Layered Cathode Materials for Lithium-Ion Batteries: Review of Computational Studies on LiNi_1–x–yCo_xMn_yO₂ and LiNi_1–x–yCo_xAl_yO₂

Abstract

At present the most successful rechargeable battery is the Li-ion battery, due to the small size, high energy density, and low reduction potential of Li. Computational materials science has become an increasingly important tool to study these batteries, and in particular cathode properties. In silico studies of cathode materials have proven to be a valuable tool to understand the workings of cathodes, without having to do sophisticated experiments. First-principles and empirical computations have been used by various groups to study key properties, such as structural stability, electronic structure, ion diffusion mechanisms, equilibrium cell voltage, thermal and electrochemical stability, and surface behavior of Li-ion battery cathode materials. Arguably, the most practical and promising Li-ion cathode materials today are layered oxide materials, and in particular LiNi 1−x−y Co x Mn y O 2 (NCM) and LiNi 1−x−y Co x Al y O 2 (NCA). Here, some of the computational approaches to studying Li-ion batteries, with special focus on issues related to layered materials, are discussed. Subsequently, an overview of theoretical and related experimental work performed on layered cathode materials, and in particular on NCM and NCA materials, is provided.

Peculiar Properties of Electrochemically Oxidized SmBaCo2−xMnxO5+δ (x = 0; 0.5 and 1) A-Site Ordered Perovskites

“…This may allow for the oxide to maintain generally unchanged structural parameters, creating a metastable configuration. This can be, to some degree, related to the peculiar structural differences observed between the electrochemically and chemically lithiated (i.e., intercalated with Li) layered oxide samples at room temperature [36][37][38].…”

Studies of Nickel-Rich LiNi0.85Co0.10Mn0.05O2 Cathode Materials Doped with Molybdenum Ions for Lithium-Ion Batteries

“…Among these power sources, advanced lithium ion batteries (LIBs) are the most appropriate ones for electrochemical propulsion, since they may provide the necessary high energy density, cycle life, stability, and reasonable safety [1][2][3][4][5][6][7][8][9][10][11]. The limiting factor of energy content in LIBs are the positive electrodes (cathodes) and their improvement is much more effective compared to other parts of batteries to get high energy density [12].…”

Enhancement of Structural, Electrochemical, and Thermal Properties of Ni‐Rich LiNi0.85Co0.1Mn0.05O2 Cathode Materials for Li‐Ion Batteries by Al and Ti Doping

“…The dopants' effects on the cathode materials are influenced by several important properties, including ionic charge, ionic size, and magnetism. [21] These effects help to explain the mechanisms through which these dopants at low concentration affect the behavior of NCM cathode materials (see later in the Results and Discussion Section).…”

“…Several studies have concluded that different dopants have distinct effects on the cathode materials, such as suppressing Li/Ni cation mixing, “pillar effect”, and impeding the intergranular cracks. The dopants’ effects on the cathode materials are influenced by several important properties, including ionic charge, ionic size, and magnetism [21] . These effects help to explain the mechanisms through which these dopants at low concentration affect the behavior of NCM cathode materials (see later in the Results and Discussion Section).…”