Allen Jan L, Crear Bria A, Choudhury Rishav, Wang Michael J, Tran Dat T, Ma Lin, Piccoli Philip M, Sakamoto Jeff, Wolfenstine Jeff
Energy Sciences Division, Sensors & Electron Devices Directorate, US Army Research Laboratory, Adelphi, MD 20783, USA.
Department of Chemistry, Howard University, Washington, DC 20059, USA.
Molecules. 2021 Apr 30;26(9):2625. doi: 10.3390/molecules26092625.
Spinel-structured solids were studied to understand if fast Li ion conduction can be achieved with Li occupying multiple crystallographic sites of the structure to form a "Li-stuffed" spinel, and if the concept is applicable to prepare a high mixed electronic-ionic conductive, electrochemically active solid solution of the Li stuffed spinel with spinel-structured Li-ion battery electrodes. This could enable a single-phase fully solid electrode eliminating multi-phase interface incompatibility and impedance commonly observed in multi-phase solid electrolyte-cathode composites. Materials of composition LiM(III)TiO, M(III) = Cr or Al were prepared through solid-state methods. The room-temperature bulk Li-ion conductivity is 1.63 × 10 S cm for the composition LiCrTiO. Addition of LiBO (LBO) increases ionic and electronic conductivity reaching a bulk Li ion conductivity averaging 6.8 × 10 S cm, a total Li-ion conductivity averaging 4.2 × 10 S cm, and electronic conductivity averaging 3.8 × 10 S cm for the composition LiCrTiO with 1 wt. % LBO. An electrochemically active solid solution of LiCrMnO and LiNiMnO was prepared. This work proves that Li-stuffed spinels can achieve fast Li-ion conduction and that the concept is potentially useful to enable a single-phase fully solid electrode without interphase impedance.
研究了尖晶石结构的固体，以了解锂占据结构的多个晶体学位置形成“锂填充”尖晶石时是否能实现快速锂离子传导，以及该概念是否适用于制备具有尖晶石结构锂离子电池电极的高混合电子 - 离子导电、电化学活性的锂填充尖晶石固溶体。这可以实现单相全固态电极，消除多相固体电解质 - 阴极复合材料中常见的多相界面不相容性和阻抗。通过固态方法制备了组成LiM(III)TiO（M(III)=Cr或Al）的材料。对于LiCrTiO组成，室温下的体相锂离子电导率为1.63×10 S cm。添加LiBO（LBO）可提高离子和电子电导率，对于含1 wt.% LBO的LiCrTiO组成，其体相锂离子电导率平均达到6.8×10 S cm，总锂离子电导率平均为4.2×10 S cm，电子电导率平均为3.8×10 S cm。制备了LiCrMnO和LiNiMnO的电化学活性固溶体。这项工作证明锂填充尖晶石可以实现快速锂离子传导，并且该概念对于实现无相间阻抗的单相全固态电极可能是有用的。
