Green Synthesis and Enhanced CO2 Capture Performance of Perfluorinated Cerium-Based Metal-Organic Frameworks with UiO-66 and MIL-140 Topology

2018 ◽  
Author(s):  
Roberto D’Amato ◽  
Anna Donnadio ◽  
Mariolino Carta ◽  
Claudio Sangregorio ◽  
Riccardo Vivani ◽  
...  
Keyword(s):  
Photoelectron Spectroscopy ◽  
Metal Organic Frameworks ◽  
Isosteric Heat ◽  
Experimental Conditions ◽  
Cerium Ammonium Nitrate ◽  
Ideal Adsorbed Solution Theory ◽  
Metal Organic ◽  
Adsorbed Solution ◽  
Better Than ◽  
The Ideal

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<sub>2</sub> 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<sub>2</sub> over N<sub>2</sub>: 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, amongst the highest ever reported for metal-organic frameworks. The calculated isosteric heat of CO<sub>2 </sub>adsorption is in the range of 38-40 kJ mol<sup>-1</sup>, indicating a strong physisorptive character.

scholarly journals Water-based Synthesis and Enhanced CO2 Capture Performance of Perfluorinated Cerium-Based Metal-Organic Frameworks with UiO-66 and MIL-140 Topology

2018 ◽  
Author(s):  
Roberto D’Amato ◽  
Anna Donnadio ◽  
Mariolino Carta ◽  
Claudio Sangregorio ◽  
Riccardo Vivani ◽  
...  
Keyword(s):  
Photoelectron Spectroscopy ◽  
Metal Organic Frameworks ◽  
Isosteric Heat ◽  
Experimental Conditions ◽  
Cerium Ammonium Nitrate ◽  
Ideal Adsorbed Solution Theory ◽  
Metal Organic ◽  
Adsorbed Solution ◽  
Better Than ◽  
The Ideal

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<sub>2</sub> 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<sub>2</sub> over N<sub>2</sub>: 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, amongst the highest ever reported for metal-organic frameworks. The calculated isosteric heat of CO<sub>2 </sub>adsorption is in the range of 38-40 kJ mol<sup>-1</sup>, indicating a strong physisorptive character.

Water-based Synthesis and Enhanced CO2 Capture Performance of Perfluorinated Cerium-Based Metal-Organic Frameworks with UiO-66 and MIL-140 Topology

2018 ◽  
Author(s):  
Roberto D’Amato ◽  
Anna Donnadio ◽  
Mariolino Carta ◽  
Claudio Sangregorio ◽  
Riccardo Vivani ◽  
...  
Keyword(s):  
Photoelectron Spectroscopy ◽  
Metal Organic Frameworks ◽  
Isosteric Heat ◽  
Experimental Conditions ◽  
Cerium Ammonium Nitrate ◽  
Ideal Adsorbed Solution Theory ◽  
Metal Organic ◽  
Adsorbed Solution ◽  
Better Than ◽  
The Ideal

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<sub>2</sub> 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<sub>2</sub> over N<sub>2</sub>: 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, amongst the highest ever reported for metal-organic frameworks. The calculated isosteric heat of CO<sub>2 </sub>adsorption is in the range of 38-40 kJ mol<sup>-1</sup>, indicating a strong physisorptive character.

Single-solute and bisolute sorption of phenol and trichloroethylene from aqueous solution onto modified montmorillonite and application of sorption models

2013 ◽  
Vol 67 (1) ◽  
pp. 152-158 ◽  
Author(s):  
C. D. Wu ◽  
L. Wang ◽  
C. X. Hu ◽  
M. H. He
Keyword(s):  
Cetyltrimethylammonium Bromide ◽  
Langmuir Model ◽  
Solution Theory ◽  
Sorption Behaviour ◽  
Freundlich Model ◽  
Ideal Adsorbed Solution Theory ◽  
Modified Montmorillonite ◽  
Adsorbed Solution ◽  
Better Than ◽  
The Ideal

The single-solute and bisolute sorption behaviour of phenol and trichloroethylene, two organic compounds with different structures, onto cetyltrimethylammonium bromide (CTAB)-montmorillonite was studied. The monolayer Langmuir model (MLM) and empirical Freundlich model (EFM) were applied to the single-solute sorption of phenol or trichloroethylene from water onto monolayer or multilayer CTAB-montmorillonite. The parameters contained in the MLM and EFM were determined for each solute by fitting to the single-solute isotherm data, and subsequently utilized in binary sorption. The extended Langmuir model (ELM) coupled with the single-solute MLM and the ideal adsorbed solution theory (IAST) coupled with the single-solute EFM were used to predict the binary sorption of phenol and trichloroethylene onto CTAB-montmorillonite. It was found that the EFM was better than the MLM at describing single-solute sorption from water onto CTAB-montmorillonite, and the IAST was better than the ELM at describing the binary sorption from water onto CTAB-montmorillonite.

scholarly journals Predicting adsorption selectivities from pure gas isotherms for gas mixtures in metal–organic frameworks

2020 ◽  
Vol 11 (3) ◽  
pp. 643-655 ◽  
Author(s):  
Arpan Kundu ◽  
Kaido Sillar ◽  
Joachim Sauer
Keyword(s):  
Geometric Mean ◽  
Metal Organic Frameworks ◽  
Gas Mixtures ◽  
Mixing Rule ◽  
Lateral Interactions ◽  
Solution Theory ◽  
Ideal Adsorbed Solution Theory ◽  
Metal Organic ◽  
Adsorbed Solution ◽  
Adsorbed Solution Theory

A new mixing rule (geometric mean) is proposed with substantial improvements compared to the widely used ideal adsorbed solution theory for adsorbates with strong lateral interactions.

scholarly journals Role of Electrostatic Effects in the Pure Component and Binary Adsorption of Ethylene and Ethane in Cu-Tricarboxylate Metal-Organic Frameworks

2007 ◽  
Vol 25 (8) ◽  
pp. 607-619 ◽  
Author(s):  
Timothy M. Nicholson ◽  
Suresh K. Bhatia
Keyword(s):  
Selective Adsorption ◽  
Isosteric Heat ◽  
Pure Component ◽  
Solution Theory ◽  
Ideal Adsorbed Solution Theory ◽  
Separation Factors ◽  
Metal Organic ◽  
Adsorbed Solution ◽  
Gcmc Simulations ◽  
Adsorbed Solution Theory

The interaction of ethane and ethylene with a Cu-tricarboxylate complex was investigated, showing that at low loadings the lighter molecule has a higher binding energy as a result of interaction with framework Cu and H-bonding with basic framework oxygen atoms. This leads to the selective adsorption of ethylene at low pressure by a factor of ca. 2. This is overcome by the stronger van der Waals interaction of ethane at high loadings, explaining recent literature data. Both experimental data and single-component Grand Canonical Monte Carlo (GCMC) simulations were fitted well with the Unilan model and mixture isotherms were satisfactorily predicted by the Ideal Adsorbed Solution Theory when compared with binary simulation results. Both binary GCMC simulations and Ideal Adsorbed Solution Theory predictions yielded separation factors of ca. 2 and a difference in isosteric heat of 3 kJ/mol. The results suggest that the Cu-BTC framework offers a possible route for the separation of ethane and ethylene, a Holy Grail of adsorption.

scholarly journals Effective Separation of Prime Olefins from Gas Stream Using Anion Pillared Metal Organic Frameworks: Ideal Adsorbed Solution Theory Studies, Cyclic Application and Stability

Catalysts ◽  
2021 ◽  
Vol 11 (4) ◽  
pp. 510
Author(s):  
Majeda Khraisheh ◽  
Fares. Almomani ◽  
Gavin Walker
Keyword(s):  
Breakthrough Curves ◽  
Isotherm Models ◽  
Regeneration Ability ◽  
Solution Theory ◽  
Experimental Conditions ◽  
Ideal Adsorbed Solution Theory ◽  
Adsorbed Solution ◽  
The Stability ◽  
Adsorption Desorption ◽  
Adsorbed Solution Theory

The separation of C3H4/C3H6 is one of the most energy intensive and challenging operations, requiring up to 100 theoretical stages, in traditional cryogenic distillation. In this investigation, the potential application of two MOFs (SIFSIX-3-Ni and NbOFFIVE-1-Ni) was tested by studying the adsorption–desorption behaviors at a range of operational temperatures (300–360 K) and pressures (1–100 kPa). Dynamic adsorption breakthrough tests were conducted and the stability and regeneration ability of the MOFs were established after eight consecutive cycles. In order to establish the engineering key parameters, the experimental data were fitted to four isotherm models (Langmuir, Freundlich, Sips and Toth) in addition to the estimation of the thermodynamic properties such as the isosteric heats of adsorption. The selectivity of the separation was tested by applying ideal adsorbed solution theory (IAST). The results revealed that SIFSIX-3-Ni is an effective adsorbent for the separation of 10/90 v/v C3H4/C3H6 under the range of experimental conditions used in this study. The maximum adsorption reported for the same combination was 3.2 mmolg−1. Breakthrough curves confirmed the suitability of this material for the separation with a 10-min gab before the lighter C3H4 is eluted from the column. The separated C3H6 was obtained with a 99.98% purity.

scholarly journals Gas Adsorption Selectivity in Topologically Disordered Metal–Organic Frameworks

2021 ◽  
Author(s):  
Adam Sapnik ◽  
Christopher W. Ashling ◽  
Lauren K. Macreadie ◽  
Seok J. Lee ◽  
Tim Johnson ◽  
...  
Keyword(s):  
Gas Adsorption ◽  
Metal Organic Frameworks ◽  
Interaction Strength ◽  
Functional Materials ◽  
Adsorption Selectivity ◽  
Guest Molecules ◽  
Sorption Behaviour ◽  
Ideal Adsorbed Solution Theory ◽  
Industrial Gases ◽  
Metal Organic

<div><p>Disordered metal–organic frameworks are emerging as an attractive class of functional materials, however their applications in gas storage and separation have yet to be fully explored. Here, we investigate gas adsorption in the topologically disordered Fe-BTC framework and its crystalline counterpart, MIL‑100. Despite their similar chemistry and local structure, they exhibit very different sorption behaviour towards a range of industrial gases, noble gases and hydrocarbons. Virial analysis reveals that Fe-BTC has enhanced interaction strength with guest molecules compared to MIL‑100. Most notably, we observe striking discrimination between the adsorption of C<sub>3</sub>H<sub>6</sub> and C<sub>3</sub>H<sub>8</sub> in Fe‑BTC, with over a twofold increase in the amount of C<sub>3</sub>H<sub>6</sub> being adsorbed than C<sub>3</sub>H<sub>8</sub>. Thermodynamic selectivity towards a range of industrially relevant binary mixtures is probed using ideal adsorbed solution theory (IAST). Together, this suggests the disordered material may possess powerful separation capabilities that are rare even amongst crystalline frameworks.</p></div>

scholarly journals Robust algorithms for the solution of the ideal adsorbed solution theory equations

AIChE Journal ◽  
2014 ◽  
Vol 61 (3) ◽  
pp. 981-991 ◽  
Author(s):  
Enzo Mangano ◽  
Daniel Friedrich ◽  
Stefano Brandani
Keyword(s):  
Solution Theory ◽  
Robust Algorithms ◽  
Ideal Adsorbed Solution Theory ◽  
Adsorbed Solution ◽  
The Ideal ◽  
Adsorbed Solution Theory
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