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Title: Investigating the Effects of Lithium Phosphorous Oxynitride Coating on Blended Solid Polymer Electrolytes

Abstract

Solid-state electrolytes are very promising to enhance the safety of lithium ion batteries. Two classes of solid electrolytes, polymer and ceramic, can be combined to yield a hybrid electrolyte that can synergistically combine the properties of both materials. Chemical stability, thermal stability, and high mechanical modulus of ceramic electrolytes against dendrite penetration can be combined with the flexibility and ease of processing of polymer electrolytes. By laminating a polymer electrolyte with a ceramic electrolyte, the stability of the solid electrolyte is expected to improve against lithium metal, and the ionic conductivity could remain close to the value of the original polymer electrolyte as long as an appropriate thickness of the ceramic electrolyte is applied. In this paper we report a bilayered lithium-ion conducting hybrid solid electrolyte consisting of a blended polymer electrolyte (BPE) laminated with a thin layer of the inorganic solid electrolyte lithium phosphorous oxynitride (LiPON). The hybrid system was thoroughly studied. First, we investigated the influence of polymer chain length and lithium salt ratio on the ionic conductivity of the BPE based on poly(ethylene oxide) (PEO) and poly(propylene carbonate) (PPC) with the salt lithium bis(trifluoromethanesulfonyl)imide (LiTFSI). The optimized BPE consisted of 100k molecular weight PEO, 50k molecular weightmore » PPC, and 25(w/w)% LiTFSI, (denoted as PEO100PPC50LiTFSI25) which exhibited an ionic conductivity of 2.11×10-5 S/cm, and the ionic conductivity showed no thermal memory effects as the PEO crystallites were well disrupted by PPC and LiTFSI. Secondly, the effects of LiPON coating on the BPE were evaluated as a function of thickness down to 20 nm. The resulting bilayer structure showed an increase in the voltage window from 5.2 to 5.5 V (vs Li/Li+) and thermal activation energies that approached the activation energy of the BPE when thinner LiPON layers were used, resulting in similar ionic conductivities for 30 nm LiPON coatings on PEO100PPC50LiTFSI25. Coating BPEs with a thin layer of LiPON is shown to be an effective strategy to improve the long-term stability against lithium.« less

Authors:
 [1]; ORCiD logo [2]; ORCiD logo [2];  [3];  [3]; ORCiD logo [2]; ORCiD logo [1]
  1. National Renewable Energy Lab. (NREL), Golden, CO (United States); Univ. of Louisiana Lafayette, LA (United States)
  2. National Renewable Energy Lab. (NREL), Golden, CO (United States)
  3. Univ. of Louisiana Lafayette, LA (United States)
Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE); National Science Foundation (NSF); Chevron Corporation; USDOE Laboratory Directed Research and Development (LDRD) Program
OSTI Identifier:
1660221
Report Number(s):
NREL/JA-5K00-76378
Journal ID: ISSN 1944-8244; MainId:6404;UUID:70b58b2c-d967-ea11-9c31-ac162d87dfe5;MainAdminID:17301
Grant/Contract Number:  
AC36-08GO28308; 1832963
Resource Type:
Accepted Manuscript
Journal Name:
ACS Applied Materials and Interfaces
Additional Journal Information:
Journal Volume: 12; Journal Issue: 36; Journal ID: ISSN 1944-8244
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; ceramic; lithium ion batteries; polymer; solid state electrolytes

Citation Formats

LaCoste, Jed, Li, Zhifei, Xu, Yun, He, Zizhou, Matherne, Drew, Zakutayev, Andriy, and Fei, Ling. Investigating the Effects of Lithium Phosphorous Oxynitride Coating on Blended Solid Polymer Electrolytes. United States: N. p., 2020. Web. https://doi.org/10.1021/acsami.0c09113.
LaCoste, Jed, Li, Zhifei, Xu, Yun, He, Zizhou, Matherne, Drew, Zakutayev, Andriy, & Fei, Ling. Investigating the Effects of Lithium Phosphorous Oxynitride Coating on Blended Solid Polymer Electrolytes. United States. https://doi.org/10.1021/acsami.0c09113
LaCoste, Jed, Li, Zhifei, Xu, Yun, He, Zizhou, Matherne, Drew, Zakutayev, Andriy, and Fei, Ling. Thu . "Investigating the Effects of Lithium Phosphorous Oxynitride Coating on Blended Solid Polymer Electrolytes". United States. https://doi.org/10.1021/acsami.0c09113. https://www.osti.gov/servlets/purl/1660221.
@article{osti_1660221,
title = {Investigating the Effects of Lithium Phosphorous Oxynitride Coating on Blended Solid Polymer Electrolytes},
author = {LaCoste, Jed and Li, Zhifei and Xu, Yun and He, Zizhou and Matherne, Drew and Zakutayev, Andriy and Fei, Ling},
abstractNote = {Solid-state electrolytes are very promising to enhance the safety of lithium ion batteries. Two classes of solid electrolytes, polymer and ceramic, can be combined to yield a hybrid electrolyte that can synergistically combine the properties of both materials. Chemical stability, thermal stability, and high mechanical modulus of ceramic electrolytes against dendrite penetration can be combined with the flexibility and ease of processing of polymer electrolytes. By laminating a polymer electrolyte with a ceramic electrolyte, the stability of the solid electrolyte is expected to improve against lithium metal, and the ionic conductivity could remain close to the value of the original polymer electrolyte as long as an appropriate thickness of the ceramic electrolyte is applied. In this paper we report a bilayered lithium-ion conducting hybrid solid electrolyte consisting of a blended polymer electrolyte (BPE) laminated with a thin layer of the inorganic solid electrolyte lithium phosphorous oxynitride (LiPON). The hybrid system was thoroughly studied. First, we investigated the influence of polymer chain length and lithium salt ratio on the ionic conductivity of the BPE based on poly(ethylene oxide) (PEO) and poly(propylene carbonate) (PPC) with the salt lithium bis(trifluoromethanesulfonyl)imide (LiTFSI). The optimized BPE consisted of 100k molecular weight PEO, 50k molecular weight PPC, and 25(w/w)% LiTFSI, (denoted as PEO100PPC50LiTFSI25) which exhibited an ionic conductivity of 2.11×10-5 S/cm, and the ionic conductivity showed no thermal memory effects as the PEO crystallites were well disrupted by PPC and LiTFSI. Secondly, the effects of LiPON coating on the BPE were evaluated as a function of thickness down to 20 nm. The resulting bilayer structure showed an increase in the voltage window from 5.2 to 5.5 V (vs Li/Li+) and thermal activation energies that approached the activation energy of the BPE when thinner LiPON layers were used, resulting in similar ionic conductivities for 30 nm LiPON coatings on PEO100PPC50LiTFSI25. Coating BPEs with a thin layer of LiPON is shown to be an effective strategy to improve the long-term stability against lithium.},
doi = {10.1021/acsami.0c09113},
journal = {ACS Applied Materials and Interfaces},
number = 36,
volume = 12,
place = {United States},
year = {2020},
month = {8}
}

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