Process design for calcination of nickel-based cathode materials by in situ characterization and multiscale modeling

Developing battery materials towards commercial use, from the early discovery through synthesis, processing, scaling up, and eventually to industrial production, may take decades. A notable example is Ni-based layered oxides, which were discovered as early as 1950s and intensively pursued as cathode active materials (CAMs) since the early 90s but have yet to realize their full commercial potential. Significant efforts have been devoted to materials development aiming at improving performance, far less to process development for large-scale synthesis and processing of CAMs. Herein, we present a rational design of calcination for scalable production of Ni-based CAMs. We start with an overview of the current understanding and knowledge gaps hindering rational process design and scaling-up of the calcination process. Then with specific examples, we demonstrate how to tackle those fundamental challenges through in situ characterization and multiscale modeling. We conclude by providing perspectives on the remaining challenges and emerging opportunities in commercial development of Ni-based cathodes, calling for more endeavors in this field. Graphical abstract