Adaptive Cation Pillar Effects Achieving High Capacity in Li-Rich Layered Oxide, Li2 MnO3-LiMeO2 (Me = Ni, Co, Mn)


Lithium-rich layered oxide (LLO) is a type of positive electrode material that is being explored for use in lithium-ion batteries. Lithium-rich layered oxide materials have a high theoretical capacity, which makes them desirable for application in high-energy density batteries. Li-rich layered oxides materials do, however, have several limitations that prevent widespread application. Their poor cycling stability, which refers to the battery’s capacity maintenance over numerous charge and discharge cycles, is one of the main problems. This may eventually result in a drop in performance and a shorter battery life. Low-rate capability, or the battery’s inability to charge and discharge at rapid rates, is another problem. This may reduce the battery’s power output and lessen its suitability for usage in high-power applications. Because of the high lithium content, the crystal structure may alter over time and become structurally unstable. This can cause the material to break down and lose capacity. Researchers are actively working to address these issues and improve the cycling stability and rate capability of Li-rich layered oxides materials.

In the study published in the peer-reviewed Journal Small, Dr. Satoshi Hiroi, Professor Koji Ohara from Japan Synchrotron Radiation Research Institute together with Dr. Masatsugu Oishi and Mr. Daiki Kabutan from Tokushima University along with Dr. Keiji Shimoda and Professor Yoshiharu Uchimoto from Kyoto University introduced a new concept that can improve the capacity and performance of Li-rich layered oxide in lithium-ion batteries. The research team focused on the structural mechanisms and performance of Li-rich layered oxide materials as cathode materials. They investigated the role of adaptive cation pillars in improving the capacity and cycling stability of Li-rich layered oxide materials using X-ray total scattering measurements and structural refinements to analyze the structural changes during charge and discharge cycles.

The authors synthesized and characterized the positive electrode material Li1.16Ni0.15Co0.19Mn0.50O2 for its utility in lithium-ion batteries. They confirmed the composition and morphology of the material using X-ray diffraction and scanning electron microscopy after synthesizing the material via a solid-state reaction that involved lithium hydroxide and nickel-cobalt-manganese carbonate. The electrochemical performance of the electrode was measured using a battery setup, where it was used as a cathode material with a lithium metal anode in an electrolyte solution. To assess the electrode’s performance as a cathode material for lithium-ion batteries, the electrode’s capacity, voltage profile, and cycling stability were examined during charge and discharge cycles. Synchrotron radiation was used to conduct X-ray total scattering studies in order to study the structural changes that occur during battery cycling. To establish the structural parameters in various charge/discharge states, the obtained data were examined utilizing structural refinements. The importance of adaptable cation pillars in enhancing the capacity and cycling stability of Li-rich layered oxide materials was revealed in their study.

Based on the authors’ findings from measurements of X-ray total scattering and structural modifications, the researchers concluded that adaptable cation pillars are key in enhancing the capacity and performance of Li-rich layered oxide materials. After the initial charge, the hard pillars became practically immovable, indicating that they were connected to the material’s rapid capacity diminishing. The high capacity of the positive electrode material, on the other hand, was a result of the adaptive pillars’ ability to migrate back and forth between the Me layer and the tetrahedral layer to promote large amount of Li desorption insertion into the Li layer.

In conclusion, the study demonstrated that Li-rich layered oxide materials excellent cathode materials for lithium-ion batteries through the use of adaptable cation pillars may be a potential strategy. However, further research is needed to optimize the synthesis and processing of these materials.


Satoshi Hiroi, Masatsugu Oishi, Koji Ohara, Keiji Shimoda, Daiki Kabutan and Yoshiharu Uchimoto. Adaptive Cation Pillar Effects Achieving High Capacity in Li-Rich Layered Oxide, Li2MnO3-LiMeO2 (Me = Ni, Co, Mn). Small, Volume 18, 2022, 2203412.

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