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Report

Teaser, summary, work performed and final results

Periodic Reporting for period 3 - ROMEO (Reactor optimisation by membrane enhanced operation)

Teaser

Summary

\"ROMEO has been developing a new reactor concept using homogeneous catalysis and membrane technology to carry out chemical synthesis and downstream processing in a single step. Process intensification for catalytic-driven and eco-friendly reaction systems will be brought to a new level thanks to this two-in-one reactor. Thus, ROMEOâ€™s reactor will improve efficiency and long-term sustainability for the process industry.

Processes for bulk chemicals and bio-energy applications have been chosen to demonstrate the efficiency of ROMEOâ€™s technology in a near industrial environment. ROMEOâ€™s reactor includes a ceramic monolith for the fixation of the homogenous catalyst with a fixed membrane on top of it. Chemical synthesis and separation are carried out in a single step thanks to the membrane. In this \"\"two-in-one\"\" reactor, the product is continuously removed from the reaction mixture as soon as it is formed.

The applicability of this revolutionary technology was demonstrated in two mini plants for hydroformylation (HyFo) and water-gas-shift (WGS) reaction. The first facility converts olefins and syngas to aldehydes. The mini plant was successfully operated for more than 5000 h showing the proposed benefits in energy savings of up to 70%, improved process outlets in an industrial near environment as well as estimated OPEX and CAPEX savings.

The demo plant for the water-gas-shift reaction uses CO or CO-containing syngas derived from biomass to generate hydrogen from biogenic waste materials, for example wood waste. The principle application of the ROMEO technology to the water-gas-shift process could also be successfully shown within the project under lab conditions applying a new membrane system for CO2 separation on a monolithic structure. However, under industrial near conditions impurities from the feed stream hindered a stable long-term process operation. To solve this, further investigations and optimization are necessary.

Besides demonstration ROMEO intended to get a detailed understanding of the processes involved in its new reactor, from nanoscale (catalyst phase, membrane, transport across and inside the membrane) to macro-scale (e.g. heat and mass flow, industrial process design). The gained know-how was used to develop a flexible reactor design methodology for ROMEO. The developed tool-box will allow to evaluate the applicability of ROMEOÂ´s technology for a wide range of further applications.

Further optimization of that technology, broadening to other applications and scale-up to pilot plant application in a production environment will be realized in the MACBETH project (GA 869896).\"

Work performed

Membrane development: After determining reaction conditions and purity requirements, available membrane systems and their applicability under the given conditions have been considered. The first separation concept of the WGS case had to be changed. A membrane coating technology for thin and dense layers on ceramic support material has been developed and samples for further processing have been prepared.

Immobilization of catalytic system: Support structures for membrane modules have been determined and optimized, samples and strategies for catalyst immobilization and characterization of the coated systems provided, and the catalyst system has been optimized.

Catalytic membrane systems feasibility: Reaction conditions have been determined and experimental and analytical set-up have been done. After catalyst tests on support structures, the catalyst and membrane system has been tested under near industrial conditions.

Methodology development: The model set-up has been discussed, boundary conditions determined and support for establishing a reaction and diffusion model provided. A short cut modelling has been performed and applied to a ROMEO tool box.

Reactor design: The reactor design was done in close cooperation between the partners. Besides general design aspects a scale and numbering-up concept was realized.

Demonstration: Two mini plants have been set up at different sites and operated for the two prominent reactions under industrial near conditions for more than 5000 h (HyFo) and 1500 h (water-gas-shift). A life time cycle assessment for the catalyst/membrane module with data from demonstration trials has been done.

Dissemination and business plan: A home page, several project newsletters, videos, press releases etc. have been done as well as a 2- day workshop on membrane reactor technology and 35 oral/poster presentations Eight scientific publications have been done, seven patent applications submitted and a proposal for a business plan has been elaborated.

Selected main results and their exploitation
- Monoliths coated with a dense and thin membrane layer. Exploitation for HyFo, WGS and other chemical reactions.
- 2D membrane reactor model in ACM. Exploitation for a priori design of gas phase membrane reactors.
- Shortcut membrane reactor model. Exploitation for optimization of gas phase membrane reactors.
- Insitu preparation and immobilization of catalytic system. Exploitation for Hyfo + further applications.
- Seven submitted patent applications for HyFo related processes. Exploitation for Hyfo.
- Membrane reactor design for monolithic supported ionic liquid phase catalysis. Exploitation for Gas-phase catalysis and separation processes in a laboratory scale.
- Four intended patent applications for reactor types, components and coating. Exploitation for WGS and other syngas applications, HyFo, oxydations, hydrogenations and gas phase catalysis.
- Hybrid SILP-CNT materials for catalysis. Exploitation for HyFo, WGS and catalytic processes.

An important activity to exploit the results is the successor project MACBETH (GA 869896 started on 01 Nov 2019) in order to bring the technology to higher TRLs and to broaden the application scope to further application cases.

Final results

The integration of reaction and downstream processing steps into a single unit is of central importance in order to achieve a new level of process intensification for catalytic driven and ecofriendly reaction systems. This disruptive technology concept is able to achieve important socio-economic impacts.

The new technology concept has been proven and demonstrated by two prominent large volume reaction types as examples for the majority of industrial relevant reaction classes:
- Processes with undesired consecutive reactions like hydroformylation (HyFo)
- Equilibrium driven reactions like water gas shift (WGS) reaction.

Thus, ROMEO has brought the innovative catalytic membrane reactor technology from TRL 3 to TRL 5, overcoming existing challenges through an inter-disciplinary approach and development of an integrated reactor technology platform. It features a broadly applicable integration of reaction and subsequent downstream processing steps into a process intensified single reactor concept.

The main socio-economic impacts of the ROMEO technology are concerning the following dimensions and an impact analysis for four application cases delivered quantitative results.
- Decrease in greenhouse gas (GHG) emission: -20 % to -45 %
- Increase in resource and energy efficiency (RE): +20 % to +70 %
- Novel modular and scalable integrated (upstream-downstream) installations with considerable decrease in CAPEX (-15 % to -50 %) and OPEX (-16 % to -80 %).