Prospects of armchair-GeSe and zigzag-GeTe as promising candidates for novel fluoride/chloride ion batteries: a first-principles exploration.
Chen Junjie J, Rao Qinyan Q, Lin Yuda Y
The development of novel rechargeable fluoride-ion batteries (FIBs) and chloride-ion batteries (CIBs) constitutes a major step forward in the field of anion-shuttle battery systems, and this work systematically explores the potential of monolayer GeX (X = Se/Te) as cathode materials for such systems. By employing first-principles calculations, we have assessed key electrochemical properties including thermodynamic stability, electronic structure, adsorption behavior, ion diffusion barriers, average open-circuit voltage (OCV), and theoretical specific capacity. Our findings reveal that both monolayer "armchair" structured GeSe and "zigzag" structured GeTe intrinsically adsorb fluoride and chloride ions, with charge transfer and electronic structure analyses indicating a strong interaction between the adsorbed F-/Cl- and the substrate. The relatively low diffusion barriers (0.11 eV for GeSe in FIBs and 0.38 eV for GeTe in CIBs) together with the high theoretical specific capacities (427.3 mA h g-1 for GeSe in FIBs and 490.8 mA h g-1 for GeTe in CIBs) suggest that monolayer GeSe is preferable as a cathode material for fluoride ion batteries, while GeTe is more favorable for chloride ion battery applications. Additionally, ab initio molecular dynamics (AIMD) simulations confirm that the monolayer GeSe and GeTe maintain structural stability and ion adsorption capability at room temperature. These results underscore the significant potential of monolayer GeX for use as a high-performance electrode material in next-generation FIBs and CIBs, while also providing a verifiable research framework that can help steer the broader anion battery field from fragmented exploration toward more systematic and in-depth investigation of materials science and electrochemical mechanisms.