First-principles calculations and automation for electrochemical device applications based on 2D materials

Abstract

In this thesis, we present the operating and design principles of two-dimensional material-based electrochemical devices through first-principles calculation. In addition, we develop a Python-based automation platform of first-principle based computational catalysis for the discovery of highly active catalytic materials by high-throughput screening. First, we find that atomically precise non-noble metal cluster can be stabilized in two-dimensional carbon nitride layers with periodic pores. The non-noble metal cluster exhibits strong metallic properties, resulting in high oxygen reduction reaction or hydrogen evolution reaction performance compared to well-known single atom or encapsulated catalyst as counterparts. Next, we demonstrate the synergistic effect between different types of nitrogen doped graphene for oxygen reduction reaction, which is considered one of the strongest candidates for metal-free catalyst. By applying systematic investigation rules, we have discovered a specific composition of nitrogen doped complexes that maximize their catalytic activity. Based on the findings, we proposed the design principle of nitrogen doped complex that changes from low activity to high activity. Finally, we develop NanoCore Catalysis that is a Python-based automation platform for first-principles calculation based computational catalysis. NanoCore Catalysis is automatically performed for catalyst atomic structure modeling, Gibbs free energy calculation, and visualization of Gibbs free energy diagram. It is also demonstrated to use high-throughput catalyst screening by oxygen reduction reaction and hydrogen evolution reaction examples. Through these researches, we show the usefulness and importance of first-principle calculations and automated workflows for computational catalysis in the development of two-dimensional electrochemical devices. We expect that understanding of operating and design principle of renewable energy related electrocatalyst will help and contribute to development of various two-dimensional material applications.