A Scalable Robust Microporous Al‐MOF for Post‐Combustion Carbon Capture

Abstract Herein, a robust microporous aluminum tetracarboxylate framework, MIL‐120(Al)‐AP, (MIL, AP: Institute Lavoisier and Ambient Pressure synthesis, respectively) is reported, which exhibits high CO 2 uptake (1.9 mmol g −1 at 0.1 bar, 298 K). In situ Synchrotron X‐ray diffraction measurements together with Monte Carlo simulations reveal that this structure offers a favorable CO 2 capture configuration with the pores being decorated with a high density of µ 2 ‐OH groups and accessible aromatic rings. Meanwhile, based on calculations and experimental evidence, moderate host‐guest interactions Q st (CO 2 ) value of MIL‐120(Al)‐AP (−40 kJ mol −1 ) is deduced, suggesting a relatively low energy penalty for full regeneration. Moreover, an environmentally friendly ambient pressure green route, relying on inexpensive raw materials, is developed to prepare MIL‐120(Al)‐AP at the kilogram scale with a high yield while the Metal‐ Organic Framework (MOF) is further shaped with inorganic binders as millimeter‐sized mechanically stable beads. First evidences of its efficient CO 2 /N 2 separation ability are validated by breakthrough experiments while operando IR experiments indicate a kinetically favorable CO 2 adsorption over water. Finally, a techno‐economic analysis gives an estimated production cost of ≈ 13 $ kg −1 , significantly lower than for other benchmark MOFs. These advancements make MIL‐120(Al)‐AP an excellent candidate as an adsorbent for industrial‐scale CO 2 capture processes.