Regulating Solvation Structures Enabled by the Mesoporous Material MCM-41 for Rechargeable Lithium Metal Batteries

For developing the reversible lithium metal anode, constructing an ideal solid electrolyte interphase (SEI) by regulating the Li⁺ solvation structure is a powerful way to overcome the major obstacles of lithium dendrite and limited Coulombic efficiency (CE). Herein, spherical mesoporous molecular sieve MCM-41 nanoparticles are coated on a commercial PP separator and used to regulate the Li⁺ solvation structure for lithium metal batteries (LMBs). The regulated solvation structure exhibits an agminated state with more contact ion pairs (CIPs) and ionic aggregates (AGGs), which successfully construct a homogeneous inorganic-rich SEI in the lithium anode. Meanwhile, the regulated solvation structure weakens the interaction between the solvents and Li⁺, resulting in low Li⁺ desolvation energy and uniform Li deposition. Thus, a high CE (～96.76%), dendrite-free Li anode, and stable Li plating/stripping cycling for approximately 1000 h are achieved in the regulated carbonate-based electrolyte without any additives. Therefore, regulating the Li⁺ solvation structure in the electrolyte by employing a mesoporous material is a forceful way to construct an ideal SEI and harness lithium metal.