2025-09-04 中国科学院（CAS）
＜関連情報＞
- https://english.cas.cn/newsroom/research_news/chem/202509/t20250904_1053898.shtml
- https://pubs.acs.org/doi/10.1021/jacs.5c10937
高温酸素発生反応のためのPrFeO3-δペロブスカイトにおけるスピン状態調整 Spin-State Tuning in PrFeO3-δ Perovskite for High-Temperature Oxygen Evolution Reaction
Jingcheng Yu,Qingxue Liu,Shuo Wang,Shiming Zhou,Rongtan Li,Weicheng Feng,Yige Guo,Xiaomin Zhang,Rile Ge,Junhu Wang,Limin Liu,Shaowei Zhang,Geng Zou,Yuefeng Song,Guoxiong Wang,and Xinhe Bao
Journal of the American Chemical Society Published: August 26, 2025
DOI:https://doi.org/10.1021/jacs.5c10937
Abstract
The electrocatalytic activity of perovskite oxides is fundamentally governed by their electronic structure. However, a deeper understanding of the relationship between the eg electron occupancy and high-temperature oxygen evolution reaction (OER) performance in solid oxide electrolysis cells (SOECs) remains underexplored. Here, A-site doped Pr0.5Ae0.5FeO3−δ (Ae = Ca, Sr, Ba) are constructed with exceptional high-temperature OER performance, and Pr0.5Ba0.5FeO3−δ achieves a current density of 3.33 A cm–2 at 2.0 V and 800 °C. X-ray absorption spectroscopy, 57Fe Mössbauer spectroscopy, and magnetic susceptibility measurements reveal that alkaline earth metal doping induces a spin-state transition from high-spin Fe3+ (t2g3eg2) to low-spin Fe4+ (t2g4eg0), with reduced eg occupancy, thus accelerating the charge transfer and oxygen transport in the OER process. This work sheds light on the critical role of the B-site Fe electronic structure in high-temperature OER performance and provides guidance for the rational design of Fe-based perovskites as SOEC anode materials.
