Activating the lattice oxygen can significantly improve the kinetics of oxygen evolution reaction (OER), however, it often results in reduced stability due to the bulk structure degradation. Here, we develop a spinel Fe0.3Co0.9Cr1.8O4 with active lattice oxygen by high-throughput methods, achieving high OER activity and stability, superior to the benchmark IrO2. The oxide exhibits an ultralow overpotential (190 mV at 10 mA cm-2) with outstanding stability for over 170 h at 100 mA cm-2. Soft X-ray absorption- and Raman-spectroscopies, combined with 18O isotope-labelling experiments, reveal that lattice oxygen activation is driven by Cr oxidation, which induces a cation migration from CrO6 octahedrons to CrO4 tetrahedrons. The geometry conversion creates accessible non-bonding oxygen states, crucial for lattice oxygen oxidation. Upon oxidation, peroxo O-O bond is formed and further stabilized by Cr6+ (CrO4 tetrahedra) via dimerization. This work establishes a new approach for designing efficient catalysts that feature active and stable lattice oxygen without compromising structural integrity.
Keywords: Active lattice oxygen; Cation migration; High-throughput methods; Oxygen evolution reaction; Spinel oxides.
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