Reduced Potential Barrier of Sodium-Substituted Disordered Rocksalt Cathode for Oxygen Evolution Electrocatalysts

Cation-disordered rocksalt (DRX) cathodes have been viewed as next-generation high-energy density materials surpassing conventional layered cathodes for lithium-ion battery (LIB) technology. Utilizing the opportunity of a better cation mixing facility in DRX, we synthesize Na-doped DRX as an efficient electrocatalyst toward oxygen evolution reaction (OER). This novel OER electrocatalyst generates a current density of 10 mA cm(−2) at an overpotential (η) of 270 mV, Tafel slope of 67.5 mV dec(−1), and long-term stability >5.5 days’ superior to benchmark IrO(2) (η = 330 mV with Tafel slope = 74.8 mV dec(−1)). This superior electrochemical behavior is well supported by experiment and sparse Gaussian process potential (SGPP) machine learning-based search for minimum energy structure. Moreover, as oxygen binding energy (O(BE)) on the surface closely relates to OER activity, our density functional theory (DFT) calculations reveal that Na-doping assists in facile O(2) evolution (O(BE) = 5.45 eV) compared with pristine-DRX (6.51 eV).