Innovation: Carbon Dioxide Capture And Hydrogen Production With Membranes

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Hydrogen membrane reactors are an attractive technology for pre-combustion carbon dioxide capture in both coal and gas fired power stations because they combine the efficient conversion of syngas into hydrogen fuel with capture of the remaining carbon dioxide in one reactor. The carbon dioxide is produced at high pressure, reducing the compression energy for transport and storage.

CACHET II project will develop innovative metallic membranes and modules for high capacity hydrogen production and separation from a number of fuel sources including natural gas and coal. The DICP membrane developed in FP6 project CACHET along with novel seal and substrate technology will be scaled up and undergo long term stability testing. An optimisation design tool will be built to include the relationship of all key operating parameters; this tool will be used to specify an optimised pilot and commercial membrane module design.

The project will research novel binary and tertiary palladium alloys for improved durability and permeance for application to solid based fuels derived syngas and high temperature integrated reforming processes. Fundamental research on high temperature sulphur removal systems will enable sulphur tolerant membranes to become an economic possibility.

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Palladium (Pd)-based hydrogen (H2) permeable membrane reactors are an attractive technology for pre-combustion carbon dioxide (CO2) capture from both coal and gas fired power stations. It can capture nearly 100% of CO2 from a combined cycle power plant, at low energy penalty. The CO2 captured is at high pressure, reducing the compression energy for transport and storage. When integrated with a water-gas-shift (WGS) reactor, it combines the efficient conversion of syngas into H2 fuel with capture of the remaining CO2 in one reactor, which has the potential to be the most cost-effective pre-combustion carbon capture technology.

The first part centred on the successful pure Pd membrane that was developed in the FP6 CACHET project. An important lesson learned from CACHET was that external mass flow limitations and concentration polarization effects may easily dominate the overall H2 permeation rate. So the development of effective membranes must always go hand in hand with the design of effective membrane separators or reactors. As WP4 develops an optimisation tool and engineering design for Pd membrane modules, WP1 provides the data for validation by carrying out realistic tests with technically viable 1 m long Pd membranes in a pilot module. Therefore the objective of WP1 in CACHET-II is to build such a scaled-down version of a full-scale membrane module (to be designed in WP4) with 1 m long Pd membranes with improved sealing technology and test this membrane unit for 1000 hours.

During the first 18 months of the project, WP1 has successfully demonstrated that Pd membranes and seals can be manufactured at 1m length scale, and produced the first permeation test results. Two types of seals have been developed, a metal to ceramic joint by IMR and compression seal by ECN, both of which can be implemented into the 1m membrane unit and withstand the tests for 1000 hours. At the moment, both seals are also being tested for even longer durability, aiming at 150 days stability target. Permeation tests of 0.5m membranes have been performed by ECN and DICP, generating data to support the modelling and reaction design activities in WP4. All of these activities will eventually contribute to the construction of the down-scaled 1m membrane module at ECN. The design of the module has been kicked off by ECN and Technip.

Efforts in WP2 have encompassed theoretical modelling, membrane manufacturing by electroless plating and magnetron sputtering followed by appropriate characterization, and extensive H2 permeation evaluation. So far >50 Pd-alloy membrane specimens have been manufactured by magnetron sputtering. Focus during the 1st 18 months of the project has been on binary Pd-Cu and ternary Pd-Cu-TM materials, and the validation of electroless plating as a feasible route for preparation of commercial scale Pd-Cu membranes. Prepared films are being characterized using SEM-EDS, XRD and XPS, while the H2 permeability is being investigated. In total 7 of the prepared ternary Pd-Cu-TM alloy membranes show a higher H2 permeability compared to their binary Pd-Cu counterpart at the same Pd content. A first selection of 3 ternary Pd-Cu-alloy systems for further optimisation has been made on the basis of permeance measurements without the presence of H2S.

Gas permeation tests have been performed between 300 and 500 C investigating the effect of CO and H2S inhibition on various Pd-alloys. It has been shown that a H2S concentration of around 20 ppm saturates the Pd-alloy surface, thereby reducing the obtained H2 flux by up to 90%. The degree of H2S inhibition is rather similar for all Pd-alloy investigated up to now, including binary Pd-Ag, Pd-Cu and Pd-Au alloy membranes. No HSE-related problems have been encountered during the H2S exposure experiments. The H2 flux through the Pd-Ag and Pd-Y alloy membranes are largely affected by CO poisoning. For these alloys, a reduction of up to 50% is obtained at a CO concentration of 5 vol%. For ternary Pd-Cu and Pd-Au alloy membranes the CO inhibition has been found to be less than 10% at the same CO concentration. The H2 permeabilities of face-centred-cubic (FCC) Pd-Cu membranes prepared by sequential electroless plating on tubular ceramic supports and subsequent alloying at 500 °C are in very
good agreement with those prepared by magnetron sputtering. This demonstrates that it will be possible to prepare Pd-Cu membranes for potential commercial applications using this facile and readily scalable preparation method.

For the development of high temperature Pd-alloys for operation at 650-750 C, a start has been made with stability investigation on pure Pd and Pd-Cu alloys. The permeance testing on pure Pd at increasing temperature from 400 to 600 C shows a decrease in selectivity of the membrane but constant permeance. More Pd-Cu alloys have been prepared and are in the process of endurance testing.

During the first 18 month period, the project has issued press release, established the project website, submitted papers and presentations at Journals and International Conferences, published the first projects newsletter and organised a dedicated CACHET-II workshop at the first International Conference of Clean Energy held in China on 10-13 April 2011. More details of these published material can be found at the project website: .

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This innovation is the result of the project

Title: Carbon Dioxide Capture And Hydrogen Production With Membranes


01.01.2010 to 31.12.2012

completed project

Organisations and people involved in this eco-innovation.

Please click on an entry to view all contact details.


(United Kingdom)

Role in project: Project Coordination

Contact person: Ms. SONG Bai


Phone: +44-019-32764176




Contact person: Dr. WANG Hua


Phone: +86-41184379023




Contact person: Dr. TONG Baiyun


Phone: +86-2423971197




Contact person: Mrs. ALATOPOULOU Despina I.

Phone: +30-2107721740




Contact person: Ms. DRAGONI Graziano

Phone: +39-223992077




Contact person: Mr. REINDERS Marinus


Phone: +31-224564455




Contact person: Mr. BUVIK Reidar


Phone: +4793051090




Contact person: Ms. BASTIDE Frank


Phone: +33-147782398