[en] 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 µ2-OH groups and accessible aromatic rings. Meanwhile, based on calculations and experimental evidence, moderate host-guest interactions Qst (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/N2 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 ≈ 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.
Disciplines :
Chemical engineering
Author, co-author :
Chen, Bingbing; Institut des Matériaux Poreux de Paris, Ecole Normale Supérieure, ESPCI Paris, CNRS, PSL University, Paris, 75005, France
Fan, Dong; ICGM, Univ. Montpellier, CNRS, ENSCM, Montpellier, 34293, France
Pinto, Rosana V; Institut des Matériaux Poreux de Paris, Ecole Normale Supérieure, ESPCI Paris, CNRS, PSL University, Paris, 75005, France ; Service de Thermodynamique et de Physique Mathématique, Faculté Polytechnique, Université de Mons, Mons, 7000, Belgium
Dovgaliuk, Iurii; Institut des Matériaux Poreux de Paris, Ecole Normale Supérieure, ESPCI Paris, CNRS, PSL University, Paris, 75005, France
Nandi, Shyamapada; Institut des Matériaux Poreux de Paris, Ecole Normale Supérieure, ESPCI Paris, CNRS, PSL University, Paris, 75005, France
Chakraborty, Debanjan; Institut des Matériaux Poreux de Paris, Ecole Normale Supérieure, ESPCI Paris, CNRS, PSL University, Paris, 75005, France
García-Moncada, Nuria; Normandie Université, ENSICAEN, UNICAEN, CNRS, Laboratoire Catalyse et Spectrochimie, Caen, 14000, France
Vimont, Alexandre; Normandie Université, ENSICAEN, UNICAEN, CNRS, Laboratoire Catalyse et Spectrochimie, Caen, 14000, France
McMonagle, Charles J; Swiss-Norwegian Beamlines, European Synchrotron Radiation Facility, 71 Avenue des Martyrs, Grenoble, 38000, France
Bordonhos, Marta; CERENA, Departamento de Engenharia Química, Instituto Superior Técnico, Universidade de Lisboa, Lisboa, 1049-001, Portugal ; CICECO- Aveiro Institute of Materials, Department of Chemistry, University of Aveiro, Campus Universitário de Santiago, Aveiro, 3810-193, Portugal
Al Mohtar, Abeer; CERENA, Departamento de Engenharia Química, Instituto Superior Técnico, Universidade de Lisboa, Lisboa, 1049-001, Portugal
Cornu, Ieuan; Centre National de la Recherche Scientifique (CNRS), UPR3079 CEMHTI, Université d'Orléans, 1D Av. Recherche Scientifique, CEDEX 2, Orléans, 45071, France
Florian, Pierre; Centre National de la Recherche Scientifique (CNRS), UPR3079 CEMHTI, Université d'Orléans, 1D Av. Recherche Scientifique, CEDEX 2, Orléans, 45071, France
Heymans, Nicolas ; Université de Mons - UMONS > Faculté Polytechnique > Service de Thermodynamique, Physique mathématiques
Daturi, Marco; Normandie Université, ENSICAEN, UNICAEN, CNRS, Laboratoire Catalyse et Spectrochimie, Caen, 14000, France
De weireld, Guy ; Université de Mons - UMONS > Faculté Polytechnique > Service de Thermodynamique, Physique mathématiques
Pinto, Moisés; CERENA, Departamento de Engenharia Química, Instituto Superior Técnico, Universidade de Lisboa, Lisboa, 1049-001, Portugal
Nouar, Farid; Institut des Matériaux Poreux de Paris, Ecole Normale Supérieure, ESPCI Paris, CNRS, PSL University, Paris, 75005, France
Maurin, Guillaume; ICGM, Univ. Montpellier, CNRS, ENSCM, Montpellier, 34293, France
Mouchaham, Georges ; Institut des Matériaux Poreux de Paris, Ecole Normale Supérieure, ESPCI Paris, CNRS, PSL University, Paris, 75005, France
Serre, Christian; Institut des Matériaux Poreux de Paris, Ecole Normale Supérieure, ESPCI Paris, CNRS, PSL University, Paris, 75005, France
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