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Published on: August 12, 2013
Tailoring Li3N-Contained Complementary Gradient Solid Electrolyte Interphase in High-Performance 3.2 V Aqueous
Fengcheng Tang1, Zhuoni Zhao1, Fangkun Li2
1School of Metallurgy and Environment, National Energy Metal Resources and New Materials Key Laboratory, Engineering Research Center of the Ministry of Education for Advanced Battery Materials, Central South University, Changsha, 410083, PR China.
Researchers developed a new method to create a stable lithium nitride (Li3N) solid electrolyte interphase (SEI) in aqueous lithium-ion batteries (ALIBs). This breakthrough enables higher voltages and longer battery life by preventing hydrolysis and improving interfacial stability.
Area of Science:
- Electrochemistry
- Materials Science
- Energy Storage
Background:
- Aqueous lithium-ion batteries (ALIBs) face limitations in operating voltage (< 3 V) and interfacial stability.
- Lithium nitride (Li3N), a key component for high-voltage solid electrolyte interphase (SEI) in non-aqueous batteries, is prone to hydrolysis in aqueous electrolytes, hindering its use in ALIBs.
- Existing ALIBs suffer from unstable electrode/electrolyte interphases and hydrogen evolution reactions at higher voltages.
Purpose of the Study:
- To overcome the limitations of low operating voltages and unstable interphases in ALIBs.
- To enable the unprecedented construction of a Li3N-containing complementary gradient SEI in aqueous media.
- To advance the development of high-voltage, long-term stable ALIBs.
Main Methods:
- Employed a two-pronged strategy involving an asymmetric amide co-solvent (N-methylformamide, NMF) and overpotential-driven interfacial engineering.
- Applied an appropriate overpotential (0.3 V) to drive the formation of a Li3N-contained complementary gradient SEI.
- Investigated the potential three-step formation mechanism of the LiF/Li3N SEI involving sequential decomposition of TFSI-, NMF, and H2O.
Main Results:
- Successfully constructed a robust complementary gradient SEI composed of an outer LiF layer and an inner, stable Li3N layer through internal self-protection in aqueous media.
- The tailored SEI structure demonstrated synergistic chemical stability and rapid formation dynamics, effectively inhibiting the hydrogen evolution reaction.
- LiMn2O4||Li4Ti5O12 cells exhibited excellent cycling stability, retaining capacity over 700 cycles at 2C and 2000 cycles at 5C (3.2 V).
Conclusions:
- Established a novel strategy for stabilizing Li3N-containing electrode/electrolyte interphases in aqueous batteries.
- Demonstrated a distinctive pathway for advancing high-voltage and long-term stable ALIBs.
- The developed method offers a promising approach for next-generation aqueous energy storage systems.
