Regulating Solvation Structures Enabled by the Mesoporous Material MCM-41 for Rechargeable Lithium Metal Batteries
Lina Zhao, Zeyu Wu, Zhenhua Wang, Zhe Bai, Wang Sun, Kening Sun
Abstract
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.