Design Lithium Exchanged Zeolite Based Multifunctional Electrode Additive for Ultra‐High Loading Electrode Toward High Energy Density Lithium Metal Battery

Abstract The practicalization of a high energy density battery requires the electrode to achieve decent performance under ultra‐high active material loading. However, as the electrode thickness increases, there is a notable restriction in ionic transport in the electrodes, limiting the diffusion kinetics of Li+ and the utilization rate of active substances. In this study, lithium‐ion‐exchanged zeolite X (Li‐X zeolite) is synthesized via Li+ exchange strategy to enhance Li+ diffusion kinetics. When incorporated Li–X zeolite into the ultra‐high loading cathodes, it possesses i) high electron conductivity with a uniform network by reducing tortuosity, ii) decent ion conductivity attributes to modulated Li+ diffusivity of Li‐X and iii) high elasticity to prevent particle‐level cracking and electrode‐level disintegration. Moreover, Li–X zeolite at the solid/liquid interface facilitates the formation of a stable cathode electrolyte interface, which effectively suppresses side reactions and mitigates the dissolution of transition cations. Therefore, an ultra‐high loading (66 mg cm−2) cathode is fabricated via dry electrode technology, demonstrating a remarkable areal capacity of 12.7 mAh cm−2 and a high energy density of 464 Wh kg−1 in a lithium metal battery. The well‐designed electrode structure with multifunctional Li–X zeolite as an additive in thick cathodes holds promise to enhance the battery's rate capability, cycling stability, and overall energy density.