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Overlapping and rate controlling electrochemical reactions for tin(IV) oxide electrodes in lithiu-ion batteries
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: 0000-0003-4440-2952
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Inorganic Chemistry.ORCID iD: 0000-0001-9292-016X
2017 (English)In: Journal of Electroanalytical Chemistry, ISSN 0022-0728, E-ISSN 1873-2569, Vol. 797, p. 47-60Article in journal (Refereed) Published
Abstract [en]

The results of this extensive electrochemical study of the electrochemical reactions of SnO2 electrodes in lithium-ion batteries demonstrate that the different reduction and oxidation reactions overlap significantly during the cycling and that the rates of the redox reactions are limited by the mass transport through the layers of oxidation or reduction products formed on the electrodes. The experiments, which were carried out in the absence and presence of the lithium alloy reactions, show that the capacity losses seen on the first cycles mainly can be explained by an incomplete oxidation of the lithium tin alloy and an incomplete reformation of SnO2. The latter can be explained by the formation of thin tin oxide layers (i.e., SnO and SnO2), protecting the remaining tin, as the oxidation current then becomes limited by the Li+ diffusion rate though these layers. The results, also show that the first cycle SnO2 reduction was incomplete for the about 20 μm thick electrodes containing 1 to 6 μm large SnO2 particles. This can be ascribed to the formation of a layer of tin and Li2O (protecting the remaining SnO2) during the reduction process. Although the regeneration of the SnO2 always was slower than the reduction of the SnO2, the results clearly show that the SnO2 conversion reaction is far from irreversible, particularly at low scan rates and increased temperatures. Electrochemical cycling at 60 °C hence gave rise to increased capacities, but also a faster capacity loss, compared to at room temperature. These new findings indicate that a full utilization of SnO2 based electrodes at a given cycling rate only can be reached with sufficiently small particles since the allowed particle size is given by the time available for the mass transport through the formed surface layers. The present results consequently provide important insights into the phenomena limiting the use of SnO2 electrodes in lithium-ion batteries.

Place, publisher, year, edition, pages
2017. Vol. 797, p. 47-60
Keyword [en]
Li-ion batteries, SnO2, electrodes, overlapping reactions
National Category
Inorganic Chemistry
Research subject
Chemistry with specialization in Inorganic Chemistry
Identifiers
URN: urn:nbn:se:uu:diva-336947ISI: 000404696900008OAI: oai:DiVA.org:uu-336947DiVA, id: diva2:1167704
Funder
Swedish Foundation for Strategic Research , EM11-0028StandUp
Available from: 2017-12-19 Created: 2017-12-19 Last updated: 2018-02-22Bibliographically approved

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Böhme, SolveigEdström, KristinaNyholm, Leif

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