Operando Monitoring and Deciphering the Structural Evolution in Oxygen Evolution Electrocatalysis

Abstract The oxygen evolution reaction (OER) acts as the bottleneck of some crucial energy conversion and storage technologies involving water electrolysis, CO 2 electrolysis, and metal‐air batteries, among others. The challenging sluggish reaction kinetics of the OER can be overcome via developing highly efficient electrocatalysts, which experience a dynamic structural evolution process during the reaction. However, the reaction mechanism of the structural transformation of electrocatalysts during the OER and the structure‐activity correlation in understanding the real active sites remain elusive. Fortunately, operando characterizations offer a platform to study the structural evolution processes and the reaction mechanisms of OER electrocatalysts. In this review, using several in situ/operando techniques some recent advances are elaborated with emphases on tracking the structural evolution processes of electrocatalysts, recording the reaction intermediates during electrocatalysis, and building a link between the structure and activity/stability of electrocatalysts. Moreover, theoretical considerations are also discussed to assist operando characterization understanding. Finally, some perspectives are provided which are expected to be helpful to tackle the current challenges in operando monitoring and unraveling the reaction mechanisms of OER electrocatalysts.