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- Title
Constructing Efficient Mg(CF<sub>3</sub>SO<sub>3</sub>)<sub>2</sub> Electrolyte via Tailoring Solvation and Interface Chemistry for High‐Performance Rechargeable Magnesium Batteries.
- Authors
Zhang, Duo; Wang, Yaru; Yang, Yang; Zhang, Yang; Zhao, Yazhen; Pan, Ming; Sun, Yukun; Chen, Shaopeng; Liu, Xiaoshuo; Wang, Jiulin; NuLi, Yanna
- Abstract
Non‐passivating and chlorine‐free electrolytes are crucial for making rechargeable magnesium batteries practically feasible. Rational design of a brand‐new electrolyte should balance both Mg salt and solvent considering that the interfacial reactions occurring at electrolyte/electrode interface involve with ion solvation structure. Herein, nitrogenous 2‐methoxyethylamine (MOEA) is employed as co‐solvent to regulate the coordination behavior of cations/anions in Mg(CF3SO3)2‐G2 electrolyte after a series of screenings, which enables significantly ameliorated physiochemical properties. In‐depth insight on the mechanism of MOEA participating in the solvation structure formation and interfacial reactions is deduced via density functional theory calculations and molecular dynamics simulations. The decompositions of MOEA‐tailored cationic/anionic complexes shield Mg anode and Mo6S8 cathode with Mg3N2 and CxNy‐rich layers, respectively, which enable to suppress side reaction and accelerate Mg2+ transportation with competing desolvation at the interfacial layer. All the merits endow remarkable performances of symmetric/asymmetric cells with ultralong‐cycle lives over 5000 h and a remarkable average Coulombic efficiency of 98.3% after 8200 cycles (≈11 months), respectively. Additionally, a cheerful discharge capacity of ≈59.3 mAh g−1 is obtained over 1000 cycles at 0.5 C in Mo6S8||Mg full cell.
- Subjects
SURFACE chemistry; INTERFACIAL reactions; LITHIUM cells; ELECTROLYTES; MOLECULAR theory; MOLECULAR dynamics; SOLVATION
- Publication
Advanced Energy Materials, 2023, Vol 13, Issue 39, p1
- ISSN
1614-6832
- Publication type
Article
- DOI
10.1002/aenm.202301795