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Influence of state-of-charge in commercial LiNi0.33Mn0.33Co0.33O2/LiMn2O4-graphite cells analyzed by synchrotron-based photoelectron spectroscopy
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
Chalmers University of Technology, Gothenburg, Sweden.
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.ORCID iD: 0000-0003-2538-8104
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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2018 (English)In: Journal of Energy Storage, ISSN 2352-152X, Vol. 15, p. 172-180Article in journal (Refereed) Published
Abstract [en]

Degradation mechanisms in 26 Ah commercial Li-ion battery cells comprising graphite as the negative electrode and mixed metal oxide of LiMn2O4 (LMO) and LiNi1/3Mn1/3Co1/3O2 (NMC) as the positive electrode are here investigated utilising extensive cycling at two different state-of-charge (SOC) ranges, 10–20% and 60–70%, as well as post-mortem analysis. To better analyze these mechanisms electrochemically, the cells were after long-term cycling reassembled into laboratory scale “half-cells” using lithium metal as the negative electrode, and thereafter cycled at different rates corresponding to 0.025 mA/cm2 and 0.754 mA/cm2. The electrodes were also analyzed by synchrotron-based hard x-ray photoelectron spectroscopy (HAXPES) using two different excitation energies to determine the chemical composition of the interfacial layers formed at different depth on the respective electrodes. It was found from the extensive cycling that the cycle life was shorter for the cell cycled in the higher SOC range, 60–70%, which is correlated to findings of an increased cell resistance and thickness of the SEI layer in the graphite electrode as well as manganese dissolution from the positive electrode.

Place, publisher, year, edition, pages
2018. Vol. 15, p. 172-180
Keywords [en]
Li-ion battery, Commercial cells, Battery ageing, Photoelectron spectroscopy
National Category
Chemical Sciences
Identifiers
URN: urn:nbn:se:uu:diva-338184DOI: 10.1016/j.est.2017.11.010ISI: 000426619500015OAI: oai:DiVA.org:uu-338184DiVA, id: diva2:1171587
Available from: 2018-01-08 Created: 2018-01-08 Last updated: 2019-04-11Bibliographically approved
In thesis
1. Avoiding ageing: Surface degradation of commercial electrode materials in lithium-ion batteries
Open this publication in new window or tab >>Avoiding ageing: Surface degradation of commercial electrode materials in lithium-ion batteries
2019 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

The battery market today expands rapidly, not least for electric vehicles. But to compete against the combustion engine, the cost of batteries must be reduced. After years of usage, the batteries degrade and need to be exchanged, increasing the cost over the vehicle lifecycle. This can be mitigated by tailoring the usage conditions and the battery materials. Understanding and avoiding ageing can be key to a more sustainable transport system. This thesis contains studies on degradation processes in Li-ion batteries utilizing the LiNixMnyCozO2 (NMC) cathode material, and suggests strategies for the improvement of battery life time.

When cycling different negative electrodes – including graphite, lithium foil and lithium titanium oxide (LTO) – against NMC electrodes, only minor capacity fading was observed in the NMC-LTO and NMC-graphite cells, in contrast to the NMC-Li-metal cells. The capacity fading for Li-metal cells was determined to be caused by degradation products formed at the lithium foil which thereafter diffused to the NMC electrode, leading to a higher resistance. Commercial NMC/LiMn2O4-graphite cells were also investigated after cycling in limited state of charge (SOC)-intervals. The cycle life was far longer in the low-SOC cell than in the high-SOC cell. Photoelectron spectroscopy revealed increased manganese dissolution in the high-SOC cell, likely causing a less stable solid electrolyte interphase layer on the negative electrode. This, in turn, limits the capacity. How temperature influence ageing in NMC-LTO was analysed in cells cycled at -10 °C, 30 °C and 55 °C. It was found that the initial side reactions at the LTO electrode limited the cell capacity, but that these also stabilized the NMC electrode. At 55 °C, excessive side reactions at LTO caused capacity fading due to loss of active lithium. At -10 °C, high cell resistance limited the capacity. Switching to a PC based electrolyte allowed stable low temperature cycling, although it was found that PC degraded and formed thick electrode surface layers. Also sulfolane-based electrolytes were investigated, showing thinner surface layers than the EC containing reference electrolyte at high potentials, thus indicating a more stable electrolyte system.

Place, publisher, year, edition, pages
Uppsala: Acta Universitatis Upsaliensis, 2019. p. 72
Series
Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology, ISSN 1651-6214 ; 1802
Keywords
Li-ion battery, Ageing, Photoelectron spectroscopy, Nickel Manganese Cobalt Oxide
National Category
Chemical Sciences
Identifiers
urn:nbn:se:uu:diva-381548 (URN)978-91-513-0639-1 (ISBN)
Public defence
2019-06-05, Room 4001, Ångströmlaboratoriet, Lägerhyddsvägen 1, Uppsala, 09:15 (English)
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Available from: 2019-05-09 Created: 2019-04-11 Last updated: 2019-06-17

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Björklund, ErikYounesi, RezaBrandell, DanielEdström, Kristina

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