Dimensionality Control of Electrocatalytic Activity in Perovskite Nickelates

Abstract

The dimensionality of the crystal structure plays an important role in the electronic structures of materials. Ruddlesden-Popper perovskite oxides offer an attractive platform for studying this role due to dimensional flexibility. The effects of dimensionality on physical properties in those oxides have been widely reported. However, the study of dimensional dependence on the chemical properties is still lacking. Here, we synthesized a series of Ruddlesden-Popper perovskite nickelates La_<i>n</i>SrNi_<i>n</i>O_3<i>n</i>+1 (<i>n</i> = 1, 2, 3, and ∞) to explore the role of dimensionality on oxygen-evolution reaction (OER) performance. As the dimensionality increased with <i>n</i>, the nickelates exhibited an enhanced OER activity. We found that the weakening of electron correlations among Ni 3<i>d</i> electrons by increasing the dimensionality induced an insulator-to-metal transition and a strengthened Ni-O hybridization, both of which accelerated the OER kinetics. This work sets up a bridge between the dimensionality and electrocatalysis, which provides guidance for designing highly efficient oxygen-evolving catalysts.