TY - JOUR
T1 - Water-Based Synthesis and Enhanced CO 2 Capture Performance of Perfluorinated Cerium-Based Metal-Organic Frameworks with UiO-66 and MIL-140 Topology
AU - D'Amato, Roberto
AU - Donnadio, Anna
AU - Carta, Mariolino
AU - Sangregorio, Claudio
AU - Tiana, Davide
AU - Vivani, Riccardo
AU - Taddei, Marco
AU - Costantino, Ferdinando
N1 - Publisher Copyright:
Copyright © 2018 American Chemical Society.
PY - 2019/1/7
Y1 - 2019/1/7
N2 - Reaction of cerium ammonium nitrate and tetrafluoroterephthalic acid in water afforded two new metal-organic frameworks with UiO-66 [F4-UiO-66(Ce)] and MIL-140 [F4-MIL-140A(Ce)] topologies. The two compounds can be obtained in the same experimental conditions, just by varying the amount of acetic acid used as crystallization modulator in the synthesis. Both F4-UiO-66(Ce) and F4-MIL-140A(Ce) feature pores with size <8 Å, which classifies them as ultramicroporous. Combination of X-ray photoelectron spectroscopy and magnetic susceptibility measurements revealed that both compounds contain a small amount of Ce(III), which is preferentially accumulated near the surface of the crystallites. The CO 2 sorption properties of F4-UiO-66(Ce) and F4-MIL-140A(Ce) were investigated, finding that they perform better than their Zr-based analogues. F4-MIL-140A(Ce) displays an unusual S-shaped isotherm with steep uptake increase at pressure <0.2 bar at 298 K. This makes F4-MIL-140A(Ce) exceptionally selective for CO 2 over N 2 : the calculated selectivity, according to the ideal adsorbed solution theory for a 0.15:0.85 mixture at 1 bar and 293 K, is higher than 1900, among the highest ever reported for metal-organic frameworks. The calculated isosteric heat of CO 2 adsorption is in the range of 38-40 kJ mol -1 , indicating a strong physisorptive character.
AB - Reaction of cerium ammonium nitrate and tetrafluoroterephthalic acid in water afforded two new metal-organic frameworks with UiO-66 [F4-UiO-66(Ce)] and MIL-140 [F4-MIL-140A(Ce)] topologies. The two compounds can be obtained in the same experimental conditions, just by varying the amount of acetic acid used as crystallization modulator in the synthesis. Both F4-UiO-66(Ce) and F4-MIL-140A(Ce) feature pores with size <8 Å, which classifies them as ultramicroporous. Combination of X-ray photoelectron spectroscopy and magnetic susceptibility measurements revealed that both compounds contain a small amount of Ce(III), which is preferentially accumulated near the surface of the crystallites. The CO 2 sorption properties of F4-UiO-66(Ce) and F4-MIL-140A(Ce) were investigated, finding that they perform better than their Zr-based analogues. F4-MIL-140A(Ce) displays an unusual S-shaped isotherm with steep uptake increase at pressure <0.2 bar at 298 K. This makes F4-MIL-140A(Ce) exceptionally selective for CO 2 over N 2 : the calculated selectivity, according to the ideal adsorbed solution theory for a 0.15:0.85 mixture at 1 bar and 293 K, is higher than 1900, among the highest ever reported for metal-organic frameworks. The calculated isosteric heat of CO 2 adsorption is in the range of 38-40 kJ mol -1 , indicating a strong physisorptive character.
KW - Carbon dioxide capture
KW - Gas separations
KW - Green synthesis
KW - Metal-organic frameworks
KW - Porous materials
UR - https://www.scopus.com/pages/publications/85059667369
U2 - 10.1021/acssuschemeng.8b03765
DO - 10.1021/acssuschemeng.8b03765
M3 - Article
AN - SCOPUS:85059667369
SN - 2168-0485
VL - 7
SP - 394
EP - 402
JO - ACS Sustainable Chemistry and Engineering
JF - ACS Sustainable Chemistry and Engineering
IS - 1
ER -
