Percorrer por autor "Serre, Christian"
A mostrar 1 - 10 de 21
Resultados por página
Opções de ordenação
- Adsorption and dynamics of linear and mono-branched hexane isomers in MIL-140 metal-organic frameworksPublication . Zhao, Hengli; Silva, José A.C.; Henrique, Adriano; Nouar, Farid; Serre, Christian; Maurin, Guillaume; Ghoufi, AzizRecent breakthrough experiments revealed the iso-reticular Zr-MOFs, MIL-140B and MIL-140C, as promising sorbents for the separation of C6 isomers. Interestingly while the ultra-small pore MIL-140B exhibited hexane isomer sorption hierarchy according to the normal boiling point order (n-C6 > 3MP (3-methyl pentane)), an uncommon shift in the elution order was observed in the larger pore MIL-140C. It was only speculated that the flexibility of the MOFs might be the origin of this intriguing behavior. Herein, flexible force field hybrid osmotic Monte Carlo combined with molecular dynamics simulations were carried out to unravel the microscopic mechanism of the adsorption and dynamics of both C6 isomers in MIL140B and MIL140C. Thermodynamically preferred adsorption of n-C6 over 3MP was predicted for MIL-140B and to a slightly less extent for MIL-140C. Interestingly while the mobility of n-C6 was found to remain higher than that of 3MP in the whole range of loading for MIL-140B, 3MP becomes more mobile than n-C6 at saturation in MIL-140C. This suggests that this kinetics order is most probably the origin of the inversion of the elution order observed experimentally for MIL-140C. The translational and rotational dynamics of the two guests in MIL-140B and MIL-140C was further understood in-depth.
- Biogas upgrading using shaped MOF MIL-160(Al) by pressure swing adsorption process: Experimental and dynamic modelling assessmentPublication . Karimi, Mohsen; Siqueira, Rafael M.; Rodrigues, Alírio; Nouar, Farid; Silva, José A.C.; Serre, Christian; Ferreira, AlexandreBiogas has been introduced as a sustainable source of energy, which is considered as a promising alternative for conventional fossil fuels. Indeed, biogas requires to be upgraded from the impurities, specifically, carbon dioxide to be commercially utilized. In this study, the potential of shaped form MIL-160(Al) as a water stable Al dicarboxylate microporous MOF has been assessed concerning the biogas upgrading application. To this end, firstly, the dynamic fixed-bed adsorption of carbon dioxide and methane was investigated at 313 K and 4.0 bar. The measured breakthrough outcomes were simulated with a developed mathematical model, which the results confirmed an acceptable potential of model predictions. Afterwards, a pressure swing adsorption (PSA) process with 5-steps was designed relying on dynamic equilibrium results, and experimentally validated by a lab-scale PSA set-up for a 50:50 CO2/CH4 mixture. Finally, an industrial PSA process was designed to have a precise knowledge on the potential of MIL-160(Al) for biogas upgrading for large scale applications. The results demonstrated the purity and recovery of methane around 99 % and 63 %, respectively, which indicated the appealing capacity of this adsorbent for such a purpose.
- A complete separation of hexane isomers by a functionalized flexible metal organic frameworkPublication . Mendes, Patrícia A.P.; Horcajada, Patricia; Rives, Sébastien; Ren, Hong; Rodrigues, Alírio; Devic, Thomas; Magnier, Emmanuel; Trens, Philippe; Jobic, Hervé; Ollivier, Jacques; Maurin, Guillaume; Serre, Christian; Silva, José A.C.The separation ability of branched alkane isomers (nHEX, 3MP, 22DMB) of the flexible and functionalized microporous iron(III) dicarboxylate MIL-53(Fe)-(CF3)2 solid is evaluated through a combination of breakthrough experiments (binary or ternary mixtures), adsorption isotherms, X-ray diffraction temperature analysis, quasi-elastic neutron scattering measurements and molecular dynamics simulations. A kinetically controlled molecular sieve separation between the di-branched isomer of hexane 22DMB from a mixture of paraffins is achieved. The reported total separation between mono- and di-branched alkanes which was neither predicted nor observed so far in any class of porous solids is spectacular and paves the way towards a potential unprecedented upgrading of the RON of gasoline.
- Developing pressure swing adsorption process for biogas upgrading using shaped MIL-160(Al)Publication . Karimi, Mohsen; Rodrigues, Alírio; Ferreira, Alexandre; Nouar, Farid; Cho, Kyung Ho; Lee, Hwang; Serre, Christian; Silva, José A.C.In this study, regarding the increasing interest on renewable sources of energy as well as considering the challenges of climate changes, the potential of shaped MOF MIL-160 (Al) for biogas upgrading has been evaluated. Accordingly, firstly the breakthrough assessments of CO2 and CH4 adsorption onto this sorbents were studied. Afterwards, a pressure swing adsorption (PSA) process to this end was designed and developed. The results showed MIL-160(Al) has an excellent potential for biogas upgrading concerning CO2 and CH4 separation.
- Functionalization of metal-organic frameworks for hexane isomers separationPublication . Mendes, Patricia; Rodrigues, Alírio; Ragon, Florence; Horcajada, Patricia; Serre, Christian; Silva, José A.C.This work shows the effect of incorporating three different organic ligands (NH2-H2BDC, NO2-H2BDC and Br-H2BDC) into UIO-66(Zr) framework viewing the separation of hexane isomers(22DMB, 23DMB, 3MP and nHEX).
- Hexane isomers separation on an isoreticular series of microporous Zr carboxylate metal organic frameworksPublication . Henrique, Adriano; Maity, Tanmoy; Zhao, Hengli; Brântuas, Pedro; Rodrigues, Alírio; Nouar, Farid; Ghoufi, Aziz; Maurin, Guillaume; Silva, José A.C.; Serre, ChristianA series of isoreticular Zr carboxylate MOFs, MIL-140A, B and C, exhibiting 1D microporous triangular shaped channels and based on different aromatic dicarboxylate ligands (1,4-BDC, 2,6-NDC and 4,4′-BPDC, respectively), were investigated by chromatographic breakthrough experiments regarding their ability to separate hexane isomers (nC6/2MP/3MP/23DMB/22DMB). Both single and equimolar multicomponent experiments were performed at the temperatures 343, 373, and 423 K and a total hydrocarbon pressure up to 50.0 kPa using the MIL-140B form. The elution order is similar to that of the normal boiling point of the compounds nC6 > 2MP > 3MP > 23DMB > 22DMB. It is noteworthy that this material enables separation of the hexane isomers by class, linear > mono-branched > di-branched, with a selectivity (linear + mono-branched isomers/di-branched isomers) up to 10 at 343 K, decreasing, however, as the temperature increases. Grand canonical Monte Carlo simulations were further performed to gain insight into the adsorption/separation mechanisms, highlighting the crucial need to consider a tiny tilting of the organic linkers for capturing the experimental observations. The impact of the pore size was finally assessed through the comparison with MIL-140A and MIL-140C, respectively, based on multicomponent experiments at 343 K. We evidenced a significant decrease of the selectivity (about 2) in both cases while the loadings were decreased or increased for MIL-140A and MIL-140C, respectively. Additionally, MIL-140C was demonstrated to exhibit an uncommon shift in the elution order occurring between nC6 and 3MP, 3MP being the last compound to saturate in the column.
- Hexane isomers sorption on a functionalized metal-organic frameworkPublication . Silva, José A.C.; Mendes, Patricia; Ragon, Florence; Rodrigues, Alírio; Horcajada, Patricia; Serre, ChristianA series of functionalized porous Zr terephthalate MOFs of the UiO-66(Zr) structure type bearing either Br, NH2 or NO2 groups have been synthesized at the multi-gram scale through an atmospheric pressure solvothermal route with the final aim of investigating the influence of functionalization on the separation of hexane isomers (22DMB, 23DMB, 3MP and nHEX). The studies performed in a fixed bed adsorption column with equimolar mixtures at temperatures between 343 and 423 K and partial pressure up to 10 kPa have shown that the Br, NO2 and NH3 forms exhibit an uptake reaching 15%, being the sorption selectivity hierarchy on the whole comparable to the bared UiO-66 solid: 22DMB approximate to 23DMB >> 3MP nHEX. The 22DMB/nHEX selectivity reaches approximately three at low uptake while the 22DMB/3MP selectivity of UiO-66_NO2 is nearly constant (1.3).
- A microporous multi‐cage metal–organic framework for an effective one‐step separation of branched alkanes feedsPublication . Zhou, Lin; Brântuas, Pedro; Henrique, Adriano; Reinsch, Helge; Wahiduzzaman, Mohammad; Grenèche, Jean‐Marc; Rodrigues, Alírio; Silva, José A.C.; Maurin, Guillaume; Serre, ChristianThe improvement of the Total Isomerization Process (TIP) for the production of high-quality gasoline with the ultimate goal of reaching a Research Octane Number (RON) higher than 92 requires the use of specific sorbents to separate pentane and hexane isomers into classes of linear, mono- and di-branched isomers. Herein we report the design of a new multi-cage microporous Fe(III)-MOF (referred to as MIP-214, MIP stands for materials of the Institute of Porous Materials of Paris) with a flu-e topology, incorporating an asymmetric heterofunctional ditopic ligand, 4-pyrazolecarboxylic acid, that exhibits an appropriate microporous structure for a thermodynamic-controlled separation of hydrocarbon isomers. This MOF produced via a direct, scalable, and mild synthesis route was proven to encompass a unique separation of C5/C6 isomers by classes of low RON over high RON alkanes with a sorption hierarchy: (n-hexane >> n-pentane approximate to 2-methylpentane>3-methylpentane)(low RON)>>(2,3-dimethylbutane approximate to i-pentane approximate to 2,2-dimethylbutane)(high RON) following the adsorption enthalpy sequence. We reveal for the first time that a single sorbent can efficiently separate such a complex mixture of high RON di-branched hexane and mono-branched pentane isomers from their low RON counterparts, which is a major achievement reported so far.
- MIL-160(Al) as a candidate for biogas upgrading and CO2 capture by adsorption processesPublication . Karimi, Mohsen; Ferreira, Alexandre; Rodrigues, Alírio; Nouar, Farid; Serre, Christian; Silva, José A.C.The microporous bioderived Al dicarboxylate MIL-160(Al) MOF in its shaped form has been evaluated as a candidate for biogas upgrading (BU) and/or carbon capture and storage (CCS) by studying adsorption isotherms of CO2, CH4, and N2 at 313, 343, and 373 K until 8 bar. The isotherms disclosed the following loading capacities: 4.2 (CO2), 2.07 (CH4), and 0.69 (N2) mol/kg at 5.8 bar and 313 K, which fitted with the dual-site Langmuir model. The linear-driving-force coefficients (LDFs) for CO2 and CH4 calculated from uptake rate experiments are in the order of 0.021-0.096 and 0.041-0.165 s-1 at 313 K between 0.11 and 2.76 bar, respectively. The Response Surface Methodology (RSM) was also applied to maximize the selectivity for mixtures CO2/CH4 and CO2/N2 with interest for BU or CCS. Breakthrough curve experiments with mixtures CO2/CH4 and CO2/N2 at the optimum selectivity conditions were developed and simulated using ASPEN Adsorption. This work clearly demonstrates the potential of MIL-160(Al) to be used in BU and/or CCS-related applications.
- Multicomponent hexane isomers sorption on MOF ZIF-8Publication . Mendes, Patricia; Silva, José A.C.; Rodrigues, Alírio; Horcajada, Patricia; Serre, ChristianThe main goal of this research focuses on the development of an adsorptive process to separate hexane isomers (kinetic diameter very similar) in order to improve the quality of gasoline measured by the octane number (RON). In this investigation, studies of sorption equilibrium of hexane isomers: n-hexane (RON 25), 3-methylpentane (RON 75), 2,3-dimethylbutane (RON 103) and 2,2-dimethylbutane (RON 94) were performed on ZIF-8. The MOF ZIF-8 was synthesized and fully characterized by XRD, TGA, IR and surface area at the Institute Lavoisier Versailles.
- «
- 1 (current)
- 2
- 3
- »