Optimizing Electrode-Electrolyte Interfaces in Lithium Batteries

Research output: ThesisDissertation (TU Delft)

Abstract

Energy storage technologies are critical to the global energy transition, given the need to reduce carbon emissions and the ever-increasing demand for energy. The need for energy storage is particularly crucial in the automotive and electricity generation sectors, where a shift from fossil fuels to renewable sources is imperative. Lithium-ion batteries are central contributors to this transition, powering electric vehicles (EVs) and supporting renewable energy integration into electricity grids. Historically, lithium-ion batteries evolved from using Li metal as a negative electrode to safer alternatives like graphite, and positive electrode materials such as LiNi0.8Mn0.1Co0.1O2 (NMC811) and LiFePO4 (LFP). However, despite these advancements, several challenges still need to be addressed.
First, increasing the energy density of lithium-ion batteries is a priority, particularly for EVs, where higher energy densities can extend the driving range and improve market adoption. Feasible solutions in this regard could be increasing the thickness of electrodes and switching to higher energy density materials such as Li metal. Second, safety remains a key concern, as current batteries use liquid electrolytes that are prone to thermal runaway, leading to fires or explosions. Solid-state electrolytes offer a safer alternative with higher thermal stability. However, they also present their own challenges at the electrode/electrolyte interfaces. Third, there is a growing emphasis on developing environmentally friendly batteries, as many of the materials and manufacturing processes for current lithium-ion batteries are not sustainable. Efforts are being made to eliminate fluorinated compounds and other toxic components from batteries, but this needs to be done without compromising performance. The optimization of the electrode-electrolyte interfaces in batteries holds the key to enabling batteries of the future. Optimizing Li morphology during plating/stripping, improving interfacial stability, and ensuring sufficient ion and electron percolation in cathode composites are key to improving battery capacity, lifetime, safety, and efficiency.
Original languageEnglish
QualificationDoctor of Philosophy
Awarding Institution
  • Delft University of Technology
Supervisors/Advisors
  • Mulder, F.M., Promotor
  • Wagemaker, M., Promotor
Award date3 Jun 2025
DOIs
Publication statusPublished - 2025

Keywords

  • Li-ion batteries
  • Lithium metal batteries
  • Solid state NMR
  • XPS
  • Phase inversion
  • Fluorine-free electrolytes
  • solid state batteries

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