Browsing by Author "Van Sint Annaland, Martin"
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Item Catalytic membrane reactor for the production of biofuels(2016-06-15) Liuzzi, Dalia; Pérez-Alonso, Francisco José; Fierro, José Luis G.; Rojas, Sergio; Van Wijk, Frank L.; Roghair, Ivo; Van Sint Annaland, Martin; Fernandez, Ekain; Viviente, Jose Luis; Tanaka, D. A.Pacheco; TECNOLOGÍAS DE HIDRÓGENO; TECNOLOGÍA DE MEMBRANAS E INTENSIFICACIÓN DE PROCESOSThe H2-distributed feeding concept using Pd/Ag-based membranes and an Ru-based catalyst in a Packed Bed Membrane Reactor (H2-PBMR) for the synthesis of biofuels via the so-called Fischer-Tropsch Synthesis has been demonstrated. The most successful approach resulted when H2-poor syngas (H2/CO = 1) typically obtained from the gasification of biomass was fed directly through the reaction chamber, i.e., to the catalyst bed, whereas the H2 needed to reach the proper stoichiometry for the FTS (H2/CO = 2) was admitted, and properly distributed, into the catalyst bed through the Pd/Ag-based membrane by flowing H2/He mixtures at the retentate side of the membrane. Under the optimum reaction conditions, the CO conversion measured with the H2-distributed feeding concept is lower than that obtained in a conventional Packed Bed Reactor with H2/CO = 2 (37.9 vs 50.7%), but significantly higher than that obtained in a conventional reactor with H2/CO = 1 (14.1%). Remarkably, the productivity towards high-molecular hydrocarbons increases by almost 70% and the methane production decreases by one order of magnitude when using the H2-distributed feeding concept in a Packed Bed Membrane Reactor.Item Development of thin Pd-Ag supported membranes for fluidized bed membrane reactors including WGS related gases(2015-03-02) Fernandez, Ekain; Helmi, Arash; Coenen, Kai; Melendez, Jon; Viviente, Jose Luis; Pacheco Tanaka, David Alfredo; Van Sint Annaland, Martin; Gallucci, Fausto; TECNOLOGÍAS DE HIDRÓGENO; Tecnalia Research & Innovation; TECNOLOGÍA DE MEMBRANAS E INTENSIFICACIÓN DE PROCESOSThis paper reports the preparation, characterization and stability tests of Pd-based thin membranes for fluidized bed membrane reactor applications. Various thin membranes have been prepared by simultaneous Pd-Ag electroless plating. A simple technique for sealing of the produced membranes is reported and discussed. The membranes have been characterized for single gas permeation, and afterwards used for permeation of mixtures of gases and under fluidization conditions. The membranes have shown very high permeation rates and perm-selectivity when used as permeators. When applied in fluidized bed reactors it has been found that the membranes are stable as long as no interaction between the fluidization catalyst and the membrane surface occurs. For some catalysts a strong chemical interaction between the catalyst and the membrane surface has been observed which caused a drastic decrease in the membrane flux.Item Effect of sweep gas on hydrogen permeation of supported Pd membranes: Experimental and modeling(2019-02-08) Nordio, Maria; Soresi, Serena; Manzolini, Giampaolo; Melendez, Jon; Van Sint Annaland, Martin; Pacheco Tanaka, D. Alfredo; Gallucci, Fausto; Tecnalia Research & Innovation; TECNOLOGÍA DE MEMBRANAS E INTENSIFICACIÓN DE PROCESOSMembrane reactor processes are being increasingly proposed as an attractive solution for pure hydrogen production due to the possibility to integrate production and separation inside a single reactor vessel. High hydrogen purity can be obtained through dense metallic membranes, especially palladium and its alloys, which are highly selective to hydrogen. The use of thin membranes seems to be a good industrial solution in order to increase the hydrogen flux while reducing the cost of materials. Typically, the diffusion through the membrane layer is the rate-limiting step and the hydrogen permeation through the membrane can be described by the Sieverts’ law but, when the membrane becomes thinner, the diffusion through the membrane bulk becomes less determinant and other mass transfer limitations might limit the permeation rate. Another way to increase the hydrogen flux at a given feed pressure, is to increase the driving force of the process by feeding a sweep gas in the permeate side. This effect can however be significantly reduced if mass transfer limitations in the permeate side exist. The aim of this work is to study the mass transfer limitation that occurs in the permeate side in presence of sweep gas. A complete model for the hydrogen permeation through Pd–Ag membranes has been developed, adding the effects of concentration polarization in retentate and permeate side and the presence of the porous support using the dusty gas model equation, which combines Knudsen diffusion, viscous flow and binary diffusion. By studying the influence of the sweep gas it has been observed that the reduction of the driving force is due to the stagnant sweep gas in the support pores while the concentration polarization in the permeate is negligible.Item N2, He and CO2 diffusion mechanism through nanoporous YSZ/γ-Al2O3 layers and their use in a pore-filled membrane for hydrogen membrane reactors(2016-06-01) Arratibel, Alba; Astobieta, Uxue; Pacheco Tanaka, David Alfredo; Van Sint Annaland, Martin; Gallucci, Fausto; TECNOLOGÍA DE MEMBRANAS E INTENSIFICACIÓN DE PROCESOSNanoporous ceramic supports for pore filled membranes were prepared on ceramic supports (α-Al2O3) with pore size of 100 nm by adding additional layers with different proportions of YSZ/γ-Al2O3 (ranging from 50% to 90% of YSZ) by dip-coating and the effect of different parameters in the preparation method have been investigated. The diffusion mechanisms of N2, He and CO2 through the supported nanoporous layers have been studied in detail with permeation measurements at a temperature range of 50-400°C and pressure difference of 30-100 kPa. It was observed that as the amount of γ-Al2O3 in the nanoporous layers increases, the adsorption of CO2 is favored at low temperatures and pressures. Finally, a pore-filled Pd/YSZ/γ-Al2O3 (60 wt%YSZ-40 wt. γ-Al2O3) membrane was successfully prepared and its permeation performance was tested over 900 h at 500 and 550 C, showing relatively low ideal H2/N2 perm-selectivity of about 50 due to low hydrogen flux.Item Pd-based metallic supported membranes: High-temperature stability and fluidized bed reactor testing(2016-06-01) Medrano, Jose Antonio; Fernandez, Ekain; Melendez, Jon; Parco, Maria; Tanaka, David Alfredo Pacheco; Van Sint Annaland, Martin; Gallucci, Fausto; TECNOLOGÍAS DE HIDRÓGENO; Tecnalia Research & Innovation; EXTREMAT; TECNOLOGÍA DE MEMBRANAS E INTENSIFICACIÓN DE PROCESOSThe present work focuses on the study of a metallic supported Pd-Ag membrane for high temperature applications with a particular attention to long-term stability. In this work, a metallic supported thin-film Pd-Ag membrane has been tested for more than 800 h and sustained hydrogen perm-selectivities higher than 200000 have been measured. Furthermore, it has been demonstrated that there is no interaction of the membrane with the Ni/CaAl2O4 reforming catalyst particles, thus resulting in a constant permeance in the fluidized bed membrane reactor mode. The membrane has been tested under steam and autothermal reforming of methane conditions and the membrane performance has been quantified in terms of the hydrogen recovery and separation factors demonstrating a good reactor performance accomplishing an enhancement in the process efficiency by in-situ selective H2 separation. A decrease in ideal perm-selectivity has been observed at high temperatures (600°C). Small defects at the Pd/Ag surface as a result of interaction of the Pd/Ag later with the metallic support have been observed in after test membrane characterization, which provides appreciated information for the improvement in the performance and production of future membranes.Item Recent Advances in Pd-Based Membranes for Membrane Reactors(2017-01-01) Arratibel Plazaola, Alba; Pacheco Tanaka, David A.; Van Sint Annaland, Martin; Gallucci, Fausto; Tecnalia Research & Innovation; TECNOLOGÍA DE MEMBRANAS E INTENSIFICACIÓN DE PROCESOSPalladium-based membranes for hydrogen separation have been studied by several research groups during the last 40 years. Much effort has been dedicated to improving the hydrogen flux of these membranes employing different alloys, supports, deposition/production techniques, etc. High flux and cheap membranes, yet stable at different operating conditions are required for their exploitation at industrial scale. The integration of membranes in multifunctional reactors (membrane reactors) poses additional demands on the membranes as interactions at different levels between the catalyst and the membrane surface can occur. Particularly, when employing the membranes in fluidized bed reactors, the selective layer should be resistant to or protected against erosion. In this review we will also describe a novel kind of membranes, the pore-filled type membranes prepared by Pacheco Tanaka and coworkers that represent a possible solution to integrate thin selective membranes into membrane reactors while protecting the selective layer. This work is focused on recent advances on metallic supports, materials used as an intermetallic diffusion layer when metallic supports are used and the most recent advances on Pd-based composite membranes. Particular attention is paid to improvements on sulfur resistance of Pd based membranes, resistance to hydrogen embrittlement and stability at high temperature.Item Techno-economic assessment of different routes for olefins production through the oxidative coupling of methane (OCM): Advances in benchmark technologies: Advances in benchmark technologies(2017-12-15) Spallina, Vincenzo; Velarde, Ildefonso Campos; Medrano Jimenez, José Antonio; Godini, Hamid Reza; Gallucci, Fausto; Van Sint Annaland, Martin; Tecnalia Research & Innovationhis paper addresses the techno-economic assessment of two technologies for olefins production from naphtha and natural gas. The first technology is based on conventional naphtha steam cracking for the production of ethylene, propylene and BTX at polymer grade. The unused products are recovered in a boiler to produce electricity for the plant. The plant has been designed to produce 1 MTPY of ethylene. In the second case, ethylene is produced from natural gas through the oxidative coupling of methane (OCM) in which natural gas is fed to the OCM reactor together with oxygen from a cryogenic air separation unit (ASU). The overall reactions are kinetically controlled and the system is designed to work at about 750–850 °C and close to 10 bar. Since the overall reaction system is exothermic, different layouts for the reactor temperature control are evaluated. For the naphtha steam cracking plant, the energy analysis shows an overall conversion efficiency of 67% (with a naphtha-to-olefins conversion of 65.7%) due to the production of different products (including electricity), with a carbon conversion rate of 70%. The main equipment costs associated with naphtha steam cracking are represented by the cracker (about 30%), but the cost of ethylene depends almost entirely on the cost associated with the fuel feedstock. In case of the OCM plant, the overall energy conversion efficiency drops to maximally 30%. In the studied plant design, CO2 capture from the syngas is also considered (downstream of the OCM reactor) and therefore the final carbon/capture efficiency is above 20%. The cost of ethylene from OCM is higher than with the naphtha steam cracking plant and the CAPEX affects the final cost of ethylene significantly, as well as the large amount of electricity required.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.