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Title: In Situ STEM-EELS Observation of Nanoscale Interfacial Phenomena in All-Solid-State Batteries

Abstract

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 systemsmore » and facilitate improved engineering of devices operated far from equilibrium.« less

Authors:
 [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). Materials Science & Technology Division
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of California, San Diego, CA (United States); Brookhaven National Lab. (BNL), Upton, NY (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; Science and Engineering Research Board (SERB) (India)
Contributing Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Amrita Vishwa Vidyapeetham Univ., Kochi (India)
OSTI Identifier:
1362191
Alternate Identifier(s):
OSTI ID: 1257962; OSTI ID: 1595355
Report Number(s):
BNL-112300-2016-JA
Journal ID: ISSN 1530-6984; KC0203020; ERKCZ06
Grant/Contract Number:  
AC05-00OR22725; SC0002357; SC0001294; SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
Nano Letters
Additional Journal Information:
Journal Volume: 16; Journal Issue: 6; Journal ID: ISSN 1530-6984
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 25 ENERGY STORAGE; in situ TEM; interfacial phenomena; Lithium ion battery; solid electrolyte; thin film battery

Citation Formats

Wang, Ziying, Santhanagopalan, Dhamodaran, Zhang, Wei, Wang, Feng, Xin, Huolin L., He, Kai, Li, Juchuan, Dudney, Nancy, and Meng, Ying Shirley. In Situ STEM-EELS Observation of Nanoscale Interfacial Phenomena in All-Solid-State Batteries. United States: N. p., 2016. Web. doi:10.1021/acs.nanolett.6b01119.
Wang, Ziying, Santhanagopalan, Dhamodaran, Zhang, Wei, Wang, Feng, Xin, Huolin L., He, Kai, Li, Juchuan, Dudney, Nancy, & Meng, Ying Shirley. In Situ STEM-EELS Observation of Nanoscale Interfacial Phenomena in All-Solid-State Batteries. United States. doi:10.1021/acs.nanolett.6b01119.
Wang, Ziying, Santhanagopalan, Dhamodaran, Zhang, Wei, Wang, Feng, Xin, Huolin L., He, Kai, Li, Juchuan, Dudney, Nancy, and Meng, Ying Shirley. Tue . "In Situ STEM-EELS Observation of Nanoscale Interfacial Phenomena in All-Solid-State Batteries". United States. doi:10.1021/acs.nanolett.6b01119. https://www.osti.gov/servlets/purl/1362191.
@article{osti_1362191,
title = {In Situ STEM-EELS Observation of Nanoscale Interfacial Phenomena in All-Solid-State Batteries},
author = {Wang, Ziying and Santhanagopalan, Dhamodaran and Zhang, Wei and Wang, Feng and Xin, Huolin L. and He, Kai and Li, Juchuan and Dudney, Nancy and Meng, Ying Shirley},
abstractNote = {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.},
doi = {10.1021/acs.nanolett.6b01119},
journal = {Nano Letters},
number = 6,
volume = 16,
place = {United States},
year = {2016},
month = {5}
}

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Works referencing / citing this record:

In Situ Transmission Electron Microscopy Studies of Electrochemical Reaction Mechanisms in Rechargeable Batteries
journal, June 2019


In Situ Transmission Electron Microscopy Studies of Electrochemical Reaction Mechanisms in Rechargeable Batteries
journal, June 2019