Amorphous LiCoO2-based Positive Electrode Active Materials with Good Formability for All-Solid-State Rechargeable Batteries

Abstract

ABSTRACTAmorphous LiCoO2-based positive electrode materials are synthesized by a mechanical milling technique. As a lithium oxy-acid, Li2SO4, Li3PO4, Li3BO3, Li2CO3, and LiNO3 are selected and milled with LiCoO2. XRD patterns indicate that reaction between LiCoO2 and these lithium oxy-acids proceeds. Amorphization mainly occurs, and several broad peaks attributable to cubic LiCoO2 are observed in all the samples. These amorphous active materials show mixed conductivities of electron and lithium ion. All-solid-state cells using the prepared amorphous active materials and the Li2.9B0.9S0.1O3.1 glass-ceramic electrolyte are fabricated and their charge-discharge properties are examined. The cells with only the 80LiCoO2·20Li2SO4 (mol%) and the 80LiCoO2·20Li3PO4 active materials function as secondary batteries. This is because higher lithium ionic conductivities are obtained in the 80LiCoO2·20Li2SO4 and 80LiCoO2·20Li3PO4 active materials than in the others. The largest capacity is obtained in the cell with the 80LiCoO2·20Li2SO4 active material because of its good formability and high lithium ionic conductivity. In addition, the cell with the 80LiCoO2·20Li2SO4 positive electrode active material shows the better cycle and rate performance than that with the crystalline LiCoO2. It is noted that the amorphization with lithium oxy-acids is a promising technique for achieving a novel active material with better electrochemical performance.