Few-shot learning for screening 2D Ga2CoS4− supported single-atom catalysts for hydrogen production

A machine learning-driven high-throughput screening reveals efficient single-atom catalysts on 2D Ga 2 CoS 4− x surfaces, optimizing hydrogen evolution reaction catalysis and providing alternatives to platinum-based catalysts. Hydrogen generation and related energy applications heavily rely on the hydrogen evolution reaction (HER), which faces challenges of slow kinetics and high overpotential. Efficient electrocatalysts, particularly single-atom catalysts (SACs) on two-dimensional (2D) materials, are essential. This study presents a few-shot machine learning (ML) assisted high-throughput screening of 2D septuple-atomic-layer Ga 2 CoS 4− x supported SACs to predict HER catalytic activity. Initially, density functional theory (DFT) calculations showed that 2D Ga 2 CoS 4 is inactive for HER. However, defective Ga 2 CoS 4− x ( x = 0–0.25) monolayers exhibit excellent HER activity due to surface sulfur vacancies (SVs), with predicted overpotentials (0–60 mV) comparable to or lower than commercial Pt/C, which typically exhibits an overpotential of around 50 mV in the acidic electrolyte, when the concentration of surface SV is lower than 8.3%. SVs generate spin-polarized states near the Fermi level, making them effective HER sites. We demonstrate ML-accelerated HER overpotential predictions for all transition metal SACs on 2D Ga 2 CoS 4− x . Using DFT data from 18 SACs, an ML model with high prediction accuracy and reduced computation time was developed. An intrinsic descriptor linking SAC atomic properties to HER overpotential was identified. This study thus provides a framework for screening SACs on 2D materials, enhancing catalyst design.