Defect Engineering, Electronic Structure, and Catalytic Properties of Perovskite Oxide La0.5Sr0.5CoO3−δ

The electronic structures of transition metal oxides play a crucial role in the physical and chemical properties of solid materials. Defect engineering is an efficient way to regulate the electronic structure and improve the performance of materials. Here, we develop a defect engineering route that is implemented by controlling the topochemical reactions between cobalt perovskite and urea to optimize the electronic structure of La0.5Sr0.5CoO3−δ (LSCO). Urea pyrolysis is able to increase the oxygen defect concentration and cause octahedral distortions. Furthermore, we can distinctly observe that the introduction of oxygen vacancies narrows the hybridization orbital between O 2p and Co 3d and optimizes the O p-band center near the Fermi level by X-ray absorption spectroscopy, which greatly improves the catalytic activity of CO oxidation and photocatalytic water splitting. These results highlight the relationship between oxygen defects, electronic structure, and catalytic activity of perovskite LSCO, and demonstrate a rational approach to defect design and reveal the importance of anion redox chemistry for the structures and properties of perovskite oxides.