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Title: Composite Metal-Ceramic Hydrogen Separation Membranes

Authors:
Publication Date:
Research Org.:
Synkera Technologies Inc., Longmont, CO
Sponsoring Org.:
USDOE
OSTI Identifier:
878904
Report Number(s):
DOE/ER/84086-1
DOE Contract Number:
FG02-04ER84086
Type / Phase:
SBIR
Resource Type:
Technical Report
Country of Publication:
United States
Language:
English
Subject:
08 HYDROGEN; 36 MATERIALS SCIENCE; 32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATION; hydrogen purification, hydrogen separation, composite membranes, fuel cells

Citation Formats

Dmitri Routkevitch. Composite Metal-Ceramic Hydrogen Separation Membranes. United States: N. p., 2006. Web.
Dmitri Routkevitch. Composite Metal-Ceramic Hydrogen Separation Membranes. United States.
Dmitri Routkevitch. Mon . "Composite Metal-Ceramic Hydrogen Separation Membranes". United States. doi:.
@article{osti_878904,
title = {Composite Metal-Ceramic Hydrogen Separation Membranes},
author = {Dmitri Routkevitch},
abstractNote = {},
doi = {},
journal = {},
number = ,
volume = ,
place = {United States},
year = {Mon Apr 10 00:00:00 EDT 2006},
month = {Mon Apr 10 00:00:00 EDT 2006}
}

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  • During this quarter, work continued on the development of high-flux palladium-silver membranes for the separation of hydrogen from carbon dioxide. Palladium-silver/poly(etherimide) composite membranes were prepared by a vacuum sputtering technique. The influence of different poly(etherimide) support membranes on the performance of palladium-silver membranes was investigated. All membranes tested showed a hydrogen/carbon dioxide selectivity lower than that of the uncoated poly(etherimide)/poly(dimethylsiloxane) membranes. This is probably due to damage of the skin layer of the asymmetric poly(etherimide) support membranes during the palladium-silver electron bombardment. Polysulfone/poly(dimethylsiloxane)/poly(ether-ester-amide) composite membranes were also prepared. Membrane samples consistently showed a carbon dioxide/hydrogen selectivity of 9 to 10more » and a normalized carbon dioxide flux of 2 to 4 {times} 10{sup {minus}4} cm{sup 3} (STP)/cm{sup 2}{center dot}sec{center dot}cmHg. These are extremely good values, superior to any commercially available membranes for this separation. 2 figs., 4 tabs.« less
  • 'The project on ceramic-supported polymer membranes focuses on the development of a novel class of membranes for the separation of organics from both organic-aqueous and organic-organic mixtures, Theses membranes are fabricated by a graft polymerization process where polymer chains are grown onto the surface of a ceramic support membrane. The surface graft polymerization process, developed at UCLA, results in the formation of a thin polymer layer covalently bonded to the membrane pore surface as a layer of terminally anchored polymeric chains. Through the selection of the polymer most appropriate for the desired separation task, the graft polymerized surface layer canmore » be synthesized to impart specific separation properties to the membrane. It is expected that this project will lead to the demonstration of a new technology for the tailor design of a new class of selective and robust ceramic-supported polymer membranes. This new approach will allow the rapid deployment of task-specific membranes for the separation of waste constituents for subsequent recovery, treatment or disposal. Progress to date includes the preparation of successful silica-polyvinylpyrrolidone (PVP) membrane for the treatment of oil-in-water emulsions and a silica-polyvinylacetate (PVAc) pervaporation membrane for the separation of organics from water. Current work is ongoing to study the performance of the pervaporation membrane for the removal of chlorinated organics from water and to develop a pervaporation membrane for organic-organic separation. In another aspect of the study, the authors are studying the hydrophilic PVP CSP membrane for oil-in-water emulsion treatment with the goal of determining the optimal membrane polymer surface structure as a function of various operating conditions (e.g., tube-side Reynolds number and transmembrane pressure), Work is also in progress to characterize the polymer layer by AFM and internal reflection FTIR, and to model the conformation of the polymer surface layer.'« less
  • 'This report summarizes the work progress over the last 1.75 years of a 3 year project. The objectives of the project have been to develop a new class of ceramic-supported polymeric membranes that could be tailored-designed for a wide-range of applications in remediation and pollution prevention. To date, a new class of chemically-modified ceramic membranes was developed for the treatment of oil-in-water emulsions and for the pervaporation removal of volatile organics from aqueous systems. These new ceramic-supported polymer (CSP) membranes are fabricated by modifying the pore surface of a ceramic membrane support by a graft polymerization process (Chaimberg and Cohen,more » 1994). The graft polymerization process consists of activating the membrane surface with alkoxy vinyl silanes onto which vinyl monomers are added via free-radical graft polymerization resulting in a thin surface layer of terminally anchored polymer chains. Reaction conditions are selected based on knowledge of the graft polymerization kinetics for the specific polymer/substrate system. The resultant ceramic-supported polymer (CSP) membrane is a composite structure in which mechanical strength is provided by the ceramic support and the selectivity is determined by the covalently bonded polymer brush layer. Thus, one of the unique attributes of the CSP membrane is that it can be used in environments where the polymer layer is swollen (or even completely miscible) in the mixture to be separated (Castro et al., 1993). It is important to note that the above modification process is carried out under mild conditions (e.g., temperature of about 70 C) and is well suited for large scale commercial application. In a series of studies, the applicability of a polyvinylpyrrolidone CSP membrane was demonstrated for the treatment of oil-in-water emulsion under a variety of flow conditions (Castro et al.,1996). Improved membrane performance was achieved due to minimization of surface adsorption of the oil components. For the special case of long surface chains, significant additional performance improvement permeate stream was attained at high Reynolds numbers. At the high Reynolds number condition, shear-induced deformation of the terminally anchored polymer chains and as a consequence the screening of the pore entry, resulted in improved permeate quality. Current studies are focused on the optimization of the polymer surface layer and quantification of chemical and hydrodynamic polymer-emulsion interactions.'« less
  • The present project was conceived to address the need for robust yet selective membranes suitable for operating in harsh ph, solvent, and temperature environments. An important goal of the project was to develop a membrane chemical modification technology that would allow one to tailor-design membranes for targeted separation tasks. The method developed in the present study is based on the process of surface graft polymerization. Using essentially the same base technology of surface modification the research was aimed at demonstrating that improved membranes can be designed for both pervaporation separation and ultrafiltration. In the case of pervaporation, the present studymore » was the first to demonstrate that pervaporation can be achieved with ceramic support membranes modified with an essentially molecular layer of terminally anchored polymer chains. The main advantage of the above approach, relative to other proposed membranes, is that the separating polymer layer is covalently attached to the ceramic support. Therefore, such membranes have a potential use in organic-organic separations where the polymer can swell significantly yet membrane robustness is maintained due to the chemical linkage of the chains to be inorganic support. The above membrane technology was also useful in developing fouling resistant ultrafiltration membranes. The prototype membrane developed in the project was evaluated for the treatment of oil-in-water microemulsions, demonstrating lack of irreversible fouling common with commercial membranes.« less
  • There is a growing need in the areas of hazardous waste treatment, remediation and pollution prevention for new processes capable of selectively separating and removing target organic species from aqueous steams. Membrane separation processes are especially suited for solute removal from dilute solutions. They have the additional advantage of requiring less energy relative to conventional separation technologies (e.g., distillation, extraction and even adsorption processes). The major difficulty with current membranes is the poor longevity of polymeric membranes under harsh conditions (high temperature, harsh solvents and pH conditions) and the lack of selectivity of ceramic membranes. In our previous work (1996more » EMSP project), a first generation of novel polymer-ceramic (PolyCer) composite membranes were developed with the goal of overcoming the above difficulties. The proposed PolyCer membranes are fabricated by a surface-graft polymerization process resulting in a molecular layer of polymer chains which are terminally and covalently anchored to the porous membrane support. The polymer imparts the desired membrane selectivity while the ceramic support provides structural integrity. The PolyCer membrane retain its structural integrity and performance even when the polymer phase is exposed to harsh solvent conditions since the polymer chains are covalently bonded to the ceramic support surface. To date, prototype PolyCer membranes were developed for two different membrane separation processes: (a) pervaporation removal of organics from aqueous systems; and (b) ultrafiltration of oil-in-water emulsions. Pervaporation PolyCer membranes were demonstrated for removal of selected organics (TCE, chloroform and MTBE) from water with permeate enrichment factors as high as 300. While the above results have been extremely encouraging, higher enrichment factors (>1000) should be sought for field applications. The above improvement is feasible by increasing the length and surface density of the grafted polymer chains. The required simultaneous increase in surface polymer graft density and chain length is beyond the capability of present free-radical graft polymerization methods. Therefore, it is proposed to develop a new approach to synthesizing the grafted polymer membrane phase via ''living'' free-radical polymerization. This approach should allow controlled growth of the grafted polymer chains while maintaining the advantage of high surface chain density possible with conventional free-radical polymerization. Optimization of the membrane surface layer will be sought by developing fundamental correlation between surface characteristics (e.g., topology, chain length and surface density) and membrane performance. The ability to tailor-design the grafted polymer surface with long polymer chains of a desired surface density is also advantageous in fabricating non-fouling ultrafiltration membranes for colloidal filtration. Using th e same ''living'' free-radical polymerization technology, as for the pervaporation membranes, ultrafiltration ceramic membranes with terminally anchored surface chains, can be produced to repel colloidal species, thus reducing membrane fouling while increasing permeate rejection. As an outcome of the 1996 EEMSP project, it was discovered that, with sufficiently long surface chains, significant increase in PolyCer UF membrane rejection is possible, especially at high tangential velocities. The fabrication, via ''living'' free-radical polymerization, and optimization of such non-fouling UF membranes is another goal of the proposed research. It is expected that this project will results in the demonstration of a commercially viable technology for the ''tailor design'' and optimization of a new class of selective and robust polymer-ceramic (PolyCer) membranes for aqueous waste treatment and water decontamination applications. The proposed PolyCer approach will allow the rapid deployment of ''field-ready'' and task-specific membranes for recovery and recycle for remediation and pollution prevention applications.« less