Machine-Learning-Driven High-Throughput Screening of Transition-Metal Atom Intercalated g-C3N4/MX2 (M = Mo, W; X = S, Se, Te) Heterostructures for the Hydrogen Evolution Reaction.

Rising global energy demand, accompanied by environmental concerns linked to conventional fossil fuels, necessitates a shift toward cleaner and sustainable alternatives. This study focuses on the machine-learning (ML)-driven high-throughput screening of transition-metal (TM) atom intercalated g-C3N4/MX2 (M = Mo, W; X = S, Se, Te) heterostructures to unravel the rich landscape of possibilities for enhancing the hydrogen evolution reaction (HER) activity. The stability of the heterostructures and the intercalation within the substrates are verified through adhesion and binding energies, showcasing the significant impact of chalcogenide selection on the interaction properties. Based on hydrogen adsorption Gibbs free energy (ΔGH) computed via density functional theory (DFT) calculations, several ML models were evaluated, particularly random forest regression (RFR) emerges as a robust tool in predicting HER activity with a low mean absolute error (MAE) of 0.118 eV, thereby paving the way for accelerated catalyst screening. The Shapley Additive exPlanation (SHAP) analysis elucidates pivotal descriptors that influence the HER activity, including hydrogen adsorption on the C site (HC), MX layer (HMX), S site (HS), and intercalation of TM atoms at the N site (IN). Overall, our integrated approach utilizing DFT and ML effectively identifies hydrogen adsorption on the N site (site-3) of g-C3N4 as a pivotal active site, showcasing exceptional HER activity in heterostructures intercalated with Sc and Ti, underscoring their potential for advancing catalytic performance.