Tuning the Electronic Structure of LaNiO3 through Alloying with Strontium to Enhance Oxygen Evolution Activity

Abstract

Abstract The perovskite oxide LaNiO3 is a promising oxygen electrocatalyst for renewable energy storage and conversion technologies. Here, it is shown that strontium substitution for lanthanum in coherently strained, epitaxial LaNiO3 films (La1−x SrxNiO3) significantly enhances the oxygen evolution reaction (OER) activity, resulting in performance at x = 0.5 comparable to the state‐of‐the‐art catalyst Ba0.5Sr0.5Co0.8Fe0.2O3−δ. By combining X‐ray photoemission and X‐ray absorption spectroscopies with density functional theory, it is shown that an upward energy shift of the O 2p band relative to the Fermi level occurs with increasing x in La1−xSrxNiO3. This alloying step strengthens Ni 3d–O 2p hybridization and decreases the charge transfer energy, which in turn accounts for the enhanced OER activity.

Keywords

• hole doping
• hybridization
• LaNiO3
• nickelates
• oxygen evolution reaction