Multi-Fidelity Computational Screening of High-Entropy MBenes for CO$_2$ Electroreduction
Abstract
High-entropy MBenes (HE-MBenes) represent a promising, unexplored class of 2D materials for electrocatalysis. In this work, we present a systematic computational screening of 56 equiatomic quinary HE-MBene compositions from the {Ti, V, Cr, Mo, Nb, Ta, Zr, Hf} pool for CO adsorption and electroreduction. Using the Monte Carlo Special Quasirandom Structure (MCSQS) algorithm, we generated disordered M-type supercells and assessed structural stability via DFT (PBE+D3) in VASP. Of the 56 candidates, 55 passed relaxation, with 45 exhibiting negative formation energies, confirming thermodynamic stability. To efficiently screen CO adsorption across disordered surfaces, we developed a machine-learning interatomic potential (MLIP) using the MACE architecture. Fine-tuned on our DFT dataset, the model achieved energy RMSEs of 3.49 and 3.0 meV/atom for adsorbed and pristine sets, respectively. Active sites were identified via PDOS analysis, matching metal d-orbital signatures with CO molecular orbitals. The rate-determining step of the CO-to-CO pathway was evaluated using the computational hydrogen electrode (CHE) model. Short-time structural integrity was assessed via AIMD at 500 K over 2.5 ps; phonon-based stability remains a priority for future work. Our results establish an integrated DFT-MLIP-AIMD framework for the rational design of high-entropy 2D materials tailored for CO conversion.
Keywords
Cite
@article{arxiv.2605.08728,
title = {Multi-Fidelity Computational Screening of High-Entropy MBenes for CO$_2$ Electroreduction},
author = {Sree Harsha Bharadwaj H and Raghavan Ranganathan},
journal= {arXiv preprint arXiv:2605.08728},
year = {2026}
}