Origin of Surface Reconstruction in Lattice Oxygen Oxidation Mechanism Based‐Transition Metal Oxides: A Spontaneous Chemical Process

Abstract A fundamental understanding of surface reconstruction process is pivotal to developing highly efficient lattice oxygen oxidation mechanism (LOM) based electrocatalysts. Traditionally, the surface reconstruction in LOM based metal oxides is believed as an irreversible oxygen redox behavior, due to the much slower rate of OH − refilling than that of oxygen vacancy formation. Here, we found that the surface reconstruction in LOM based metal oxides is a spontaneous chemical reaction process, instead of an electrochemical reaction process. During the chemical process, the lattice oxygen atoms were attacked by adsorbed water molecules, leading to the formation of hydroxide ions (OH − ). Subsequently, the metal‐site soluble atoms leached from the oxygen‐deficient surface. This work also suggests that the enhancement of surface hydrophilicity could accelerate the surface reconstruction process. Hence, such a finding could add a new layer for the understanding of surface reconstruction mechanism.