Adverse Effects of Trace Non-polar Binder on Ion Transport in Free-standing Sulfide Solid Electrolyte Separators

Anna Mills; Guang Yang; Wan Yu Tsai; X. Chelsea Chen; Robert L. Sacci; Beth L. Armstrong; Daniel T. Hallinan; Jagjit Nanda

doi:10.1149/1945-7111/aced24

Adverse Effects of Trace Non-polar Binder on Ion Transport in Free-standing Sulfide Solid Electrolyte Separators

Anna Mills, Guang Yang, Wan Yu Tsai, X. Chelsea Chen, Robert L. Sacci, Beth L. Armstrong, Daniel T. Hallinan, Jagjit Nanda

Research output: Contribution to journal › Article › peer-review

5 Scopus citations

Abstract

Sulfide solid-state electrolyte (SE) possesses high room-temperature ionic conductivity. However, fabrication of the free-standing, sheet-type thin sulfide SE film electrolyte to enable all-solid-state batteries to deliver high energy and power density remains challenging. Herein we show that argyrodite sulfide (Li₆PS₅Cl) SE can be slurry cast to form free-standing films with low (≤5 wt%) loadings of poly(isobutylene) (PIB) binder. Two factors contribute to a lower areal specific resistance (ASR) of the thin film SEs benchmarked to the pristine powder pellet SSE counterparts: i) 1-2 orders reduced thickness and ii) reasonably comparable ionic conductivity at room temperature after the isostatic pressing process. Nevertheless, an increasing polymer binder loading inevitably introduced voids in the thin film SEs, compromising anode/electrolyte interfacial ion transport. Our findings highlight that electrolyte/electrode interfacial stability, as well as the selection of slurry components, including sulfide SE, binder, and solvent, play essential roles in thin film sulfide electrolyte development.

Original language	English
Article number	080513
Journal	Journal of the Electrochemical Society
Volume	170
Issue number	8
DOIs	https://doi.org/10.1149/1945-7111/aced24
State	Published - Aug 1 2023

Funding

This research was conducted at Oak Ridge National Laboratory, managed by UT Battelle, LLC, for the U.S. Department of Energy (DOE) and is sponsored by the Office of Energy Efficiency and Renewable Energy (EERE) in the Vehicle Technologies Office (VTO) through the Advanced Battery Materials Research (BMR) Program. This manuscript has been authored by UT-Battelle, LLC under Contract No. DE-AC05–00OR22725 with the U.S. Department of Energy. SEM measurement was conducted as part of a user project at the Center for Nanophase Materials Sciences (CNMS), which is a US Department of Energy, Office of Science User Facility at Oak Ridge National Laboratory. We would like to thank Ethan Self, Teerth Brahmbhatt, Frank Delnick, and Andrew Westover for their fruitful discussions. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a non-exclusive, paid-up, irrevocable, world-wide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan. ( http://energy.gov/downloads/doe-public-access-plan ). This research was conducted at Oak Ridge National Laboratory, managed by UT Battelle, LLC, for the U.S. Department of Energy (DOE) and is sponsored by the Office of Energy Efficiency and Renewable Energy (EERE) in the Vehicle Technologies Office (VTO) through the Advanced Battery Materials Research (BMR) Program. This manuscript has been authored by UT-Battelle, LLC under Contract No. DE-AC05-00OR22725 with the U.S. Department of Energy. SEM measurement was conducted as part of a user project at the Center for Nanophase Materials Sciences (CNMS), which is a US Department of Energy, Office of Science User Facility at Oak Ridge National Laboratory. We would like to thank Ethan Self, Teerth Brahmbhatt, Frank Delnick, and Andrew Westover for their fruitful discussions. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a non-exclusive, paid-up, irrevocable, world-wide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan. (http://energy.gov/downloads/doe-public-access-plan).

Funders	Funder number
United States Government
U.S. Department of Energy
Office of Science
Office of Energy Efficiency and Renewable Energy	DE-AC05–00OR22725
Oak Ridge National Laboratory
UT-Battelle

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10.1149/1945-7111/aced24

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title = "Adverse Effects of Trace Non-polar Binder on Ion Transport in Free-standing Sulfide Solid Electrolyte Separators",

abstract = "Sulfide solid-state electrolyte (SE) possesses high room-temperature ionic conductivity. However, fabrication of the free-standing, sheet-type thin sulfide SE film electrolyte to enable all-solid-state batteries to deliver high energy and power density remains challenging. Herein we show that argyrodite sulfide (Li6PS5Cl) SE can be slurry cast to form free-standing films with low (≤5 wt%) loadings of poly(isobutylene) (PIB) binder. Two factors contribute to a lower areal specific resistance (ASR) of the thin film SEs benchmarked to the pristine powder pellet SSE counterparts: i) 1-2 orders reduced thickness and ii) reasonably comparable ionic conductivity at room temperature after the isostatic pressing process. Nevertheless, an increasing polymer binder loading inevitably introduced voids in the thin film SEs, compromising anode/electrolyte interfacial ion transport. Our findings highlight that electrolyte/electrode interfacial stability, as well as the selection of slurry components, including sulfide SE, binder, and solvent, play essential roles in thin film sulfide electrolyte development.",

author = "Anna Mills and Guang Yang and Tsai, {Wan Yu} and Chen, {X. Chelsea} and Sacci, {Robert L.} and Armstrong, {Beth L.} and Hallinan, {Daniel T.} and Jagjit Nanda",

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AU - Mills, Anna

AU - Yang, Guang

AU - Tsai, Wan Yu

AU - Chen, X. Chelsea

AU - Sacci, Robert L.

AU - Armstrong, Beth L.

AU - Hallinan, Daniel T.

AU - Nanda, Jagjit

PY - 2023/8/1

Y1 - 2023/8/1

N2 - Sulfide solid-state electrolyte (SE) possesses high room-temperature ionic conductivity. However, fabrication of the free-standing, sheet-type thin sulfide SE film electrolyte to enable all-solid-state batteries to deliver high energy and power density remains challenging. Herein we show that argyrodite sulfide (Li6PS5Cl) SE can be slurry cast to form free-standing films with low (≤5 wt%) loadings of poly(isobutylene) (PIB) binder. Two factors contribute to a lower areal specific resistance (ASR) of the thin film SEs benchmarked to the pristine powder pellet SSE counterparts: i) 1-2 orders reduced thickness and ii) reasonably comparable ionic conductivity at room temperature after the isostatic pressing process. Nevertheless, an increasing polymer binder loading inevitably introduced voids in the thin film SEs, compromising anode/electrolyte interfacial ion transport. Our findings highlight that electrolyte/electrode interfacial stability, as well as the selection of slurry components, including sulfide SE, binder, and solvent, play essential roles in thin film sulfide electrolyte development.

AB - Sulfide solid-state electrolyte (SE) possesses high room-temperature ionic conductivity. However, fabrication of the free-standing, sheet-type thin sulfide SE film electrolyte to enable all-solid-state batteries to deliver high energy and power density remains challenging. Herein we show that argyrodite sulfide (Li6PS5Cl) SE can be slurry cast to form free-standing films with low (≤5 wt%) loadings of poly(isobutylene) (PIB) binder. Two factors contribute to a lower areal specific resistance (ASR) of the thin film SEs benchmarked to the pristine powder pellet SSE counterparts: i) 1-2 orders reduced thickness and ii) reasonably comparable ionic conductivity at room temperature after the isostatic pressing process. Nevertheless, an increasing polymer binder loading inevitably introduced voids in the thin film SEs, compromising anode/electrolyte interfacial ion transport. Our findings highlight that electrolyte/electrode interfacial stability, as well as the selection of slurry components, including sulfide SE, binder, and solvent, play essential roles in thin film sulfide electrolyte development.

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Adverse Effects of Trace Non-polar Binder on Ion Transport in Free-standing Sulfide Solid Electrolyte Separators

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