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Title: Energy Efficient Membrane Reactor for Fuel Reforming

Publication Date:
Research Org.:
Materials & Electrochemical Research (MER) Corp.
Sponsoring Org.:
USDOE - Office of Energy Efficiency and Renewable Energy (EE-2F)
OSTI Identifier:
Report Number(s):
Final Report
DOE Contract Number:
Type / Phase:
Resource Type:
Technical Report
Country of Publication:
United States
08 HYDROGEN; microchannel, catalytic, membrane, fuel reformer, hydrogen, fuel cells

Citation Formats

Dr. Raouf Loutfy Dr. Lev Tuchinskiy. Energy Efficient Membrane Reactor for Fuel Reforming. United States: N. p., 2006. Web.
Dr. Raouf Loutfy Dr. Lev Tuchinskiy. Energy Efficient Membrane Reactor for Fuel Reforming. United States.
Dr. Raouf Loutfy Dr. Lev Tuchinskiy. Mon . "Energy Efficient Membrane Reactor for Fuel Reforming". United States. doi:.
title = {Energy Efficient Membrane Reactor for Fuel Reforming},
author = {Dr. Raouf Loutfy Dr. Lev Tuchinskiy},
abstractNote = {},
doi = {},
journal = {},
number = ,
volume = ,
place = {United States},
year = {Mon Jan 23 00:00:00 EST 2006},
month = {Mon Jan 23 00:00:00 EST 2006}

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  • GTI developed a plan where efforts were concentrated in 4 major areas: membrane material development, membrane module development, membrane process development, and membrane gasifier scale-up. GTI assembled a team of researchers to work in each area. Task 1.1 Ceramic Membrane Synthesis and Testing was conducted by Arizona State University (ASU), Task 1.2 Metallic Membrane Synthesis and Testing was conducted by the U.S. National Energy Technology Laboratory (NETL), Task 1.3 was conducted by SCHOTT, and GTI was to test all membranes that showed potential. The initial focus of the project was concentrated on membrane material development. Metallic and glass-based membranes weremore » identified as hydrogen selective membranes under the conditions of the biomass gasification, temperatures above 700C and pressures up to 30 atmospheres. Membranes were synthesized by arc-rolling for metallic type membranes and incorporating Pd into a glass matrix for glass membranes. Testing for hydrogen permeability properties were completed and the effects of hydrogen sulfide and carbon monoxide were investigated for perspective membranes. The initial candidate membrane of Pd80Cu20 chosen in 2008 was selected for preliminary reactor design and cost estimates. Although the H2A analysis results indicated a $1.96 cost per gge H2 based on a 5A (micron) thick PdCu membrane, there was not long-term operation at the required flux to satisfy the go/no go decision. Since the future PSA case yielded a $2.00/gge H2, DOE decided that there was insufficient savings compared with the already proven PSA technology to further pursue the membrane reactor design. All ceramic membranes synthesized by ASU during the project showed low hydrogen flux as compared with metallic membranes. The best ceramic membrane showed hydrogen permeation flux of 0.03 SCFH/ft2 at the required process conditions while the metallic membrane, Pd80Cu20 showed a flux of 47.2 SCFH/ft2 (3 orders of magnitude difference). Results from NETL showed Pd80Cu20 with the highest flux, therefore it was chosen as the initial and eventually, final candidate membrane. The criteria for choice were high hydrogen flux, long-term stability, and H2S tolerance. Results from SCHOTT using glass membranes showed a maximum of 0.25 SCFH/ft2, that is an order of magnitude better than the ceramic membrane but still two orders of magnitude lower than the metallic membrane. A membrane module was designed to be tested with an actual biomass gasifier. Some parts of the module were ordered but the work was stopped when a no go decision was made by the DOE.« less
  • We propose to develop an inorganic metal-metal composite membrane to study reforming of liquid hydrocarbons and methanol by equilibrium shift in membrane-reactor configuration, viewed as fuel processor. Based on our current understanding and experience in the Pd-ceramic composite membrane, we propose to further develop this membrane to a Pd and Pd-Ag alloy membrane on microporous stainless steel support to provide structural reliability from distortion due to thermal cycling. Because of the metal-metal composite structure, we believe that the associated end-seal problem in the Pd-ceramic composite membrane in tubular configuration would not be an issue at all. We plan to testmore » this membrane as membrane-reactor-separator for reforming liquid hydrocarbons and methanol for simultaneous production and separation of high-purity hydrogen for PEM fuel cell applications. To improve the robustness of the membrane film and deep penetration into the pores, we have used osmotic pressure field in the electroless plating process. Using this novel method, we deposited thin Pd-film on the inside of microporous stainless steel tube and the deposited film appears to robust and defect free. Work is in progress to evaluate the hydrogen perm-selectivity of the Pd-stainless steel membrane.« less
  • In this work, asymmetric dense Pd/porous stainless steel composite membranes were fabricated by depositing palladium on the outer surface of the tubular support. The electroless plating method combined with an osmotic pressure field was used to deposit the palladium film. Surface morphology and microstructure of the composite membranes were characterized by SEM and EDX. The SEM and EDX analyses revealed strong adhesion of the plated pure palladium film on the substrate and dense coalescence of the Pd film. Membranes were further characterized by conducting permeability experiments with pure hydrogen, nitrogen, and helium gases at temperatures from 325 to 450 Cmore » and transmembrane pressure differences from 5 to 45 psi. The permeation results showed that the fabricated membranes have both high hydrogen permeability and selectivity. For example, the hydrogen permeability for a composite membrane with a 20 {micro}m Pd film was 3.02 x 10{sup -5} moles/m{sup 2}.s.Pa{sup 0.765} at 450 C. Hydrogen/nitrogen selectivity for this composite membrane was 1000 at 450 C with a transmembrane pressure difference of 14.7 psi. Steam reforming of methane is one of the most important chemical processes in hydrogen and syngas production. To investigate the usefulness of palladium-based composite membranes in membrane-reactor configuration for simultaneous production and separation of hydrogen, steam reforming of methane by equilibrium shift was studied. The steam reforming of methane using a packed-bed inert membrane tubular reactor (PBIMTR) was simulated. A two-dimensional pseudo-homogeneous reactor model with parallel flow configuration was developed for steam reforming of methane. The shell volume was taken as the feed and sweep gas was fed to the inside of the membrane tube. Radial diffusion was taken into account for concentration gradient in the radial direction due to hydrogen permeation through the membrane. With appropriate reaction rate expressions, a set of partial differential equations was derived using the continuity equation for the reaction system and then solved by finite difference method with appropriate boundary and initial conditions. An iterative scheme was used to obtain a converged solution. Membrane reactor performance was compared to that in a traditional non-membrane packed-bed reactor (PBR). Their performances were also compared with thermodynamic equilibrium values achievable in a conventional non-membrane reactor. Numerical results of the models show that the methane conversions in the PBIMTR are always higher than that in the PBR, as well as thermodynamic equilibrium conversions. For instance, at a reaction pressure of 6 atm, a temperature of 650 C, a space velocity of 900/16.0 SCCM/gm{sub cat}, a steam to methane molar feed ratio of 3.0, a sweep ratio of 0.15, the conversion in the membrane reactor is about 86.5%, while the conversion in the non-membrane reactor is about 50.8%. The corresponding equilibrium conversion is about 56.4%. The effects on the degree of conversion and hydrogen yield were analyzed for different parameters such as temperature, reactor pressure, feed and sweep flow rate, feed molar ratio, and space time. From the analysis of the model results, it is obvious that the membrane reactor operation can be optimized for conversion or yield through the choice of proper operating and design parameters. Comparisons with available literature data for both membrane and non-membrane reactors showed a good agreement.« less
  • Ethylene and propylene are two of the largest commodity chemicals in the United States and are major building blocks for the petrochemicals industry. These olefins are separated currently by cryogenic distillation which demands extremely low temperatures and high pressures. Over 75 billion pounds of ethylene and propylene are distilled annually in the US at an estimated energy requirement of 400 trillion BTU`s. Non-domestic olefin producers are rapidly constructing state-of-the-art plants. These energy-efficient plants are competing with an aging United States olefins industry in which 75% of the olefins producers are practicing technology that is over twenty years old. New separationmore » opportunities are therefore needed to continually reduce energy consumption and remain competitive. Amoco has been a leader in incorporating new separation technology into its olefins facilities and has been aggressively pursuing non-cryogenic alternatives to light gas separations. The largest area for energy reduction is the cryogenic isolation of the product hydrocarbons from the reaction by-products, methane and hydrogen. This separation requires temperatures as low as {minus}150{degrees}F and pressures exceeding 450 psig. This CRADA will focus on developing a capillary condensation process to separate olefinic mixtures from light gas byproducts at temperatures that approach ambient conditions and at pressures less than 250 psig; this technology breakthrough will result in substantial energy savings. The key technical hurdle in the development of this novel separation concept is the precise control of the pore structure of membrane materials. These materials must contain specially-shaped channels in the 20-40A range to provide the driving force necessary to remove the condensed hydrocarbon products. In this project, Amoco is the technology end-user and provides the commercialization opportunity and engineering support.« less