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Surface Characterization of the Carbon Cathode and the Lithium Anode of Li-O2 Batteries using LiClO4 or LiBOB salts
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.
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
2013 (English)In: ACS Applied Materials and Interfaces, ISSN 1944-8244, E-ISSN 1944-8252, Vol. 5, no 4, 1333-1341 p.Article in journal (Refereed) Published
Abstract [en]

The surface compositions of a MnO2 catalyst containing carbon cathode and a Li anode in a Li–O2 battery were investigated using synchrotron-based photoelectron spectroscopy (PES). Electrolytes comprising LiClO4 or LiBOB salts in PC or EC:DEC (1:1) solvents were used for this study. Decomposition products from LiClO4 or LiBOB were observed on the cathode surface when using PC. However, no degradation of LiClO4 was detected when using EC/DEC. We have demonstrated that both PC and EC/DEC solvents decompose during the cell cycling to form carbonate and ether containing compounds on the surface of the carbon cathode. However, EC/DEC decomposed to a lesser degree compared to PC. PES revealed that a surface layer with a thickness of at least 1–2 nm remained on the MnO2 catalyst at the end of the charged state. It was shown that the detachment of Kynar binder influences the surface composition of both the carbon cathode and the Li anode of Li–O2 cells. The PES results indicated that in the charged state the SEI on the Li anode is composed of PEO, carboxylates, carbonates, and LiClO4 salt.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2013. Vol. 5, no 4, 1333-1341 p.
Keyword [en]
Li-O2 battery, XPS, Carbon Cathode, Lithium Anode, Perchlorate, Lithium/Air, Photoelectron Spectroscopy, lithium bis(oxalato)borate
National Category
Materials Chemistry Physical Chemistry Inorganic Chemistry
Research subject
Chemistry with specialization in Inorganic Chemistry
Identifiers
URN: urn:nbn:se:uu:diva-183885DOI: 10.1021/am3026129ISI: 000315619100022OAI: oai:DiVA.org:uu-183885DiVA: diva2:564954
Funder
StandUp
Available from: 2012-11-05 Created: 2012-11-05 Last updated: 2017-12-07Bibliographically approved
In thesis
1. Characterization of Reaction Products in the Li-O2 Battery Using Photoelectron Spectroscopy
Open this publication in new window or tab >>Characterization of Reaction Products in the Li-O2 Battery Using Photoelectron Spectroscopy
2012 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

The rechargeable Li-O2 battery has attracted interest due to its high theoretical energy density (about 10 times better than today’s Li-ion batteries). In this PhD thesis the cycling instability of the Li-O2 battery has been studied. Degradation of the battery has been followed by studying the interface between the electrodes and electrolyte and determining the chemical composition and quantity of degradation products formed after varied cycling conditions. For this in-house and synchrotron based Photoelectron Spectroscopy (PES) were used as a powerful surface sensitive technique. Using these methods quantitative and qualitative information was obtained of both amorphous and crystalline compounds. To make the most realistic studies the carbon cathode pore structure was optimised by varying the binder to carbon ratio. This was shown to have an effect on improving the discharge capacity. For Li-O2 batteries electrolyte decomposition is a major challenge. The stability of different electrolyte solvents and salts were investigated. Aprotic carbonate and ether based solvents such as PC, EC/DEC, TEGDME, and PEGDME were found to decompose during electrochemical cycling of the cells. The carbonate based electrolytes decompose to form a 5-10 nm thick surface layer on the carbon cathode during discharge which was then removed during battery charging. The degradation products of the ether based electrolytes consisted mainly of ether and carbonate based surface species. It is also shown that Li2O2 as the final discharge product of the cell is chemically reactive and decomposes carbonate and ether based solvents. The stability of lithium electrolyte salts (such as LiPF6, LiBF4, LiB(CN)4, LiBOB, and LiClO4) was also studied. The PES results revealed that all salts are unstable during the cell cycling and in contact with Li2O2. Decomposition layers thinner than 5 nm were observed on Li2O2. Furthermore, it is shown that the stability of the interface on the lithium anode is a chief issue. When compared to Li batteries (where oxygen levels are below 10 ppm) working in the presence of excess oxygen leads to the decomposition of carbonate based electrolytes to a larger degree.

Place, publisher, year, edition, pages
Uppsala: Acta Universitatis Upsaliensis, 2012. 65 p.
Series
Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology, ISSN 1651-6214 ; 1001
Keyword
Li-O2 Battery, Surface Characterization, Lithium-Air Battery, Photoelectron Spectroscopy, XPS
National Category
Materials Chemistry Physical Chemistry
Research subject
Chemistry with specialization in Materials Chemistry; Chemistry with specialization in Physical Chemistry
Identifiers
urn:nbn:se:uu:diva-183887 (URN)978-91-554-8544-3 (ISBN)
Public defence
2012-12-19, Polhemsalen, Ångström Laboratory, Lägerhyddsvägen 1, Uppsala, 10:15 (English)
Opponent
Supervisors
Available from: 2012-11-27 Created: 2012-11-05 Last updated: 2016-04-26Bibliographically approved

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Publisher's full texthttp://www.ncbi.nlm.nih.gov/pubmed/23336349

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Younesi, RezaHahlin, MariaEdström, Kristina

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