title: Compositional engineering of perovskite oxides for highly efficient oxygen reduction reactions.
abstract: Mixed conducting perovskite oxides are promising catalysts for high-temperature oxygen reduction reaction. Pristine SrCoO(3-δ) is a widely used parent oxide for the development of highly active mixed conductors. Doping a small amount of redox-inactive cation into the B site (Co site) of SrCoO(3-δ) has been applied as an effective way to improve physicochemical properties and electrochemical performance. Most findings however are obtained only from experimental observations, and no universal guidelines have been proposed. In this article, combined experimental and theoretical studies are conducted to obtain fundamental understanding of the effect of B-site doping concentration with redox-inactive cation (Sc) on the properties and performance of the perovskite oxides. The phase structure, electronic conductivity, defect chemistry, oxygen reduction kinetics, oxygen ion transport, and electrochemical reactivity are experimentally characterized. In-depth analysis of doping level effect is also undertaken by first-principles calculations. Among the compositions, SrCo0.95Sc0.05O(3-δ) shows the best oxygen kinetics and corresponds to the minimum fraction of Sc for stabilization of the oxygen-vacancy-disordered structure. The results strongly support that B-site doping of SrCoO(3-δ) with a small amount of redox-inactive cation is an effective strategy toward the development of highly active mixed conducting perovskites for efficient solid oxide fuel cells and oxygen transport membranes.
authors: †State Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing Tech University, Nanjing 210009, China.|§Department of Mechanical and Aerospace Engineering, The Hong Kong University of Science and Technology, Hong Kong, China.
authors: Dengjie
authors: D
authors: Chen
authors: §Department of Mechanical and Aerospace Engineering, The Hong Kong University of Science and Technology, Hong Kong, China.
authors: Chi
authors: C
authors: Chen
authors: †State Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing Tech University, Nanjing 210009, China.
authors: Zhenbao
authors: Z
authors: Zhang
authors: §Department of Mechanical and Aerospace Engineering, The Hong Kong University of Science and Technology, Hong Kong, China.
authors: Zarah Medina
authors: ZM
authors: Baiyee
authors: §Department of Mechanical and Aerospace Engineering, The Hong Kong University of Science and Technology, Hong Kong, China.|⊥Department of Chemical and Biomolecular Engineering, The Hong Kong University of Science and Technology, Hong Kong, China.
authors: Francesco
authors: F
authors: Ciucci
authors: †State Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing Tech University, Nanjing 210009, China.
authors: Zongping
authors: Z
authors: Shao
keywords: SrCoO3−δ; compositional engineering; first-principles calculations; oxygen reduction kinetics; oxygen transport membranes; solid oxide fuel cells