Laboratory of Chemical Reaction Engineering: Overview

Research Focus and Overview

The research focus of the group is on controlling the transport trajectories in chemical reactors by structuring at different length and time scales. Therefore, porous catalysts and multiphase reactors are structured and systematically studied under dynamic operation conditions. The inherent interplay between transport properties and structure is evaluated by combination of physical as well as numerical experiments with emphasis on syngas reactions for chemical energy conversion and storage. Hence, the chemical utilization and storage of hydrogen (H2) and turning carbon dioxide (CO2) into value is the major focus of our research activities.

The expertise in the group covers synthesis and characterization of porous, solid catalysts, experimental evaluation of chemical reactors, modeling and simulation of multiphase reactors as well as unsteady-state process operation.

Head of Laboratory: Prof. Dr.-Ing. Robert Güttel

Chemical Utilization of Hydrogen and Upcycling of Carbon Dioxide

Power-to-X processes are key to use hydrogen (H2) as energy carrier and as raw material in the chemical value chain. By hydrogenating carbon dioxide (CO2) or nitrogen (N2) available world wide via separation from air, a sustainable production of chemicals and transportation of H2 across the the globe is possible. We focus our research to develop catalysts and reactors for enhanced Methanation, Fischer-Tropsch and Ammonia synthesis processes.

Key Publications:

  1. Gäßler, M., Stahl, J., Schowalter, M., Pokhrel, S., Rosenauer, A., Mädler, L., Güttel, R. (2022). The Impact of Support Material of Cobalt-Based Catalysts Prepared by Double Flame Spray Pyrolysis on CO2 Methanation Dynamics. ChemCatChem, accpeted. doi:10.1002/cctc.202200286
  2. Cholewa, T., Semmel, M., Mantei, F., Güttel, R., Salem, O. (2022). Process Intensification Strategies for Power-to-X Technologies. ChemEngineering 6 (1) 13. doi:10.3390/chemengineering6010013
  3. Straß-Eifert, A., Sheppard, T.L., Becker, H., Friedland, J., Zimina, A., Grunwaldt, J.-D., Güttel, R. (2021). Cobalt-based Nanoreactors in Combined Fischer-Tropsch Synthesis and Hydroprocessing: Effects on Methane and CO2 Selectivity. ChemCatChem 13 (24) 5216-5227. doi: 10.1002/cctc.202101053
  4. Straß-Eifert, A., van der Wal, L., Hernandez, Mejia, C., Weber, L., Yoshida, H., Zecevic, J., de Jong, K., Güttel, R. (2021). Bifunctional Co-based Catalysts for Fischer-Tropsch Synthesis: Descriptors affecting the product distribution. ChemCatChem 13 (11) 2726-2742. doi: 10.1002/cctc.202100270
  5. Sánchez, A., Milt, V.G., Miró, E.E., Güttel, R. (2020). Ceramic fiber-based structures as catalyst supports: a study on mass and heat transport behavior applied to CO2 methanation. Industrial & Engineering Chemistry Research 59 (38) 16539-16552. doi: 10.1021/acs.iecr.0c01997
  6. Theurich, S., Rönsch, S., Güttel, R. (2020). Transient Flow Rate Ramps for Methanation of Carbon Dioxide in an Adiabatic Fixed-Bed Recycle Reactor. Energy Technology, 8 (3) 1901116. doi:10.1002/ente.201901116

Unsteady-State Reactor Operation

Unsteady-state reactor operation is one of the main challenges for the efficient utilization of renewable ressources in the chemical value chain, since it requires a deep understanding of the involved processes at multiple time and length scales (doi: 10.1002/nadc.20204097163). From scientific viewpoint the systematic analysis of reactor dynamics provides a high information density, which can only be evaluated by sophisticated combination of physical and numerical experimentation. The project aims at developing such methods in order to allow for application in Power-to-X processes.

Key Publications:

  1. Gäßler, M., Stahl, J., Schowalter, M., Pokhrel, S., Rosenauer, A., Mädler, L., Güttel, R. (2022). The Impact of Support Material of Cobalt-Based Catalysts Prepared by Double Flame Spray Pyrolysis on CO2 Methanation Dynamics. ChemCatChem, accepted. doi:10.1002/cctc.202200286
  2. Schumacher, J., Meyer, D., Friedland, J., Güttel, R. (2022). Evaluation of the application of different diffusion models for the methanation of CO/CO2 mixtures. Results in Engineering 13, 100355. doi:10.1016/j.rineng.2022.100355
  3. Meyer, D., Schumacher, J., Friedland, J., Güttel, R. (2022). Frequency Response Analysis of the Unsteady-State CO/CO2 Methanation Reaction: An Experimental Study. Industrial & Engineering Chemistry Research 61 (5) 2045-2054. doi:10.1021/acs.iecr.1c04547, preprint: 10.26434/chemrxiv-2022-zrnbx
  4. Meyer, D., Friedland, J., Schumacher, J., Gäßler, M., Güttel, R. (2022). Hydrogenation of CO/CO2 mixtures under unsteady-state conditions: Effect of the carbon oxides on the dynamic methanation process. Chemical Engineering Science 250, 117405. doi:10.1016/j.ces.2021.117405, preprint: 10.26434/chemrxiv-2021-pzfrv
  5. Meyer, D., Friedland, J., Schumacher, J., Güttel, R. (2021). The periodic transient kinetics method for investigation of kinetic process dynamics under realistic conditions: Methanation as an example. Chemical Engineering Research and Design 173, 253-266. doi:10.1016/j.cherd.2021.07.011, preprint: 10.26434/chemrxiv.14653395.v1
  6. Theurich, S., Rönsch, S., Güttel, R. (2020). Transient Flow Rate Ramps for Methanation of Carbon Dioxide in an Adiabatic Fixed-Bed Recycle Reactor. Energy Technology, 8 (3) 1901116. doi:10.1002/ente.201901116
  7. Matthischke, S., Rönsch, S., Güttel, R. (2018). Start-up time and load range for the methanation of carbon dioxide in a fixed-bed recycle reactor. Industrial & Engineering Chemistry Research 57 (18) 6391–6400. doi:10.1021/acs.iecr.8b00755
  8. Meyer, D., Friedland, J., Kohn, T., Güttel, R. (2017). Transfer Functions for Periodic Reactor Operation: Fundamental Methodology for Simple Reaction Networks. Chemical Engineering & Technology 40 (11) 2096-2103. doi:10.1002/ceat.201700122
  9. Güttel, R. (2013). Study of Unsteady-State Operation of Methanation by Modeling and Simulation. Chemical Engineering & Technology 36 (10) 1675-1682. doi:10.1002/ceat.201300223

Structured Catalysts and Reactors

The spatial structuring of catalysts and reactors is possible on different length scales, which offers the opportunity to intensify heterogeneously catalyzed reactions (doi: 10.1002/ente.201500257). Therefore, we work on the development of nanostructured core-shell catalysts for syngas reactions (Fischer-Tropsch synthesis, CO/CO2 methanation), which are robust under the harsh reaction conditions and thus stable for long operation periods. Furthermore, these materials are proven to allow tuning the product selectivity for Fischer-Tropsch synthesis. In order to transfer the promising features into application, we also immobilize the novel materials on support structures, such as honeycombs or ceramic fibers.

Key Publications:

  1. Straß-Eifert, A., Sheppard, T.L., Becker, H., Friedland, J., Zimina, A., Grunwaldt, J.-D., Güttel, R. (2021). Cobalt-based Nanoreactors in Combined Fischer-Tropsch Synthesis and Hydroprocessing: Effects on Methane and CO2 Selectivity. ChemCatChem 13 (24) 5216-5227. doi: 10.1002/cctc.202101053
  2. Straß-Eifert, A., van der Wal, L., Hernandez, Mejia, C., Weber, L., Yoshida, H., Zecevic, J., de Jong, K., Güttel, R. (2021). Bifunctional Co-based Catalysts for Fischer-Tropsch Synthesis: Descriptors affecting the product distribution. ChemCatChem 13 (11) 2726-2742. doi: 10.1002/cctc.202100270
  3. Straß-Eifert, A., Sheppard, T.L., Damsgaard, C.D., Grunwaldt, J.-D., Güttel, R. (2021). Stability of Cobalt Particles in and outside HZSM‐5 under CO Hydrogenation Conditions Studied by ex situ and in situ Electron Microscopy. ChemCatChem 13 (2) 718-729. doi: 10.1002/cctc.202001533
  4. Sánchez, A., Milt, V.G., Miró, E.E., Güttel, R. (2020). Ceramic fiber-based structures as catalyst supports: a study on mass and heat transport behavior applied to CO2 methanation. Industrial & Engineering Chemistry Research 59 (38) 16539-16552. doi: 10.1021/acs.iecr.0c01997
  5. Kirchner, J., Zambrzycki, C., Baysal, Z., Kureti, S., Güttel, R. (2020). Fe based core-shell model catalysts for the reaction of CO2 with H2. Reaction Kinetics, Mechanisms and Catalysis 131 (1) 119-128. doi:10.1007/s11144-020-01859-9
  6. Ilsemann, J., Straß-Eifert, A., Friedland, J., Kiewidt, L., Thöming, J., Bäumer, M., Güttel, R. (2019). Cobalt@Silica core-shell catalysts for hydrogenation of CO/CO2 mixtures to methane. ChemCatChem 11, 4884-4893. doi:10.1002/cctc.201900916
  7. Güttel, R., Turek, T. (2016). Improvement of Fischer-Tropsch Synthesis through Structuring on Different Scales. Energy Technology 4 (1) 44-54. doi:10.1002/ente.201500257
  8. Kruse, N., Machoke, A. G., Schwieger, W., Güttel, R. (2015). Nanostructured Encapsulated Catalysts for Combination of Fischer-Tropsch Synthesis and Hydroprocessing. ChemCatChem 7 (6) 1018-1022. doi:10.1002/cctc.201403004

Multiphase Reactions and Reactors

Gas-liquid reactions for stoichiometric conversion and heterogeneously catalyzed reactions are of great importance in the chemical industry. For very fast kinetics and highly exothermic reactions the design of suitable reactors with superior efficiency is highly demanding, as convective and conductive heat and mass transfer depend on often chaotic hydrodynamics. The aim is the development of experimental equipment and simulation models to gather reliable kinetic data for reactor design and scale up.

Key Publications:

  1. Sánchez, A., Milt, V.G., Miró, E.E., Güttel, R. (2022). Impact of heat transport properties and configuration of ceramic fibrous catalyst structures for CO2 methanation: A simulation study. Journal of Environmental Chemical Engineering 10 (2) 107148. doi: 10.1016/j.jece.2022.107148
  2. Friedland, J., Güttel, R. (2021). Challenges in transfer of gas-liquid reactions from batch to continuous operation: Dimensional analysis and simulations for aerobic oxidation. Journal of Flow Chemistry 11 (3) 625-640. doi:10.1007/s41981-021-00176-z
  3. Friedland, J., Brandt, A., Leopold, K., Güttel, R. (2021). Atomization of gold nanoparticles in graphite furnace AAS: Modelling and simulative exploration of experimental results. Spectrochimica Acta Part B: Atomic Spectroscopy, 182, 106249. doi:10.1016/j.sab.2021.106249
  4. Meyer, D., Schumacher, J., Friedland, J., Güttel, R. (2020). Hydrogenation of CO/CO2 Mixtures on Nickel Catalysts: Kinetics and Flexibility for Nickel Catalysts. Industrial & Engineering Chemistry Research 59 (33) 14668-14678. doi:10.1021/acs.iecr.0c02072
  5. Lechner, M., Kastner, K., Chan, C. J., Güttel, R., Streb, C. (2018). Aerobic Oxidation Catalysis by a Molecular Barium Vanadium Oxide. Chemistry - A European Journal 24 (19) 4952-4956. doi:10.1002/chem.201706046
  6. Lechner, M., Güttel, R., Streb, C. (2016). Challenges in polyoxometalate-mediated aerobic oxidation catalysis: catalyst development meets reactor design. Dalton Transactions 45, 16716-16726. doi:10.1039/C6DT03051C

Highlights and News

New project on Ammonia synthesis

[08/22] The Federal Ministry of Education and Research (BMBF) and the Project Management Jülich (PtJ) fund our project on process intensification of Ammonia synthesis for hydrogen conversion and distribution, where we collaborate with our colleagues from Fraunhofer ISE.

Poster Prize in Würzburg

[07/22] Max received the poster prize of the Annual Meeting on Reaction Engineering in Würzburg. Congratulations, well deserved!

Project funded by DBU

[07/22] The German Federal Environmental Foundation (DBU) funds our member Hannes to work on the application of artificial neural networks (aNN) for modeling the kinetics of methanation.

Methanation in July

[07/22] We got three papers accepted on methanation: The first compares fiber-based supporting structures with conventional packed-beds based on simulations (10.1007/s11244-022-01675-6). The second is on investigating Nickel-surfaces by pulse-experimentation with CO/H2 mixtures under reactive conditions (10.1002/cctc.202200298). The third investigates nanostructured Fe@SiO2 core-shell model catalysts with respect to deactivation during CO and CO2 methanation (10.3390/reactions3030027).

Support effect in CO2 Methanation

[06/22] Together with our colleagues from Bremen University we studied the support effects during dynamic methanation of CO2. Titania seems to provide sorption-enhancement in CH4 formation. The paper is open access here: 10.1002/cctc.202200286

Unsteady-State CO/CO2 Methanation

[01/22] We recently published three papers in one month on hydrogenation of CO/CO2 mixtures into methane on Nickel catalysts. Two focus on experimental step response studies (10.1016/j.ces.2021.117405, 10.1021/acs.iecr.1c04547), while one focuses on modeling and simulation (10.1016/j.rineng.2022.100355).

Review on Power-to-X

[01/22] With our colleagues from Fraunhofer ISE we published a review on process intensification strategies for Power-to-X technologies here: 10.3390/chemengineering6010013

Chemische Reaktionstechnik

[03/21] Our new textbook is available in print and online. Unbelievable to hold it in my hands...
Now, we fill the book website with examples based on the simulation tool Python.

Robert Güttel and Thomas Turek (2021), Chemische Reaktionstechnik, Springer Spektrum, Berlin, Heidelberg. ISBN 978-3-662-63149-2