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Title: In Situ STEM-EELS observation of nanoscale interfacial phenomena in all-solid-state batteries

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 LiCoO 2/LiPON/Si thin film battery, an unexpected structurally disordered interfacial layer between LiCoO 2 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 LiCoO 2/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 storagemore » and conversion systems and facilitate improved engineering of devices operated far from equilibrium.« less
 [1] ;  [2] ;  [3] ;  [3] ;  [3] ;  [3] ;  [4] ;  [4] ;  [1]
  1. Univ. of California, San Diego, CA (United States). Dept. of NanoEngineering
  2. Univ. of California, San Diego, CA (United States). Dept. of NanoEngineering; Amrita Vishwa Vidyapeetham Univ., Kochi (India). Amrita Centre for Nanosciences and Molecular Medicine
  3. Brookhaven National Lab. (BNL), Upton, NY (United States)
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Material Science and Technology Division
Publication Date:
Report Number(s):
Journal ID: ISSN 1530-6984; KC0403020
Grant/Contract Number:
SC0002357; SC0001294; SC0012704; AC05-00OR22725
Accepted Manuscript
Journal Name:
Nano Letters
Additional Journal Information:
Journal Volume: 16; Journal Issue: 6; Journal ID: ISSN 1530-6984
American Chemical Society
Research Org:
Univ. of California, San Diego, CA (United States); Brookhaven National Lab. (BNL), Upton, NY (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE Laboratory Directed Research and Development (LDRD) Program; Science and Engineering Research Board (SERB) (India)
Contributing Orgs:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Amrita Vishwa Vidyapeetham Univ., Kochi (India)
Country of Publication:
United States
36 MATERIALS SCIENCE; in situ TEM; interfacial phenomena; Lithium ion battery; solid electrolyte; thin film battery
OSTI Identifier:
Alternate Identifier(s):
OSTI ID: 1362191