Additive strongly-coordinated solvation structure towards high-voltage 600 Wh/kg-class lithium metal pouch cell.

Anions involved solvation structures have been widely designed to construct inorganic enriched interfaces to enable wide voltage window, which, however, sacrifices the anions and effective Li+ conductivity. Here we propose an additive-coordinated solvation structure of Li+, with the preferred sacrifice of additive rather than anions, to realize stable cycling of 600 Wh kg⁻¹-scale Li metal batteries. Leveraging the molecular design of additives, even a trace amount addition allows for its coordination within the inner sheath of Li+ solvation structure. This not only attenuates the excessive consumption of anions and solvent molecules, but also facilitates the formation of robust protective interface. Benefiting from these advantages, a 550.7 Wh kg⁻¹ Li | |LiNi0.8Co0.1Mn0.1O2 pouch cell maintains 80.0% capacity retention over 180 cycles at 0.1 C charge and 0.5 C discharge rate. Furthermore, the paired Li | | lithium-rich manganese-based layered oxide pouch cell achieves a specific energy of 602.5 Wh kg⁻¹, sustaining 80% capacity retention for 60 cycles at 0.1 C charge/discharge rate, thus validating the suitability of additive coordinated solvation structure.