Structural changes in the silver-carbon composite anode interlayer of solid-state batteries

Dominic Spencer-Jolly; Varnika Agarwal; Christopher Doerrer; Bingkun Hu; Shengming Zhang; Dominic L.R. Melvin; Hui Gao; Xiangwen Gao; Paul Adamson; Oxana V. Magdysyuk; Patrick S. Grant; Robert A. House; Peter G. Bruce

doi:10.1016/j.joule.2023.02.001

Structural changes in the silver-carbon composite anode interlayer of solid-state batteries

Dominic Spencer-Jolly, Varnika Agarwal, Christopher Doerrer, Bingkun Hu, Shengming Zhang, Dominic L.R. Melvin, Hui Gao, Xiangwen Gao, Paul Adamson, Oxana V. Magdysyuk, Patrick S. Grant, Robert A. House, Peter G. Bruce^*

^*Corresponding author for this work

Metallurgy and Materials

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Abstract

Ag-carbon composite interlayers have been reported to enable Li-free (anodeless) cycling of solid-state batteries. Here, we report structural changes in the Ag-graphite interlayer, showing that on charge, Li intercalates electrochemically into graphite, subsequently reacting chemically with Ag to form Li-Ag alloys. Discharge is not the reverse of charge but rather passes through Li-deficient Li-Ag phases. At higher charging rates, Li intercalation into graphite outpaces the chemical reactions with Ag, delaying the formation of the Li-Ag phases and resulting in more Li metal deposition at the current collector. At and above 2.5 mA·cm⁻², Li dendrites are not suppressed. Ag nanoparticles do not suppress dendrites more effectively than does an interlayer of graphite alone. Instead, Ag in the carbon interlayer results in more homogeneous Li and Li-Ag formation on the current collector during charge.

Original language	English
Pages (from-to)	503-514
Number of pages	12
Journal	Joule
Volume	7
Issue number	3
Early online date	24 Feb 2023
DOIs	https://doi.org/10.1016/j.joule.2023.02.001
Publication status	Published - 15 Mar 2023

Bibliographical note

Funding Information:
P.G.B. is indebted to the Faraday Institution (FIRG02), 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, and EP/R010145/1). We thank Diamond Light Source, Didcot, United Kingdom for use of synchrotron radiation facilities and experimental support (experiment no. mg26082).

Publisher Copyright:
© 2023 The Author(s)

Keywords

anodeless
dendrites
interfaces
interlayers
operando PXRD
solid-state batteries

ASJC Scopus subject areas

General Energy

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SpencerJolly2023StructuralFinal published version, 2.66 MBLicence: Creative Commons: Attribution (CC BY)

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title = "Structural changes in the silver-carbon composite anode interlayer of solid-state batteries",

abstract = "Ag-carbon composite interlayers have been reported to enable Li-free (anodeless) cycling of solid-state batteries. Here, we report structural changes in the Ag-graphite interlayer, showing that on charge, Li intercalates electrochemically into graphite, subsequently reacting chemically with Ag to form Li-Ag alloys. Discharge is not the reverse of charge but rather passes through Li-deficient Li-Ag phases. At higher charging rates, Li intercalation into graphite outpaces the chemical reactions with Ag, delaying the formation of the Li-Ag phases and resulting in more Li metal deposition at the current collector. At and above 2.5 mA·cm−2, Li dendrites are not suppressed. Ag nanoparticles do not suppress dendrites more effectively than does an interlayer of graphite alone. Instead, Ag in the carbon interlayer results in more homogeneous Li and Li-Ag formation on the current collector during charge.",

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author = "Dominic Spencer-Jolly and Varnika Agarwal and Christopher Doerrer and Bingkun Hu and Shengming Zhang and Melvin, {Dominic L.R.} and Hui Gao and Xiangwen Gao and Paul Adamson and Magdysyuk, {Oxana V.} and Grant, {Patrick S.} and House, {Robert A.} and Bruce, {Peter G.}",

note = "Funding Information: P.G.B. is indebted to the Faraday Institution (FIRG02), 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, and EP/R010145/1). We thank Diamond Light Source, Didcot, United Kingdom for use of synchrotron radiation facilities and experimental support (experiment no. mg26082). Publisher Copyright: {\textcopyright} 2023 The Author(s)",

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AU - Spencer-Jolly, Dominic

AU - Agarwal, Varnika

AU - Doerrer, Christopher

AU - Hu, Bingkun

AU - Zhang, Shengming

AU - Melvin, Dominic L.R.

AU - Gao, Hui

AU - Gao, Xiangwen

AU - Adamson, Paul

AU - Magdysyuk, Oxana V.

AU - Grant, Patrick S.

AU - House, Robert A.

AU - Bruce, Peter G.

N1 - Funding Information: P.G.B. is indebted to the Faraday Institution (FIRG02), 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, and EP/R010145/1). We thank Diamond Light Source, Didcot, United Kingdom for use of synchrotron radiation facilities and experimental support (experiment no. mg26082). Publisher Copyright: © 2023 The Author(s)

PY - 2023/3/15

Y1 - 2023/3/15

N2 - Ag-carbon composite interlayers have been reported to enable Li-free (anodeless) cycling of solid-state batteries. Here, we report structural changes in the Ag-graphite interlayer, showing that on charge, Li intercalates electrochemically into graphite, subsequently reacting chemically with Ag to form Li-Ag alloys. Discharge is not the reverse of charge but rather passes through Li-deficient Li-Ag phases. At higher charging rates, Li intercalation into graphite outpaces the chemical reactions with Ag, delaying the formation of the Li-Ag phases and resulting in more Li metal deposition at the current collector. At and above 2.5 mA·cm−2, Li dendrites are not suppressed. Ag nanoparticles do not suppress dendrites more effectively than does an interlayer of graphite alone. Instead, Ag in the carbon interlayer results in more homogeneous Li and Li-Ag formation on the current collector during charge.

AB - Ag-carbon composite interlayers have been reported to enable Li-free (anodeless) cycling of solid-state batteries. Here, we report structural changes in the Ag-graphite interlayer, showing that on charge, Li intercalates electrochemically into graphite, subsequently reacting chemically with Ag to form Li-Ag alloys. Discharge is not the reverse of charge but rather passes through Li-deficient Li-Ag phases. At higher charging rates, Li intercalation into graphite outpaces the chemical reactions with Ag, delaying the formation of the Li-Ag phases and resulting in more Li metal deposition at the current collector. At and above 2.5 mA·cm−2, Li dendrites are not suppressed. Ag nanoparticles do not suppress dendrites more effectively than does an interlayer of graphite alone. Instead, Ag in the carbon interlayer results in more homogeneous Li and Li-Ag formation on the current collector during charge.

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Structural changes in the silver-carbon composite anode interlayer of solid-state batteries

Abstract

Bibliographical note

Keywords

ASJC Scopus subject areas

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