Community Research and Development Information Service - CORDIS

Periodic Report Summary 2 - GREEN-CC (Graded Membranes for Energy Efficient New Generation Carbon Capture Process)

Project Context and Objectives:
The objective of the project is the development of a new generation high-efficiency capture process based on oxyfuel combustion utilizing novel oxygen transport membranes.
All scenarios about the future global energy requirements anticipate an increasing demand for electricity, which in 2030 is predicted to be twice the current demand. Increasing global population and fast growing economies especially in developing countries are identified as main drivers for this development. These scenarios also indicate that this increase can only be met by considerable use of the fossil fuels coal, natural gas and oil. It becomes clear that fossil fuels will contribute to more than 60 % of future electricity generation. However, fossil fuel power plants are by far the biggest point sources of CO2 and contribute more than 40% of the worldwide anthropogenic CO2 emissions. Carbon Capture and Utilization (CCU) or Storage (CCS) in fossil power plants is an important strategy to reduce CO2 emissions in order to counteract global warming, offering a key contribution to allow future electricity supply to be environmentally safe and sustainable.
Major sources for human made CO2 emissions comprise the energy and the industrial sector including cement, glass and steel production. One of the most appropriate concepts to capture CO2 from such point sources is the oxyfuel combustion. The main energy demand for this method results from the O2 generation, which is usually done by air liquefaction. This energy demand can substantially be lowered using thermally integrated separation modules based on ceramic oxygen transport membranes (OTM). It is least if the OTM is integrated in a 4-end mode, which entails that the permeating oxygen is swept and directly diluted using recirculated flue gas. Up to 60% reduction in capture energy demand compared to cryogenic air separation and up to 40% reduction compared to post-combustion capture approaches can be achieved. GREEN-CC provides a new generation high-efficiency capture process based on oxyfuel combustion. The focus lies on the development of clear integration approaches for OTM-modules in power plants and cement industry considering minimum energy penalty related to common CO2 capture and integration in existing plants with minimum capital investment. This is attained by using advanced process simulations and cost calculations. GREEN-CC also explores the use of OTM-based oxyfuel combustion in different energy-demanding industrial processes, e.g. oil refining and petrochemical industry.
Oxygen transport membranes consist of gastight Mixed Ionic Electronic Conductors (MIEC), which allow oxygen diffusion through vacancies in the crystal lattice and simultaneous transport of electrons in the opposite direction, thus obviating the need for an external electrical short circuit. Their major advantage is infinite oxygen selectivity, providing that leakage through the membrane layer or the sealing is prevented, resulting in high purity oxygen. However, highly permeable membrane materials show a chemical instability against CO2 and other flue gas components. One major challenge faced by GREEN-CC is therefore to identify and develop membrane materials, components, and a Proof-of-Concept-module for the 4-end mode OTM integration. The desired membrane assembly will consist of a thin membrane layer supported on substrates with engineered porosity and oxygen reduction catalysts with high and stable activity in flue gas. As proof of concept, a planar membrane module will be developed which opens up challenging hurdles like joining technology. Modelling at all levels will support the development ranging from gas transport modelling through the membrane assembly, finite element modelling of the Proof-of-Concept- module as well as process simulations of the targeted applications, i.e. power plant and cement industry. Specific attention is paid to cost efficiency in terms of capital and operational costs.

Project Results:
The aim of the project is to develop membranes and a PoC-module for an integrated oxygen generation in cement production and for Oxyfuel- and IGCC fossil power plants. As these industries have a range of different requirements for incorporation of a membrane module into their specific process environment, one of the first steps was to establish a list of boundary conditions (e.g. Temperature, Pressure, Gasses, Dust, Durability, Maintenance etc.), which serves as a guideline for the material development and testing of the membranes. It turned out that the amount of harmful elements and dust is very different in the different applications, so that dependent on the membrane stability process modifications in the flue gas cleaning may be required. In addition, process simulations for an optimal integration of the membranes were performed. The calculations allow a comparison of the newly designed processes with existing processes in terms of net-efficiency and investment and operating costs for selected cases. The IGCC-case was identified to be inefficient due to additional technology required independent of membrane performance and cost. Therefore, it will not be continued in the project.
Four design concepts for the asymmetric planar pilot Proof-of-Concept-module were investigated by numerical modeling (Computational Fluid Dynamics and FEM stress analysis). Advantages and disadvantages of each concept were evaluated, and the most promising concept was selected at month 24 (MS 3). Also our Australian partner, the University of Queensland, contributed to these modeling activities. Two tape-cast asymmetric membranes and an interlayer providing stability elements have to be laminated, sintered, and sealed into the metallic housing.
A wide range of membrane materials were identified and manufactured at lab scale, aiming at high performance and stability. Consequently, permeation experiments and stability tests in CO2 and SOx were carried out. La0,58Sr0,4Co0,2Fe0,8O3-δ (LSCF) was decided to be scaled up for the PoC-module as a reference material because it is stable in CO2 and are successfully sealed to metallic housing materials using Ag/CuO-based reactive air brazing.. However, stability towards SOx is a critical issue. In the recent period membrane components are developed in medium size for additional tests (joining, performance). Scale up to final PoC-module size based on the final design of the module is ongoing but delayed. The respective D1.7 was shifted from M36 to M40, which was agreed between all partners to be acceptable in order to meet the project target, i.e. demonstration of the proof of concept operation for 1000 hours in application relevant conditions. In addition, a lot of dual phase composites were investigated, because of a high stability in CO2 and SOx. In the recent period one favorite composition (Ce0,8Gd0.2O2-δ - FeCo2O4) was selected from this research which is proven to be stable in the targeted conditions. To increase the performance of the membranes several catalytic materials were tested and selected for porous surface layers on top of the membranes. Also for these materials stability tests in CO2 and SOx containing atmospheres were carried out and the electrochemical behavior was measured.
In the first period of 18 months all deliverables and milestones were fulfilled according to the work plan in Annex I. In the second period D3.2 had 6 months delay which is uncritical for the project. The interaction between the work packages and partners is very effective. The project has a high potential to achieve its goals developing a membrane, stable at operation conditions defined by the industrial partners. An operating 4-end proof of concept module is expected to be available by the end of the project. Operation time of 1000 h of the PoC module under realistic atmosphere has to be demonstrated in the last period of the project.

Potential Impact:
The reduction or elimination of CO2 emissions from power plants fuelled by fossil fuels (coal, gas) and cement production plants is a major target in the current socio-economic, environmental and political situation and discussion to reduce greenhouse gas emissions. This mission can be achieved by introducing gas separation techniques using membrane technology, which is associated with significantly lower efficiency losses in the power plant process compared to conventional separation technologies. To reduce CO2-emissions by 50 to 60% before 2050, a significant contribution of carbon capture and storage or use is required. Concerning the emissions from European fossil fuel power plants, the “European Industrial Initiative on CCS” wants to reach a near zero level until 2020 by means of economic feasible CCS technologies. After a further optimisation the technology will be transferred to other carbon-intensive industries. A significant cost reduction for oxygen production is expected to be achieved by Oxygen Transport Membranes (OTM), including lower efficiency losses as compared to today’s best cryogenic technology. This is a key requirement to make oxyfuel concepts a feasible future option for emission-free energy generation. The GREEN-CC process concept offers a very promising solution that has great potential in reducing the cost of CO2 capture. Companies like Linde AG, Thyssen Krupp Industrial Solutions, Shell worldwide leaders in their fields, will strongly participate in the GREEN-CC project in order to reinforce technology transfer. In addition to storage CO2 use is a relevant topic for future activities. In a world of increasing amount of renewable energies highly stable oxygen transport membranes like dual phase composites can be also used for “Power/Heat to X (Fuels or Chemicals)” technologies in a membrane reactor.
In the chemical industry, process intensification can be achieved through the integration of catalytic converters and membrane separators. High product selectivity is obtained through the control of oxygen dosing into the catalyst and reducing the risk derived from explosive mixtures air/methane in fixed bed reactor with concomitant reactant feeding. Process intensification strategy permits dramatic reductions in the size of operation units in chemical plants, in order to combine given production objectives with waste and energy consumption reduction. Air separation using OTMs operating at process temperature of the chemical reactions considered in this project – Oxidative coupling of methane – makes the use of methane as feedstock economically and ecologically attractive by energy saving, resulting in mitigation of CO2 emission.
Results from research work related to material development (WP1 and 2) and modelling (WP1.5, 2.1 and WP5) within GREEN-CC provide the basis for further technological development and industrial application. Development of membranes with high flux, high selectivity and stability, and a commercial level of throughput require (i) deep understanding of the physico-chemical and thermo-mechanical properties of complex multicomponent perovskites and thin films under application conditions, which is achieved here by computer modelling and (ii) reliable processing of thin film membranes with sufficient long-time stability in application conditions. The close to application or actual application condition material testing will be also be studied thoroughly (WP3). Another focus will be on the development and construction of a proof-of-concept module (WP4 and WP5). To achieve the overall goals of the project and to open up the perspective towards industrial implementation, it is very important to build a bridge between research and a potential industrial application.
The project partners are working towards commercialization of membrane technology, and acknowledges that open dissemination channels are the best means of gathering forces for this cause. GREEN-CC targets in the demonstration of an asymmetric thin-film oxygen transport membrane with superior performance with regard to high oxygen permeation, infinite oxygen selectivity, and high stability.

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