Dissertation: "Exploring Reaction Pathways in Li-ion Batteries with Operando Gas Analysis"

  • Date:
  • Location: Ångströmlaboratoriet, Lägerhyddsvägen 1 Polhemsalen
  • Doctoral student: Robin Lundström
  • About the dissertation
  • Organiser: Department of Chemistry - Ångström Laboratory
  • Contact person: Erik Berg
  • Disputation

Robin Lundström defends his PhD thesis with the title "Exploring Reaction Pathways in Li-ion Batteries with Operando Gas Analysis" in the subject of Chemistry with a specialisation in Materials Chemistry.

Opponent: Dr. Isidora Cekic-Laskovic, Forschungszentrum Jülich GmbH, Germany

Supervisor: Prof. Erik Berg, Structural Chemistry, Department of Chemistry - Ångström, Uppsala University

Link to the thesis in full text in DiVA.


The reliance on Li-ion batteries is increasing as we transition from fossil fuels to renewable energy sources. Despite their widespread use, a gap remains in understanding certain processes within these batteries, especially regarding the solid electrolyte interphase (SEI) and the impact of side reactions on Li-ion batteries. A custom-made Online Electrochemical Mass Spectrometry (OEMS) instrument was designed to explore these aspects. The OEMS instrument was validated through the study of gas-evolving reactions in the classic LiCoO2 | Graphite system. In-depth studies focusing on the reaction pathways of ethylene carbonate, the archetype Li-ion battery electrolyte solvent, identified the specific reaction pathways contributing to SEI formation. Moreover, ethylene carbonate’s interaction with residual contaminants like OH– from H2O reduction was explored. It was revealed that the integrity of the SEI can be compromised by minor amounts of contaminants, establishing a competitive dynamic at the negative electrode surface between ethylene carbonate and residual contaminants such as H2O and HF. Additionally, the roles of additives like vinylene carbonate and lithium bis(oxolato) borate in SEI formation were explored. Vinylene carbonate was shown to form a layer on the negative electrode, but also scavenge protons and H2O, revealing that it is a multi-functional additive. Lithium bis(oxolato) borate on the other hand formed an SEI layer before H2O reduction, blocking the residual contaminant and ethylene carbonate from reaching the electrode surface. By providing insights into the negative electrode’s interphase and SEI formation through a custom-made OEMS instrument, this research underscores the complexity of reaction pathways and the necessity of considering both major and minor, as well as, primary and secondary reactions for a holistic understanding of Li-ion batteries.


Image of the thesis.