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Accelerated Discovery of Nitrogen-Coordinated Dual-Atom Hydrogen Evolution Reaction Electrocatalysts via Machine Learning Potentials

cond-mat.mtrl-sci2026-05v1license

Abstract

The hydrogen evolution reaction (HER) is central to sustainable hydrogen production, and nitrogen coordinated dual atom catalysts (DACs) offer a promising route to noble metal activity at low cost. Yet their vast compositional and coordination design space remains underexplored, as density functional theory (DFT) screening at scale is prohibitive. Here, we map the HER landscape of graphene supported TM2@Nx-Gr DACs, screening 23 transition metals across 20 nitrogen coordination motifs using a machine learning potential (MLP) benchmarked against DFT. Intermediate coordination (2N to 4N) consistently yields near-optimal {\Delta}GH*, with Ti2@2Na, Mn2@2Na, Fe2@2Na, Cu2@2Na, Rh2@2Na, Zr2@2Na, Zr2@2Nb, Zr2@2Nc, Nb2@2Nc, Zr2@2Nd, Mn2@2Ne, Mn2@2Nf, Ti2@3Na, Au2@3Na, Fe2@3Na, Pd2@3Nb, Rh2@3Nc, Rh2@3Nd, Au2@3Nd, V2@4Na, Ti2@4Nb, Pd2@4Nb, Ti2@4Nc, Cr2@4Nd, Ni2@4Nd, Cu2@4Nd emerging as standout, synthesizable candidates, most exhibiting metallic or narrow gap (<0.25 eV) character. The MLP reaches near-DFT accuracy, with a mean absolute error of 80 meV for Gibbs binding free energies at orders of magnitude lower computational cost, establishing MLP driven screening as a practical engine for next-generation catalyst discovery.

Comments: Research article, 32 pages, 18 figures

Cite

@article{arxiv.2605.29821,
  title  = {Accelerated Discovery of Nitrogen-Coordinated Dual-Atom Hydrogen Evolution Reaction Electrocatalysts via Machine Learning Potentials},
  author = {Yanmei Zang and Hyun Gyu Park and Gi Beom Sim and Tae Hyeon Park and Ho Jin Lee and Xiaorong Zou and D. ChangMo Yang and Soohaeng Yoo Willow and Hye Jung Kim and Chang Woo Myung},
  journal= {arXiv preprint arXiv:2605.29821},
  year   = {2026}
}