Lightweight energy storage is a must for increased driving range of electric vehicles. โMass-lessโ energy storage can be achieved by directly storing energy in structural components. In such multifunctional devices called structural composite batteries, carbon fibres carry mechanical load and simultaneously act as negative battery electrode by hosting lithium ions in its microstructure. Little is known of how the microstructure of carbon fibres is optimised for multifunctionality, and deeper understanding of the configuration and the distribution of atoms in carbon fibres is needed.Here synchrotron hard X-ray photoelectron spectroscopy and atom probe tomography are used to reveal the chemical states and three-dimensional distribution of atoms in commercial carbon fibres. This thesis presents the first ever guide for how to perform atom probe tomography on carbon fibres, and the first ever three-dimensional atomic reconstruction of a carbon fibre.The results show that the chemical states and distribution of nitrogen heteroatoms in carbon fibres affect the electrochemical performance of the fibres. Carbon fibres performed electrochemically better with higher amount of nitrogen with pyridinic and pyrrolic configurations. Additionally, the nitrogen concentration varies throughout the carbon fibre, which may suggest that the electrochemical properties also vary throughout the carbon fibre. The knowledge provided by this thesis can lead to future carbon fibre designs with enhanced electrochemical performance for multifunctional applications
