The Importance of Structural Uniformity and Chemical Homogeneity in Cobalt‐Free Lithium Excess Nickel Manganese Oxide Cathodes

Abstract This study explores the relationships between material quench rate during processing and the resulting structural and electrochemical properties of Li[Ni_0.25Li_0.167Mn_0.583]O₂. Samples of this lithium‐rich material are prepared with highly contrasting postfiring cooling methods: a rapid water emersion quench or closed‐door oven cooling. The contrasting approaches result in samples with different structural, chemical, and electrochemical behaviors; after cycling the rapidly quenched material yields greater capacity, greater stability, and initially lower, but more stable voltages than the slower cooled samples. Through the use of scanning tunneling electron microscopy, X‐Ray Diffraction (XRD), and X‐ray photoelectron spectroscopy (XPS) it is demonstrated that rapidly quenched powders are more structurally uniform and chemically homogenous before cycling. By comparing these precycling sample to postcycling samples, it is then examined how this increased structural uniformity and chemical homogeneity leads to the superior electrochemical properties of the rapidly quenched samples.