Dynamics of Both Active Phase and Catalysis Pathway for Spinel Water‐Oxidation Catalysts

Abstract The active structure and catalysis pathway of catalytic materials jointly dominate the thermodynamic energy barrier and kinetic rate during the reactions, which severely restrict their catalysis service behaviors. Herein, the whole dynamic process covering both the structural evolution and the catalysis pathway evolution of model catalyst spinel NiCo 2 O 4 during water oxidation via in situ experiments and theoretical calculations is investigated. Based on the identified authentic terminated active phase NiOOH and figured lattice oxygen oxidation pathway, an effective expedition and optimization of this reconfiguration with a proper doping approach is sufficiently evidenced, to finally establish a life‐time dynamic structure–performance correlation of catalysts and acquire outstanding catalysis activity. Results indicate synergistic deliberation of two critical issues regarding the dynamics of both catalyst structure and catalysis pathway can truthfully benefit the in‐depth understanding of advanced catalysts design and render their performance.