TY - JOUR AU - Jinhyuk Lee AU - Daniil A Kitchaev AU - Deok-Hwang Kwon AU - Chang-Wook Lee AU - Joseph K Papp AU - Yi-Sheng Liu AU - Zhengyan Lun AU - Raphaële J Clément AU - Tan Shi AU - Bryan D McCloskey AU - Jinghua Guo AU - Mahalingam Balasubramanian AU - Gerbrand Ceder AB -

There is an urgent need for low-cost, resource-friendly, high-energy-density cathode materials for lithium-ion batteries to satisfy the rapidly increasing need for electrical energy storage. To replace the nickel and cobalt, which are limited resources and are associated with safety problems, in current lithium-ion batteries, high-capacity cathodes based on manganese would be particularly desirable owing to the low cost and high abundance of the metal, and the intrinsic stability of the Mn4+ oxidation state. Here we present a strategy of combining high-valent cations and the partial substitution of fluorine for oxygen in a disordered-rocksalt structure to incorporate the reversible Mn2+/Mn4+ double redox couple into lithium-excess cathode materials. The lithium-rich cathodes thus produced have high capacity and energy density. The use of the Mn2+/Mn4+ redox reduces oxygen redox activity, thereby stabilizing the materials, and opens up new opportunities for the design of high-performance manganese-rich cathodes for advanced lithium-ion batteries.

BT - Nature DA - 04/2018 DO - 10.1038/s41586-018-0015-4 IS - 7700 LA - eng N2 -

There is an urgent need for low-cost, resource-friendly, high-energy-density cathode materials for lithium-ion batteries to satisfy the rapidly increasing need for electrical energy storage. To replace the nickel and cobalt, which are limited resources and are associated with safety problems, in current lithium-ion batteries, high-capacity cathodes based on manganese would be particularly desirable owing to the low cost and high abundance of the metal, and the intrinsic stability of the Mn4+ oxidation state. Here we present a strategy of combining high-valent cations and the partial substitution of fluorine for oxygen in a disordered-rocksalt structure to incorporate the reversible Mn2+/Mn4+ double redox couple into lithium-excess cathode materials. The lithium-rich cathodes thus produced have high capacity and energy density. The use of the Mn2+/Mn4+ redox reduces oxygen redox activity, thereby stabilizing the materials, and opens up new opportunities for the design of high-performance manganese-rich cathodes for advanced lithium-ion batteries.

PY - 2018 SP - 185 EP - 190 ST - Nature T2 - Nature TI - Reversible Mn2+/Mn4+ double redox in lithium-excess cathode materials VL - 556 SN - 0028-0836 ER -