Large-scale Simulations of Catalysis at the Interface of Electrodes and Electrolytes

Electrocatalytic reactions are being applied more widely to reduce the carbon footprint of industries, such as steel and concrete, for potential high density energy storage, as well as synthesis of advanced organic bioactive molecules.

While accurate atomistic models are available for solution phase and clean surface reactions, they are largely absent for interfaces between solids and liquids.

During electrocatalysis large electric fields are present at the electrode, which will affect all species close to the reactive center.

We will develop and apply models to understand the impact of such inhomogeneous local environments on key reaction steps.

The two main reactions in focus are the reduction of carbon dioxide to formic acid, carbon monoxide, or methanol, and the water oxidation reaction to generate molecular oxygen.

We recently demonstrated that three key reaction steps can be simulated using dynamic large-scale systems in water and organic solvents, to carbon surfaces interfacing organic solvent, electrolyte solutions, and reactions in the electric double layer.

Herein, we will expand our previous models to describe all potentially limiting reaction steps, we aim at replacing precious metals with iron, and we will develop models for studying diffusion, reactions, and electron transfer in electrocatalytic porous materials.

We will take the next step in understanding the impact of the dynamic structural complexity and the interface of an electrode and an electrolyte.