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Title: A Silica-Aerogel-Reinforced Composite Polymer Electrolyte with High Ionic Conductivity and High Modulus

Abstract

High-energy all-solid-state lithium (Li) batteries have great potential as next-generation energy-storage devices. Among all choices of electrolytes, polymer-based systems have attracted widespread attention due to their low density, low cost, and excellent processability. However, they are generally mechanically too weak to effectively suppress Li dendrites and have lower ionic conductivity for reasonable kinetics at ambient temperature. Here, an ultrastrong reinforced composite polymer electrolyte (CPE) is successfully designed and fabricated by introducing a stiff mesoporous SiO 2 aerogel as the backbone for a polymer-based electrolyte. The interconnected SiO 2 aerogel not only performs as a strong backbone strengthening the whole composite, but also offers large and continuous surfaces for strong anion adsorption, which produces a highly conductive pathway across the composite. As a consequence, a high modulus of ≈0.43 GPa and high ionic conductivity of ≈0.6 mS cm -1 at 30°C are simultaneously achieved. Furthermore, LiFePO 4–Li full cells with good cyclability and rate capability at ambient temperature are obtained. Full cells with cathode capacity up to 2.1 mAh cm -2 are also demonstrated. The aerogel-reinforced CPE represents a new design principle for solid-state electrolytes and offers opportunities for future all-solid-state Li batteries.

Authors:
 [1];  [2];  [1];  [1];  [1];  [1]; ORCiD logo [3]
  1. Stanford Univ., CA (United States). Dept. of Materials Science and Engineering
  2. Stanford Univ., CA (United States). Dept. of Mechanical Engineering
  3. Stanford Univ., CA (United States). Dept. of Materials Science and Engineering; SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Institute for Materials and Energy Science (SIMES)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); National Science Foundation (NSF)
OSTI Identifier:
1470755
Alternate Identifier(s):
OSTI ID: 1457072
Grant/Contract Number:  
AC02-76SF00515; ECCS-1542152
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Materials
Additional Journal Information:
Journal Volume: 30; Journal Issue: 32; Journal ID: ISSN 0935-9648
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 25 ENERGY STORAGE; composite polymer electrolytes; SiO2 aerogels; solid-state batteries

Citation Formats

Lin, Dingchang, Yuen, Pak Yan, Liu, Yayuan, Liu, Wei, Liu, Nian, Dauskardt, Reinhold H., and Cui, Yi. A Silica-Aerogel-Reinforced Composite Polymer Electrolyte with High Ionic Conductivity and High Modulus. United States: N. p., 2018. Web. doi:10.1002/adma.201802661.
Lin, Dingchang, Yuen, Pak Yan, Liu, Yayuan, Liu, Wei, Liu, Nian, Dauskardt, Reinhold H., & Cui, Yi. A Silica-Aerogel-Reinforced Composite Polymer Electrolyte with High Ionic Conductivity and High Modulus. United States. doi:10.1002/adma.201802661.
Lin, Dingchang, Yuen, Pak Yan, Liu, Yayuan, Liu, Wei, Liu, Nian, Dauskardt, Reinhold H., and Cui, Yi. Mon . "A Silica-Aerogel-Reinforced Composite Polymer Electrolyte with High Ionic Conductivity and High Modulus". United States. doi:10.1002/adma.201802661. https://www.osti.gov/servlets/purl/1470755.
@article{osti_1470755,
title = {A Silica-Aerogel-Reinforced Composite Polymer Electrolyte with High Ionic Conductivity and High Modulus},
author = {Lin, Dingchang and Yuen, Pak Yan and Liu, Yayuan and Liu, Wei and Liu, Nian and Dauskardt, Reinhold H. and Cui, Yi},
abstractNote = {High-energy all-solid-state lithium (Li) batteries have great potential as next-generation energy-storage devices. Among all choices of electrolytes, polymer-based systems have attracted widespread attention due to their low density, low cost, and excellent processability. However, they are generally mechanically too weak to effectively suppress Li dendrites and have lower ionic conductivity for reasonable kinetics at ambient temperature. Here, an ultrastrong reinforced composite polymer electrolyte (CPE) is successfully designed and fabricated by introducing a stiff mesoporous SiO2 aerogel as the backbone for a polymer-based electrolyte. The interconnected SiO2 aerogel not only performs as a strong backbone strengthening the whole composite, but also offers large and continuous surfaces for strong anion adsorption, which produces a highly conductive pathway across the composite. As a consequence, a high modulus of ≈0.43 GPa and high ionic conductivity of ≈0.6 mS cm-1 at 30°C are simultaneously achieved. Furthermore, LiFePO4–Li full cells with good cyclability and rate capability at ambient temperature are obtained. Full cells with cathode capacity up to 2.1 mAh cm-2 are also demonstrated. The aerogel-reinforced CPE represents a new design principle for solid-state electrolytes and offers opportunities for future all-solid-state Li batteries.},
doi = {10.1002/adma.201802661},
journal = {Advanced Materials},
number = 32,
volume = 30,
place = {United States},
year = {2018},
month = {6}
}

Journal Article:
Free Publicly Available Full Text
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Citation Metrics:
Cited by: 16 works
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Figures / Tables:

Figure 1 Figure 1: Material synthesis and characterizations. a) Schematic showing the synthetic procedures of the SiO2-aerogel-reinforced CPE. With the SiO2 aerogel as the framework, LiTFSl dissolved in liquid PEGDA/SCN mixture was infused into the aerogel under vacuum, followed by ultraviolet photocuring to afford crosslinked PEO within the aerogel framework. The magnifiedmore » drawing in the right shows the detailed microstructure of the composite electrolyte. b,c) Digital photo images showing the pristine SiO2 aerogel film (b) and the final composite electrolyte film (c), where the infusion of the materials increases the transparency of the film. d,e) SEM images showing the surface morphologies of pristine SiO2 aerogel (d) and composite electrolyte (e). The high-volume pores are fully filled after infusion and photocuring. f,g) BET surface area (f) and pore size distribution (g) of the SiO2 aerogel, which exhibits high surface area of 701 m2 g-1 with most of the pores <30 nm.« less

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    Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.