Solving Electrochemistry Puzzles by First-Principles Multi-Scale Modeling

Here we present, how computational modeling based on first-principles can make a significant contribution to achieving this goal. Starting from a basic understanding of electrochemical reaction thermodynamics from a quantum chemical perspective, we highlight the importance of the electric double layer in linking the atomistic to a macroscopic scale. By analyzing a wide range of catalysts exemplarily for the electrochemical reduction of CO₂, we derive general descriptors for electrochemical activity and selectivity which can be used to computationally screen materials in a high-throughput manner. Further, we discuss the role of mass transport and kinetics at the example of CO₂ reduction and stress the importance of the interplay between different time and size scales. Finally, results are presented from experimental collaborations that can help to further solve the multi-scale challenge in electrochemistry.