Bifunctional Single Atom Catalysts for Rechargeable Zinc–Air Batteries: From Dynamic Mechanism to Rational Design

Abstract Ever‐growing demands for rechargeable zinc–air batteries (ZABs) call for efficient bifunctional electrocatalysts. Among various electrocatalysts, single atom catalysts (SACs) have received increasing attention due to the merits of high atom utilization, structural tunability, and remarkable activity. Rational design of bifunctional SACs relies heavily on an in‐depth understanding of reaction mechanisms, especially dynamic evolution under electrochemical conditions. This requires a systematic study in dynamic mechanisms to replace current trial and error modes. Herein, fundamental understanding of dynamic oxygen reduction reaction and oxygen evolution reaction mechanisms for SACs is first presented combining in situ and/or operando characterizations and theoretical calculations. By highlighting structure–performance relationships, rational regulation strategies are particularly proposed to facilitate the design of efficient bifunctional SACs. Furthermore, future perspectives and challenges are discussed. This review provides a thorough understanding of dynamic mechanisms and regulation strategies for bifunctional SACs, which are expected to pave the avenue for exploring optimum single atom bifunctional oxygen catalysts and effective ZABs.