Atomistic Structure Generation and Neural-Network Screening of Hard Carbons to Identify High-Capacity Sodium Storage

Abstract

Hard carbons are established anodes for lithium-ion batteries and leading candidates for sodium-ion batteries, yet their electrochemical performance is governed by a heterogeneous network of graphitic domains, defects, and nanopores that conventional atomistic methods cannot model at the required length scales. We combine universal machine-learned interatomic potentials with the RAFFLE structure-generation framework to construct 13,096 realistic hard carbon models containing up to 4,378 atoms, matching experimentally measured densities, porosities, and sp$^2$/sp$^3$ bonding fractions. Explicit sodium intercalation of representative structures reproduces the characteristic sloping-to-plateau voltage profiles, revealing that capacity increases with decreasing carbon density and increasing porosity. To screen the full library, we train a lightweight neural-network surrogate that predicts capacity directly from the host using frozen universal-potential descriptors augmented by geometric void features. The surrogate identifies high-capacity candidates exceeding 800 mAh g$^{-1}$, which are validated by full intercalation calculations. This scalable framework links hard carbon microstructure to sodium-storage performance and provides atomistic design principles for high-capacity anodes. More broadly, the workflow enables systematic exploration of synthesis-dependent amorphous microstructures, including precursor chemistry, pyrolysis, heteroatom doping, and pore engineering, providing a route toward atomistically informed hard carbon design.