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

Wang, Ziying; Santhanagopalan, Dhamodaran; Zhang, Wei; Wang, Feng; Xin, Huolin L.; He, Kai; Li, Juchuan; Dudney, Nancy; Meng, Ying Shirley

doi:10.1021/acs.nanolett.6b01119

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

Journal Article · Tue May 03 00:00:00 EDT 2016 · Nano Letters

DOI:https://doi.org/10.1021/acs.nanolett.6b01119· OSTI ID:1257962

Wang, Ziying ^[1]; Santhanagopalan, Dhamodaran ^[2]; Zhang, Wei ^[3]; Wang, Feng ^[3]; Xin, Huolin L. ^[3]; He, Kai ^[3]; Li, Juchuan ^[4]; Dudney, Nancy ^[4]; Meng, Ying Shirley ^[1]

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). Material Science and 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.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Lab. (BNL), Upton, NY (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Univ. of California, San Diego, CA (United States)

Sponsoring Organization:: Science and Engineering Research Board (SERB) (India); Science and Engineering Research Board (SERB), India; USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Contributing Organization:: Amrita Vishwa Vidyapeetham Univ., Kochi (India); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Grant/Contract Number:: AC05-00OR22725; SC0001294; SC0002357; SC0012704

OSTI ID:: 1257962

Alternate ID(s):: OSTI ID: 1362191
OSTI ID: 1595355

Report Number(s):: BNL--112300-2016-JA; KC0403020

Journal Information:: Nano Letters, Journal Name: Nano Letters Journal Issue: 6 Vol. 16; ISSN 1530-6984

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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25 ENERGY STORAGE
36 MATERIALS SCIENCE
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In Situ STEM-EELS observation of nanoscale interfacial phenomena in all-solid-state batteries

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