Browsing by Keyword "Carbon membranes"
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Item Carbon molecular sieve membranes for selective CO2 separation at elevated temperatures and pressures(2023-02) Rahimalimamaghani, A.; Godini, H.R.; Mboussi, M.; Pacheco Tanaka, A.; Llosa Tanco, M.; Gallucci, F.; TECNOLOGÍA DE MEMBRANAS E INTENSIFICACIÓN DE PROCESOSThe use of Carbon Molecular Sieve Membranes (CMSM) for selective CO2 separation from post-combustion CO2-rich streams from steel plant was experimentally evaluated and reported in this paper. Efficient CMSMs were developed for such application and their promising potentials in operating at elevated temperatures and pressures were experimentally demonstrated. The best performance in terms of flux as well as perm-selectivity, above the Robeson upper bound, was obtained using a CMSM developed with ethylenediamine in the dip-coating stage of the fabrication. In fact, adding ethylenediamine was proven to be particularly important in narrowing down the pore size distribution to ultra-micropore and establishing effective CO2 adsorption site over the membrane surface and the pores wall. It was shown that using a tailored CMSM with a precursor synthesized by co-polymerization of ethylenediamine with Novolac can improve the CO2/N2 ideal perm-selectivity from 33 to 97 at operational conditions of 200 °C and 20 bar.Item Composite-alumina-carbon molecular sieve membranes prepared from novolac resin and boehmite. Part I: Preparation, characterization and gas permeation studies(2015-05-04) Llosa Tanco, Margot A.; Pacheco Tanaka, David A.; Rodrigues, Sandra C.; Texeira, Miguel; Mendes, Adélio; TECNOLOGÍA DE MEMBRANAS E INTENSIFICACIÓN DE PROCESOSAbstract Supported composite alumina-carbon molecular sieve membranes (c-CMSM) were prepared from in house prepared novolac phenolic resin loaded with boehmite nanoparticles in a single dipping-drying-carbonization step. A porous α-alumina tube support was dipped into a N-methyl-2-pyrrolidone solution containing polymerized novolac resin loaded with boehmite, subsequently dried at 100 C and carbonized at 500 C under nitrogen environment. The structure, morphology and performance of the membranes were examined by scanning electron microscopy (SEM), X-ray diffraction (XRD), thermogravimetric analysis (TGA), carbon dioxide adsorption and permeation of N2, O2, He, H2 and CO2. SEM showed carbon membranes with a thin and very uniform layer with a thickness of ca. 3 μm CO2 adsorption isotherms indicated that the produced carbon membranes presented a microporous structure. The c-CMSM exhibited good gas separation properties. The permselectivity surpass the Robeson upper bound for polymeric membranes, especially regarding ideal permselectivities of pairs H2/N2 = 117, and He/O2 = 49. Aging effects were observed after membrane exposure to ambient air. However with a thermal treatment under nitrogen atmosphere the permeance of nitrogen increases.Item Composite-alumina-carbon molecular sieve membranes prepared from novolac resin and boehmite. Part II: Effect of the carbonization temperature on the gas permeation properties(2015-03-02) Llosa Tanco, Margot A.; Pacheco Tanaka, David A.; Mendes, Adélio; TECNOLOGÍA DE MEMBRANAS E INTENSIFICACIÓN DE PROCESOSThe influence of carbonization temperature on the permeation properties and aging of thin (4 μm) supported carbon molecular sieve membranes (c-CMSM), prepared from in house synthesized novolac phenolic resin loaded with boehmite nanoparticles, were studied. Just after membrane carbonization (fresh membrane), high permeance to N2 and O2 and low O2/N2 permselectivities were observed; the highest permeations were observed for carbonization end temperatures between 500 °C and 700 °C. After leaving the c-CMSM 1 day in the air, a large decrease in the permeation and considerable increase in the permselectivity were observed due to the reduction of the pore size by oxygen chemisorption and water physical adsorption; the permeability to H2 and H2/N2 ideal permselectivity for a membrane carbonized at 550 °C are close to palladium membranes for low temperature (<100 °C). The effect of the permeation characteristics of the membranes carbonized at various temperatures and the removal of water adsorbed in the pores by heat treatment were studied.Item Effect of aluminium acetyl acetonate on the hydrogen and nitrogen permeation of carbon molecular sieves membranes(2022-04-15) Rahimalimamaghani, A.; Pacheco Tanaka, D.A.; Llosa Tanco, M.A.; Neira D'Angelo, F.; Gallucci, F.; TECNOLOGÍA DE MEMBRANAS E INTENSIFICACIÓN DE PROCESOSWith a growing interest in hydrogen as energy carrier, the efficient purification of hydrogen from gaseous mixtures is very important. This paper addresses the separation of hydrogen using Carbon Molecular Sieves Membranes (CMSM), which show an attractive combination of high permeability, selectivity and stability. Supported CMSM containing various amounts of aluminium have been prepared from novolac and aluminium acetyl acetonate (Al(acac)3) as carbon and alumina precursors. The thickness of the CMSM layers depend on the content of Al(acac)3 in the dipping solution, which also has influence in the pore size and pore size distribution of the membranes. The permeation properties of the membranes against the Al content in the membrane follows a volcano shape, where the membrane containing 4 wt (%) of Al(acac)3 has the best properties and was stable during 720 h for hydrogen at 150 °C and 6 bar pressure difference. All the CMSM have permeation properties well above the Robeson Upper limit.Item New hydrophilic carbon molecular sieve membranes for bioethanol dehydration via pervaporation(2022-05-01) Rahimalimamaghani, A.; Pacheco Tanaka, D.A.; Llosa Tanco, M.A.; Neira D'Angelo, F.; Gallucci, F.; TECNOLOGÍA DE MEMBRANAS E INTENSIFICACIÓN DE PROCESOSTubular supported carbon molecular sieve membranes (CMSMs) with high hydrophilicity and perm-selectivities for water suitable for ethanol dehydration were developed from a Novolac oligomer phenolic resin as precursor. Alpha alumina supported CMSMs resulted in 1.69 times higher surface roughness than zirconia supports. The higher surface roughness resulted in 48% higher selective layer thickness. According to pervaporation results, water permeance decreased by the increase in selective layer thickness and mole based selectivity of water- ethanol was enhanced. The oligomer with 3982 g/mol molecular weight enabled membrane to reach high selectivity with one-layer coating. Performance of the membranes are compared with literature data in terms of mole-based selectivity vs. water permeance. CMSMs could be a potential substitution for traditional ethanol dehydration methods with offering higher performance and as a result reducing the final price of bioethanol to be used as a sustainable energy source.Item Tailoring pore structure and surface chemistry of microporous Alumina-Carbon Molecular Sieve Membranes (Al-CMSMs) by altering carbonization temperature for optimal gas separation performance: An investigation using low-field NMR relaxation measurements: An investigation using low-field NMR relaxation measurements(2021-11-15) Forster, Luke; D'Agostino, Carmine; Anabell Llosa-Tanco, Margot; Spallina, Vincenzo; Brencio, Camilla; Gallucci, Fausto; Lindley, Matthew; Haigh, Sarah J.; Alfredo Pacheco-Tanaka, David; Tecnalia Research & Innovation; TECNOLOGÍA DE MEMBRANAS E INTENSIFICACIÓN DE PROCESOSIn this work we applied low-field, NMR spin-lattice measurements to evaluate for the first time the effect of carbonization temperature (range 600 - 1000 ℃) on the preparation of Alumina-Carbon Molecular Sieve Membranes (Al-CMSMs), providing new insights into intra-pore fluid interactions. The results show that the average Al-CMSM pore size generally increases with carbonization temperature whilst the hydrophilicity of the pore surface, and the amount of strongly adsorbed H2O, decreases with an increasing carbonization temperature. As such, lower carbonization temperatures produce more hydrophilic membranes, with further evidence provided by FTIR measurements demonstrating the presence of polar functional groups on the surface, with water interacting more strongly with the membrane surface, as evidenced by NMR. It was found that the Al-CMSM carbonization temperature significantly affected permeance and H2O/CH4 permselectivity by altering the membrane pore size distribution and pore hydrophilicity. H2O permeance values are seen to be up to 100 times larger than respective CH4 permeance values. The greater permeance of H2O is attributed to the larger kinetic diameter of CH4 relative to H2O and the adsorption of water in the hydrophilic pores enhancing the adsorption-diffusion transport mechanism. Optimal water permeation temperatures are thus higher for the more hydrophilic membranes, obtained at lower carbonization temperatures, as more energy is required to remove strongly adsorbed water blocking the pores. At higher carbonization temperatures, the Knudsen diffusion mechanism of permeance dominates over the adsorption-diffusion mechanism thereby reducing permeance as diffusion slows due to collisions between gas molecules and the pore walls. CH4 permeation always occurs via Knudsen diffusion with CH4 permeance increasing with permeation temperature due to the increased rate of CH4 diffusion.Item Ultra-Selective CMSMs Derived from Resorcinol-Formaldehyde Resin for CO2 Separation(2022-08-30) Rahimalimamaghani, Arash; Pacheco Tanaka, David Alfredo; Llosa Tanco, Margot A.; Neira D’Angelo, Maria Fernanda; Gallucci, Fausto; Tecnalia Research & Innovation; TECNOLOGÍA DE MEMBRANAS E INTENSIFICACIÓN DE PROCESOSA resorcinol-formaldehyde precursor was synthesized to fabricate the CO2 selective Carbon Molecular Sieve Membranes (CMSMs) developed in this study. The degree of polymerization (DP) was analyzed via Gel Permeation Chromatography (GPC) and its effect on the CO2/N2 perm-selectivity and CO2 permeance was investigated. The membrane that was polymerized at 80 °C (named R80) was selected as the best performing CMSM after a preliminary test. The post treatment with oxidative atmosphere was performed to increase the CO2 permeance and CO2/N2 perm-selectivity on membrane R80. The gas permeation results and Pore Size Distribution (PSD) measurements via perm-porometry resulted in selecting the membrane with an 80 °C polymerization temperature, 100 min of post treatment in 6 bar pressure and 120 °C with an oxygen concentration of 10% (named R80T100) as the optimum for enhancing the performance of CMSMs. The 3D laser confocal microscopy results confirmed the reduction in the surface roughness in post treatment on CMSMs and the optimum timing of 100 min in the treatment. CMSM R80T100 exhibiting CO2/N2 ideal selectivity of 194 at 100 °C with a CO2 permeability of 4718 barrier was performed higher than Robeson’s upper bound limit for polymeric membranes and also the other CMSMs fabricated in this work.Item Upgrading biogas with novel composite carbon molecular sieve (CCMS) membranes: Experimental and techno-economic assessment: Experimental and techno-economic assessment(2020-08-15) Medrano, J.A.; Llosa-Tanco, M.A.; Cechetto, V.; Pacheco-Tanaka, D.A.; Gallucci, F.; TECNOLOGÍA DE MEMBRANAS E INTENSIFICACIÓN DE PROCESOSThe use of biogas as feedstock for hydrogen production was widely proposed in the literature in the last years as a strategy to reduce anthropogenic carbon emissions. However, its lower heating value compared to natural gas hampers the revamping of existing reforming plants. The use of composite carbon molecular sieve membranes for biogas upgrading (CO2 removal from biogas) was investigated experimentally in this work. In particular, ideal perm-selectivities and permeabilities above the Robeson plot for CO2/CH4 mixtures have been obtained. These membranes show better performances compared to polymeric membranes, which are nowadays commercialized for CO2 separation in natural gas streams. Compared to polymeric membranes, carbon membranes do not show deactivation by plasticization when exposed to CO2, and thus can find industrial application. This work was extended with a techno-economic analysis where carbon membranes are installed in a steam methane reforming plant. Results have been first validated with data from literature and show that the use of biogas increases the costs of hydrogen production to a value of 0.25 €/Nm3 compared to the benchmark technology (0.21 €/Nm3). On the other hand, the use of biogas leads to a decrease in carbon emissions up to 95%, thus the use of biogas for hydrogen production is foreseen as a very interesting alternative to conventional technologies in view of the reduction in the carbon footprint in the novel technologies that are to be installed in the near future.Item Vapor/gas separation through carbon molecular sieve membranes: Experimental and theoretical investigation: Experimental and theoretical investigation(2022-03-08) Poto, Serena; Endepoel, Joost G.H.; Llosa-Tanco, Margot Anabell; Pacheco-Tanaka, David Alfredo; Gallucci, Fausto; Neira d’Angelo, M. Fernanda; Tecnalia Research & Innovation; TECNOLOGÍA DE MEMBRANAS E INTENSIFICACIÓN DE PROCESOSThe separation of H2O vapor from (hydrogen-rich) gaseous streams is a topic of increasing interest in the context of CO2 valorisation, where the in situ water removal increases product yield and catalyst stability. In this work, composite alumina carbon molecular sieve membranes (Al-CMSM) were prepared from phenolic resin solutions loaded with hydrophilic boehmite (γ-AlO(OH)) nanosheets (0.4–1.4 wt. % in solution) which partially transform to γ-Al2O3 nanosheets upon thermal decomposition of the resin, improving the hydrophilicity and thus the adsorption-diffusion contribution of the H2O permeation. The γ-Al2O3 nanosheets showed no influence on the pore size distribution of the membranes in the range of micropores, but they increased the membrane hydrophilicity. In addition, the use of boehmite in the resin solution causes an increase in the viscosity and thus an increase in the carbon layers thickness deposited on the porous α-Al2O3 support (from 1 to 3.3 μm). Furthermore, the alumina sheets introduce defects in the carbon matrix, increasing the tortuosity of the active layer, as concluded via phenomenological modelling and parametric fitting of the experimental results. As a consequence, the water permeability exhibits a maximum (1.3ꞏ10−6 molꞏs−1 Pa−1 m−1 at 150 °C) with boehmite/alumina content of ca. 0.8 wt. %, as the combined effects of increasing hydrophilicity (which favour H2O permeability) and increasing thickness and tortuosity (which hamper permeability) upon increasing boehmite loading. Similarly, the H2O/gas perm-selectivity is optimum at 1.2 wt. % boehmite loading. We further investigated the H2O permeation mechanism by modelling the mono- and multi-layer adsorption and capillary condensation of water in microporous media, which result as the main transport mechanisms in the explored conditions.