High energy-density lithium-ion batteries are in demand for portable electronic devices and electrical vehicles. Since the energy density of the batteries relies heavily on the cathode material used, major research efforts have been made to develop alternative cathode materials with a higher degree of lithium utilization and specific energy density. In particular, layered, Ni-rich, lithium transition-metal oxides can deliver higher capacity at lower cost than the conventional LiCoO2 . However, for these Ni-rich compounds there are still several problems associated with their cycle life, thermal stability, and safety. Herein the performance enhancement of Ni-rich cathode materials through structure tuning or interface engineering is summarized. The underlying mechanisms and remaining challenges will also be discussed.

Nickel‐Rich Layered Lithium Transition‐Metal Oxide for High‐Energy Lithium‐Ion Batteries

The ever-growing demand for advanced rechargeable lithium-ion batteries in portable electronics and electric vehicles has spurred intensive research efforts over the past decade. The key to sustaining the progress in Li-ion batteries lies in the quest for safe, low-cost positive electrode (cathode) materials with desirable energy and power capabilities. One approach to boost the energy and power densities of batteries is to increase the output voltage while maintaining a high capacity, fast charge–discharge rate, and long service life. This review gives an account of the various emerging high-voltage positive electrode materials that have the potential to satisfy these requirements either in the short or long term, including nickel-rich layered oxides, lithium-rich layered oxides, high-voltage spinel oxides, and high-voltage polyanionic compounds. The key barriers and the corresponding strategies for the practical viability of these cathode materials are discussed along with the optimization of electrolytes and other cell components, with a particular emphasis on recent advances in the literature. A concise perspective with respect to plausible strategies for future developments in the field is also provided.

High-voltage positive electrode materials for lithium-ion batteries

https://iopscience.iop.org/article/10.1149/2.0021707jes/pdf

Oxygen Release and Its Effect on the Cycling Stability of LiNixMnyCozO2 (NMC) Cathode Materials for Li-Ion Batteries

Understanding reactions at the electrode/electrolyte interface (EEI) is essential to developing strategies to enhance cycle life and safety of lithium batteries. Despite research in the past four decades, there is still limited understanding by what means different components are formed at the EEI and how they influence EEI layer properties. We review findings used to establish the well-known mosaic structure model for the EEI (often referred to as solid electrolyte interphase or SEI) on negative electrodes including lithium, graphite, tin, and silicon. Much less understanding exists for EEI layers for positive electrodes. High-capacity Li-rich layered oxides yLi2–xMnO3·(1–y)Li1–xMO2, which can generate highly reactive species toward the electrolyte via oxygen anion redox, highlight the critical need to understand reactions with the electrolyte and EEI layers for advanced positive electrodes. Recent advances in in situ characterization of well-defined electrode surfaces can provide mechanistic insights an...

/pdf/electrode-electrolyte-interface-in-li-ion-batteries-current-3tj6h3u310.pdf

Electrode–Electrolyte Interface in Li-Ion Batteries: Current Understanding and New Insights

Future generations of electrified vehicles require driving ranges of at least 300 miles to successfully penetrate the mass consumer market. A significant improvement in the energy density of lithium batteries is mandatory, maintaining at the same time similar, or improved, rate capability, lifetime, cost, and safety. Several new cathode materials have been claimed over the last decade to allow for this energy improvement. The possibility that some of them will find application in the future automotive batteries is critically evaluated here by first considering their theoretical and experimentally demonstrated energy densities at the material level. For selected candidates, the energy density at the automotive battery cell level for electric vehicle applications is calculated using an in-house developed software. For the selected cathodes, literature results concerning their power capability and lifetime are also discussed with reference to the automotive targets.

Future generations of cathode materials: an automotive industry perspective

Toward uniform and ultrathin carbon layer coating on lithium iron phosphate using liquid carbon dioxide for enhanced electrochemical performance

We use transmission electron microscopy (TEM) to investigate the evolution of the surface structure of LixNi0.8Co0.15Al0.05O2 cathode materials (NCA) as a function of the extent of first charge at room temperature using a combination of high-resolution electron microscopy (HREM) imaging, selected area electron diffraction (SAED), and electron energy loss spectroscopy (EELS). It was found that the surface changes from the layered structure (space group R3m) to the disordered spinel structure (Fd3m), and eventually to the rock-salt structure (Fm3m), and that these changes are more substantial as the extent of charge increases. EELS indicates that these crystal structure changes are also accompanied by significant changes in the electronic structure, which are consistent with delithiation leading to both a reduction of the Ni and an increase in the effective electron density of oxygen. This leads to a charge imbalance, which results in the formation of oxygen vacancies and the development of surface poros...

Investigation of Changes in the Surface Structure of LixNi0.8Co0.15Al0.05O2 Cathode Materials Induced by the Initial Charge

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Toward uniform and ultrathin carbon layer coating on lithium iron phosphate using liquid carbon dioxide for enhanced electrochemical performance

Investigation of Changes in the Surface Structure of LixNi0.8Co0.15Al0.05O2 Cathode Materials Induced by the Initial Charge