typical adsorption behavior instead of chemical reaction is observed. The existence of Cs+ cation in the electrolyte does not change the components and structure of the Li surface film and this is consistent with the projection of the SHES mechanism. Various factors affecting the effectiveness of SHES mechanism are also discussed. The morphologies of Li films deposited is smooth and uniform during the repeated deposition-stripping cycles and at various current densities (from 0.1 to 1.0 mA cm-2) by adding just a small amount (0.05 M) of Cs+-additive in the electrolyte.