Surface distortion as a unifying concept and descriptor in oxygen reduction reaction electrocatalysis

• Published in: Nature materials Vol. 17; no. 9; pp. 827 - 833
• Main Authors: Chattot, Raphaël, Le Bacq, Olivier, Beermann, Vera, Kühl, Stefanie, Herranz, Juan, Henning, Sebastian, Kühn, Laura, Asset, Tristan, Guétaz, Laure, Renou, Gilles, Drnec, Jakub, Bordet, Pierre, Pasturel, Alain, Eychmüller, Alexander, Schmidt, Thomas J., Strasser, Peter, Dubau, Laetitia, Maillard, Frédéric
• Format: Journal Article
• Language: English
• Published: London Nature Publishing Group UK 01.09.2018; Nature Publishing Group
• Subjects: 119/118; 639/301/357/354; 639/638/161/886; 639/638/77/887; Atomic structure; Biomaterials; Catalysis; Chemical Sciences; Chemistry; Chemistry and Materials Science; Computer simulation; Condensed Matter Physics; Cristallography; Crystal structure; Design defects; Electrocatalysis; Fuel cells; Grain boundaries; Laboratories; Low temperature; Materials Science; Nanocatalysis; Nanomaterials; Nanoparticles; Nanotechnology; Optical and Electronic Materials; Oxygen reduction reactions; Particle size; Proton exchange membrane fuel cells; Reference materials; Stability criteria; Surface defects; Surface distortion; Surface structure; Transmission electron microscopy
• ISSN: 1476-1122; 1476-4660
• DOI: 10.1038/s41563-018-0133-2

Tuning the surface structure at the atomic level is of primary importance to simultaneously meet the electrocatalytic performance and stability criteria required for the development of low-temperature proton-exchange membrane fuel cells (PEMFCs). However, transposing the knowledge acquired on extended, model surfaces to practical nanomaterials remains highly challenging. Here, we propose ‘surface distortion’ as a novel structural descriptor, which is able to reconciliate and unify seemingly opposing notions and contradictory experimental observations in regards to the electrocatalytic oxygen reduction reaction (ORR) reactivity. Beyond its unifying character, we show that surface distortion is pivotal to rationalize the electrocatalytic properties of state-of-the-art of PtNi/C nanocatalysts with distinct atomic composition, size, shape and degree of surface defectiveness under a simulated PEMFC cathode environment. Our study brings fundamental and practical insights into the role of surface defects in electrocatalysis and highlights strategies to design more durable ORR nanocatalysts. Tuning surface structure is key for electrocatalytic performance and stability of proton-exchange membrane fuel cells. Surface distortion as a structural descriptor can help to clarify the role of surface defects and to design enhanced nanocatalysts.