A Data-Driven Framework to Accelerate the Discovery of Hybrid Cathode Materials for Metal-Based Batteries

Selecting materials for hybrid cathodes, which involve a combination of intercalation and conversion materials, has gained interest due to their combined synergistic and compromised properties that are not attainable by their homogeneous counterparts. Herein, we present a data-driven framework for discovering hybrid cathode materials for metal-based batteries. This framework systematically explores the potential materials space for any given working ion, evaluates the candidate’s stability, and identifies the growth modes/adsorption of the components for a stable hybrid cathode. To demonstrate the application of the framework and its various possible outcomes, we performed a case study whose main design objective was to discover hybrid cathode materials with an average gravimetric energy density surpassing that of the widely used high energy density NMC333 cathode material. The framework identified LiCr₄GaS₈-Li₂S as a promising hybrid cathode material that achieves an average energy density of 1,424 Wh/kg (on a lithiated cathode basis) that exceeds NMC333’s maximum theoretical energy density of 1,028 Wh/kg. Furthermore, LiCr₄GaS₈-Li₂S has several desirable features: 1) the lithiated and delithiated intercalation and conversion phases are thermodynamically stable; 2) the marginal volume change of the intercalation material upon (de)lithiation mitigates the high-volume change of the conversion material; 3) the conversion material possesses high energy density that ameliorates the low energy density of the intercalation material; 4) the intercalation material can act as both a conductive additive and immobilizer of S to mitigate sulfur species shuttling, while actively contributing to the energy density of the cathode; 5) the intercalation material serves as an ideal support for the soft sulfur species and finally, 6) we anticipate that the life span, self-discharge, mechanical integrity, and capacity fading are better than those of conventional Li-S batteries. The developed framework was instrumental for exploring materials within the enormous potential hybrid cathode material space with pre-defined battery material design objectives.