C4 - Space- and time-resolved investigation of the gas phase and the active surface/bulk

Objective

This project focusses on the structural and concentration gradients that evolve during operation inside the channels and walls of monolithic catalysts in an emission control system. Therefore, new in situ techniques capable of simultaneously probing spatial and temporal changes in the gas phase and the catalyst will be developed. For the first time, non-invasive laser and X-ray based methods will be combined to investigate the catalyst using planar laser induced fluorescence (PLIF) and X-ray absorption spectroscopy (XAS). On basis of detailed reaction mechanisms and CFD simulations, the reactor behavior will be modeled and catalyst activation/regeneration strategies developed.

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 NO_x emission of hydrogen fueled combustion engines by NO_x 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, Spatially-resolved investigation of CO₂ methanation over Ni/γ-Al₂O₃ and Ni_3.2Fe/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 NO_x 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

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 NO_x emission of hydrogen fueled combustion engines by NO_x 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, Spatially-resolved investigation of CO₂ methanation over Ni/γ-Al₂O₃ and Ni_3.2Fe/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 NO_x 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

Project Area C - Catalytic reactors