System-level comparison and techno-economic evaluation of structured metal–organic framework adsorbents for post-combustion CO₂ capture by vacuum/pressure swing adsorption

Shaping micron-sized metal–organic framework (MOF) powders into millimeter-sized structures addresses handling and processing challenges for practical CO₂ capture. However, most studies focus on simple metrics such as CO₂ uptake capacity and CO₂/N₂ selectivity, often neglecting system-level cost considerations. Additionally, system-level modeling frequently relies on data generated from MOFs in powder form, without considering their structured variants. This study presents a systematic approach for data generation and evaluation of MOFs, namely UiO-66, MIL-101@GO, and ZIF-8, that have undergone polymer-aided structuring, using dynamic simulations of a cyclic vacuum/pressure swing adsorption (V/PSA) process for CO₂ capture and compression from the flue gas of a 550 MW coal-fired power plant. Parametric sensitivity analyses were performed, and the V/PSA process was optimized to maximize CO₂ purity and recovery while minimizing costs. Results show that the structured UiO-66 achieves a cost of $72.50 per ton of CO₂ captured with 95 % purity and 88.8 % recovery, which drops to $60.60 per ton with 80 % recovery. Structured MIL-101@GO costs $75.00 per ton for 96.4 % purity and 88.6 % recovery, while structured ZIF-8 costs $80.20 per ton with 91.2 % purity and 74.4 % recovery. This study highlights the importance of using cost as a primary evaluation metric for structured adsorbents integrating data from such adsorbents into system-level modeling and optimizing cyclic adsorption processes with detailed equipment sizing and column scheduling to assess their feasibility for commercial-scale CO₂ capture.