In Situ STEM-EELS Observation of Nanoscale Interfacial Phenomena in All-Solid-State Batteries
- Univ. of California, San Diego, CA (United States). Dept. of NanoEngineering
- Univ. of California, San Diego, CA (United States). Dept. of NanoEngineering; Amrita Vishwa Vidyapeetham Univ., Kochi (India). Amrita Centre for Nanosciences and Molecular Medicine
- Brookhaven National Lab. (BNL), Upton, NY (United States)
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
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. In this paper, 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. Finally, 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.
- Research Organization:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Univ. of California, San Diego, CA (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States)
- Sponsoring Organization:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Laboratory Directed Research and Development (LDRD) Program; Science and Engineering Research Board (SERB), India; Science and Engineering Research Board (SERB) (India)
- Contributing Organization:
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Amrita Vishwa Vidyapeetham Univ., Kochi (India)
- Grant/Contract Number:
- AC05-00OR22725; SC0002357; SC0001294; SC0012704
- OSTI ID:
- 1362191
- Alternate ID(s):
- OSTI ID: 1257962; OSTI ID: 1595355
- Report Number(s):
- BNL-112300-2016-JA; KC0203020; ERKCZ06
- Journal Information:
- Nano Letters, Vol. 16, Issue 6; ISSN 1530-6984
- Publisher:
- American Chemical SocietyCopyright Statement
- Country of Publication:
- United States
- Language:
- English
Web of Science
Similar Records
Effects of cathode electrolyte interfacial (CEI) layer on long term cycling of all-solid-state thin-film batteries
All Solid-State Li/LLZO/LCO Battery Enabled by Alumina Interfacial Coating