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

摘要

The active structure and catalysis pathway of catalytic materials jointly dominatethe thermodynamic energy barrier and kinetic rate during the reactions,which severely restrict their catalysis service behaviors. Herein, the wholedynamic process covering both the structural evolution and the catalysispathway evolution of model catalyst spinel NiCo_2O_4 during water oxidationvia in situ experiments and theoretical calculations is investigated. Based onthe identified authentic terminated active phase NiOOH and figured latticeoxygen oxidation pathway, an effective expedition and optimization of thisreconfiguration with a proper doping approach is sufficiently evidenced, tofinally establish a life-time dynamic structure–performance correlation ofcatalysts and acquire outstanding catalysis activity. Results indicate synergisticdeliberation of two critical issues regarding the dynamics of bothcatalyst structure and catalysis pathway can truthfully benefit the in-depthunderstanding of advanced catalysts design and render their performance.