Cross-contamination; Membrane permeance; Microreactor; PDMS; Solution-diffusion model; Cross contamination; Desaturation; Direct synthesis; Liquid reaction; Mass-transport process; Membrane reactor; Micro-reactor; Reaction media; Chemistry (all); Chemical Engineering (all); Industrial and Manufacturing Engineering; Applied Mathematics; General Chemical Engineering; General Chemistry
Abstract :
[en] Microstructured membrane reactors present a promising approach to master the productivity and safety challenges during the direct synthesis of hydrogen peroxide. However, various mass transport processes occur in this complex system. In order to gain a deeper understanding of these processes, the saturation and desaturation behaviour of the liquid reaction medium with the gaseous reactants is investigated experimentally to examine possible cross-contamination. Moreover, the employed PDMS membrane's permeances to hydrogen and oxygen are researched at different pressures, by using a variable-pressure/constant-volume setup for the behaviour at ambient pressure and a constant-pressure/variable-volume setup for the behaviour at elevated pressures. A mathematical model in MATLAB is applied to simulate the results. It is shown that a certain desaturation of the gasses through the membrane occurs, and the results are underlined by the modelled ones using a solution-diffusion model in MATLAB. Thus a constant flushing of the gas channels of the reactor is required for safety reasons. Moreover, the measured permeance values indicate that the species transport is mainly limited by the diffusion in the liquid phase and not the membrane resistance.
Disciplines :
Chemical engineering
Author, co-author :
Trinkies, Laura L. ; Institute for Micro Process Engineering (IMVT), Karlsruhe Institute of Technology, Germany
Düll, Andrea; Institute for Micro Process Engineering (IMVT), Karlsruhe Institute of Technology, Germany
Zhang, Jinju; Institute for Micro Process Engineering (IMVT), Karlsruhe Institute of Technology, Germany
Urban, Sebastian ; Laboratory for Sensors, IMTEK - Department of Microsystems Engineering, University of Freiburg, Freiburg, Germany
Deschner, Benedikt J. ; Institute for Micro Process Engineering (IMVT), Karlsruhe Institute of Technology, Germany
Kraut, Manfred ; Institute for Micro Process Engineering (IMVT), Karlsruhe Institute of Technology, Germany
LADEWIG, Bradley Paul ; University of Luxembourg > Faculty of Science, Technology and Medicine (FSTM) > Department of Engineering (DoE) ; Institute for Micro Process Engineering (IMVT), Karlsruhe Institute of Technology, Germany
Weltin, Andreas ; Laboratory for Sensors, IMTEK - Department of Microsystems Engineering, University of Freiburg, Freiburg, Germany
Kieninger, Jochen ; Laboratory for Sensors, IMTEK - Department of Microsystems Engineering, University of Freiburg, Freiburg, Germany
Dittmeyer, Roland ; Institute for Micro Process Engineering (IMVT), Karlsruhe Institute of Technology, Germany ; Institute of Catalysis Research and Technology (IKFT), Karlsruhe Institute of Technology, Germany
External co-authors :
yes
Language :
English
Title :
Investigation of mass transport processes in a microstructured membrane reactor for the direct synthesis of hydrogen peroxide
This work was performed with the help of the Large Scale Data Facility at the Karlsruhe Institute of Technology funded by the Ministry of Science, Research and the Arts Baden-Württemberg and by the Federal Ministry of Education and Research. The authors would like to thank Uta Gerhards and Florian Messerschmidt (KIT, IMVT-MAT) for SEM studies and Paul Kant for support with the gas chromatograph.This work was performed with the help of the Large Scale Data Facility at the Karlsruhe Institute of Technology funded by the Ministry of Science, Research and the Arts Baden-Württemberg and by the Federal Ministry of Education and Research. The authors would like to thank Uta Gerhards and Florian Messerschmidt (KIT, IMVT-MAT) for SEM studies and Paul Kant for support with the gas chromatograph.This research was funded by Deutsche Forschungsgemeinschaft (DFG) (FOR 2383, under Grant No. DI 696/13-2).
Campos-Martin, J., Blanco-Brieva, G., Fierro, J.G., Hydrogen Peroxide Synthesis: an Outlook Beyond the Anthraquinone Process. Angew. Chem. 45 (2006), 6962–6984, 10.1002/anie.200503779.
Centi, G., Perathoner, S., Abate, S., 2009. Direct Synthesis of Hydrogen Peroxide: Recent Advances: Design, Reactions and Characterization. In: Mizuno (Hg.) 2009 - Modern Heterogeneous Oxidation Catalysis, pp. 253–287. doi:10.1002/9783527627547.ch8.
Ciriminna, R., Albanese, L., Meneguzzo, F., Pagliaro, M., Hydrogen Peroxide: A Key Chemical for Today's Sustainable Development. ChemSusChem 9 (2016), 3374–3381, 10.1002/cssc.201600895.
Flaherty, D., Direct Synthesis of H2O2 from H2 and O2 on Pd Catalysts: Current Understanding, Outstanding Questions, and Research Needs. ACS Catal. 8 (2018), 1520–1527, 10.1021/acscatal.7b04107.
Fuller, E., Schettler, P., Giddings, J., New Method for Prediction of Binary Gas-Phase Diffusion Coefficients. Ind. Eng. Chem. 58 (1966), 18–27, 10.1021/ie50677a007.
García-Serna, J., Moreno, T., Biasi, P., Cocero, M.J., Mikkola, J.P., Salmi, T.O., Engineering in Direct Synthesis of Hydrogen Üeroxide: Targets, Reactors and Guidelines for Operational Conditions. Green Chem., 16, 2014, 2320, 10.1039/c3gc41600c.
Goor, G., Glenneberg, J., Jacobi, S., Dadabhoy, J., Candido, E., 2000. Hydrogen Peroxide. In: Ullmann's Encyclopedia of Industrial Chemistry. Wiley-VCH Verlag GmbH & Co. KGaA: Weinheim, Germany, pp. 1–40. doi:10.1002/14356007.a13_443.pub3.
Hägg, M., Membrane Purification of Cl2 gas I. Permeabilities as a Function of Temperature for Cl2,O2,N2,H2 in two Types of PDMS Membranes. J. Membr. Sci. 170 (2000), 173–190, 10.1016/S0376-7388(99)00371-3.
Li, J., Šimek, H., Ilioae, D., Jung, N., Bräse, S., Zappe, H., Dittmeyer, R., Ladewig, B.P., In Situ Sensors for Flow Reactors - a Review. Reaction Chem. Eng., 2021, 10.1039/D1RE00038A.
Merkel, T., Bondar, V., Nagai, K., Freeman, B., Pinnau, I., Gas Sorption, Diffusion, and Permeation in Polydimethylsiloxane. J. Polym. Sci., Part B: Polym. Phys. 38 (2000), 415–434, 10.1002/(SICI)1099-0488(20000201)38:3<415::AID-POLB8>3.0.CO;2-Z.
Nagy, E., Basic Equations of the Mass Transport Through a Membrane Layer. 1st ed., 2012, Elsevier Insights, Elsevier, Amsterdam and Boston.
Pashkova, A., Svajda, K., Dittmeyer, R., Direct Synthesis of Hydrogen Peroxide in a Catalytic Membrane Contactor. Chem. Eng. J. (Amsterdam, Neth.) 139 (2008), 165–171, 10.1016/j.cej.2007.09.003.
Pashkova, A., Dittmeyer, R., Kaltenborn, N., Richter, H., Experimental Study of Porous Tubular Catalytic Membranes for Direct Synthesis of Hydrogen Peroxide. Chem. Eng. J. (Amsterdam, Neth.) 165 (2010), 924–933, 10.1016/j.cej.2010.10.011.
Pashkova, A., Greiner, L., Krtschil, U., Hofmann, C., Zapf, R., Direct Synthesis of Hydrogen Peroxide Over Supported Pd Catalysts: Turning to Dense CO2 as an Alternative Solvent. Appl. Catal., A 464–465 (2013), 281–287, 10.1016/j.apcata.2013.06.007.
Paunovic, V., Schouten, J., Nijhuis, T.A., Direct Synthesis of Hydrogen Peroxide Using Concentrated H2 and O2 Mixtures in a Wall-Coated Microchannel – Kinetic Study. Appl. Catal., A 248 (2015), 160–168, 10.1016/j.cattod.2014.04.007.
Samanta, C., Direct Synthesis of Hydrogen Peroxide from Hydrogen and Oxygen: An Overview of Recent Developments in the Process. Appl. Catal., A 350 (2008), 133–149, 10.1016/j.apcata.2008.07.043.
Sander, R., Compilation of Henry's Law Constants (Version 4.0) for Water as Solvent. Atmos. Chem. Phys. 15 (2015), 4399–4981, 10.5194/acp-15-4399-2015.
Selinsek, M., Bohrer, M., Vankayala, B.K., Haas-Santo, K., Kraut, M., Dittmeyer, R., Towards a New Membrane Micro Reactor System for Direct Synthesis of Hydrogen Peroxide. Catal. Today 268 (2016), 85–94, 10.1016/j.cattod.2016.02.003.
Selinsek, M., Kraut, M., Dittmeyer, R., Experimental Evaluation of a Membrane Micro Channel Reactor for Liquid Phase Direct Synthesis of Hydrogen Peroxide in Continuous Flow Using Nafion Membranes for Safe Utilization of Undiluted Reactants. Catalysts, 8, 2018, 556, 10.3390/catal8110556.
Shoghl, S., Raisi, A., Aroujalian, A., Modeling of Gas Solubility and Permeability in Glassy and Rubbery Membranes Using Lattice Fluid Theory. Polymer 115 (2017), 184–196, 10.1016/j.polymer.2017.03.032.
Urban, S., Weltin, A., Flamm, H., Kieninger, J., Deschner, B.J., Kraut, M., Dittmeyer, R., Urban, G.A., Electrochemical Multisensor System for Monitoring Hydrogen Peroxide, Hydrogen and Oxygen in Direct Synthesis Microreactors. Sens. Actuators, B 273 (2018), 973–982, 10.1016/j.snb.2018.07.014.
Urban, S., Tamilselvi Sundaram, V., Kieninger, J., Urban, G., Weltin, A., Microsensor Electrodes for 3D Inline Process Monitoring in Multiphase Microreactors. Sensors, 20, 2020, 4876, 10.3390/s20174876.
Urban, S., Deschner, B.J., Trinkies, L.L., Kieninger, J., Kraut, M., Dittmeyer, R., Urban, G.A., Weltin, A., In Situ Mapping of H2, O2, and H2O2 in Microreactors: A Parallel, Selective Multianalyte Detection Method. ACS Sens. 6 (2021), 1583–1594, 10.1021/acssensors.0c02509.
VDI-Wärmeatlas: Mit 320 Tabellen, 11. ed.; VDI-Buch, Springer Vieweg and Springer, Berlin Heidelberg: Berlin, doi:10.1007/978-3-642-19981-3.
Wilson, N., Bregante, D., Priyadarshini, P., Flaherty, D., Production and Use of H2O2 for Atom-efficient Functionalization of Hydrocarbons and Small Molecules. Catal. 29 (2017), 122–212, 10.1039/9781788010634-00122.
Yampolskii, Y.P., Pinnau, I., Freeman, B.D., Materials Science of Membranes for Gas and Vapor Separation. 2006, Wiley, Chichester England and Hoboken NJ.
Yang, S., Verdaguer-Casadevall, A., Arnarson, L., Silvioli, L., Colic, V., Toward the Decentralized Electrochemical Production of H2O2: A Focus on the Catalysis. ACS Catal. 8 (2018), 4064–4081, 10.1021/acscatal.8b00217.
Yi, Y., Wang, L., Li, G., Guo, H., A Review on Research Progress in the Direct Synthesis of Hydrogen Peroxide from Hydrogen and Oxygen: Noble-Metal Catalytic Method, Fuel-Cell Method and Plasma Method. Catal Sci. Technol. 6 (2016), 1593–1610, 10.1039/C5CY01567G.
