One of the largest challenges in achieving the energy transition is the conversion and storage of sustainable energy in energy-rich compounds such as hydrogen, hydrocarbons or alcohols produced from water and CO2. The key limiting factor in making these reactions more efficient is the lack of detailed understanding of how these reactions proceed on the nanoscale. In particular, detailed knowledge of the hydrogen-bond structure and molecular dynamics in the interfacial region near the electrode surface is missing. In this project we will combine advanced nonlinear optical femtosecond vibrational spectroscopy with scanning probe microscopy to investigate the water structure on the molecular scale near an operating electrode surface. We will also use these advanced techniques to investigate the dynamic distribution of ions and reactants in the region near the electrode surface. With these studies we will obtain novel insights in the structure of the electrical double layer near a biased electrode surface, which will be of great value in optimizing electrochemical reactions for the conversion and storage of sustainable energy.