A Numerical Investigation of Electrically-Heated Methane Steam Reforming Over Structured Catalysts

The use of electric energy as an alternative system to provide heat of reaction enables the cut-off of CO2 emissions of several chemical processes. Among these, electrification of steam methane reforming results in a cleaner production method of hydrogen. In this work, we perform for the first time a numerical investigation of a compact steam reforming unit that exploits the electrical heating of the catalyst support. First, for such unit we consider the optimal thermodynamic conditions to perform the power to hydrogen conversion; the process should be run at atmospheric pressure and in a close temperature range. Then, among possible materials currently used for manufacturing structured supports we identify silicon carbide as the best material to run electrified steam reforming at moderate voltages and currents. The temperature and concentration profiles in idealized units are studied to understand the impact of the catalyst geometry on the process performances and open-cell foams, despite lower surface to volume show the best potential. Finally, the impact of heat losses is analyzed by considering different operative conditions and reactor geometries, showing that it is possible to obtain relatively high thermal efficiencies with the proposed methodology

A fundamental investigation of gas/solid mass transfer in open-cell foams using a combined experimental and CFD approach

In this work, we combine numerical (CFD) simulations and experimental measurements in a fundamental investigation of the fluid-solid mass transfer properties of open-cell foams, which are promising support for catalytic applications limited by external heat and mass transfer. CFD simulations are exploited to gain insight into the complex transport mechanisms and to enable a parametric analysis of the geometrical features by means of virtually-generated structures. Catalytic activity experiments under diffusion control are used to validate the CFD results and to extend the range of conditions and foam morphologies investigated. Analysis of the flow field by CFD simulations provides a rational basis for the choice of the average strut size as a physically sound characteristic length for mass transfer correlations. Results from both numerical simulations and experimental tests are interpreted according to a fully-theoretically based geometrical model for the prediction of the specific surface area, which accounts for the detailed node-strut geometry. The effects of cell size and strut shape are properly included in the functional dependence of the Sherwood number on the Reynolds number. The effect of porosity requires one additional dependence, wherein the Sherwood number is inversely proportional to the square of the void fraction. The resulting Sherwood–Reynolds correlation is in excellent agreement with experimental data and CFD simulations. It enables accurate (±15%) estimation of the external mass transfer coefficients for open-cell foams when coupled with the proposed geometrical model from two readily accessible pieces of geometrical information, i.e. the void fraction and either the cell size or the pore diameter of the foam. The derived correlation can be applied to the design of novel enhanced open-cell foam catalyst substrates and structured reactors

A systematic procedure for the virtual reconstruction of open-cell foams

Open-cell foams are considered a potential candidate as an innovative catalyst support in many processes of the chemical industry. In this respect, a deeper understanding of the transport phenomena in such structures can promote their extensive application. In this contribution, we propose a general procedure to recover a representative open-cell structure starting from some easily obtained information. In particular, we adopt a realistic description of the foam geometry by considering clusters of solid material at nodes and different strut-cross sectional shapes depending on the void fraction. The methodology avoids time-consuming and expensive measuring techniques, such as micro-computed tomography (μCT) or magnetic resonance imaging (MRI). Computational Fluid Dynamics (CFD) could be a powerful instrument to enable accurate analyses of the complex flow field and of the gas-to-solid heat and mass transport. The reconstructed geometry can be easily exploited to generate a suitable computational domain allowing for the detailed investigation of the transport properties on a realistic foam structure by means of CFD simulations. Moreover, the proposed methodology easily allows for parametric sensitivity analysis of the foam performances, thus being an instrument for the advanced design of these structures. The geometrical properties of the reconstructed foams are in good agreement with experimental measurements. The flow field established in complex tridimensional geometries reproduces the real foam behavior as proved by the comparison between numerical simulations and experiments

Electrified CO2 valorization driven by direct Joule heating of catalytic cellular substrates

The growing environmental concerns have driven catalytic CO2 valorization as a forward-looking solution to mitigate the carbon footprint of valuable chemical products. CO2 conversion processes into synthesis gas, such as CO2 reforming of methane (CRM) or reverse water–gas shift (RWGS), may have a strategic role for the future sustainable production of chemicals and energy carriers. However, fuel combustion to supply the heat of the associated endothermic reactions would result in unwanted CO2 emissions, frustrating the overall objective. Electrification of the endothermic processes may represent the technological solution to such an issue. Here we report a promising approach for the direct electrification of the CO2 reforming of methane (eCRM) and reverse water–gas shift (eRWGS) processes in washcoated structured reactors. We employ catalytically activated open-cell foams that provide optimal heat and mass transfer properties and serve as Joule heating substrates for the catalytic conversion of CO2 via reaction with methane or hydrogen. The proposed reactor system with Joule-heated Rh/Al2O3-coated foam exhibited excellent catalytic and electrical stability for more than 75 h, operating up to 800 °C and approaching equilibrium conversion at high space velocity, i.e., GHSV of 600 and 100 kNl/kgcat/h for eRWGS and eCRM, respectively. Such a reactor concept has potential to ensure remarkably low specific energy demand for CO2 valorization. Assuming an optimized process configuration approx. 0.7 kWh/Nm3CO2 is calculated for eRWGS. By replacing fuel combustion with Joule heating driven by renewable electricity, the electrified CO2 valorization processes provide an important approach for dealing with the intermittent nature of renewable sources by storing the energy in chemicals with a low carbon footprint

Investigation of packed conductive foams as a novel reactor configuration for methane steam reforming

Abstract In this work, a novel fixed bed reactor configuration is proposed and tested for the steam reforming of methane; the proposed solution consists of filling the voids of highly conductive metallic open-cell foams with small catalytic pellets. This reactor layout aims at enhancing the radial heat transfer of the tubular reactor by exploiting the thermal conductivity of the solid interconnected matrix, while keeping a target catalyst inventory and avoiding issues related to washcoating of metallic structures. Tests were performed using a Rh/Al2O3 catalyst in the form of alumina egg-shell particles, with diameter of 600 μm. FeCrAlY open cell foams of 12 PPI and copper open cell foams of 10 and 40 PPI were compared to a conventional packed bed system; experiments were performed at GHSV of 5000 and 10000 h−1 at oven temperatures in the 600–800 °C range. Experiments demonstrated a benefit in terms of the thermal management of the reactor and an increase of productivity at the same furnace temperature in kinetically-limited conditions. A heat transfer model of the packed foams was developed based on the approach of electric equivalent circuit; the model incorporates independently estimated lumped or effective parameters and provides an engineering rationale of the observed reduction of temperature gradients across the catalytic bed

Adoption of 3D printed highly conductive periodic open cellular structures as an effective solution to enhance the heat transfer performances of compact Fischer-Tropsch fixed-bed reactors

Abstract Heat transfer is universally recognized as a key challenge for the intensification of the Fischer-Tropsch (FT) process in compact fixed-bed reactors. For the first time in the scientific literature we demonstrate experimentally that the adoption of a highly conductive periodic open cellular structure (POCS, 3D-printed in AlSi7Mg0.6 by Selective Laser Melting) packed with catalysts pellets is a promising solution to boost heat exchange in fixed-bed FT reactors. This reactor configuration enabled us to assess the performances of a highly active Co/Pt/Al2O3 catalyst packed into the POCS at process conditions relevant to industrial Fischer-Tropsch operation. Unprecedented performances (CO conversion ≈ 80%) could be thus achieved thanks to an outstanding heat management. In fact, almost flat axial and radial temperature profiles were measured along the catalytic bed even under the most severe process conditions (i.e. high CO conversions corresponding to high volumetric heat duties), demonstrating the effective potential of this reactor concept to manage the strong exothermicity of the FT reaction. The heat transfer of the packed-POCS reactor outperformed both packed-bed and packed-foam reactors, granting smaller radial temperature gradients in the catalytic bed, as well as smaller temperature differences at the reactor wall, with larger volumetric power releases. The strengths of the packed-POCS reactor configuration are its regular geometry, which enhances the effective radial thermal conductivity, and the improved contact between the structure and the reactor wall, which governs the limiting wall heat transfer coefficient

Development of a Catalytic Fuel Processor for a 10 kW Combined Heat and Power System: Experimental and Modeling Analysis of the Steam Reforming Unit

In this work, we address the development of a combined heat and power unit for residential applications, fed by natural gas, air and H2O; focus is on the design of the first catalytic stage of the fuel processor, that is the steam reforming unit. A commercial catalyst was tested at the laboratory scale, under kinetically controlled conditions in order to derive information on the reaction kinetics and support the basic engineering of the full scale reactor. Analogous tests after long term steam reforming ageing were then performed to quantify the evolution of the catalyst activity under real operating conditions and estimate a lumped deactivation factor. A modelling analysis was performed to predict the expected performance of the fuel processor at varying input parameters and catalyst activity profiles. It was verified that at a space velocity below 5000 Nl/kgcat/h, the reactor output is fully controlled by the thermodynamics at 650 °C, which guarantees the best operability and efficiency of the whole fuel processo