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energies Article Kinetics and Reactor Design Aspects of Selective Methanation of CO over a Ru/γ-Al2O3 Catalyst in CO2/H2 Rich Gases † Panagiota Garbis, Christoph Kern and Andreas Jess * Chair of Chemical Engineering, Center of Energy Technology, University Bayreuth, 95440 Bayreuth, Germany; panagiota.garbis@uni-bayreuth.de (P.G.); christoph.kern@uni-bayreuth.de (C.K.) * Correspondence:jess@uni-bayreuth.de;Tel.:+49-(0)-921-55-7430 † The original paper was presented in: Garbis, P., Kern, C., Jess, A. Selective CO methanation for PEMFC applications. Riehl, R., Preißinger, M., Eames, I., Tierney, M., Eds. In Proceedings of the Heat Powered Cycles Conference 2018, Bayreuth, Germany, 16–19 September 2018. ISBN: 978-0-9563329-6-7. Received: 11 January 2019; Accepted: 30 January 2019; Published: 1 February 2019 Abstract: Polymer electrolyte membrane fuel cells (PEMFCs) for household applications utilize H2 produced from natural gas via steam reforming followed by a water gas shift (WGS) unit. The H2-rich gas contains CO2 and small amounts of CO, which is a poison for PEMFCs. Today, CO is mostly converted by addition of O2 and preferential oxidation, but H2 is then also partly oxidized. An alternative is selective CO methanation, studied in this work. CO2 methanation is then a highly unwanted reaction, consuming additional H2. The kinetics of CO methanation in CO2/H2 rich gases were studied with a home-made Ru catalyst in a fixed bed reactor at 1 bar and 160–240 ◦C. Both CO and CO2 methanation can be well described by a Langmuir Hinshelwood approach. The rate of CO2 methanation is slow compared to CO. CO2 is directly converted to methane, i.e., the indirect route via reverse water gas shift (WGS) and subsequent CO methanation could be excluded by the experimental data and in combination with kinetic considerations. Pore diffusion may affect the CO conversion (>200 ◦C). The kinetic equations were applied to model an adiabatic fixed bed methanation reactor of a fuel cell appliance. Keywords: ruthenium catalyst; CO methanation; kinetic modeling; fixed bed reactor; process simulation 1. Introduction In recent years, the interest in proton-exchange membrane fuel cells (PEMFCs), also known as polymer electrolyte membrane fuel cells, for stationary applications such as households or office buildings has increased [1]. PEMFCs cogenerate electrical power and heat (heated water) from hydrogen (and O2/air) and reach about 80% overall efficiency. Home fuel cells cannot generate at all times exactly the needed amount of both heat and electricity, and are typically combined with a traditional furnace (e.g., with natural gas as fuel) and households are also connected to the electrical grid to cover the need of heat and electricity not produced by the fuel cell. Today, pure H2 is rarely directly available. Hence, home fuel cells currently use H2 produced from natural gas from the gas grid. Natural gas is firstly converted by steam reforming (CH4 + H2O ↔ CO + 3H2) followed by a water gas shift (WGS) reactor (CO + H2O ↔ CO2 + H2) to decrease the concentration of CO (and to increase the output of H2). However, the WGS is limited by thermodynamic constraints, and the H2 rich gas still contains small amounts of CO at the outlet of the WGS, typically 0.5–1 vol% CO [2,3]. Unfortunately, even traces of CO deactivate the anode electro-catalyst of the PEMFC. Therefore, the CO content must not exceed 10 ppm for Pt-anodes and Energies 2019, 12, 469; doi:10.3390/en12030469 www.mdpi.com/journal/energiesPDF Image | Selective Methanation of CO over a Ru-y-AI2O3 Catalyst in CO2 H2
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