Browsing by Author "Pacheco Tanaka, David Alfredo"
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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 Hydrogen permeation and stability in ultra-thin Pd-Ru supported membranes(2020-03-04) Liu, Jinxia; Bellini, Stefano; de Nooijer, Niek C.A.; Sun, Yu; Pacheco Tanaka, David Alfredo; Tang, Chunhua; Li, Hui; Gallucci, Fausto; Caravella, Alessio; Tecnalia Research & Innovation; TECNOLOGÍA DE MEMBRANAS E INTENSIFICACIÓN DE PROCESOSIn this paper, we report the performance of supported PdRu membranes for possible applications to hydrogen purification and/or production. For this purpose, we fabricated three ultra-thin α-alumina-supported membranes by combined plating techniques: a PdAg membrane (3 μm-thick ca.) and two PdRu (1.8 μm-thick ca.). The former is set as a benchmark for comparison. The membranes were characterised using different methodologies: permeation tests, thermal treatment and SEM analysis. Preliminary leakage tests performed with nitrogen has revealed that the two PdRu membranes, namely PdRu#1 and PdRu#2, show a non-ideal (non-infinite) selectivity, which is relatively low for the former (around 830 at 400 °C) and sufficiently high for the latter (2645 at 400 °C). This indicates a relevant presence of defects in the PdRu#2 membrane, differently from what observed for the PdAg and PdRu#1 ones. The permeation tests show that the hydrogen permeating flux is stable up to around 550 °C, with an apparently unusual behaviour at higher temperatures (600 °C), where we observe a slightly decrease of hydrogen flux with an increase of the nitrogen one. Moreover, a peculiar bubble-shaped structure is observed in the metal layer of all membranes after usage by means of SEM image analysis. This is explained by considering the effect of the Pd-alloy grain surface energy, which tends to minimise the exposed surface area of the grain interface by creating sphere-like bubble in the lattice, similar to what occurs for soap bubbles in water. The above-mentioned decrease in hydrogen flux at 600 °C is explained to be caused by the bubble formation, which pushes the alloy deeper in the support pores.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 Water Adsorption Effect on Carbon Molecular Sieve Membranes in H2-CH4 Mixture at High Pressure(2020-07) Nordio, Maria L. V.; Medrano, José A.; van Sint Annaland, Martin; Pacheco Tanaka, David Alfredo; Llosa Tanco, Margot; Gallucci, Fausto; Tecnalia Research & Innovation; TECNOLOGÍA DE MEMBRANAS E INTENSIFICACIÓN DE PROCESOSCarbon molecular sieve membranes (CMSMs) are emerging as promising solution to overcome the drawbacks of Pd-based membranes for H2 separation since (i) they are relatively easy to manufacture; (ii) they have low production and raw material costs; (iii) and they can work at conditions where polymeric and palladium membranes are not stable. In this work CMSMs have been investigated in pure gas and gas mixture tests for a proper understanding of the permeation mechanism, selectivity and purity towards hydrogen. No mass transfer limitations have been observed with these membranes, which represents an important advantage compared to Pd-Ag membranes, which suffer from concentration polarization especially at high pressure and low hydrogen concentrations. H2, CH4, CO2 and N2 permeation at high pressures and different temperatures in presence of dry and humidified stream (from ambient and water vapour) have been carried out to investigate the effect of the presence of water in the feed stream. Diffusion is the main mechanism observed for hydrogen, while methane, nitrogen and especially carbon dioxide permeate through adsorption-diffusion at low temperatures and high pressures. Finally, H2 permeation from H2-CH4 mixtures in presence of water has been compared at different temperatures and pressure, which demonstrates that water adsorption is an essential parameter to improve the performance of carbon molecular sieve membranes, especially when working at high temperature. Indeed, a hydrogen purity of 98.95% from 10% H2—90% CH4 was achieved. The main aim of this work is to understand the permeation mechanisms of CMSMs in different operating conditions and find the best conditions to optimize the separation of hydrogen.