Local Structure and Cation Ordering in O3 Lithium Nickel Manganese Oxides with Stoichiometry LiNi[sub xMnsub (2−x)/3Lisub (1−2x)/3]Osub 2

Key Points

• Investigate short-range cation ordering and local atomic configurations in O3-type lithium nickel manganese oxide cathode materials.
• Analyzed local cation coordination and site preferences across varying nickel contents using nuclear magnetic resonance (NMR) spectroscopy.
• Performed first-principles electronic structure computations to determine ground-state atomic ordering and calculate thermal phase disordering temperatures.
• NMR spectroscopy revealed that lithium in transition metal layers preferentially coordinates near manganese and avoids nickel, creating nonrandom cation distributions.
• First-principles computations demonstrated a ground-state arrangement of zigzag metal rows with a calculated disordering temperature of approximately 1000 K.
• Ordered structural fragments persisted above the disordering transition temperature, preserving significant short-range order even when rapidly quenched.