Abstract

Tuning catalysis at solid–solid interfaces is critical for the development of next-generation energy storage devices such as Li–O2 batteries, where solid lithium–oxygen species are formed and dissociated on a solid catalyst. Herein, atomically controlled synthesis is combined with theoretical calculations, electrochemical studies, and detailed characterization measurements to show that the interface between an oxide catalyst and the solid products is key to selectively control discharge product distribution, consequently affecting charge overpotentials. A surface structure-dependent electrochemical performance for nonprecious metal-containing, nanostructured lanthanum nickelate oxide (La2NiO4+δ, LNO) electrocatalysts is demonstrated. LNO nanostructures with (001) NiO-terminated surfaces exhibit lower charge overpotentials, as opposed to irregularly terminated polyhedral-shaped oxides of the same composition. It is found that these LNO nanostructures, with controlled surface structure, enhance the performa...

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