Abstract

The development of solid electrolytes with the combination of high ionic conductivity, electrochemical stability, and resistance to Li dendrites continues to be a challenge. A promising approach is to create inorganic–organic composites, where multiple components provide the needed properties, but the high sintering temperature of materials such as ceramics precludes close integration or co-sintering. Here, new ceramic–salt composite electrolytes that are cold sintered at 130 °C are demonstrated. As a model system, composites of Li 1.5 Al 0.5 Ge 1.5 (PO 4 ) 3 (LAGP) or Li 1+ x + y Al x Ti 2− x Si y P 3− y O 12 (LATP) with bis(trifluoromethanesulfonyl)imide (LiTFSI) salts are cold sintered. The resulting LAGP–LiTFSI and LATP–LiTFSI composites exhibit high relative densities of about 90% and ionic conductivities in excess of 10 −4 S cm −1 at 20 °C, which are comparable with the values obtained from LAGP and LATP sintered above 800 °C. It is also demonstrated that cold sintered LAGP–LiTFSI is electrochemically stable in Li symmetric cells over 1800 h at 0.2 mAh cm −2 . Cold sintering provides a new approach for bridging the gap in processing temperatures of different materials, thereby enabling high-performance composites for electrochemical systems.

Original languageEnglish (US)
Article number1807872
JournalAdvanced Functional Materials
Volume29
Issue number20
DOIs
StatePublished - May 16 2019

Fingerprint

Electrolytes
sintering
Sintering
electrolytes
composite materials
Composite materials
Ionic conductivity
ion currents
imides
Solid electrolytes
solid electrolytes
dendrites
Salts
ceramics
salts
Temperature
temperature
Processing
cells

All Science Journal Classification (ASJC) codes

  • Electronic, Optical and Magnetic Materials
  • Biomaterials
  • Chemistry(all)
  • Materials Science(all)
  • Condensed Matter Physics
  • Electrochemistry

Cite this

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title = "Ceramic–Salt Composite Electrolytes from Cold Sintering",
abstract = "The development of solid electrolytes with the combination of high ionic conductivity, electrochemical stability, and resistance to Li dendrites continues to be a challenge. A promising approach is to create inorganic–organic composites, where multiple components provide the needed properties, but the high sintering temperature of materials such as ceramics precludes close integration or co-sintering. Here, new ceramic–salt composite electrolytes that are cold sintered at 130 °C are demonstrated. As a model system, composites of Li 1.5 Al 0.5 Ge 1.5 (PO 4 ) 3 (LAGP) or Li 1+ x + y Al x Ti 2− x Si y P 3− y O 12 (LATP) with bis(trifluoromethanesulfonyl)imide (LiTFSI) salts are cold sintered. The resulting LAGP–LiTFSI and LATP–LiTFSI composites exhibit high relative densities of about 90{\%} and ionic conductivities in excess of 10 −4 S cm −1 at 20 °C, which are comparable with the values obtained from LAGP and LATP sintered above 800 °C. It is also demonstrated that cold sintered LAGP–LiTFSI is electrochemically stable in Li symmetric cells over 1800 h at 0.2 mAh cm −2 . Cold sintering provides a new approach for bridging the gap in processing temperatures of different materials, thereby enabling high-performance composites for electrochemical systems.",
author = "Wonho Lee and Lyon, {Christopher K.} and Seo, {Joo Hwan} and Raymond Lopez-Hallman and Yongjun Leng and Chao-yang Wang and Hickner, {Michael Anthony} and Randall, {Clive A.} and Gomez, {Enrique Daniel}",
year = "2019",
month = "5",
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Ceramic–Salt Composite Electrolytes from Cold Sintering. / Lee, Wonho; Lyon, Christopher K.; Seo, Joo Hwan; Lopez-Hallman, Raymond; Leng, Yongjun; Wang, Chao-yang; Hickner, Michael Anthony; Randall, Clive A.; Gomez, Enrique Daniel.

In: Advanced Functional Materials, Vol. 29, No. 20, 1807872, 16.05.2019.

Research output: Contribution to journalArticle

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T1 - Ceramic–Salt Composite Electrolytes from Cold Sintering

AU - Lee, Wonho

AU - Lyon, Christopher K.

AU - Seo, Joo Hwan

AU - Lopez-Hallman, Raymond

AU - Leng, Yongjun

AU - Wang, Chao-yang

AU - Hickner, Michael Anthony

AU - Randall, Clive A.

AU - Gomez, Enrique Daniel

PY - 2019/5/16

Y1 - 2019/5/16

N2 - The development of solid electrolytes with the combination of high ionic conductivity, electrochemical stability, and resistance to Li dendrites continues to be a challenge. A promising approach is to create inorganic–organic composites, where multiple components provide the needed properties, but the high sintering temperature of materials such as ceramics precludes close integration or co-sintering. Here, new ceramic–salt composite electrolytes that are cold sintered at 130 °C are demonstrated. As a model system, composites of Li 1.5 Al 0.5 Ge 1.5 (PO 4 ) 3 (LAGP) or Li 1+ x + y Al x Ti 2− x Si y P 3− y O 12 (LATP) with bis(trifluoromethanesulfonyl)imide (LiTFSI) salts are cold sintered. The resulting LAGP–LiTFSI and LATP–LiTFSI composites exhibit high relative densities of about 90% and ionic conductivities in excess of 10 −4 S cm −1 at 20 °C, which are comparable with the values obtained from LAGP and LATP sintered above 800 °C. It is also demonstrated that cold sintered LAGP–LiTFSI is electrochemically stable in Li symmetric cells over 1800 h at 0.2 mAh cm −2 . Cold sintering provides a new approach for bridging the gap in processing temperatures of different materials, thereby enabling high-performance composites for electrochemical systems.

AB - The development of solid electrolytes with the combination of high ionic conductivity, electrochemical stability, and resistance to Li dendrites continues to be a challenge. A promising approach is to create inorganic–organic composites, where multiple components provide the needed properties, but the high sintering temperature of materials such as ceramics precludes close integration or co-sintering. Here, new ceramic–salt composite electrolytes that are cold sintered at 130 °C are demonstrated. As a model system, composites of Li 1.5 Al 0.5 Ge 1.5 (PO 4 ) 3 (LAGP) or Li 1+ x + y Al x Ti 2− x Si y P 3− y O 12 (LATP) with bis(trifluoromethanesulfonyl)imide (LiTFSI) salts are cold sintered. The resulting LAGP–LiTFSI and LATP–LiTFSI composites exhibit high relative densities of about 90% and ionic conductivities in excess of 10 −4 S cm −1 at 20 °C, which are comparable with the values obtained from LAGP and LATP sintered above 800 °C. It is also demonstrated that cold sintered LAGP–LiTFSI is electrochemically stable in Li symmetric cells over 1800 h at 0.2 mAh cm −2 . Cold sintering provides a new approach for bridging the gap in processing temperatures of different materials, thereby enabling high-performance composites for electrochemical systems.

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