Publication date: 10th April 2024
High-entropy materials have been exploited in various applications including thermo-electrics, catalysis, energy storage and conversion performance. Benefits from the structural flexibility of perovskite materials, we successfully synthesize high-entropy materials by introducing multi-dopants into the B-site of the host oxides via a simple sol-gel method. Notably, our study reveals the formation of high-entropy alloy nanoparticles during the reduction. These metal nanoparticles are believed to serve as active sites, further enhancing catalytic performance[1,2]. The evolution of these multi-metallic species through reduction analysis was investigated by reduction analysis, XPS, elemental mapping, and high-temperature XRD. To elucidate their formation, we propose an oxidation-driven mechanism based on the control of temperature and oxygen partial pressure. The effects of entropy were studied by fabricating the material into high-temperature solid oxide cells. The incorporation of high entropy not only enhances the catalytic activity of the electrodes but also improves the stability of solid oxide cells. The area-specific resistance of the cells was reduced about 10 times from singly dopant material to high-entropy perovskite oxides. The cell with Ni-doped perovskites displays about 23 % deterioration while the high-entropy electrode possesses only 1 % deterioration for a 50-h stability test. We utilized DFT calculations to elucidate the superior performance of high-entropy alloy (HEA) metals in solid oxide cells (SOCs). Our findings suggest that HEAs can efficiently modulate surface-adsorption interactions towards the high-activity region compared to their ternary or single-element counterparts.
This work presents a synthesis route for high-entropy perovskite oxides, furthermore, it sheds light on the design of materials featuring multi-metallic species. These materials exhibit enhanced efficiency and stability as electrodes, contributing to advancements in energy conversion technologies.