Work

First-principles design of YGaTe3 for bidirectional catalysis and shuttle suppression in lithium–sulfur batteries

Year: 2025

Type: article

Abstract: Lithium-sulfur (Li-S) batteries suffer from sluggish redox kinetics and polysulfide shuttle, which hinder their practical applications. Herein, first-principles calculations are employed to design and evaluate YGaTe 3 as a high-performance sulfur host. The Y-side surface exhibits nearly metallic conductivity (band gap = 0.0186 eV), providing efficient electron transport channels. Gibbs free energy profiles reveal uniformly low energy barriers (<0.20 eV) for the stepwise S 8 → Li 2 S conversion on the Y-side, whereas the Ga-side exhibits a 0.45 eV barrier in the Li 2 S 2 → Li 2 S step. Furthermore, the continuous and thermodynamically favorable energy profiles during the charging process ensure the feasibility of LiPS oxidation and the capability of bidirectional catalysis. The NEB results demonstrate that the lower energy barrier on the Y-side (0.43 eV) compared to the Ga-side (0.72 eV) facilitates easier Li 2 S activation and faster decomposition kinetics. The Bader charge analysis and −pCOHP results indicate the enhanced charge transfer and robust Te-Li bonding on the Y-side, while the p-band center calculations show stable and favorable electronic coupling for polysulfide adsorption. This combination of high conductivity, bidirectional catalysis, and shuttle suppression highlights YGaTe 3 as a promising candidate for stable and efficient Li-S batteries.

Source: Journal of Catalysis

DOI: 10.1016/j.jcat.2025.116638