Novel nanocomposite materials for oxygen and hydrogen separation membranes

Design of oxygen and hydrogen separation membranes is the point of current interest in producing syngas from biofuels. Nanocomposites with a high mixed ionic-electronic conductivity are known to be promising materials for these applications. This work aims at studying performance of oxygen and hydrogen separation membranes based on nanocomposites PrNi_0.5Co_0.5O_3-δ + Ce_0.9Y_0.1O_2-δ and Nd_5.5WO_11.25-δ + NiCu alloy, respectively. A high and stable performance promising for the practical application was demonstrated for these membranes. For oxygen separation membrane CH₄ conversion is up to 50% with H₂ content in the outlet feed being up to 25% at 900 °C. For reactor with hydrogen separation membrane complete EtOH conversion was achieved at T ∼ 700 °C even at the highest flow rate, and a high hydrogen permeation (≥1 ml H₂ cm⁻² min⁻¹) was revealed.     

Aluminizing and oxidation treatments on the porous stainless steel substrate for preparation of H2-permeable composite palladium membranes

Composite palladium membranes based on porous stainless steel (PSS) substrate are idea hydrogen separators and purifiers for hydrogen energy systems, and the surface modification of the PSS is of key importance. In this work, the macroporous PSS tubes were aluminized through pack cementation at 850 °C in argon, followed by an oxidation with air at 600 °C. Palladium membranes were prepared by electroless plating. Their permeation performances were tested, and the hydrogen permeation kinetics was discussed. The substrate materials and the palladium membranes were characterized by means of scanning electron microscopy (SEM), energy dispersive spectroscopy (EDS), X-ray diffraction (XRD). An Al₂O₃-enriched surface layer with small pore size was created through aluminizing and oxidation treatments, which greatly improves the membrane integrity. The intermetallic diffusion between the palladium membranes and the PSS substrate material was not observed after a heat-treatment at 500 °C under hydrogen for 200 h. However, the aluminizing and oxidation treatments still need to be further optimized in order to improve the membrane permeability and selectivity, and particularly, the high diffusion resistance of the substrate materials greatly limited the hydrogen flux.     

Incorporation of thermally labile additives in polyimide carbon membrane for hydrogen separation

In this study, three thermally labile additives microcrystalline cellulose (MCC), nanocrystalline cellulose (NCC), and polyvinylpyrrolidone (PVP) were introduced to the P84-copolyimide (PI) solution. PI-based carbon tubular membranes were fabricated using dip-coating method, followed by sample characterizations in order to determine their structural morphologies, thermal stability and gas permeation performance. NCC was added as the membrane pore former for the hydrogen gas (H₂) separation. While tests involving pure H₂ and N₂ permeation were carried out at room temperature, carbon membranes were carbonized at a final temperature of 800 °C, with the heating rate of 3 °C/min under the Ar flow. Excellent result of H₂/N₂ selectivity was obtained with value of 430.06 ± 4.16. Addition of NCC has significantly increased the number of pore channels in the membrane, hence, contributing to high gas permeance and selectivity. NCC has shown potential as a good additive for an enhanced hydrogen separation performance.     

Coating the porous Al2O3 substrate with a natural mineral of Nontronite-15A for fabrication of hydrogen-permeable palladium membranes

Substrate surface modification is a key pretreatment during fabrication of composite palladium membranes for hydrogen purification in hydrogen energy applications. The suspension of a natural porous material, Nontronite-15A mineral, without any organic additives was employed in dip-coating of the porous Al₂O₃ substrate. The Nontronite-15A mineral was characterized by SEM, XRD, TG−DSC and granulometry analysis. The surface and cross-section of the coated porous Al₂O₃ tubes were observed by SEM, and their pore size distribution and nitrogen flux were also measured. Palladium membranes were fabricated over the coated Al₂O₃ tubes by a suction-assisted electroless plating. The optimal loading amount of the Nontronite-15A mineral is just to fill in and level up the surface cavities of the Al₂O₃ substrate rather than to form an extra continuous layer. A thin and selective palladium membrane was successfully obtained, and its permeation performances were tested. The kinetic analyses on the hydrogen flux indicate that the hydrogen permeation behavior exhibits typical characteristics for most of the palladium membranes. During the stability test at 450 °C for 192 h, no membrane damage was detected, and the hydrogen flux increased slightly.     

Hydrogen permeation through the Pd-Nb-Pd composite membrane: Surface effects and thermal degradation

The composite membranes based on Group 5 metals are capable of H₂ separation with the high speed and infinite selectivity. The chemical and thermal stability are critical issues for the application of such membranes in the field of hydrogen energy. In order to understand the degradation mechanisms, the H₂ permeation through composite Pd_2μm-Nb_100μm-Pd_2μm membranes was investigated in a very wide pressure range: (10⁻⁵-10⁴) Pa. At higher pressures the surface contaminations only moderately decreased the permeation. However the permeation experiments at lower pressures demonstrated that an orders of magnitude change in the probability of H₂ molecule dissociative sticking is actually hidden behind this relatively moderate effect. The membranes poisoned by the surface contaminations could be recovered by their exposure to O₂ at (300-400) °C. Heating at temperature higher than 500 °C resulted in the irreversible decrease of permeation and in the pronounced change of permeation behavior at the variation of H₂ pressure. An extremely high permeation was observed at lower pressures at the clean surface of Pd coating. That allows developing an effective membrane pump for hydrogen isotopes.     

Carbon molecular sieve membranes supported on non-modified ceramic tubes for hydrogen separation in membrane reactors

Supported carbon membranes have been regarded as more competitive than traditional gas separation materials due to the versatile combination of different pyrolyzable polymers and supports which in turn leads to high separation factors and mechanical stability. In order to determine the extent to which supported carbon membranes are more competitive, the transport mechanism of supported carbon membranes was investigated in the range 32–150 °C and 1–2.5 bar. Polyimide (Matrimid 5218) material was coated and pyrolyzed under N₂ atmosphere on TiO₂-ZrO₂ macroporous tubes (Tami) that had not been structurally modified in any way. The supported carbon membrane was studied to determine its permeation for low molecular weight gases such as H₂, CH₄, CO, N₂ and CO₂. For these gases, the permeance of the composite supported carbon membranes obtained after pyrolysis at 550 °C increased with inverse square root of molecular weight. The temperature dependence of the permeance was described using an Arrhenius law with the negative activation energies for hydrogen, carbon dioxide and nitrogen providing evidence of a non-activated process. The ideal separation selectivity computed from single gas measurements leads to values slightly lower than the Knudsen because of the influence of viscous flow. The coexistence of more than one transport mechanism in the composite membrane was confirmed. After plugging the possible defects with Polydimethylsiloxane (PDMS), the supported carbon membranes obtained at a pyrolysis temperature of 650 °C showed evidence of a molecular sieving mechanism. This paper shows the separation properties of a crack-free supported carbon membrane obtained using a simple fabrication method that does not require modification of the mesoporous support. The permeance and selectivity values were compared with those of other hydrogen selective materials. Finally, the membranes were applied to methanol steam reforming (MSR).     

Influence of water vapor on hydrogen permeation through 2.5 μm Pd-Ag membranes

Hydrogen permeation experiments were performed to evaluate the influence of water vapor on hydrogen permeability in 80-20% by weight Pd-Ag membranes of 2.5 μm thickness. In particular, hydrogen flux was measured in pure hydrogen permeation tests as well as in experiments with binary mixtures containing also nitrogen or water vapor, that were performed at temperatures ranging from 473 to 723 K and at a transmembrane pressure differences up to about 3 bar. The membranes, supplied by NGK Insulator Ltd., Japan, showed a very high hydrogen permeance and lifetime, as well as virtually infinite selectivity (exceeding 10000 for H₂-N₂ mixtures). The experiments in hydrogen-nitrogen mixtures were carried out at different temperatures, hydrogen concentrations and feed flow rates and confirmed the existence of a non-negligible concentration polarization phenomenon in the experimental module. The gas phase mass transport and the module fluid dynamics were thus analyzed and the dimensionless numbers characterizing these processes were evaluated at the different operative conditions; a linear correlation was found to hold between Sherwood and Péclet numbers. Interestingly, the hydrogen permeate fluxes measured with feeds containing H₂-H₂O mixtures resulted always lower than those obtained for the nitrogen-hydrogen mixtures performed at the same hydrogen mole fraction and operative conditions: in particular, the hydrogen flux depletion increased with decreasing temperature and/or increasing the concentration of water vapor. All the experimental evidences suggest a clear interaction between water vapor and metallic layer, causing a lower hydrogen adsorption capacity of the membrane surface. That phenomenon is reversible, since the original permeance of the membrane was restored once the water vapor was removed from the feed, and is apparently due to a competitive H₂-H₂O adsorption on the Pd-Ag surface. The hydrogen flux depletion was then modeled by considering the simultaneous effects of gas phase resistance and competitive adsorption on the surface, obtaining a rather good agreement between experimental data and calculated results.     

Co-based zeolitic imidazolate framework ZIF-9 membranes prepared on α-Al2O3 tubes through covalent modification for hydrogen separation

Hydrogen has been regarded as the most promising clean and renewable energy. Beside the production of the hydrogen, the separation of hydrogen is also an import issue before it can be used in fuel cells. Membrane-based separation technologies have gained considerable attentions due to its high efficiency and low energy consumption. Zeolite imidazolate framework (ZIF) membranes have drawn intense interest due to their zeolite-like properties such as permanent porosity, uniform pore size and exceptional thermal and chemical stability. It is rather challenged to prepare well-intergrown Co-based zeolitic imidazolate frameworks (ZIFs) membranes on porous α-Al₂O₃ tubes since Co-based ZIFs prefer to form crystals in the synthesis solution rather than grow as membrane layer on the support surface. In this work, we report the preparation of high-quality ZIF-9 membrane with high H₂/CO₂ selectivity and excellent thermal stability by using 3-aminopropyltriethoxysilane (APTES) as a covalent linker to modify the α-Al₂O₃ tube. Due to the formation of covalent bonds between APTES and ZIF-9, ZIF-9 nutrients are bound to the support surface, thus promoting the growth of dense and phase-pure ZIF-9 membrane with a thin thickness of about 4.0 μm. The gas separation performances of the ZIF-9 membrane were evaluated by single gas permeation and mixture gas separation of H₂/CO₂, H₂/N₂ and H₂/CH₄, respectively. The mixture separation factors of H₂/CO₂, H₂/CH₄, and H₂/N₂ of the ZIF-9 membrane are 21.5, 8.2 and 14.7, respectively, which by far exceeds corresponding Knudsen coefficients. Moreover, the as-prepared ZIF-9 membrane exhibits excellent stability at a relatively broad range of operating temperature, which is beneficial for the industrial application of hydrogen separation or further membrane reactor.     

Development of selective Pd–Ag membranes on porous metal filters

Metallic supports with sufficient surface quality to achieve highly selective thin Pd–Ag membranes require specific pre-treatments, are not readily available on the market and are generally very expensive. To reduce costs, rough and large media grade Hastelloy X filters have been acquired and pre-treated via polishing and chemical etching. The loss in gas permeance given by the polishing treatment proved fully recovered after chemical etching. A method to fill the large pores of the filters via aspiration of α-Al₂O₃ water-powder suspension has been applied and characterized via imaging of the filled pores, inferential statistics, and capillary flow porometry measurements. The most suitable filler particle size for pore size distribution reduction has been identified as 18 μm, while a 5 μm filler proved optimal for further pore morphology improvement. The wide pore size distribution of the filters has thus been reduced up to 200 nm by filling with α-Al₂O₃ particles of decreasing size, similarly to the ceramic supports used for thin Pd–Ag membranes deposition. A boehmite based interdiffusion barrier has been deposited, achieving further surface roughness reduction. A highly H₂ selective membrane has been obtained via simultaneous Pd–Ag plating on the pre-treated filter.     

Investigation on properties of BaZr0.6Hf0.2Y0.2O3-δ with sintering aids (ZnO,NiO, Li2O) and its application for hydrogen permeation

BaZr_0.8Y_0.2O_3-δ proton conductor has the characteristics of excellent chemical stability, but its impoverished sinterability and low conductivity hinder its applications in fuel cell and hydrogen separation. Hf doping in Zr site improves BaZr_0.6Hf_0.2Y_0.2O_3-δ sinterability and conductivity. To further enhance BaZr_0.6Hf_0.2Y_0.2O_3-δ properties, three kinds of sintering aids ZnO, NiO or Li₂O were introduced and their effect on the sinterability, microstructure and conductivity of BaZr_0.6Hf_0.2Y_0.2O_3-δ were studied. The experimental results display that 4 mol% ZnO can enhance the sinterability and conductivity of BaZr_0.6Hf_0.2Y_0.2O_3-δ sample sintered at 1400 °C. Compared with BaZr_0.6Hf_0.2Y_0.2O_3-δ sintered at 1600 °C, BaZr_0.6Hf_0.2Y_0.2O_3-δ with 4 mol% ZnO is of larger grain size, higher relative density (95.5%) and lower sintering temperature (reducing by 200 °C). Meanwhile, the conductivity of BaZr_0.6Hf_0.2Y_0.2O_3-δ with 4 mol% ZnO reaches 4.17 × 10^?3 S cm^?1 in wet 5% H₂/Ar at 700 °C, due to the reduction of the grain boundary resistance of sample. BaZr_0.6Hf_0.2Y_0.2O_3-δ with 4 mol% ZnO membrane for hydrogen separation via external short circuit was developed. The membrane with a thickness of 1.08 mm gives a hydrogen permeation flux of 0.098 mL min^?1cm^?2 at 800 °C with 50% H₂/He as feed gas. The presence of water vapor significantly promotes the hydrogen permeability of the membrane. In addition, introduction of 3% CO₂ or 100 ppm H₂S into feed gas does not decrease the hydrogen permeation flux of the membrane.     

Hydrogen permeation measurements of Pd and Pd-Cu membranes using dynamic pressure difference method

Hydrogen permeation across membranes is measured using a dynamic pressure difference method. In the method, a transient system for continuously monitoring hydrogen flux of a membrane is conducted. Three different membranes, consisting of two pure palladium (Pd) membranes with different thicknesses and one palladium-copper (Pd-Cu) membrane supported by porous stainless steel (PSS) tubes, are taken into account. Three different operating temperatures of 320, 350 and 380 °C as well as two different initial pressure differences of 5 and 10 atm are considered to evaluate the effects of the operating parameters upon the hydrogen permeation. The results suggest that a threshold of pressure difference is always exhibited at the end of the permeation process, regardless of which membrane is tested. The hydrogen permeation rate can be predicted well for the pressure exponent in the range of 0.1-1.0; however, the optimal pressure exponent is located between 0.5 and 0.8. The theoretical analysis indicates that the characteristic time of hydrogen permeation in the present system ranges from 245 to 460 s and the entire permeation period is longer than the characteristic time by an order of magnitude. In regard to the effect of membrane temperature on the permeation, the activation energies of the three membranes range from 11 to 18 kJ mol⁻¹.     

Impact of vacuum operation on hydrogen permeation through a palladium membrane tube

Palladium (Pd) membranes are characterized by their high permselectivity to hydrogen and easy operation, and are promising devises for separating hydrogen from hydrogen-rich gases. The membranes are normally operated with atmospheric pressure at the permeate side. Instead of this common operation, hydrogen permeation through a Pd membrane under vacuum operation at the permeate side is investigated and compared with that under normal operation. In this study, two membrane operating temperatures (320 and 380 °C), four H₂ partial pressure differences (2, 3, 4, and 5 atm) across the membrane, and four feed gases are considered. The results suggest that the vacuum operation can efficiently intensify the H₂ permeation rate. The improvement in H₂ permeation rate due to the vacuum operation can be increased up to 136%. The positive effect of the vacuum operation is especially pronounced when the gas mixtures are used as the feed gases, stemming from the effective attenuation of the concentration polarization. An increase in membrane temperature raises the H₂ permeation rate, but its influence in enhancing the H₂ permeation rate with the vacuum operation is not as significant as that without the vacuum one. It is found that the retardation effect of impurities on the mass transfer is always ranked as CO > CO₂ > N₂, regardless of with/without vacuum operation.     

Pd–Cu alloy membrane deposited on CeO2 modified porous nickel support for hydrogen separation

In this study, the hydrogen permeation behavior of a Pd₉₃–Cu₇ alloy membrane deposited on ceria-modified porous nickel support (PNS) was evaluated. PNS, which has an average pore size of 600 nm, was modified by alumina sol. Alumina sol was prepared using precursors that had a mean particle size of 300 nm. Alumina-modified PNS was further treated with ceria sol modification to produce a smoother surface morphology and narrow surface pores. A 7 μm thick Pd₉₃–Cu₇ alloy membrane was made on an alumina-modified PNS and a ceria-finished membrane was fabricated by magnetron sputtering followed by Cu-reflow at 700 °C for 2 h. SEM analysis showed that the membrane deposited on a ceria-finished PNS contained more clear grain boundaries than the membrane deposited on the alumina-modified PNS. The membrane was mounted in a stainless steel permeation cell with a gold-plated stainless steel O-ring. Permeation tests were then conducted using pure hydrogen and helium at temperatures ranging from 673 to 773 K and feed side pressures ranging from 100 to 400 kPa. These tests showed that the membrane had a hydrogen permeation flux of 2.8 × 10⁻¹ mol m⁻² s⁻¹ with H₂/He selectivity of >50,000 at a temperature of 773 K and pressure difference of 400 kPa.     

A mixed electronic and protonic conducting hydrogen separation membrane with asymmetric structure

In this work, highly doped ceria with lanthanum, La_0.5Ce_0.5O_2−δ (LDC), are developed as hydrogen separation membrane material. LDC presents a mixed electronic and protonic conductivity in reducing atmosphere and good stability in moist CO₂ environment. LDC separation membranes with asymmetrical structure are fabricated by a cost-saving co-pressing method, using NiO + LDC + corn starch mixture as substrate and LDC as top membrane layer. Hydrogen permeation properties are systemically studied, including the influence of operating temperature, hydrogen partial pressure in feed stream and water vapor in both sides of the membrane on hydrogen permeating fluxes. Hydrogen permeability increases as the increasing of temperature and hydrogen partial pressure in feed gas. Using 20% H₂/N₂ (with 3% of H₂O) as feed gas and dry high purity argon as sweep gas, an acceptable flux of 2.6 × 10⁻⁸ mol cm⁻² s⁻¹ is achieved at 900 °C. The existing of water in both sides of membrane has significant effect on hydrogen permeation and the corresponding reasons are analyzed and discussed.     

Production strategies of asymmetric BaCe0.65Zr0.20Y0.15O3-δ – Ce0.8Gd0.2O2-δ membrane for hydrogen separation

Mixed proton and electron conductor ceramic composites are among the most promising materials for hydrogen separation membrane technology especially if designed in an asymmetrical configuration (thin membrane supported onto a thicker porous substrate). However a precise processing optimization is needed to effectively obtain planar and crack free asymmetrical membranes with suitable microstructure and composition without affecting their hydrogen separation efficiency. This work highlights for the first time the most critical issues linked to the tape casting process used to obtain BaCe_0.65Zr_0.20Y_0.15O_3-δ – Ce_0.8Gd_0.2O_2-δ (BCZY-GDC) asymmetrical membranes for H₂ separation. The critical role of the co-firing process, sintering aid and atmosphere was critically investigated. The optimization of the production strategy allowed to obtain asymmetric membranes constituted by a dense 20 μm-thick ceramic-ceramic composite layer supported by a porous (36%) 750 μm-thick BCZY-GDC substrate. The asymmetric membranes here reported showed H₂ fluxes (0.47 mL min⁻¹ cm⁻² at 750 °C) among the highest obtained for an all-ceramic membrane.     

Hydrogen permeation studies of composite supported alumina-carbon molecular sieves membranes: Separation of diluted hydrogen from mixtures with methane

One 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%.     

Development of hydrogen-selective CAU-1 MOF membranes for hydrogen purification by ‘dual-metal-source’ approach

Hydrogen provides reliable, sustainable, environmental and climatic friendly energy to meet world's energy requirement and it also has high energy density. Hydrogen is relevant to all of the energy sectors-transportation, buildings, utilities and industry. In all of these sectors, hydrogen-rich gas streams are needed. Thus, hydrogen-selective membrane technology with superior performances is highly demanded for separation and purification of hydrogen gas mixtures. In this study, novel [Al₄(OH)₂(OCH₃)₄(H₂N-BDC)₃]·xH₂O (CAU-1) MOF membranes with accessible pore size of 0.38 nm are evaluated for this goal of hydrogen purification. High-quality CAU-1 membranes have been successfully synthesized on α-Al₂O₃ hollow ceramic fibers (HCFs) by secondary growth assisted with the homogenously deposited CAU-1 nanocrystals with a size of 500 nm as seeds. The energy-dispersive X-ray spectroscopy study shows that the HCFs substrates play dual roles in the membrane preparation, namely aluminum source and as a support. The crystals in the membrane are intergrown together to form a continuous and crack-free layer with a thickness of 4 μm. The gas sorption ability of CAU-1 MOF materials is examined by gas adsorption measurement. The isosteric heats of adsorption with average values of 4.52 kJ/mol, 12.90 kJ/mol, 12.82 kJ/mol and 27.99 kJ/mol are observed for H₂, N₂, CH₄, and CO₂ respectively, indicating different interactions between CAU-1 framework and these gases. As-prepared HCF supported CAU-1 membranes are tested by single and binary gas permeation of H₂/CO₂, H₂/N₂ and H₂/CH₄ at different temperatures, feed pressures and testing time. The permeation results show preferential permeance of H₂ over CO₂, N₂, and CH₄ with high separation factors of 12.34, 10.33, and 10.42 for H₂/CO₂, H₂/N₂, H₂/CH₄, respectively. The temperature, pressure and test time dependent studies reveal that HCFs supported CAU-1 membranes possess high stability, resistance to cracking, temperature cycling, high reproducibility, these of which combined with high separation efficiency make this type of MOF membranes are promising for hydrogen recycling from industrial exhausts.     

Preparation of thin Pd membrane on porous stainless steel tubes modified by a two-step method

Thin Pd membranes for hydrogen filtration were deposited on modified porous stainless steel (PSS) tubes using an electroless plating technique. Alumina oxide (Al₂O₃) particles of two different sizes were subsequently used to modify the non-uniform pore distribution and the surface roughness of the PSS tubes. The principle of the modification was to use large Al₂O₃ particles (∼10 μm) to fill larger pores on the surface, and leave the smaller pores intact. Small Al₂O₃ particles (∼1 μm) were then used to further decrease the surface roughness. The detailed manufacturing steps of the Al₂O₃ modification were investigated and optimized to achieve a continuous dense Pd membrane with a minimum thickness of 4.4 μm on the modified PSS tubes. The highest hydrogen permeance of the membrane was 2.94 × 10⁻³ mol/m²-s-kPa^0.5 at 773 K, with a selectivity coefficient (H₂/He) of 1124 under a pressure difference of 800 kPa. In comparison, the thickness and hydrogen permeance of a dense Pd membrane on unmodified PSS tubes were 31.5 μm and 5.97 × 10⁻⁴ mol/m²-s-kPa^0.5, respectively, at 773 K under an 800 kPa pressure difference. The stability of the membranes at high temperatures was also investigated. The hydrogen permeation flux at 773 K was stable during a test period of 500 h. These results demonstrate that the two-step method modifies the surface of PSS tubes in a relatively simple way and results in thin, dense Pd membranes with high hydrogen permeance and good thermal stability.     

Pre-activation of SBA-15 intermediate barriers with Pd nuclei to increase thermal and mechanical resistances of pore-plated Pd-membranes

Thermal and mechanical resistances of palladium composite membranes prepared by Electroless Pore-Plating (ELP-PP) and containing SBA-15 as intermediate layer were improved by doping the silica material with Pd nuclei before its incorporation on the composite membrane. Textural properties of synthesized SBA-15 materials (both raw and doped ones) were analyzed by XRD, N₂ adsorption-desorption at 77 K and TEM, while the main properties of the composite membrane were determined by SEM and gravimetric analyses. Moreover, membrane permeation tests were also carried out with pure gases, hydrogen and nitrogen, and binary mixtures of them at temperature of 400 °C and pressure driving forces in the range of 0.5–2.5 bar. The use of bare SBA-15 intermediate layer leads to the appearance of cracks on the Pd layer during permeation experiments at high temperature. In contrast, the use of Pd-doped SBA-15 particles avoids this problem, thus improving both thermal and mechanical resistances of the composite ELP-PP Pd-membrane. Following this preparation method, an estimated Pd thickness of 7.1 μm was obtained, reaching a hydrogen permeance of 3.81·10^?4 mol s^?1 m^?2 Pa^?0.5 and ensuring an ideal H₂/N₂ separation factor higher than 2550 at 400 °C.