Strategies to suppress the shuttle effect of redox mediators in lithium-oxygen batteries

Abstract Rechargeable lithium-oxygen (Li-O2) batteries are the next generation energy storage devices due to their ultrahigh theoretical capacity. Redox mediators (RMs) are widely used as a homogenous electrocatalyst in non-aqueous Li-O2 batteries to enhance their discharge capacity and reduce charge overpotential. However, the shuttle effect of RMs in the electrolyte solution usually leads to corrosion of the Li metal anode and uneven Li deposition on the anode surface, resulting in unwanted consumption of electrocatalysts and deterioration of the cells. It is therefore necessary to take some measures to prevent the shuttle effect of RMs and fully utilize the soluble electrocatalysts. Herein, we summarize the strategies to suppress the RM shuttle effect reported in recent years, including electrolyte additives, protective separators and electrode modification. The mechanisms of these strategies are analyzed and their corresponding requirements are discussed. The electrochemical properties of Li-O2 batteries with different strategies are summarized and compared. The challenges and perspectives on preventing the shuttle effect of RMs are described for future study. This review provides guidance for achieving shuttle-free redox mediation and for designing Li-O2 cells with a long cycle life, high energy efficiency and highly reversible electrochemical reactions.