Journal
ACS NANO
Volume 16, Issue 12, Pages 20891-20901Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.2c08441
Keywords
Dendrite-free lithium metal anode; Solvation structure; Inorganic-rich SEI; Multifunctional separators; Mesoporous materials
Categories
Funding
- National Natural Science Foundation of China
- [22179007]
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Regulating the solvation structure of lithium ions is a powerful approach to overcome the challenges of lithium dendrite and limited Coulombic efficiency in developing reversible lithium metal anodes. In this study, mesoporous MCM-41 nanoparticles are used to regulate the solvation structure, resulting in a homogeneous inorganic-rich solid electrolyte interphase (SEI) and improved lithium deposition. The regulated solvation structure enhances the Coulombic efficiency and stability of 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.
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