Computational Screening of Layered Materials for Multivalent Ion Batteries

[Image: see text] Batteries based on multivalent ion (such as Al(3+), Ca(2+), and Mg(2+)) intercalation materials have attracted extensive research interest due to their impressive capacity improvement and cost reduction compared with Li-ion batteries. However, the materials for state-of-the-art multivalent ion batteries still suffer from drawbacks such as sluggish ion mobility, poor rate performance, and low cyclic stability, bringing challenges for the design and investigation of new materials. Layered cathode materials are widely applied in current commercial batteries due to their outstanding ionic conductivity and structural stability, which may also hold the key for the cathodes of multivalent batteries. Therefore, combining database screening and density functional theory computations, we evaluated the layered compounds in Materials Project database by theoretical capacity, thermodynamic stability, experimental availability, voltage, volume variation, electronic conductivity, and ionic migration barrier and achieved over 20 kinds of layered cathode materials for multivalent batteries. Through Mg ion substitution for Ca sites, we further achieved several kinds of cathode materials for Mg-ion batteries with ideal stability, voltage, and ion diffusion barriers. We hope the methodology and screened materials could promote the development of multivalent ion batteries.