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Understanding the SEI Formation at Pristine Li-Ion Cathodes: Chemisorption and Reaction of DEC on LiCoO2 Surfaces Studied by a Combined SXPS/HREELS Approach

Späth, Thomas ; Becker, Dirk ; Schulz, Natalia ; Hausbrand, René ; Jaegermann, Wolfram (2017)
Understanding the SEI Formation at Pristine Li-Ion Cathodes: Chemisorption and Reaction of DEC on LiCoO2 Surfaces Studied by a Combined SXPS/HREELS Approach.
In: Advanced Materials Interfaces, 4 (23)
doi: 10.1002/admi.201700567
Artikel, Bibliographie

Kurzbeschreibung (Abstract)

Reactions and solid electrolyte interface (SEI) formation at electrode–electrolyte interfaces are crucial for the stability and performance of Li‐ion batteries, but are still not fully understood on a fundamental level. For improving battery properties, a detailed understanding of these degradation processes is needed. In this contribution, the interface formation between a thin film LiCoO2 cathode material and diethyl carbonate (DEC) as typical battery electrolyte solvent is presented. A surface‐science approach is used performing a stepwise adsorption of DEC onto LiCoO2 at low temperatures. The interface is studied after each step by synchrotron‐based X‐ray photoemission spectroscopy (SXPS) and high‐resolution electron energy loss spectroscopy. The results demonstrate that the decomposition of carbonate solvents in contact with fully lithiated cathode materials as observed in adsorption experiments is complex, including the reduction of solvent, subsequent decomposition reactions, and also catalytic effects. In the present case, lithium ethyl carbonate, lithium ethoxide, and lithium oxides are assigned as reaction products. The spectra provide indications for partial electron transfer coupled to covalent interaction involving surface oxygen O2p orbital and DEC lowest unoccupied molecular orbital (LUMO) states.

Typ des Eintrags: Artikel
Erschienen: 2017
Autor(en): Späth, Thomas ; Becker, Dirk ; Schulz, Natalia ; Hausbrand, René ; Jaegermann, Wolfram
Art des Eintrags: Bibliographie
Titel: Understanding the SEI Formation at Pristine Li-Ion Cathodes: Chemisorption and Reaction of DEC on LiCoO2 Surfaces Studied by a Combined SXPS/HREELS Approach
Sprache: Englisch
Publikationsjahr: 2017
Verlag: Wiley-VCH Verlag GmbH, Weinheim
Titel der Zeitschrift, Zeitung oder Schriftenreihe: Advanced Materials Interfaces
Jahrgang/Volume einer Zeitschrift: 4
(Heft-)Nummer: 23
DOI: 10.1002/admi.201700567
URL / URN: https://doi.org/10.1002/admi.201700567
Kurzbeschreibung (Abstract):

Reactions and solid electrolyte interface (SEI) formation at electrode–electrolyte interfaces are crucial for the stability and performance of Li‐ion batteries, but are still not fully understood on a fundamental level. For improving battery properties, a detailed understanding of these degradation processes is needed. In this contribution, the interface formation between a thin film LiCoO2 cathode material and diethyl carbonate (DEC) as typical battery electrolyte solvent is presented. A surface‐science approach is used performing a stepwise adsorption of DEC onto LiCoO2 at low temperatures. The interface is studied after each step by synchrotron‐based X‐ray photoemission spectroscopy (SXPS) and high‐resolution electron energy loss spectroscopy. The results demonstrate that the decomposition of carbonate solvents in contact with fully lithiated cathode materials as observed in adsorption experiments is complex, including the reduction of solvent, subsequent decomposition reactions, and also catalytic effects. In the present case, lithium ethyl carbonate, lithium ethoxide, and lithium oxides are assigned as reaction products. The spectra provide indications for partial electron transfer coupled to covalent interaction involving surface oxygen O2p orbital and DEC lowest unoccupied molecular orbital (LUMO) states.

Freie Schlagworte: HREELS, LiCoO2 cathode material, SEI formation, XPS
Fachbereich(e)/-gebiet(e): 11 Fachbereich Material- und Geowissenschaften
11 Fachbereich Material- und Geowissenschaften > Materialwissenschaft
11 Fachbereich Material- und Geowissenschaften > Materialwissenschaft > Fachgebiet Oberflächenforschung
Hinterlegungsdatum: 01 Nov 2017 17:20
Letzte Änderung: 26 Jun 2018 12:07
PPN:
Sponsoren: The authors thank HZB for the allocation of synchrotron radiation beamline at the SoLiAS workstation at the U49 II/PGM 2 beamline., Furthermore, the authors thankfully acknowledge the financial support by HZB, DFG (project HA 6128/1-1), and the Hesse Graduate Program for scientific-technological fundamentals for electromobility (HGP-E).
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