Abstract
Isothermal conditions are a prerequisite for the accurate determination of kinetics in heterogeneous catalysis. In this work, an integral fixed-bed lab reactor with 5 mm inner diameter placed inside an aluminum heating block is used. Temperature profiles were recorded with a single but axially movable thermocouple in a fixed bed of a highly loaded supported Ni catalyst (15.4 wt% Ni on γ-Al2O3) for the Sabatier reaction, i.e., the methanation of CO2, under elevated pressures and without carrier gas dilution. The corresponding conversions of CO2 were determined at the reactor outlet. Depending on the reaction conditions, temperature profiles can show significant deviations from isothermal conditions and even a light-off phenomenon with fluctuating conversions seems to occur. Based on our results, an experimental approach based on the use of one single thermocouple in the fixed bed is recommended which allows to exclude the occurrence of hotspots with a high degree of certainty.
Similar content being viewed by others
References
Berger RJ, Stitt EH, Marin GB, Kapteijn F, Moulijn JA (2001) CatTech 5:30–60
Kapteijn F, Berger RJ, Moulijn JA (2008) In: Ertl G, Knözinger H, Schüth F, Weitkamp J (eds) Handbook of heterogeneous catalysis, 2nd edn. Wiley, Weinheim
Kapteijn F, Moulijn JA (2008) In: Ertl G, Knözinger H, Schüth F, Weitkamp J (eds) Handbook of heterogeneous catalysis, 2nd edn. Wiley, Weinheim
Froment GF, Bischoff KB, DeWilde J (2010) Chemical reactor analysis and design, 3rd edn. Wiley, New York
Anderson JR, Pratt KC (1985) Introduction to characterization and testing of catalysts. Academic Press, Sydney
Weekman VW (1974) AlChE J 20:833–840
Rase HF (1990) Fixed-bed reactor design and diagnostics: gas-phase reactions. Butterworths, Stoneham
Dautzenberg M (1989) In: Bradley SA, Gattuso MJ, Bertolacini RJ (eds) Characterization and catalyst development. ASC, Washington, DC
Satterfield CN (1970) Mass transfer in heterogeneous catalysis. MIT Press, Cambridge
Berger RJ, Pérez-Ramírez J, Kapteijn F, Moulijn JA (2002) Chem Eng Sci 57:4921–4932
van den Bleek CV, van der Wiele K, Berg PJ (1969) Chem Eng Sci 24:681–694
Perego C, Peratello S (1999) Catal Today 52:133–145
Götz M, Lefebvre J, Mörs F, McDaniel Koch A, Graf F, Bajohr S, Reimert R, Kolb T (2016) Renew Energy 85:1371–1390
Guerra L, Rossi S, Rodrigues J, Gomes J, Puna J, Santos MT (2018) J Environ Chem Eng 6:671–676
Kopyscinski J, Schildhauer TJ, Vogel F, Biollaz SMA, Wokaun A (2010) J Catal 271:262–279
Li Y, Zhang Q, Chai R, Zhao G, Liu Y, Lu Y, Cao F (2015) AIChE J 61:4323–4331
Schüler C, Hinrichsen O (2016) Chem Ing Tech 88:1693–1702
Tauer G, Kern C, Jess A (2017) In: Preprints 2017-2 of the DGMK-conference, petrochemistry and refining in a changing raw materials landscape, ISBN 978-3-941721-74-6
Belimov M, Metzger D, Pfeifer P (2017) AIChE J 63:120–129
Gao J, Wang Y, Ping Y, Hu D, Xu G, Gu F, Su F (2012) RSC Adv 2:2358–2368
Schouten EPS, Borman PC, Westerterp KR (1994) Chem Eng Sci 49:4725–4747
Anastasov AI (2002) Chem Eng J 86:287–297
Lange T, Neher F, Klemm E, Heinrich S, Balcazar E, Liebner C (2014) In: Preprints 2014-3 of the DGMK-conference, selective oxidation and functionalization, classical and alternative routes and sources, ISBN 978-3-941721-44-9
Heinrich S, Edeling F, Liebner C, Hieronymus H, Lange T, Klemm E (2012) Chem Eng Sci 84:540–543
Weatherbee GD, Bartholomew CH (1984) J Catal 87:352–362
Moulijn JA, Tarfaoui A, Kapteijn F (1991) Catal Today 11:1–12
Acknowledgements
The authors thank Mirko Peifer, Dr. Thomas Schwarz and Prof. Dr. Klaus Stöwe for providing the catalyst. This work was supported by ThyssenKrupp Industrial Solutions TKIS.
Author information
Authors and Affiliations
Corresponding author
Rights and permissions
About this article
Cite this article
Beierlein, D., Schirrmeister, S., Traa, Y. et al. Experimental approach for identifying hotspots in lab-scale fixed-bed reactors exemplified by the Sabatier reaction. Reac Kinet Mech Cat 125, 157–170 (2018). https://doi.org/10.1007/s11144-018-1402-4
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s11144-018-1402-4