Research Article 2026-04-22 posted v1

Machine-Learned Interatomic Potential Insights into the Effect of H₂O on CO₂ Adsorption in HEU-Type Zeolites

A
Anthony Pembere 1 Department of Physical Sciences, Jaramogi Oginga Odinga University of Science and Technology, P.O Box 210 Bondo 40601, Kenya 2Michigan Institute for Data and AI in Society, University of Michigan. Weiser Hall, 500 Church Street, Suite 600, Ann Arbor, MI 48109-1042
F
Fred Sifuna Department of Pure and Applied Chemistry, Masinde Muliro University of Science and Technology, P.O Box 190 Kakamega 50100, Kenya

Abstract

The rapid increase in atmospheric CO₂ concentrations remains a major driver of global climate change, making the development of high-performance carbon capture materials essential. These materials must be capable of operating efficiently under realistic conditions including humidity and industrial gases. Understanding the influence of water on CO₂ adsorption in zeolite structures is therefore crucial for developing robust carbon capture technologies. In this study, the impact of water on CO₂ adsorption in HEU-type zeolites is examined using a machine-learned interatomic potential (MLIP) trained on high-fidelity ab initio data. MLIPs enable atomistic simulations with near-density functional theory (DFT) accuracy while also providing access to extended timescales and lengths. Radial distribution functions (RDFs) and cumulative coordination numbers of HEU zeolite co-loaded with H₂O and CO₂ show that the structure is preserved, as indicated by the absence of changes in the Si–O and Si–Si peaks. The O–O distribution broadens, reflecting the aggregation of hydrogen-bonded water molecules within the pores. The reduction in C–network correlations indicates that water preferentially occupies the adsorption sites, displacing CO₂ and weakening its interaction with the network. These results highlight competitive adsorption and pore obstruction under humid conditions. Therefore, improving the hydrophobicity of the zeolite surface or pre-drying the gas streams may be necessary to maintain adsorption efficiency.

Citation Information

@article{anthonypembere2026,
  title={Machine-Learned Interatomic Potential Insights into the Effect of H₂O on CO₂ Adsorption in HEU-Type Zeolites},
  author={Anthony Pembere and Fred Sifuna},
  journal={Research Square},
  year={2026},
  doi={https://doi.org/10.21203/rs.3.rs-9475077/v1}
}
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