Enhanced oxygen evolution reaction by modulating the electronic states of a flexible van der Waals membranous catalyst with infinite-layer phase

Abstract

The precise stoichiometry and lattice ordering of perovskite transition metal oxide (TMO) thin films enable the atomic-level catalytic mechanisms in the process of oxygen evolution reaction (OER), accordingly facilitating the creation and refinement potentially effective catalysts. Nevertheless, the fundamental understanding of the interaction between the electronic and structural properties of infinite-layer structured electrocatalysts, as well as their catalytic efficiency, remains lacking. Herein, the successful acquisition of the membranous LaNiO2 catalysts with infinite-layer phase were achieved via topological reconstruction. Subsequent electrochemical testing revealed a decrease in the OER performance of nickelate after reduction, attributed to the diminished bonding strength between catalyst and oxygen intermediates. Given these unexpected findings, this study aimed to leverage surface strains to manipulate electronic states, thereby modulating the OER performance of LaNiO2. Applying either compressive or tensile strains to LaNiO2 enabled the restoration of its performance to pre-reduction levels induced by hydrogen, owing to the reinforced bond strength between catalyst and oxygen intermediates. This research provides both experimental evidence and theoretical guidance for understanding the importance of defect and stress engineering in OER, offering valuable insights for improving OER performance in flexible nano-membranous electrocatalysts with infinite-layer phase for practical applications.