Browsing by Author "Nouar, Farid"
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- 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.
- 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.
- 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.
- 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.
- Separation of branched alkanes feeds by a synergistic action of zeolite and metal-organic frameworkPublication . Brântuas, Pedro; Henrique, Adriano; Wahiduzzaman, Mohammad; Wedelstedt, Alexander von; Maity, Tanmoy; Rodrigues, Alírio; Nouar, Farid; Lee, U-Hwang; Cho, Kyung Ho; Silva, José A.C.; Serre, Christian; Maurin, GuillaumeZeolites and metal-organic frameworks (MOFs) are considered as “competitors” for new separation processes. The production of high-quality gasoline is currently achieved through the total isomerization process that separates pentane and hexane isomers while not reaching the ultimate goal of a research octane number (RON) higher than 92. This work demonstrates how a synergistic action of the zeolite 5A and the MIL-160(Al) MOF leads to a novel adsorptive process for octane upgrading of gasoline through an efficient separation of isomers. This innovative mixed-bed adsorbent strategy encompasses a thermodynamically driven separation of hexane isomers according to the degree of branching by MIL-160(Al) coupled to a steric rejection of linear isomers by the molecular sieve zeolite 5A. Their adsorptive separation ability is further evaluated under real conditions by sorption breakthrough and continuous cyclic experiments with a mixed bed of shaped adsorbents. Remarkably, at the industrially relevant temperature of 423 K, an ideal sorption hierarchy of low RON over high RON alkanes is achieved, i.e., n-hexane ≫n-pentane ≫2-methylpentane > 3-methylpentane⋙ 2,3-dimethylbutane > isopentane ≈ 2,2-dimethylbutane, together with a productivity of 1.14 mol dm−3 and a high RON of 92, which is a leap-forward compared with existing processes.
- Separation of CO2/N2 mixture by pressure swing adsorption process using shaped MI-160(Al) for CO2 post-combustion capturePublication . Karimi, Mohsen; Rodrigues, Alírio; Ferreira, Alexandre; Nouar, Farid; Cho, Kyung Ho; Lee, Hwang; Serre, Christian; Silva, José A.C.Breakthrough experiments were properly simulated with ASPEN ADSIM. Cyclic steady state were developed after 10 cycles. Shaped MOF MIL-160(Al) showed and excellent capacity for Post-combustion CO2 Capture. Life cycle assessment (LCA) of MIL-160 for Postcombustion CO2 Capture can be considered as a future direction.
- Separation of CO2/N2 onto Shaped MOF MIL-160(Al) Using the Pressure Swing Adsorption Process for Post-combustion ApplicationPublication . Karimi, Mohsen; Siqueira, Rafael M.; Rodrigues, Alírio; Nouar, Farid; Silva, José A.C.; Serre, Christian; Ferreira, Alexandre F.P.Adsorption processes have already been considered as an appealing technology for carbon capture and climate change mitigation. Accordingly, this work investigated the capacity of shaped MIL-160(Al) as a water stable bioderived Al dicarboxylate microporous metal-organic framework for separation of carbon dioxide and nitrogen concerning postcombustion application. First, breakthrough experiments of carbon dioxide and nitrogen were accomplished at 313 K and 4.0 bar. Then, a set of equations/relations were considered to model the dynamic fixed-bed tests, in which the outcomes proved the capacity of the developed model for such a purpose. Next, a pressure swing adsorption (PSA) process with five steps, including pressurization, feed, rinse, blowdown, and purge, was planned and validated using performed experiments in a laboratory-scale PSA setup. In the end, an industrial PSA process was designed to attain a better grasp of the capacity of MIL-160(Al) for postcombustion application. The results indicated an exciting potential of this adsorbent for postcombustion carbon capture, with the purity and recovery of carbon dioxide around 67.3 and 99.1%, respectively.
- Separation performance of shaped MOF MIL-160(AL) for double applications of pre and post combustion carbon capturePublication . Karimi, Mohsen; Ferreira, Alexandre; Rodrigues, Alírio; Nouar, Farid; Cho, Kyung Ho; Lee, Hwang; Serre, Christian; Silva, José A.C.The world currently faces the dual challenges: climate changes caused by global warming and a high energy demand regarding the exponential population expansion and industrial development [1, 2]. Carbon dioxide, methane, nitrogen oxide and halogenated components are the main anthropogenic greenhouse gases (GHGs) [1]. The challenge of reducing GHGs emission can be overcome by successful developing post-combustion CO2 capture also advancing the green and renewable sources of energy including biogas [3]. Nevertheless, the main drawback concerning the biogas is its high content on carbon dioxide (it might be as high as 40% or more), which significantly reduces its heating capacity. Therefore, for biogas applications, a previous separation step is required to reduce the CO2 content [2,3]. Among the different methodologies for biogas upgrading and postcombustion CO2 capture, adsorption is among the most attractive ones