Concurrent Amorphization and Nanocatalyst Formation in Cu‐Substituted Perovskite Oxide Surface: Effects on Oxygen Reduction Reaction at Elevated Temperatures

Authors: SungHyun Jeon, Wan‐Gil Jung, Hohan Bae, Sejong Ahn, Bonjae Koo, WonJeong Yu, Seunghyun Kim, DongHwan Oh, Uisik Kim, Scott A. Barnett, Jongsu Seo, Bong‐Joong Kim, WooChul Jung

Published: 2024-08-09

DOI: 10.1002/adma.202404103

Source: Full article


Abstract

AbstractThe activity and durability of chemical/electrochemical catalysts are significantly influenced by their surface environments, highlighting the importance of thoroughly examining the catalyst surface. Here, Cu‐substituted La0.6Sr0.4Co0.2Fe0.8O3‐δ is selected, a state‐of‐the‐art material for oxygen reduction reaction (ORR), to explore the real‐time evolution of surface morphology and chemistry under a reducing atmosphere at elevated temperatures. Remarkably, in a pioneering observation, it is discovered that the perovskite surface starts to amorphize at an unusually low temperature of approximately 100 °C and multicomponent metal nanocatalysts additionally form on the amorphous surface as the temperature raises to 400 °C. Moreover, this investigation into the stability of the resulting amorphous layer under oxidizing conditions reveals that the amorphous structure can withstand a high‐temperature oxidizing atmosphere (≥650 °C) only when it has undergone sufficient reduction for an extended period. Therefore, the coexistence of the active nanocatalysts and defective amorphous surface leads to a nearly 100% enhancement in the electrode resistance for the ORR over 200 h without significant degradation. These observations provide a new catalytic design strategy for using redox‐dynamic perovskite oxide host materials.