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Limitations of polyacrylic acid binders when employed in thick LNMO Li-ion battery electrodes
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.ORCID iD: 0000-0002-0512-6820
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.ORCID iD: 0000-0003-0763-5239
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
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2024 (English)In: Journal of the Electrochemical Society, ISSN 0013-4651, E-ISSN 1945-7111, Vol. 171, no 2, article id 020531Article in journal (Refereed) Published
Abstract [en]

Polyacrylic acid (PAA) is here studied as a binder material for LiNi0.5Mn1.5O4 (LNMO) cathodes for lithium-ion batteries. When the LNMO electrodes are fabricated with an active mass loading of similar to 10 mg cm-2 (similar to 1.5 mA h cm-2), poor discharge capacity and short cycle life is obtained in full-cells with graphite electrodes. The electrochemical results with PAA are compared with a commonly used water-based binder, sodium carboxymethyl cellulose (CMC), which shows better electrochemical performance. The main cause for these problems in PAA based cells is identified to be the high internal resistance in the initial cycles, caused by factors such as contact resistance, inhomogeneous binder distribution and poor electrolyte wetting of the active material.

Place, publisher, year, edition, pages
Institute of Physics Publishing (IOPP), 2024. Vol. 171, no 2, article id 020531
National Category
Materials Chemistry
Identifiers
URN: urn:nbn:se:uu:diva-498898DOI: 10.1149/1945-7111/ad242bISI: 001163284700001OAI: oai:DiVA.org:uu-498898DiVA, id: diva2:1744803
Funder
VinnovaEU, Horizon 2020, 875126Swedish Research CouncilAvailable from: 2023-03-20 Created: 2023-03-20 Last updated: 2024-03-05Bibliographically approved
In thesis
1. LiNi0.5Mn1.5O4 cathodes for lithium-ion batteries: Exploring strategies for a stable electrode-electrolyte interphase
Open this publication in new window or tab >>LiNi0.5Mn1.5O4 cathodes for lithium-ion batteries: Exploring strategies for a stable electrode-electrolyte interphase
2023 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Climate change, a pressing global issue, can be partially addressed by using electric vehicles to reduce CO2 emissions. In this context, high-energy and high-power density batteries are vital. The LiNi0.5Mn1.5O4 (LNMO)-based cell is in this regard appealing as it fulfils several requirements, but is unfortunately constrained by capacity fading, especially at elevated temperatures. LNMO operates at ~ 4.7 V (vs. Li+/Li) at which conventional Li-ion battery (LIB) electrolytes are not thermodynamically stable.

This thesis investigates the degradation mechanisms in LNMO cells and various practical strategies to tackle these problems. In the first part, a technique named synthetic charge-discharge profile voltammetry (SCPV) is developed to better understand the oxidative stability of some of the common electrolytes. The second part focuses on the use of binders that could potentially enable the formation of an artificial cathode-electrolyte interphase in LNMO cells. Polyacrylonitrile (PAN), which is often considered to be oxidatively stable, is however shown to degrade under the operating voltages of LNMO. A second polymer, polyacrylic acid (PAA), was studied for higher electrode mass loadings, but a high internal resistance resulted in poor initial discharge capacity as compared to the carboxymethyl cellulose (CMC) benchmark.

In order to effectively mitigate capacity fading, three different electrolytes were explored in LNMO cells in the third section. First, an ionic liquid-based electrolyte, 1.2 M lithium bis(fluorosulfonyl)imide (LiFSI) in N-Propyl-N-methylpyrrolidinium bis(fluorosulfonyl)imide (PYR13FSI), was used. X-ray photoelectron spectroscopy (XPS) analysis revealed that this electrolyte stabilized the electrode by forming robust and predominantly inorganic surface layers which stabilized the electrode. Second, the study of an electrolyte containing sulfolane showed that, despite initial cycles displaying a higher degradation, the passivation layers created on the electrodes enable stable cycling. In a third study, tris(trimethylsilyl)phosphite (TMSPi) and lithium difluoro(oxalato)borate (LiDFOB) were investigated as electrolyte additives in a conventional electrolyte, and 1 wt.% and 2 wt.% of the additives, respectively, showed improved electrochemical performance in LNMO-graphite full cells, highlighting the role of these additives in enabling interphase layers at both the positive and negative electrodes. Collectively, these studies offer insights on how crucial the interfacial chemistry is for stable operation of LNMO cells, and pinpoint strategies to tailor this further.

Place, publisher, year, edition, pages
Uppsala: Acta Universitatis Upsaliensis, 2023. p. 68
Series
Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology, ISSN 1651-6214 ; 2252
National Category
Materials Chemistry
Identifiers
urn:nbn:se:uu:diva-498904 (URN)978-91-513-1757-1 (ISBN)
Public defence
2023-05-11, Polhemsalen, Ångströmlaboratoriet, Lägerhyddsvägen 1, Uppsala, 09:15 (English)
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Supervisors
Available from: 2023-04-18 Created: 2023-03-20 Last updated: 2023-04-18

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Mathew, Almavan Ekeren, WesselAndersson, RassmusYounesi, RezaBrandell, Daniel

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