Observing what cannot be observed: computational electrochemistry from carbon to hydrogen

Hanselman, S.R. (2022)

Doctoral Thesis

In this thesis, we consider various (electro)chemical phenomena at surfaces and nanoparticles and their underlying atomistic processes, which we studied using first-principles methods such as density functional theory. These phenomena range from CO2 reduction to C2 and C3 species, through solvation of adsorbates on various surface features of late transition metals, to the impact of graphene on hydrogen evolution reaction, cathodic corrosion and surface oxidation of Pt. With our thermodynamic and kinetic calculations, we provide explanations for experimental observations by unraveling underlying phenomena, support novel computational methods and techniques, and propose new atomic structures that explain prior findings and provide inroads into future electrocatalytic research.

• Density functional theory
• Surface chemistry
• Graphene
• Cathodic corrosion
• CO2 reduction
• Solvation modelling
• Sustainable energy storage
• Transition metal catalysts

• All authors: Hanselman, S.R.
• Supervisor: Koper, M.T.M.
• Co-supervisor: Calle-Vallejo, F.
• Committee: Kroes, G.J.; Doblhoff-Dier, K.; Filot, I.; Rossmeisl, J.; Ubbink, M.
• Qualification: Doctor (dr.)
• Awarding Institution: Leiden Institute of Chemistry (LIC), Faculty of Science, Leiden University
• Date: 2022-12-20
• Sponsorship: NWO Solar Fuels Graduate Program; HPC-Europa3 (INFRAIA-2016-1-730897)