Surface Curvature Effect on Dual-Atom Site Electrocatalysis

Abstract

Oxygen, nitrogen, and carbon electrocatalysis are central in power-to-x innovations. Overpotentials of underlying processes are defined by the scaling relations between the adsorption energies of intermediates and, in turn, determine their efficiency. Our research explores the possibility of switching and tuning the scaling relations by applying metal-nitrogen-carbon (M-N-C) catalysts.In this presentation, we introduce dual-atom site models and demonstrate the effect of surface curvature on oxygen and nitrogen electrocatalysis. Our Density Functional Theory (DFT) calculations show how curving the surface switches the scaling and significantly lowers overpotentials. For instance, we predict a bifunctional overpotential as low as 0.45 V, markedly lower than the theoretical limit of 0.74 V given by the OOH–OH scaling. [1]Our study is among the first to investigate the surface curvature effect beyond the common scaling limitations. It will inspire the community to explore further this effect on oxygen electrocatalysis at M-N-C catalysts, as well as other challenging reactions and similarly curved materials. Funding V.I. and J.R. acknowledge the Danish National Research Foundation Centers of Excellence, The Center for High Entropy Alloys Catalysis (Project DNRF149), and the Independent Research Fund Denmark, grant no. 0217-00014B. V.I. receives funding from the European Union’s Horizon 2020 research and innovation program under the Marie Skłodowska–Curie grant agreement no. 101031656. This research was also supported by the Estonian Research Council grant PSG250 and the EU through the European Regional Development Fund (TK141).