期刊
NANO LETTERS
卷 16, 期 6, 页码 3760-3767出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.6b01119
关键词
Lithium ion battery; thin film battery; in situ TEM; interfacial phenomena; solid electrolyte
类别
资金
- U.S. Department of Energy, Office of Basic Energy Sciences [DE-SC0002357]
- Northeastern Center for Chemical Energy Storage, an Energy Frontier Research Center - U.S. Department of Energy, Office of Basic Energy Sciences [DE-SC0001294]
- U.S. Department of Energy, Office of Science, Basic Energy Sciences (BES), Materials Sciences and Engineering Division
- Laboratory Directed Research and Development (LDRD) program at Brookhaven National Laboratory [13-022]
- SERB, India
- [DE-SC0012704]
Behaviors of functional interfaces are crucial factors in the performance and safety of energy storage and conversion devices. Indeed, solid electrode solid electrolyte interfacial impedance is now considered the main limiting factor in all-solid-state batteries rather than low ionic conductivity of the solid electrolyte. Here, we present a new approach to conducting in situ scanning transmission electron microscopy (STEM) coupled with electron energy loss spectroscopy (EELS) in order to uncover the unique interfacial phenomena related to lithium ion transport and its corresponding charge transfer. Our approach allowed quantitative spectroscopic characterization of a galvanostatically biased electrochemical system under in situ conditions. Using a LiCoO2/LiPON/Si thin film battery, an unexpected structurally disordered interfacial layer between LiCoO2 cathode and LiPON electrolyte was discovered to be inherent to this interface without cycling. During in situ charging, spectroscopic characterization revealed that this interfacial layer evolved to form highly oxidized Co ions species along with lithium, oxide and lithium peroxide species. These findings suggest that the mechanism of interfacial impedance at the LiCoO2/LiPON interface is caused by chemical changes rather than space charge effects. Insights gained from this technique will shed light on important challenges of interfaces in all-solid-state energy storage and conversion systems and facilitate improved engineering of devices operated far from equilibrium.
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