In this study, a sustainable NH2-MIL-101(Al) is synthesized and subjected to characterization for cryogenic CO2 adsorption, isotherms, and thermodynamic study. The morphology revealed a highly porous surface. The XRD showed that NH2-MIL-101(Al) was crystalline. The NH2-MIL-101(Al) decomposes at a temperature (>500 °C) indicating excellent thermal stability. The BET investigation revealed the specific surface area of 2530 m2/g and the pore volume of 1.32 cm3/g. The CO2 adsorption capacity was found to be 9.55 wt to 2.31 wt within the investigated temperature range. The isotherms revealed the availability of adsorption sites with favorable adsorption at lower temperatures indicating the thermodynamically controlled process. The thermodynamics showed that the process is non-spontaneous, endothermic, with fewer disorders, chemisorption. Finally, the breakthrough time of NH2-MIL-101(Al) is 31.25 more than spherical glass beads. The CO2 captured by the particles was 2.29 kg m�3. The CO2 capture using glass packing was 121 less than NH2-MIL-101(Al) under similar conditions of temperature and pressure. © 2021 Elsevier Ltd