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Simultaneous Monitoring of Crystalline Active Materials and Resistance Evolution in Lithium-Sulfur Batteries
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.ORCID iD: 0000-0003-4767-9471
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.ORCID iD: 0000-0002-8658-8938
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.ORCID iD: 0000-0002-8019-2801
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2020 (English)In: Journal of the American Chemical Society, ISSN 0002-7863, E-ISSN 1520-5126, Vol. 142, no 3, p. 1449-1456Article in journal (Refereed) Published
Abstract [en]

Operando X-ray diffraction (XRD) is a valuable tool for studying secondary battery materials as it allows for the direct correlation of electrochemical behavior with structural changes of crystalline active materials. This is especially true for the lithium-sulfur chemistry, in which energy storage capability depends on the complex growth and dissolution kinetics of lithium sulfide (Li2S) and sulfur (S-8) during discharge and charge, respectively. In this work, we present a novel development of this method through combining operando XRD with simultaneous and continuous resistance measurement using an intermittent current interruption (ICI) method. We show that a coefficient of diffusion resistance, which reflects the transport properties in the sulfur/carbon composite electrode, can be determined from analysis of each current interruption. Its relationship to the established Warburg impedance model is validated theoretically and experimentally. We also demonstrate for an optimized electrode formulation and cell construction that the diffusion resistance increases sharply at the discharge end point, which is consistent with the blocking of pores in the carbon host matrix. The combination of XRD with ICI allows for a direct correlation of structural changes with not only electrochemical properties but also energy loss processes at a nonequilibrium state and, therefore, is a valuable technique for the study of a wide range of energy storage chemistries.

Place, publisher, year, edition, pages
AMER CHEMICAL SOC , 2020. Vol. 142, no 3, p. 1449-1456
National Category
Condensed Matter Physics
Identifiers
URN: urn:nbn:se:uu:diva-407127DOI: 10.1021/jacs.9b11500ISI: 000509425600042PubMedID: 31889440OAI: oai:DiVA.org:uu-407127DiVA, id: diva2:1415958
Funder
Swedish Energy Agency, 42762-1Swedish Energy Agency, 42031-1Swedish Foundation for Strategic Research Available from: 2020-03-20 Created: 2020-03-20 Last updated: 2020-03-20Bibliographically approved

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Chien, Yu-ChuanMenon, Ashok S.Brant, WilliamBrandell, DanielLacey, Matthew

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