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On the Capacity Losses Seen for Optimized Nano-Si Composite Electrodes in Li-Metal Half-Cells
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström.
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Inorganic Chemistry. Karlsruhe Inst Technol, Dept Appl Biol, Inst Appl Biosci, Kaiserstr 12, D-76131 Karlsruhe, Germany.ORCID iD: 0000-0003-2394-287X
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström.
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - BMC, Analytical Chemistry.ORCID iD: 0000-0003-4764-1246
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2019 (English)In: Advanced Energy Materials, ISSN 1614-6832, Vol. 9, no 33, article id 1901608Article in journal (Refereed) Published
Abstract [en]

While the use of silicon‐based electrodes can increase the capacity of Li‐ion batteries considerably, their application is associated with significant capacity losses. In this work, the influences of solid electrolyte interphase (SEI) formation, volume expansion, and lithium trapping are evaluated for two different electrochemical cycling schemes using lithium‐metal half‐cells containing silicon nanoparticle–based composite electrodes. Lithium trapping, caused by incomplete delithiation, is demonstrated to be the main reason for the capacity loss while SEI formation and dissolution affect the accumulated capacity loss due to a decreased coulombic efficiency. The capacity losses can be explained by the increasing lithium concentration in the electrode causing a decreasing lithiation potential and the lithiation cut‐off limit being reached faster. A lithium‐to‐silicon atomic ratio of 3.28 is found for a silicon electrode after 650 cycles using 1200 mAhg−1 capacity limited cycling. The results further show that the lithiation step is the capacity‐limiting step and that the capacity losses can be minimized by increasing the efficiency of the delithiation step via the inclusion of constant voltage delithiation steps. Lithium trapping due to incomplete delithiation consequently constitutes a very important capacity loss phenomenon for silicon composite electrodes.

Place, publisher, year, edition, pages
2019. Vol. 9, no 33, article id 1901608
Keywords [en]
asymmetric cycling, hard X-ray photoelectron spectroscopy, lithium trapping, silicon, solid electrolyte interphase layer
National Category
Materials Chemistry
Identifiers
URN: urn:nbn:se:uu:diva-398839DOI: 10.1002/aenm.201901608ISI: 000477265600001OAI: oai:DiVA.org:uu-398839DiVA, id: diva2:1377232
Funder
Swedish Research Council, VR-2015-04421Swedish Research Council, VR-2017-06320StandUp
Note

De 2 första författarna delar förstaförfattarskapet.

Available from: 2019-12-11 Created: 2019-12-11 Last updated: 2019-12-11Bibliographically approved

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Lindgren, FredrikRehnlund, DavidPan, RuijunPettersson, JeanYounesi, RezaXu, ChaoGustafsson, TorbjörnEdström, KristinaNyholm, Leif

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