Solvent Sieving via 2D Silicalite‐1 Zeolite for High Energy Density Lithium Metal Batteries

Traditional strategies for constructing artificial interface layers typically via physical isolation to suppress lithium (Li) dendrite growth and interfacial side reactions while neglecting interactions with electrolyte, struggling to generate stable solid electrolyte interphase (SEI) and prevent continuous Li consumption upon long‐term cycling. Here we propose to regulate electrolyte solvation structure via a thin layer (∼490 nm thick) of two‐dimensional (2D) silicalite‐1 zeolite, which acts as solvent sieves to induce a solvent‐poor and anion‐rich solvation structure within its micropores, promoting the formation of an inorganic‐rich SEI. The unique 2D architecture not only enhances interfacial contact with electrode, thereby effectively suppressing parasitic side reactions, but also provides short‐range pathways for Li‐ion transport and homogenizes Li‐ion flux, facilitating uniform Li deposition. Moreover, the ordered micropores potently suppress shuttling of transition metal ions and scavenge residual H 2 O and generated HF, ensuring stable operation of Li metal batteries (LMBs) under practical conditions. As a result, the 4.1 Ah Li||NCM811 pouch cell delivered an energy density of 492 Wh kg −1 and stably cycled 90 cycles with a capacity retention of 95.7%. The design of 2D ultrathin artificial interface layers with solvation structure regulation capability offers new insights for advancing high‐energy density LMBs.