Multiscale evaluation of metal-organic framework-based adsorbents for shipboard carbon capture: Simulation,...

Shipboard carbon capture requires adsorbents capable of selectively removing CO₂ from complex exhaust mixtures containing CO, NO, and SO₂ under dynamically varying thermal and pressure conditions. Metal-organic frameworks (MOFs), with their tunable porosity and well-defined structures, offer strong potential for such applications, yet systematic multiscale evaluations remain limited. To address this gap, we systematically evaluated a curated dataset of 7419 pore-accessible MOFs-derived from an initial pool of 12,021 structures-using molecular simulations, machine learning, and experimental validation to identify materials with robust performance and scalability for practical marine deployment.

High-throughput grand canonical Monte Carlo (GCMC) simulations quantified multigas adsorption behavior for a curated dataset of 7419 pore-accessible MOFs (derived from an initial pool of 12,021 structures), revealing strong structure-performance correlations governed by surface area, pore metrics, and metal identity. Machine learning models trained on these data achieved R² values exceeding 0.98, enabling rapid prediction of adsorption capacities. HKUST-1 emerged as a representative candidate based on metal prevalence and synthetic feasibility. Density functional theory (DFT) calculations confirmed that partial Zn substitution enhances structural stability, while experiments validated improved binding performance in ZnHKUST-1 and its activated-carbon composite. A 3D-printed monolithic adsorbent displayed increased thermal conductivity and maintained CO₂ selectivity despite partial pore blockage. Multiphysics simulations further demonstrated efficient heat dissipation during pressurized gas charging and preferential CO₂ adsorption under multicomponent breakthrough conditions, highlighting robust gas-separation behavior under realistic operating environments.

This study provides an integrated multiscale framework that connects molecular-level screening with experimental synthesis, structural optimization, and system-level evaluation. The resulting insights establish clear design rules for enhancing stability, selectivity, and thermal management in MOF-based adsorbents. By demonstrating consistent performance under conditions relevant to marine exhaust treatment, the work advances practical pathways for implementing MOF-enabled shipboard carbon-capture technologies.