Rational designs of crystal solid‐solution materials for lithium‐ion batteries

Abstract We present a new strategy for computer‐aided rational design of quantum supercells of crystal solid‐solution (SS) materials for lithium‐ion batteries. Layered SS materials Li(NixCoyMn1−x−y)O2 are used to demonstrate our design strategy. Crystal structures obtained by rational design agree well with those fully optimized by quantum total‐energy calculations and real materials measured from experiments. Compared with conventional first‐principles determination of structures, our approach achieves a significant increase in efficiency without loss of reliability and predictability for searching new structures. We further discuss the necessary steps to develop a generic strategy to rationally design new composite electrode materials.