Interfaces between Ceramic and Polymer Electrolytes: A Comparison of Oxide and Sulfide Solid Electrolytes for Hybrid Solid-State Batteries

Dominic Spencer jolly; Dominic L. R. Melvin; Isabella D. R. Stephens; Rowena H. Brugge; Shengda D. Pu; Junfu Bu; Ziyang Ning; Gareth O. Hartley; Paul Adamson; Patrick S. Grant; Ainara Aguadero; Peter G. Bruce

doi:10.3390/inorganics10050060

Interfaces between Ceramic and Polymer Electrolytes: A Comparison of Oxide and Sulfide Solid Electrolytes for Hybrid Solid-State Batteries

Dominic Spencer jolly, Dominic L. R. Melvin, Isabella D. R. Stephens, Rowena H. Brugge, Shengda D. Pu, Junfu Bu, Ziyang Ning, Gareth O. Hartley, Paul Adamson, Patrick S. Grant, Ainara Aguadero, Peter G. Bruce^*

^*Corresponding author for this work

Metallurgy and Materials

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Abstract

Hybrid solid-state batteries using a bilayer of ceramic and solid polymer electrolytes may offer advantages over using a single type of solid electrolyte alone. However, the impedance to Li⁺ transport across interfaces between different electrolytes can be high. It is important to determine the resistance to Li⁺ transport across these heteroionic interfaces, as well as to understand the underlying causes of these resistances; in particular, whether chemical interphase formation contributes to giving high resistances, as in the case of ceramic/liquid electrolyte interfaces. In this work, two ceramic electrolytes, Li₃PS₄ (LPS) and Li_6.5La₃Zr_1.5Ta_0.5O₁₂ (LLZTO), were interfaced with the solid polymer electrolyte PEO₁₀:LiTFSI and the interfacial resistances were determined by impedance spectroscopy. The LLZTO/polymer interfacial resistance was found to be prohibitively high but, in contrast, a low resistance was observed at the LPS/polymer interface that became negligible at a moderately elevated temperature of 50 °C. Chemical characterization of the two interfaces was carried out, using depth-profiled X-ray photoelectron spectroscopy and time-of-flight secondary ion mass spectrometry, to determine whether the interfacial resistance was correlated with the formation of an interphase. Interestingly, no interphase was observed at the higher resistance LLZTO/polymer interface, whereas LPS was observed to react with the polymer electrolyte to form an interphase.

Original language	English
Article number	60
Number of pages	13
Journal	Inorganics
Volume	10
Issue number	5
DOIs	https://doi.org/10.3390/inorganics10050060
Publication status	Published - 26 Apr 2022

Bibliographical note

Funding:
P.G.B. is indebted to the Faraday Institution All-Solid-State Batteries with Li and Na Anodes (FIRG007, FIRG008), the Engineering and Physical Sciences Research Council (EP/M009521/1) and The Henry Royce Institute for Advanced Materials for financial support (EP/R00661X/1, EP/S019367/1, EP/R010145/1). R.H.B. wishes to acknowledge the EPSRC for funding from grant numbers EP/R024006/1 and EP/P003532/1. A.A. acknowledges funding from EPSRC ICSF “Genesis: garnet electrolytes for new energy storage integrated solutions” (EP/R024006/1) and Horizon 2020 FETPROACT-2018-2020 “HARVESTORE”.

Keywords

solid-state battery
hybrid battery
interfaces
polymer electrolyte
solid electrolyte
solid-polymer electrolyte interphase

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10.3390/inorganics10050060Licence: Creative Commons: Attribution (CC BY)

JollyD2022InterfacesFinal published version, 5.36 MBLicence: Creative Commons: Attribution (CC BY)

ICSF Wave 1: GENESIS: Garnet Electrolytes for New Energy Storage Integrated Solutions
Ding, Y., Slater, P. & Li, Y.
Engineering & Physical Science Research Council
1/10/17 → 28/02/21
Project: Research Councils

Cite this

Spencer jolly, D., Melvin, D. L. R., Stephens, I. D. R., Brugge, R. H., Pu, S. D., Bu, J., Ning, Z., Hartley, G. O., Adamson, P., Grant, P. S., Aguadero, A., & Bruce, P. G. (2022). Interfaces between Ceramic and Polymer Electrolytes: A Comparison of Oxide and Sulfide Solid Electrolytes for Hybrid Solid-State Batteries. Inorganics, 10(5), Article 60. https://doi.org/10.3390/inorganics10050060

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title = "Interfaces between Ceramic and Polymer Electrolytes: A Comparison of Oxide and Sulfide Solid Electrolytes for Hybrid Solid-State Batteries",

abstract = "Hybrid solid-state batteries using a bilayer of ceramic and solid polymer electrolytes may offer advantages over using a single type of solid electrolyte alone. However, the impedance to Li+ transport across interfaces between different electrolytes can be high. It is important to determine the resistance to Li+ transport across these heteroionic interfaces, as well as to understand the underlying causes of these resistances; in particular, whether chemical interphase formation contributes to giving high resistances, as in the case of ceramic/liquid electrolyte interfaces. In this work, two ceramic electrolytes, Li3PS4 (LPS) and Li6.5La3Zr1.5Ta0.5O12 (LLZTO), were interfaced with the solid polymer electrolyte PEO10:LiTFSI and the interfacial resistances were determined by impedance spectroscopy. The LLZTO/polymer interfacial resistance was found to be prohibitively high but, in contrast, a low resistance was observed at the LPS/polymer interface that became negligible at a moderately elevated temperature of 50 °C. Chemical characterization of the two interfaces was carried out, using depth-profiled X-ray photoelectron spectroscopy and time-of-flight secondary ion mass spectrometry, to determine whether the interfacial resistance was correlated with the formation of an interphase. Interestingly, no interphase was observed at the higher resistance LLZTO/polymer interface, whereas LPS was observed to react with the polymer electrolyte to form an interphase.",

keywords = "solid-state battery, hybrid battery, interfaces, polymer electrolyte, solid electrolyte, solid-polymer electrolyte interphase",

author = "{Spencer jolly}, Dominic and Melvin, {Dominic L. R.} and Stephens, {Isabella D. R.} and Brugge, {Rowena H.} and Pu, {Shengda D.} and Junfu Bu and Ziyang Ning and Hartley, {Gareth O.} and Paul Adamson and Grant, {Patrick S.} and Ainara Aguadero and Bruce, {Peter G.}",

note = "Funding: P.G.B. is indebted to the Faraday Institution All-Solid-State Batteries with Li and Na Anodes (FIRG007, FIRG008), the Engineering and Physical Sciences Research Council (EP/M009521/1) and The Henry Royce Institute for Advanced Materials for financial support (EP/R00661X/1, EP/S019367/1, EP/R010145/1). R.H.B. wishes to acknowledge the EPSRC for funding from grant numbers EP/R024006/1 and EP/P003532/1. A.A. acknowledges funding from EPSRC ICSF “Genesis: garnet electrolytes for new energy storage integrated solutions” (EP/R024006/1) and Horizon 2020 FETPROACT-2018-2020 “HARVESTORE”.",

year = "2022",

month = apr,

day = "26",

doi = "10.3390/inorganics10050060",

language = "English",

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T1 - Interfaces between Ceramic and Polymer Electrolytes

T2 - A Comparison of Oxide and Sulfide Solid Electrolytes for Hybrid Solid-State Batteries

AU - Spencer jolly, Dominic

AU - Melvin, Dominic L. R.

AU - Stephens, Isabella D. R.

AU - Brugge, Rowena H.

AU - Pu, Shengda D.

AU - Bu, Junfu

AU - Ning, Ziyang

AU - Hartley, Gareth O.

AU - Adamson, Paul

AU - Grant, Patrick S.

AU - Aguadero, Ainara

AU - Bruce, Peter G.

N1 - Funding: P.G.B. is indebted to the Faraday Institution All-Solid-State Batteries with Li and Na Anodes (FIRG007, FIRG008), the Engineering and Physical Sciences Research Council (EP/M009521/1) and The Henry Royce Institute for Advanced Materials for financial support (EP/R00661X/1, EP/S019367/1, EP/R010145/1). R.H.B. wishes to acknowledge the EPSRC for funding from grant numbers EP/R024006/1 and EP/P003532/1. A.A. acknowledges funding from EPSRC ICSF “Genesis: garnet electrolytes for new energy storage integrated solutions” (EP/R024006/1) and Horizon 2020 FETPROACT-2018-2020 “HARVESTORE”.

PY - 2022/4/26

Y1 - 2022/4/26

N2 - Hybrid solid-state batteries using a bilayer of ceramic and solid polymer electrolytes may offer advantages over using a single type of solid electrolyte alone. However, the impedance to Li+ transport across interfaces between different electrolytes can be high. It is important to determine the resistance to Li+ transport across these heteroionic interfaces, as well as to understand the underlying causes of these resistances; in particular, whether chemical interphase formation contributes to giving high resistances, as in the case of ceramic/liquid electrolyte interfaces. In this work, two ceramic electrolytes, Li3PS4 (LPS) and Li6.5La3Zr1.5Ta0.5O12 (LLZTO), were interfaced with the solid polymer electrolyte PEO10:LiTFSI and the interfacial resistances were determined by impedance spectroscopy. The LLZTO/polymer interfacial resistance was found to be prohibitively high but, in contrast, a low resistance was observed at the LPS/polymer interface that became negligible at a moderately elevated temperature of 50 °C. Chemical characterization of the two interfaces was carried out, using depth-profiled X-ray photoelectron spectroscopy and time-of-flight secondary ion mass spectrometry, to determine whether the interfacial resistance was correlated with the formation of an interphase. Interestingly, no interphase was observed at the higher resistance LLZTO/polymer interface, whereas LPS was observed to react with the polymer electrolyte to form an interphase.

AB - Hybrid solid-state batteries using a bilayer of ceramic and solid polymer electrolytes may offer advantages over using a single type of solid electrolyte alone. However, the impedance to Li+ transport across interfaces between different electrolytes can be high. It is important to determine the resistance to Li+ transport across these heteroionic interfaces, as well as to understand the underlying causes of these resistances; in particular, whether chemical interphase formation contributes to giving high resistances, as in the case of ceramic/liquid electrolyte interfaces. In this work, two ceramic electrolytes, Li3PS4 (LPS) and Li6.5La3Zr1.5Ta0.5O12 (LLZTO), were interfaced with the solid polymer electrolyte PEO10:LiTFSI and the interfacial resistances were determined by impedance spectroscopy. The LLZTO/polymer interfacial resistance was found to be prohibitively high but, in contrast, a low resistance was observed at the LPS/polymer interface that became negligible at a moderately elevated temperature of 50 °C. Chemical characterization of the two interfaces was carried out, using depth-profiled X-ray photoelectron spectroscopy and time-of-flight secondary ion mass spectrometry, to determine whether the interfacial resistance was correlated with the formation of an interphase. Interestingly, no interphase was observed at the higher resistance LLZTO/polymer interface, whereas LPS was observed to react with the polymer electrolyte to form an interphase.

KW - solid-state battery

KW - hybrid battery

KW - interfaces

KW - polymer electrolyte

KW - solid electrolyte

KW - solid-polymer electrolyte interphase

U2 - 10.3390/inorganics10050060

DO - 10.3390/inorganics10050060

M3 - Article

SN - 2304-6740

VL - 10

JO - Inorganics

JF - Inorganics

IS - 5

M1 - 60

ER -

Interfaces between Ceramic and Polymer Electrolytes: A Comparison of Oxide and Sulfide Solid Electrolytes for Hybrid Solid-State Batteries

Abstract

Bibliographical note

Keywords

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Projects

ICSF Wave 1: GENESIS: Garnet Electrolytes for New Energy Storage Integrated Solutions

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