Toward zero-excess lithium sulfur batteries: a systematic cell parameter study

Zero-excess lithium (ZEL) or ‘anode-free’ batteries aim to minimize negative electrode material and address the challenges associated with handling thin lithium metal foils during fabrication. To date, most studies in the field of ZEL cells have primarily focused on lithium-ion chemistry, with consi...

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Main Authors: Joshua H Cruddos, James B Robinson, Paul R Shearing, Alexander J E Rettie
Format: Article
Language:English
Published: IOP Publishing 2025-01-01
Series:JPhys Energy
Subjects:
Online Access:https://doi.org/10.1088/2515-7655/ada700
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author Joshua H Cruddos
James B Robinson
Paul R Shearing
Alexander J E Rettie
author_facet Joshua H Cruddos
James B Robinson
Paul R Shearing
Alexander J E Rettie
author_sort Joshua H Cruddos
collection DOAJ
description Zero-excess lithium (ZEL) or ‘anode-free’ batteries aim to minimize negative electrode material and address the challenges associated with handling thin lithium metal foils during fabrication. To date, most studies in the field of ZEL cells have primarily focused on lithium-ion chemistry, with considerably fewer systematic investigations into ZEL-sulfur (ZELiS) cell fabrication and optimization. Here we develop a ZELiS battery, comprising a Li _2 S-based composite positive electrode on carbon paper paired with a Ni foil current collector (CC) and evaluate the effects of various CC materials, electrolyte volume to Li _2 S mass ratio and C-rate. The developed cells reproducibly achieve an average Coulombic efficiency of 99% from cycles 2 to 200, and a final capacity of 272 mAh g ^−1 _Li2S at a C/10 rate. Furthermore, we employ x-ray computed tomography to elucidate the morphological changes and degradation processes occurring within the positive electrode composite, revealing the irreversible loss of Li _2 S/S _8 during cycling, which is exacerbated at high rates. These results should be useful in the development of commercially viable ZEL energy storage devices.
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spelling doaj-art-ac9c6f66907942ab8a266891cacd697d2025-01-22T10:22:21ZengIOP PublishingJPhys Energy2515-76552025-01-017202500610.1088/2515-7655/ada700Toward zero-excess lithium sulfur batteries: a systematic cell parameter studyJoshua H Cruddos0https://orcid.org/0000-0002-0757-8337James B Robinson1https://orcid.org/0000-0002-6509-7769Paul R Shearing2https://orcid.org/0000-0002-1387-9531Alexander J E Rettie3https://orcid.org/0000-0002-2482-9732Electrochemical Innovation Lab, Department of Chemical Engineering, University College London , London WC1E 6DH, United Kingdom; Advanced Propulsion Lab, Marshgate, University College London , London E20 2AE, United Kingdom; The Faraday Institution Quad One, Harwell Science and Innovation Campus , Didcot OX11 0RA, United KingdomElectrochemical Innovation Lab, Department of Chemical Engineering, University College London , London WC1E 6DH, United Kingdom; Advanced Propulsion Lab, Marshgate, University College London , London E20 2AE, United Kingdom; The Faraday Institution Quad One, Harwell Science and Innovation Campus , Didcot OX11 0RA, United KingdomThe ZERO Institute, University of Oxford , Holywell House, Osney Mead, Oxford OX2 0ES, United Kingdom; The Faraday Institution Quad One, Harwell Science and Innovation Campus , Didcot OX11 0RA, United KingdomElectrochemical Innovation Lab, Department of Chemical Engineering, University College London , London WC1E 6DH, United Kingdom; Advanced Propulsion Lab, Marshgate, University College London , London E20 2AE, United Kingdom; The Faraday Institution Quad One, Harwell Science and Innovation Campus , Didcot OX11 0RA, United KingdomZero-excess lithium (ZEL) or ‘anode-free’ batteries aim to minimize negative electrode material and address the challenges associated with handling thin lithium metal foils during fabrication. To date, most studies in the field of ZEL cells have primarily focused on lithium-ion chemistry, with considerably fewer systematic investigations into ZEL-sulfur (ZELiS) cell fabrication and optimization. Here we develop a ZELiS battery, comprising a Li _2 S-based composite positive electrode on carbon paper paired with a Ni foil current collector (CC) and evaluate the effects of various CC materials, electrolyte volume to Li _2 S mass ratio and C-rate. The developed cells reproducibly achieve an average Coulombic efficiency of 99% from cycles 2 to 200, and a final capacity of 272 mAh g ^−1 _Li2S at a C/10 rate. Furthermore, we employ x-ray computed tomography to elucidate the morphological changes and degradation processes occurring within the positive electrode composite, revealing the irreversible loss of Li _2 S/S _8 during cycling, which is exacerbated at high rates. These results should be useful in the development of commercially viable ZEL energy storage devices.https://doi.org/10.1088/2515-7655/ada700zero excess Lianode freeLi sulfurLi sulfide
spellingShingle Joshua H Cruddos
James B Robinson
Paul R Shearing
Alexander J E Rettie
Toward zero-excess lithium sulfur batteries: a systematic cell parameter study
JPhys Energy
zero excess Li
anode free
Li sulfur
Li sulfide
title Toward zero-excess lithium sulfur batteries: a systematic cell parameter study
title_full Toward zero-excess lithium sulfur batteries: a systematic cell parameter study
title_fullStr Toward zero-excess lithium sulfur batteries: a systematic cell parameter study
title_full_unstemmed Toward zero-excess lithium sulfur batteries: a systematic cell parameter study
title_short Toward zero-excess lithium sulfur batteries: a systematic cell parameter study
title_sort toward zero excess lithium sulfur batteries a systematic cell parameter study
topic zero excess Li
anode free
Li sulfur
Li sulfide
url https://doi.org/10.1088/2515-7655/ada700
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AT alexanderjerettie towardzeroexcesslithiumsulfurbatteriesasystematiccellparameterstudy