Browsing by Keyword "Hydrogen separation"
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Item Achievements of European projects on membrane reactor for hydrogen production(2017-09-10) Di Marcoberardino, Gioele; Binotti, Marco; Manzolini, Giampaolo; Viviente, José Luis; Arratibel, Alba; Roses, Leonardo; Gallucci, Fausto; TECNOLOGÍA DE MEMBRANAS E INTENSIFICACIÓN DE PROCESOSMembrane reactors for hydrogen production can increase both the hydrogen production efficiency at small scale and the electric efficiency in micro-cogeneration systems when coupled with Polymeric Electrolyte Membrane fuel cells. This paper discusses the achievements of three European projects (FERRET, FluidCELL, BIONICO) which investigate the application of the membrane reactor concept to hydrogen production and micro-cogeneration systems using both natural gas and biofuels (biogas and bio-ethanol) as feedstock. The membranes, used to selectively separate hydrogen from the other reaction products (CH4, CO2, H2O, etc.), are of asymmetric type with a thin layer of Pd alloy (<5 μm), and supported on a ceramic porous material to increase their mechanical stability. In FERRET, the flexibility of the membrane reactor under diverse natural gas quality is validated. The reactor is integrated in a micro-CHP system and achieves a net electric efficiency of about 42% (8% points higher than the reference case). In FluidCELL, the use of bio-ethanol as feedstock for micro-cogeneration Polymeric Electrolyte Membrane based system is investigated in off-grid applications and a net electric efficiency around 40% is obtained (6% higher than the reference case). Finally, BIONICO investigates the hydrogen production from biogas. While BIONICO has just started, FERRET and FluidCELL are in their third year and the two prototypes are close to be tested confirming the potentiality of membrane reactor technology at small scale.Item Attrition-resistant membranes for fluidized-bed membrane reactors: Double-skin membranes: Double-skin membranes(2018-10-01) Arratibel, Alba; Medrano, Jose Antonio; Melendez, Jon; Pacheco Tanaka, D. Alfredo; van Sint Annaland, Martin; Gallucci, Fausto; TECNOLOGÍA DE MEMBRANAS E INTENSIFICACIÓN DE PROCESOS; Tecnalia Research & InnovationPd-Ag supported membranes have been prepared by coating a ceramic interdiffusion barrier onto a Hastelloy X (0.2 µm media grade) porous support followed by deposition of the hydrogen selective Pd-Ag (4–5 µm) layer by electroless plating. To one of the membranes an additional porous Al2O3-YSZ layer (protective layer with 50 wt% of YSZ) was deposited by dip-coating followed by calcination at 550 °C on top of the Pd-Ag layer, and this membrane is referred to as a double-skin membrane. Both membranes were integrated at the same time in a single reactor in order to assess and compare the performance of both membranes under identical conditions. The membranes have first been tested in an empty reactor with pure gases (H2 and N2) and afterwards in the presence of a catalyst (rhodium onto promoted alumina) fluidized in the bubbling regime. The membranes immersed in the bubbling bed were tested at 400 °C and 500 °C for 115 and 500 h, respectively. The effect of the protective layer on the permeation properties and stability of the membranes were studied. The double-skinned membraned showed a H2 permeance of 1.55·10−6 mol m−2 s−1 Pa−1 at 500 °C and 4 bar of pressure difference with an ideal perm-selectivity virtually infinite before incorporation of particles. This selectivity did not decay during the long term test under fluidization with catalyst particles.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 Development of Pd-based double-skinned membranes for hydrogen production in fluidized bed membrane reactors(2018-03-15) Arratibel, Alba; Pacheco Tanaka, Alfredo; Laso, Iker; van Sint Annaland, Martin; Gallucci, Fausto; TECNOLOGÍA DE MEMBRANAS E INTENSIFICACIÓN DE PROCESOSThis paper reports the preparation and performance characterization of new PdAg supported membranes with a porous protecting layer to protect the membrane surface from particles in a fluidized bed membrane reactor. Supported membranes with a selective layer of 1 µm and a protective layer have been prepared. Outstanding H2 permeance (5·10−6 mol m−2 s−1 Pa−1) and H2/N2 perm-selectivity (over 25,000) were measured at 400 °C and 1 bar of pressure difference. One membrane has been tested for more than 750 h in the presence of fluidized glass beads showing a decay in the perm-selectivity to approximately 5000, mainly due to sealing leakage. However, the protective layer was removed during this long-term test. Another membrane has been tested for more than 2000 h in a fluidized bed membrane reactor with a Rh reforming catalyst supported on promoted alumina in the bubbling fluidization regime. During tests with binary mixtures mass transfer limitations toward the membrane were observed due to large H2 permeance of the membranes.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 H2 production via ammonia decomposition in a catalytic membrane reactor(2021-06-01) Cechetto, Valentina; Di Felice, Luca; Medrano, Jose A.; Makhloufi, Camel; Zuniga, Jon; Gallucci, Fausto; TECNOLOGÍA DE MEMBRANAS E INTENSIFICACIÓN DE PROCESOSThe membrane reactor is proposed in this work as a system with high potential to efficiently recover the hydrogen (H2) stored in ammonia (NH3), which has been recently proposed as an alternative for H2 storage. With this technology, NH3 decomposition and high-purity H2 separation are simultaneously performed within the same unit, and high H2 separation efficiency is achieved at lower temperature compared to conventional systems, leading to energetic and economic benefits. NH3 decomposition was experimentally performed in a Pd-based membrane reactor over a Ru-based catalyst and the performance of the conventional packed bed reactor were used as benchmark for a comparison. The results demonstrate that the introduction of a membrane in a conventional reactor enhances its performance and allows to achieve conversion higher than the thermodynamic equilibrium conversion for sufficiently high temperatures. For temperatures from and above 425 °C, full NH3 conversion was achieved and more than 86% of H2 fed to the system as ammonia was recovered with a purity of 99.998%. The application of vacuum at the membrane permeate side leads to higher H2 recovery and NH3 conversions beyond thermodynamic restrictions. On the other hand, the reactor feed flow rate and operating pressure have not shown major impacts on NH3 conversion.Item Hydrogen permeation studies of composite supported alumina-carbon molecular sieves membranes: Separation of diluted hydrogen from mixtures with methane: Separation of diluted hydrogen from mixtures with methane(2021-05-28) Llosa Tanco, Margot A.; Medrano, Jose A.; Cechetto, Valentina; Gallucci, Fausto; Pacheco Tanaka, David A.; TECNOLOGÍA DE MEMBRANAS E INTENSIFICACIÓN DE PROCESOSOne alternative for the storage and transport of hydrogen is blending a low amount of hydrogen (up to 15 or 20%) into existing natural gas grids. When demanded, hydrogen can be then separated, close to the end users using membranes. In this work, composite alumina carbon molecular sieves membranes (Al-CMSM) supported on tubular porous alumina have been prepared and characterized. Single gas permeation studies showed that the H2/CH4 separation properties at 30 °C are well above the Robeson limit of polymeric membranes. H2 permeation studies of the H2–CH4 mixture gases, containing 5–20% of H2 show that the H2 purity depends on the H2 content in the feed and the operating temperature. In the best scenario investigated in this work, for samples containing 10% of H2 with an inlet pressure of 7.5 bar and permeated pressure of 0.01 bar at 30 °C, the H2 purity obtained was 99.4%.Item Techno-economic evaluation on a hybrid technology for low hydrogen concentration separation and purification from natural gas grid(2021-07-01) Nordio, Maria; Wassie, Solomon Assefa; Van Sint Annaland, Martin; Pacheco Tanaka, D. Alfredo; Viviente Sole, José Luis; Gallucci, Fausto; Tecnalia Research & Innovation; TECNOLOGÍA DE MEMBRANAS E INTENSIFICACIÓN DE PROCESOSHydrogen can be stored and distributed by injecting into existing natural grids, then, at the user site separated and used in different applications. The conventional technology for hydrogen separation is pressure swing adsorption (PSA). The recent NREL study showed the extraction cost for separating hydrogen from a 10% H2 stream with a recovery of 80% is around 3.3–8.3 US$/kg. In this document, new system configurations for low hydrogen concentration separation from the natural gas grid by combining novel membrane-based hybrid technologies will be described in detail. The focus of the manuscript will be on the description of different configurations for the direct hydrogen separation, which comprises a membrane module, a vacuum pump and an electrochemical hydrogen compressor. These technological combinations bring substantial synergy effect of one-another while improving the total hydrogen recovery, purity and total cost of hydrogen. Simulation has been carried out for 17 different configurations; according to the results, a configuration of two-stage membrane modules (in series) with a vacuum pump and an electrochemical hydrogen compressor (EHC) shows highest hydrogen purity (99.9997%) for 25 kg/day of hydrogen production for low-pressure grid. However, this configuration shows a higher electric consumption (configuration B) due to the additional mechanical compressor between the two-stage membrane modules and the EHC. Whereas, when the compressor is excluded, and a double skin Pd membrane (PdDS) module is used in a single-stage while connected to a vacuum pump (configuration A5), the hydrogen purity (99.92%) slightly decreases yet the power consumption considerably improves (1.53 times lower). Besides to these two complementary configurations, the combination of a single membrane module, a vacuum pump and the electrochemical compressor has been also carried out (configuration A) and results show that relatively higher purity can be achieved. Based on four master configurations, this document presents a different novel hybrid system by integrating two to three technologies for hydrogen purification combined in a way that enhances the strengths of each of them.Item Ultra-pure hydrogen production via ammonia decomposition in a catalytic membrane reactor(2022-06-08) Cechetto, Valentina; Di Felice, Luca; Gutierrez Martinez, Rocio; Arratibel Plazaola, Alba; Gallucci, Fausto; Tecnalia Research & Innovation; TECNOLOGÍA DE MEMBRANAS E INTENSIFICACIÓN DE PROCESOSIn this work two alternatives are presented for increasing the purity of hydrogen produced in a membrane reactor for ammonia decomposition. It is experimentally demonstrated that either increasing the thickness of the membrane selective layer or using a small purification unit in the permeate of the membranes, ultra-pure hydrogen can be produced. Specifically, the results show that increasing the membrane thickness above 6 μm ultra-pure hydrogen can be obtained at pressures below 5 bar. A cheaper solution, however, consists in the use of an adsorption bed downstream the membrane reactor. In this way, ultra-pure hydrogen can be achieved with higher reactor pressures, lower temperatures and thinner membranes, which result in lower reactor costs. A possible process diagram is also reported showing that the regeneration of the adsorption bed can be done by exploiting the heat available in the system and thus introducing no additional heat sources.Item Unravelling the transport mechanism of pore-filled membranes for hydrogen separation(2018-09-12) Arratibel, Alba; Pacheco Tanaka, David A.; Slater, Thomas J.A.; Burnett, Timothy L.; van Sint Annaland, Martin; Gallucci, Fausto; TECNOLOGÍA DE MEMBRANAS E INTENSIFICACIÓN DE PROCESOSThe permeation characteristics of palladium pore filled (PF) membranes have been investigated with gas permeation and structural characterization of the membranes. PF membranes have been prepared by filling with Pd the nanoporous γ-Al2O3/YSZ (or pure YSZ) layer supported onto porous α-Al2O3 and ZrO2. The number of nanoporous layers and the applied vacuum level during the electroless plating process have been studied. Gas permeation properties of the PF membranes have been determined in a temperature range of 300-550 °C. The measured hydrogen permeances have been found to be lower than previously reported for similar membranes. It has been found that the hydrogen fluxes do not depend on the thickness of the nanoporous layers (γ-Al2O3/YSZ or pure YSZ) or on the vacuum pump employed for filling with Pd. The physicochemical characterization performed showed that the palladium deposited does not form a percolated network across the mesoporous layer(s), leading to low hydrogen permeances and thus low H2/N2 perm-selectivities.