Periodic Open Cellular Structures Research Articles

Conceptual study on the intensification of gas–liquid mass transfer in trickle bed reactors by the application of strut-based and novel sheet-based periodic open cellular structures (POCS)

Rapid progress in the development of additive manufacturing technology enables the production of structured reactor internals of complex geometry. To address mass transport limitations structured internals can be used in trickle bed reactors (TBRs) as the most frequently used reactor for heterogeneously catalyzed multiphase reactions. However, reactions in TBRs are frequently limited by gas–liquid mass transfer.As periodic open cellular structures (POCS) as reactor internals were not addressed regarding g–l mass transfer yet, this contribution provides first data on gas–liquid mass transfer for different types of POCS. Therefore, desorption of dissolved oxygen in water with nitrogen gas and the two-phase pressure drop were measured. Strut-based Kelvin and diamond unit cell POCS were compared to a sphere random packed bed as a benchmark. A novel sheet-based unit cell was developed realizing meandering channels demonstrating a fivefold increase in volumetric mass transfer coefficient compared to the benchmark. To compare the performance of the setup with literature data, state of the art neural network correlations were used for comparison. This proof of concept highlights the potential of additively manufactured POCS for intensified processes in trickle bed reactors, and demonstrates their versatility in application.

Periodic Open Cellular Structures in Chemical Engineering: Application in Catalysis and Separation Processes.

Periodic open cellular structures (POCS) represent a promising new class of structured internals as next-generation catalyst supports in reactors or structured packing elements in separation columns. POCS feature a well-defined morphology and can be fabricated with high reproducibility even for complex geometries by means of additive manufacturing. This results in a uniform and easily controllable flow field, which allows for adjusting the heat and mass transport processes to realize optimal process conditions. We review the fundamentals of POCS, including design and manufacturing as well as transport phenomena for single- and multiphase systems. Moreover, we review recent POCS applications in reaction and separation processes and consider promising future application fields. The exceptional transport characteristics of POCS facilitate the design of highly efficient, flexible, resilient, and safe processes, which is key for achieving process intensification toward a sustainable future.

Modelling of heat transfer and pressure drop during flow boiling of CO2 in a horizontal tube with periodic open cellular inserts

During flow boiling in horizontal tubes, highly porous inserts can improve the wetting of the tube wall and the convective boiling. The literature focuses on solid sponge structures with irregular cell geometries. Hence, in this work the local heat transfer and pressure drop during flow boiling of CO2 in periodic open cellular structures with cubic and Kelvin cell geometry were investigated. A strong influence of the cell geometry on the heat transfer and pressure drop was found. By combining the Forchheimer term with a two-phase flow method (homogeneous model, drift flux model) a new pressure drop model is proposed. The model has a mean absolute percentage error (MAPE) of 12%. Regarding the heat transfer, high-speed video recordings and an evaluation of the local heat transfer were used to test the tube segments for complete wetting. Thereafter, the convective boiling contribution was extracted from the local data of completely wetted tube segments by subtracting the nucleate boiling contribution. A separate model of the convective boiling is proposed for each cell type. The models have a MAPE of 20%. Finally, the circumferentially averaged heat transfer coefficient was found to follow a superposition of the heat transfer of the liquid and vapor phase.

Comparison of thermo-hydraulic performance among different 3D printed periodic open cellular structures

As additive manufacturing of periodic open cellular structures (POCS) is gaining interest in structured catalytic reactor research, this work seeks to thermohydraulically compare the well-known Kelvin lattice structure with the lesser-researched BCC and gyroid lattice structures. Using a combined CFD (Computational Fluid Dynamic) and experimental approach, the selected POCS are fabricated through Laser Powder Bed Fusion (LPBF), characterized, and subsequently subjected to numerical analysis. From the manufacturability point of view, the 3D printed samples closely matched their CAD designs, showing a maximum porosity deviation of 15% below design values. A CFD model, validated through pressure drop experiment, was employed to compare the POCS designs on shared geometric attributes such as specific surface area and porosity. While all structures exhibited comparable performance in term of heat and momentum transfer, our findings suggest that the Gyroid lattice may provide the optimal balance between momentum and heat transfer rates in low-velocity region. Conversely, the BCC configuration may be more favourable at higher velocity. An Ergun-like correlation was also developed and validated for each lattice type, with a Mean Absolute Percentage Error (MAPE) below 10%. Our pressure drop results align quite well with existing literature correlations, showing a MAPE under 20%. Concerning heat transfer, the values forecasted in this research show a reasonable alignment with literature’s results, though they tend to be on the lower spectrum.

Periodic open cellular structures (POCS) as catalyst support for intensified heat transport in the partial oxidation of methanol to formaldehyde

Heat transport in catalytic reactors is one of the most important factors in reactor design, especially for highly endo- or exothermic reactions. The limited thermal conductivity of randomly packed beds can be significantly improved when alternative catalyst supports are used. A new generation thereof are periodic open cellular structures (POCS), which are used in this study as catalyst support for the partial oxidation of methanol to formaldehyde, an exothermic gas phase reaction. A comparison to traditional packed bed reactors revealed that a POCS made of the highly conductive alloy AlSi10Mg can significantly reduce the hot-spot temperature, allowing almost isothermal operation at optimal reaction conditions. The improved temperature control allows for operation with higher methanol inlet concentrations and wall temperatures as compared to the commercial process. The beneficial heat transport properties of POCS were used to conduct isothermal kinetic measurements at elevated temperature. Based on these findings and the design freedom of additive manufacturing, an optimized cellular structure was designed and fabricated, which improved the heat transport especially in the critical inlet section of the reactor.

Reactor design via scan line patterning: An implicit approach to create scalable microstructured parts in selective laser melting

The adaptation of additive manufacturing for chemical flow reactors has recently gained momentum as the methods become more advanced and equipment is increasingly affordable. With the design of periodic open cellular structures (POCS) from metal selective laser melting (SLM), structured catalyst substrates can be realized in a much more ordered fashion than well-established metal foams with a random structure. Hence, tailored transport properties are achieved and flow profiles are homogenized, eliminating flow channeling and stagnant flow zones.However, with current SLM methods, the minimal achievable feature size and therewith the specific surface area is still limited. Moreover, the size of finely resolved STL files that define the structure grows exponentially with decreasing feature sizes, further limiting the scalability of methods with direct structure definition.In this work, we present a method for implicit structure design by metal SLM with specific surface areas and porosities that compete with established catalyst substrates. The definition of the microstructure is realized by control of the laser scan lines, where single scan lines create fine struts. The general applicability of our method to various metal materials is demonstrated by production from stainless steel and copper. In a numerical study for a model steam reforming application, we show that the POCS provide mass transfer coefficients and volumetric reaction rates that compete with benchmark substrates.Scan line patterning therefore provides a promising method to create highly ordered, well-scalable substrates for heterogeneous catalysis from a wide range of materials, e.g., for the application in highly efficient small-scale reactors.

Detailed numerical investigations of the in operando adjustable flow field in a diamond unit cell-based interpenetrating periodic open cellular structure (interPOCS)

In the field of heterogeneous catalysis, additively manufactured so-called Periodic Open Cellular Structures (POCS) applied as catalyst supports have demonstrated their advantages over conventional randomly packed bed reactors in terms of heat management and pressure drop (Busse et al., 2018; Inayat et al., 2016). Since the internal flow field and the pressure drop are mainly influenced by the geometrical properties of the unit cell (unit cell type, strut diameter and cell size), the resulting transport characteristics of the structure is already determined during the design phase of the unit cell (Horneber, 2015). By inserting one POCS based on a diamond unit cell (offset structure) into the cavities of a second diamond cell structure (fix structure), a completely new type of so-called interpenetrating Periodic Open Cellular Structures (interPOCS) is formed which allows for an in operando adjustment of the global and local morphological properties of the structure (Do et al., 2017; Do et al., 2020). With detailed, spatially resolved computational fluid dynamics (CFD) simulations using the open source toolbox OpenFOAM® (Weller et al., 1998) and an additional in-house random-walk particle tracking implementation called disTrackFoam (Trunk et al., 2021), we systematically investigated the local and global flow characteristics within the interPOCS in dependency of the relative positioning of the fixed and offset structure. The obtained results show that this highly adjustable structure allows for a broad variation of flow characteristics in a chemical reactor without changing the system’s periphery. This study demonstrates that interPOCS represent a completely new application of additively manufactured catalyst support structures enabling highly flexible in operando tuning of the flow field and mass transport in a heterogeneously catalyzed reactor system.

Process intensification in mass-transfer limited catalytic reactors through anisotropic periodic open cellular structures

We propose an advanced design of catalyst supports based on Periodic Open Cellular Structures (POCS) with a modified diamond unit cell. The diamond unit cell is modified by changing the angle between the struts and the fluid direction, thus changing the fluid-solid interaction and consequently the gas-solid mass and momentum transfer properties. Computational Fluid Dynamics is employed to fundamentally investigate the transport phenomena, and to carry out a parametric investigation of the effects of the morphological properties (i.e., struts angle, porosity and unit cell size). A drastic reduction of the friction factor (i.e., up to 50%) at moderate reduction of the mass transfer coefficient (i.e., up to 30%) is observed in the modified configuration upon progressively aligning the struts with the flow direction. This results in an overall improvement of the trade-off between the two properties leading to superior overall performances compared to state-of-the-art structured substrates. Unifying engineering correlations are then developed based on the numerical results for the evaluation of mass transfer coefficients and friction factors of the POCS, describing the behaviour of both the conventional and the modified cellular structure.

CFD Investigation of an Innovative Additive Manufactured POCS Substrate as Electrical Heated Solution for After-Treatment Systems

In the last decade, additive manufacturing (AM) techniques have been progressively applied to the manufacturing of many mechanical components. Compared to traditional techniques, this technology is characterized by disruptive potential in terms of the complexity of the objects that can be produced. This opens new frontiers in terms of design flexibility, making it possible to create new components with optimized performances in terms of mechanical properties and weight. In this work, the focus is on a specific field of application: the development of novel porous media structures which can be the basis of advanced after-treatment systems for internal combustion engines. In particular, the possibility to design periodic open cellular structures (POCSs) that can be applied as catalytic substrates opens new perspectives in terms of flexibility and integrated functionalities. The present study investigates an innovative solution where the catalytic substrates are located in the pipes of the exhaust manifolds of a high-performance engine. A preliminary characterization of the pressure drop induced by the POCS structure is carried out, with a particular focus on the impact of the backpressure on the engine performances. Moreover, each POCS integrates an electrical circuit which is used to promote the heating of the device, with beneficial effects on the light-off of the catalytic reactions. An advanced CFD model is applied to evaluate the potential of the solution, comparing the pollutant conversion with that of the baseline configuration equipped with a standard after-treatment system solution.

3D-Printed Raney-Cu POCS as Promising New Catalysts for Methanol Synthesis

Simultaneous generation and activation of Raney-type periodic open cellular structures (POCS) is a highly promising approach for generating novel structured methanol synthesis catalysts. In detail, we produced stable and highly active POCS from a Cu50Al50 alloy by additive manufacturing via Powder Bed Fusion by Electron Beam (PBF-EB) and activated them via selective leaching of aluminum in a sodium hydroxide/sodium zincate solution. The Raney-type Cu structures possessed catalytic methanol productivities of up to 2.2 gMeOHgnp-Cu h−1 (PBF-EB sticks) and 1.9 gMeOHgnp-Cu h−1 (PBF-EB POCS), respectively. Moreover, it was found that besides the nanoporous layer thickness, an optimum Zn/Cu ratio of 0.3–0.4 can also by adjusted by the leaching conditions.

Periodic Open Cellular Structures (POCS) as Catalyst Supports—A Review

Periodic open cellular structures (POCS) are becoming increasingly popular as catalyst carriers due to favorable properties: mixing flow, intense heat/mass transfer and low flow resistance. Their design and manufacturing are relatively easy and cheap. The presented paper focuses on the characterization of POCS in relation to their definition, types, classification and properties. Next, the design and manufacturing methods are described. Finally, the literature review dealing with the application of POCS in catalytic processes are presented.

Modelling steady-state convective heat transfer in different periodic open cellular structures (POCS) – A superposition approach

Additively manufactured periodic open cellular structures (POCS) offer promising attributes for the intensification of heat transfer processes. Their geometry and consequently thermal transport properties are highly customizable resulting in a vast design freedom. To fully exploit their potential, a detailed understanding of the relationship between their geometric and thermal transport properties is crucial. Therefore, in this contribution the convective heat transfer in four different unit cell geometries and varying cell dimensions during fully developed laminar steady-state flow is investigated. Numerical simulations are used to get a detailed insight of the local flow structures and heat flux density distributions. A correlation between the heat transfer coefficient of each unit cell and the heat transfer capability of unconnected strut arrangements with similar flow paths is introduced. On this basis, a new modelling approach is established in combination with the concept of superposition. It takes into account the detailed geometry of the porous medium and shows good agreement with the simulation data of all unit cell geometries studied in this work with porosities above 79.1%. Thus, it is the first model applicable to different types of unit cells.

In Search of an Effective Workability Zone during the 3D Printing of Polymeric Periodic Open Cellular Structures Potentially Useful as Microreactors

The question of how easy the transition is between design and manufacturing by the 3D printing of periodic open cellular structures occurs from the analysis of cases in which additive manufacturing and heterogeneous catalysis merge. The synergy between these two fields suggests that one of the great advantages that the catalysis of this manufacturing methodology can take advantage of is the obtaining of advanced designs that would allow improving the processes from the geometry of the reactors. However, not all 3D-printing techniques offer the same degree of resolution, and this uncertainty grows when using more complex materials to work with, such as ceramics or metals. Therefore, the present work seeks to answer this question by finding experimentation strategies, starting with a simple case study inspired by the additive manufacturing–catalysis combination, in which a ceramic polymer resin of high thermal resistance is used to obtain POCSs that are potentially useful in thermochemical or adsorption processes. This exploration concludes on the need to define limits for what we have called an “effective work zone” that combines both design criteria and the real possibility of printing and manipulating the pieces, making sweeps in structural parameters such as cell size and the diameter of struts in the POCS. Similarly, the possibility of coating these systems with inorganic oxides is explored, using a generic oxide (Al2O3) to analyse this scenario. Finally, a cartridge-type assembly of these systems is proposed so that they can be explored in future processes by other researchers.

Improving the radial heat transport and heat distribution in catalytic gas-solid reactors

Improving the radial heat transport or the heat distribution is a paramount aspect for the sustainable and safe operation of catalytic gas-solid reaction systems. In this perspective, the recent advances in this field are summarized and critically discussed, i.e., particle shape modification of random packed beds, structured reactors including foams, monoliths, and periodic open cellular structures, internals in packed beds, as well as alternative concepts for energy input like induction, Ohmic, and microwave heating. The role of detailed modeling to advance this field will be emphasized and future research needs are presented.

Numerical and Experimental Investigation of Pressure Drop in Periodic Open Cellular Structures for Intensification of Catalytic Processes

Periodic Open Cellular Structures are envisioned as potential enhanced catalyst substrates for heat and mass transfer-limited processes. To enable their rational design, in this study, we propose a combined numerical and experimental approach to assess the pressure drop in the tetrakaidekahedral and diamond lattices since generalized correlations are not present in the literature. Deviations are observed between the model predictions available in the literature, which are possibly due to the different methods of investigation, that is, numerical on ideal geometries and experimental on reproductions. To reconcile the two approaches and prevent discrepancies, careful attention is paid here to the quality of 3D-printed replicas for experimental investigation to obtain results representative of ideal lattices. Computational Fluid Dynamics simulations and experiments are then employed together to cross-validate the results and then to perform a parametric analysis of the effect of the morphological properties on the pressure drop. The effect of the cell size and the porosity are discussed, enabling the derivation of engineering correlations for the prediction of the pressure drop across the lattices within the range of 1 < Reds < 300. Finally, the performances of lattice materials are compared with those of conventional structured supports by evaluating the trade-off between the fluid–solid mass transfer rate and the pressure drop, which is crucial for several catalytic processes. Results show that the diamond lattice outperforms other cellular materials and can outperform ceramic honeycomb monoliths at low Reynolds numbers.

Recent Advances in the Development of Highly Conductive Structured Supports for the Intensification of Non-adiabatic Gas-Solid Catalytic Processes: The Methane Steam Reforming Case Study

Structured catalysts are strong candidates for the intensification of non-adiabatic gas-solid catalytic processes thanks to their superior heat and mass transfer properties combined with low pressure drops. In the past two decades, different types of substrates have been proposed, including honeycomb monoliths, open-cell foams and, more recently, periodic open cellular structures produced by additive manufacturing methods. Among others, thermally conductive metallic cellular substrates have been extensively tested in heat-transfer limited exo- or endo-thermic processes in tubular reactors, demonstrating significant potential for process intensification. The catalytic activation of these geometries is critical: on one hand, these structures can be washcoated with a thin layer of catalytic active phase, but the resulting catalyst inventory is limited. More recently, an alternative approach has been proposed, which relies on packing the cavities of the metallic matrix with catalyst pellets. In this paper, an up-to-date overview of the aforementioned topics will be provided. After a brief introduction concerning the concept of structured catalysts based on highly conductive supports, specific attention will be devoted to the most recent advances in their manufacturing and in their catalytic activation. Finally, the application to the methane steam reforming process will be presented as a relevant case study of process intensification. The results from a comparison of three different reactor layouts (i.e. conventional packed bed, washcoated copper foams and packed copper foams) will highlight the benefits for the overall reformer performance resulting from the adoption of highly conductive structured internals.

Development of a generalized thermal resistance model for the calculation of effective thermal conductivities in periodic open cellular structures (POCS)

Periodic open cellular structures (POCS) are a group of porous media with promising attributes for the use in heat transfer enhancement. They consist of a periodic arrangement of unit cells that offer a vast design freedom and therefore high adaptability to the needs of a specific application. In order to use POCS efficiently, a fundamental understanding of the relation between their geometry and thermal transport properties is essential.This contribution focuses on the investigation and modeling of the effective thermal conductivity. It is based on a homogenization approach that averages the heat conduction properties over an entire unit cell, while neglecting the influence of the fluid. To this end, the investigation provides detailed insight and an important component for the subsequent model development on the overall heat transfer capabilities of POCS, including convection and conjugate heat transfer. A numerical simulation setup is developed, which allows the determination of this quantity in isotropic as well as anisotropic POCS with varying unit cell type, porosity, tapering and strut cross-sectional shape. The results indicate the impact of both struts as well as nodes, on the heat transfer and form the foundation for a new generalized thermal resistance network model. In contrast to similar approaches, the impact of multidimensional heat transfer within the nodes is considered enabling an accurate prediction of the effective thermal conductivity of all POCS investigated in this work. Due to its modularity, it is easily transferable to other unknown geometries, thus contributing to the toolbox for the efficient design of POCS.

Detailed investigation of liquid distribution and holdup in periodic open cellular structures using computed tomography

Periodic open cellular structures (POCS) show great potential for process intensification in catalytic reactors due to their favorable properties regarding heat transfer, pressure drop and liquid distribution. In multiphase applications, POCS can be employed as multifunctional catalyst carrier with integrated liquid distribution function for enhancing the performance of heterogeneously catalyzed reactions. This applies particularly to trickle bed reactors where a uniform liquid distribution is of great importance. In this contribution, the liquid distribution of three POCS of different unit cell geometry is investigated using a custom-made computed tomography scanner with high spatial resolution. POCS with the Kelvin, diamond and DiaKel unit cell, respectively, were manufactured via fused deposition modeling out of acrylonitrile butadiene styrene. The liquid distribution was examined in dependence of the unit cell as well as for different liquid and gas flow rates. The three POCS show different behavior for the liquid distribution and holdup within the structures. POCS with Kelvin and DiaKel unit cell geometry show a higher liquid holdup as well as a more uniform liquid distribution compared to diamond unit cell POCS. Also, the liquid filling between the individual POCS that are stacked in the column is dependent on the unit cell.

A Fundamental Investigation of Gas/Solid Heat and Mass Transfer in Structured Catalysts Based on Periodic Open Cellular Structures (POCS).

In this work, we investigate the gas–solid heat and mass transfer in catalytically activated periodic open cellular structures, which are considered a promising solution for intensification of catalytic processes limited by external transport, aiming at the derivation of suitable correlations. Computational fluid dynamics is employed to investigate the Tetrakaidekahedral and Diamond lattice structures. The influence of the morphological features and flow conditions on the external transport properties is assessed. The strut diameter is an adequate characteristic length for the formulation of heat and mass transfer correlations; accordingly, a power-law dependence of the Sherwood number to the Reynolds number between 0.33 and 0.67 was found according to the flow regimes in the range 1–128 of the Reynolds number. An additional −1.5-order dependence on the porosity is found. The formulated correlations are in good agreement with the simulation results and allow for the accurate evaluation of the external transfer coefficients for POCS.

Development and evaluation of a new particle tracking solver for hydrodynamic and mass transport characterization of porous media – A case study on periodic open cellular structures

The detailed understanding of local mass transport characteristics in porous catalyst supports is essential for the evaluation of their performance in reaction engineering applications. This applies particularly for the development and assessment of novel concepts such as additively manufactured periodic open cellular structures (POCS). A major drawback of the frequently used Eulerian based mass transport simulation methods is their tendency to overestimate molecular diffusion due to artificial numerical diffusion, especially in the range of high Péclet numbers (boundary-layer dispersion and pure mechanical dispersion regime) that is often encountered in industrial applications.To overcome this problem, we present a new efficient solver implementation for the OpenFOAM® simulation toolbox based on the Lagrangian Random Walk Particle Tracking method to calculate the mass transport via a deterministic convective and a stochastic diffusion term. Besides the numerical calculation of effective diffusion as well as dispersion coefficients, the new solver is also capable of analyzing residence time behavior, flow tortuosity and contact patterns with catalytically active surfaces of catalyst support structures in detail. Following a thorough validation study, we demonstrate the evaluation options provided by the results of this new solver named disTrackFoam on the example of three POCS with distinct unit cell types.