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INTENT Report Summary

Project ID: 694910
Funded under: H2020-EU.1.1.

Periodic Reporting for period 1 - INTENT (Structured Reactors with INTensified ENergy Transfer for Breakthrough Catalytic Technologies)

Reporting period: 2016-11-01 to 2018-04-30

Summary of the context and overall objectives of the project

Critically important heterogeneous catalytic reactions for energy conversion and chemicals production have been run for decades in fixed bed reactors randomly packed with catalyst pellets, whose operation is intrinsically limited by slow heat removal/supply. There is urgent need for a new generation of process equipment and chemical reactors to address the current quest for process intensification.

In the INTENT project, we propose that a game-changing alternative is provided by structured reactors wherein the catalyst is washcoated onto or packed into structured substrates, like honeycomb monoliths, open-cell foams or other cellular materials, fabricated with highly conductive metallic (Al, Cu) materials.

The goal of INTENT is to fully elucidate fundamental and engineering properties of such novel conductive structured catalysts, investigate new concepts for their design, manufacturing, catalytic activation and operation (e.g. 3D printing, packed foams, energy supply by solar irradiation), and demonstrate their potential for a quantum leap in the intensification of three crucial catalytic processes for the production of energy vectors:

i) distributed Hydrogen generation via efficient small-size methane reformers

ii) conversion of syngas to clean synthetic fuels in compact (e.g. skid-mounted) Fischer-Tropsch Synthesis reactors

iii) production of solar Hydrogen.

To this purpose we will combine advanced CFD modelling with lab-scale experimentation in order to identify the optimal structure-performance relation of existing and novel substrates, use such new knowledge to design optimized prototypes, apply unconventional additive manufacturing technologies for their production, and construct a semi-industrial tubular pilot reactor to test them at a representative scale.

The project results will enable novel reactor designs based on tuning geometry, materials and configurations of the conductive internals to match the activity – selectivity demands of specific process applications, while impacting also other research areas.
The new reactor technology will have significant impact on both the Energy and on the Environmental scenarios. Just as an example, it will enable compact Gas-to-Liquids process technologies with potential to drastically reduce flaring of associated and remote Natural Gas.

Work performed from the beginning of the project to the end of the period covered by the report and main results achieved so far

Task 1 - As a first step in the fundamental investigation of the transport properties of open-cell foams, viewed as enhanced catalyst substrates, an original procedure for the digital reconstruction of foams starting from two easily accessible pieces of information, i.e. porosity and pore size, has been developed and validated. It produces faithful replicas of real foams, but can be used also to generate virtual foams with variable geometric features, suitable for numerical simulations aimed at analysis and optimization work.
Accordingly, pressure drops, heat and mass transfer properties of open-cell foams have been extensively investigated using an original approach combining dedicated experiments with CFD simulations. This has enabled covering a very broad, unprecedented range of geometric and flow variables. The results have been fully rationalized, producing a dimensionless correlation for fluid/solid mass transfer coefficients and an engineering analysis of heat conduction in open-cell foams. The latter provided indications on the optimal design of the foam matrix in order to maximize the effective thermal conductivity for a given solid mass.
Two papers have been already published on these topics, three more are submitted or in preparation.
The fundamental research is continuing in three different directions: i) characterization of the heat transfer properties of washcoated foams under reactive conditions: to this purpose, an existing rig for heat transfer measurements has been converted to run CO oxidation experiments while measuring the temperature field in the coated foam catalysts; ii) characterization of the heat transfer properties of foams packed with catalyst microparticles as an alternative method for catalytic activation; iii) characterization of the transport properties of Periodic Open Cellular Structures (POCS) fabricated by 3D printing.

Task 2 - Right at the beginning of the project, work has been devoted to develop effective washcoating methods for the catalytic activation of open-cell metallic foams, both in view of the general goals of INTENT and in order to prepare foam catalysts suitable for testing in the other Tasks of the project. Specifically, the innovative method of spin coating has been systematically compared to the conventional dip coating approach, revealing improved uniformity of the deposited catalytic layers and better control of the coating characteristics. Spin coating has been therefore identified as the method of choice for the preparation of coated structured catalysts in INTENT. One publication on this topic is in preparation. The alternative method for catalytic activation of cellular substrates investigated in INTENT relies on packing the structures (open-cell foams, POCS) with catalyst micro-particles. A fundamental study of the factors which influence the loading of the catalyst particles into the cellular structures, determining e.g. the overall catalyst inventory per unit volume, has recently started.
Additive manufacturing (3D printing) of Periodic Open Cellular Structures (POCS) made of aluminium has started early in the project thanks to a collaboration with the group of Professor Stefano Beretta at the Department of Mechanical Engineering of Politecnico di Milano. Such regular cellular materials offer additional degrees of freedom over open-cell foams for the design of optimized catalyst substrates, and look therefore very promising for process intensification. A few samples with different geometrical and structural features have been produced so far: their geometries are suitable for testing in the existing rigs, and they will be characterized in the near future by pressure drop, heat and mass transfer measurements, also in combination with CFD simulations. A mechanical characterization is being also performed at the Department of Mechanical Engineering.

Task 3 - A test facility including a pilot-scale jacketed tubular reactor has been designed in details, in view of

Progress beyond the state of the art and expected potential impact (including the socio-economic impact and the wider societal implications of the project so far)

"Significant progress beyond the state of the art existing at the beginning of the INTENT project has been achieved so far in the following areas:

- Geometrical and digital characterization of open-cell foams and other cellular substrates: in particular, the developed methodology for the virtual reconstruction of foams is fully original, and is already attracting attention.

- Analysis of the transport properties of cellular substrates: the combination of experiments and CFD simulations is a methodological approach first successfully demonstrated in INTENT for the investigation of gas/solid heat and mass transfer in open-cell foams.

- Activation of cellular substrates by packing them with catalyst particles: data on the transport properties of ""packed foams"" and ""packed POCS"", a new concept, was not available and is now being collected and rationalized.

- Application of conductive packed foams to the Fischer-Tropsch synthesis: in INTENT we have demonstrated experimentally for the first time that the adoption of thermally conductive cellular internals enables to run the extremely exothermic and temperature-sensitive Fischer-Tropsch synthesis in lab-scale tubular reactors up to very high CO conversion levels, corresponding to very large heat duties; this is impossible using a conventional packed-bed reactor configuration, which becomes unstable already at much lower CO conversion levels.

The above listed preliminary results seem very promising in view of the identification, realization and demonstration of enhanced reactor technologies for the intensification of key catalytic processes in the area of energy conversion, which is the final goal of the INTENT project.

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