Journal
ACS APPLIED MATERIALS & INTERFACES
Volume 13, Issue 43, Pages 51048-51056Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsami.1c15742
Keywords
overcrowded solvation structure; aqueous lithium-ion batteries; LiF-enriched interphase; 1,4-dioxane; wide electrochemical window
Funding
- National Natural Science Foundation of China [21905265]
- Fundamental Research Funds for the Central Universities [WK3430000007, WK2060140026]
- National Key R&D Program of China [2016YFB0901500, 51771094]
- Ministry of Education of China [B12015, IRT13R30]
- Tianjin High-Tech [18JCZDJC31500]
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The study introduces an overcrowded electrolyte using 1,4-dioxane as an agent to improve the performance of aqueous batteries, achieving a robust LiF-enriched SEI and wide electrolyte operation window. This strategy shows promise for developing low-cost and stable high-voltage aqueous batteries.
The water-in-salt electrolyte (WISE) features intimate interactions between a cation and anion, which induces the formation of an anion-derived solid electrolyte interphase (SEI) and expands the aqueous electrolyte voltage window to >3.0 V. Although further increasing the salt concentration (even to >60 molality (m)) can gradually improve water stability, issues about cost and practical feasibility are concerned. An alternative approach is to intensify ion-solvent interactions in the inner solvation structure by shielding off outward electrostatic attractions from nearby ions. Here, we design an overcrowded electrolyte using the non-polar, hydrogen-bonding 1,4-dioxane (DX) as an overcrowding agent, thereby achieving a robust LiF-enriched SEI and wide electrolyte operation window (3.7 V) with a low salt concentration (<2 m). As a result, the electrochemical performance of aqueous Li4Ti5O12/LiMn2O4 full cells can be substantially improved (88.5% capacity retention after 200 cycles, at 0.57 C). This study points out a promising strategy to develop low-cost and stable high-voltage aqueous batteries.
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