C04 – Space- and Time-Resolved Investigation of the Gas Phase and the Active Surface/Bulk

The project investigates structural and gas phase concentration gradients that develop in the channels and walls of monolithic catalysts during operation. In-situ and operando methods are developed and applied to simultaneously investigate spatial and temporal changes in the gas phase and in the catalyst. These include non-invasive laser and X-ray methods combined in a specially developed in situ cell to study the gas phase by planar laser-induced fluorescence and the catalyst by X-ray absorption spectroscopy. Detailed reaction mechanisms are used to model the reactor behavior and to develop strategies for re-/activation of the catalyst focusing first on NH3 and VOC oxidation.

Project-related publications by participating researchers

Project- and subject-related list of publications

J. Becher, D.F. Sanchez, D. Doronkin, D. Zengel, D.M. Meira, S. Pascarelli, J.-D. Grunwaldt, T.L. Sheppard, Chemical gradients in automotive Cu-SSZ-13 catalysts for NOx removal revealed by operando X-ray spectrotomography. Nature Catal. 2021, 4 (1), 46-53.

DOI: 10.1038/s41929-020-00552-3.

P. Dolcet, F. Maurer, M. Casapu, J.-D. Grunwaldt, Insights into the Structural Dynamics of Pt/CeO2 Single-Site Catalysts during CO Oxidation. Catalysts 2021, 11, 617.

DOI: 0.3390/catal11050617.

P. Lott, M. Casapu, J.-D. Grunwaldt, O. Deutschmann, A review on exhaust gas after-treatment of lean-burn natural gas engines - From fundamentals to application. Appl. Catal. B: Environmental 2023, 123241.

DOI: 10.1016/j.apcatb.2023.123241.

K. Keller, S. Wan, M. Borchers, P. Lott, R. Suntz, O. Deutschmann, Treating NOx emission of hydrogen fueled combustion engines by NOx storage and reduction catalysts: A transient kinetic study including PLIF measurements. Proc. Comb. Inst. 2023, 39, 4247-4256.

DOI: 10.1016/j.proci.2022.07.027.

V. Marchuk, X. H. Huang, J.-D. Grunwaldt, D. E. Doronkin, Structure sensitivity of alumina- and zeolite-supported platinum ammonia slip catalysts. Catal. Sci. Technol. 2023, 13, 2946-2965.

DOI: 10.1039/d2cy02095e

F. Maurer, A. Gänzler, P. Lott, B. Betz, M. Votsmeier, S. Loridant, P. Vernoux, V. Murzin, B. Bornmann, R. Frahm, O. Deutschmann, M. Casapu, J.-D. Grunwaldt, Spatiotemporal Investigation of the Temperature and Structure of a Pt/CeO2 Oxidation Catalyst for CO and Hydrocarbon Oxidation during Pulse Activation. Ind. Eng. Chem. Res. 2021, 60, 6662-6675.

DOI: 10.1021/acs.iecr.0c05798.

B. B. Sarma, F. Maurer, D. E. Doronkin, J.-D. Grunwaldt, Design of Single-Atom Catalysts and Tracking Their Fate Using Operando and Advanced X-ray Spectroscopic Tools. Chem. Rev. 2022, 123, 379–444.

DOI: 10.1021/acs.chemrev.2c00495.

A. B. Shirsath, M. L. Schulte, B. Kreitz, S. Tischer, J.-D. Grunwaldt, O. Deutschmann, Spa-
tially-resolved investigation of CO2 methanation over Ni/γ-Al2O3 and Ni3.2Fe/γ-Al2O3 catalysts
in a packed-bed reactor. Chem. Eng. J. 2023, 469, 143847.

DOI: 10.1016/j.cej.2023.143847.

S. Wan; K. Keller; P. Lott; A.B. Shirsath; S. Tischer; T. Häber; R. Suntz; O. Deutschmann. Experimental and numerical investigation of NO oxidation on Pt/Al2O3- and NOx storage on Pt/BaO/Al2O3-catalysts. Catal. Sci. Technol. 2022, 12, 4456–4470.

DOI: 10.1039/D2CY00572G.

S. Wan, T. Häber, P. Lott, R. Suntz, O. Deutschmann, Experimental investigation of NO reduction by H2 on Pd using planar laser-induced fluorescence. Appl. Energy Comb. Sci. 2023, 16, 100229.

DOI: 10.1016/j.jaecs.2023.100229

 

The project is funded since 2021 and is now in the second funding phase.