Unraveling the Stability of Layered Intercalation Compounds through First-Principles Calculations: Establishing a Linear Free Energy Relationship with Aqueous Ions

Abstract

Layered intercalation compounds, where atoms or molecules (intercalants) are inserted into layered materials (hosts), hold great potential for diverse applications. However, the lack of a systematic understanding of stable host–intercalant combinations poses challenges in materials design due to the vast combinatorial space. In this study, we performed first-principles calculations on 9024 compounds, unveiling a novel linear regression equation based on the principle of hard and soft acids and bases. This equation, incorporating the intercalant ion formation energy and ionic radius, quantitatively reveals the stability factors. Additionally, employing machine learning, we predicted regression coefficients from host properties, offering a comprehensive understanding and a predictive model for estimating the intercalation energy. Our work provides valuable insights into the energetics of layered intercalation compounds, facilitating targeted materials design.