Laser desorption/ionization-mass spectrometry for the analysis of interphases in lithium ion batteries

Valentin Göldner; Linda Quach; Egy Adhitama; Arne Behrens; Luisa Junk; Martin Winter; Tobias Placke; Frank Glorius; Uwe Karst

doi:10.1016/j.isci.2023.107517

Laser desorption/ionization-mass spectrometry for the analysis of interphases in lithium ion batteries

iScience. 2023 Jul 31;26(9):107517. doi: 10.1016/j.isci.2023.107517. eCollection 2023 Sep 15.

Authors

Valentin Göldner^{1

2}, Linda Quach^{2

3}, Egy Adhitama^{2

4}, Arne Behrens^{1

5}, Luisa Junk¹, Martin Winter^{2

4

6}, Tobias Placke^{2

4}, Frank Glorius^{2

3}, Uwe Karst^{1

2}

Affiliations

¹ Institute of Inorganic and Analytical Chemistry, University of Münster, Corrensstraße 48, 48149 Münster, Germany.
² International Graduate School for Battery Chemistry, Characterization, Analysis, Recycling and Application (BACCARA), University of Münster, Corrensstraße 40, 48149 Münster, Germany.
³ Institute of Organic Chemistry, University of Münster, Corrensstraße 36, 48149 Münster, Germany.
⁴ MEET Battery Research Center, Institute of Physical Chemistry, University of Münster, Corrensstaße 46, 48149 Münster, Germany.
⁵ Bruker Daltonics GmbH & Co. KG, Fahrenheitstraße 4, 28359 Bremen, Germany.
⁶ Helmholtz Institute Münster, IEK-12, Forschungszentrum Jülich GmbH, Corrensstraße 46, 48149 Münster, Germany.

Abstract

Laser desorption/ionization-mass spectrometry (LDI-MS) is introduced as a complementary technique for the analysis of interphases formed at electrode|electrolyte interfaces in lithium ion batteries (LIBs). An understanding of these interphases is crucial for designing interphase-forming electrolyte formulations and increasing battery lifetime. Especially organic species are analyzed more effectively using LDI-MS than with established methodologies. The combination with trapped ion mobility spectrometry and tandem mass spectrometry yields additional structural information of interphase components. Furthermore, LDI-MS imaging reveals the lateral distribution of compounds on the electrode surface. Using the introduced methods, a deeper understanding of the mechanism of action of the established solid electrolyte interphase-forming electrolyte additive 3,4-dimethyloxazolidine-2,5-dione (Ala-N-CA) for silicon/graphite anodes is obtained, and active electrochemical transformation products are unambiguously identified. In the future, LDI-MS will help to provide a deeper understanding of interfacial processes in LIBs by using it in a multimodal approach with other surface analysis methods to obtain complementary information.

Keywords: Analytical Electrochemistry; Electrochemical energy storage; Interfacial electrochemistry; Organic chemistry.