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

BACKGROUND: 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. RESULTS: 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. SIGNIFICANCE: 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.