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 CO2 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 CO2 capture configuration with the pores being decorated with a high density of mu (2)-OH groups and accessible aromatic rings. Meanwhile, based on calculations and experimental evidence, moderate host-guest interactions Q(st) (CO2) 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 CO2/N-2 separation ability are validated by breakthrough experiments while operando IR experiments indicate a kinetically favorable CO2 adsorption over water. Finally, a techno-economic analysis gives an estimated production cost of approximate to 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 CO2 capture processes.

keywords

METAL-ORGANIC FRAMEWORK; CO2 CAPTURE; ALUMINUM PYROMELLITATE; POROUS MATERIALS; DIOXIDE; ADSORPTION; SORBENTS; REMOVAL

subject category

Chemistry; Science & Technology - Other Topics; Materials Science

authors

Chen, BB; Fan, D; Pinto, RV; Dovgaliuk, I; Nandi, S; Chakraborty, D; Garcia-Moncada, N; Vimont, A; Mcmonagle, CJ; Bordonhos, M; Al Mohtar, A; Cornu, I; Florian, P; Heymans, N; Daturi, M; De Weireld, G; Pinto, M; Nouar, F; Maurin, G; Mouchaham, G; Serre, C

Groups

Projects

CICECO - Aveiro Institute of Materials (UIDB/50011/2020)

CICECO - Aveiro Institute of Materials (UIDP/50011/2020)

Associated Laboratory CICECO-Aveiro Institute of Materials (LA/P/0006/2020)

acknowledgements

The authors acknowledge the European Union's Horizon 2020 research and innovation program under grant agreement No. 831975 (MOF4AIR project) for providing financial support. M.P., M.B., and A.A.M. acknowledge Portuguese FCT/MCTES, and when applicable ERDF under the PT2020 partnership agreement, for the funding of the projects UIDB/04028/2020 and UIDP/04028/2020 (CERENA) and UIDB/50011/2020, UIDP/50011/2020 and LA/P/0006/2020 (CICECO). The computational work was performed using HPC resources from GENCI-CINES (Grant A0140907613). B.C. is grateful for support from a CSC grant (grant number 201804910475). M.B. gratefully acknowledges FCT for the PhD grant ref. SFRH/BD/147239/2019. The authors are thankful to the Swiss-Norwegian Beamlines (SNBL) staff at the European Synchrotron Radiation Facility (ESRF). We thank Dr. Antoine Tissot for his help in remeasuring the SCXRD structure of MIL-120(Al)-HP. M. Masheer Ul-Haq is acknowledged for his contribution to the synthesis part.