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

Prof. Dr. Olaf Deutschmann
O. Deutschmann, J.-D.Grunwaldt, Exhaust gas aftertreatment in mobile systems: status, challenge, and perspectives. Chem. Ing. Tech. 2013, 85, 595-617 DOI: 10.1002/cite.201200188
D. Chan, S. Tischer, J. Heck, C. Diehm, O. Deutschmann, Correlation between catalytic activity and catalytic surface area of Pt/Al₂O₃ DOC: An experimental and microkinetic modeling study. Appl. Catal. B. 2014, 165, 153-165 DOI: 10.1016/j.apcatb.2014.03.009
S. Kannepalli, A. Gremminger, S. Tischer, O. Deutschmann, Optimization of axial catalyst loading in transient-operated zone-structured monoliths: Reduction of cumulative emissions in automotive oxidation catalysts. Chem. Eng. Sci. 2017, 174, 189-202 DOI: 10.1016/j.ces.2017.09.013
A. Zellner, R. Suntz, O. Deutschmann, Two dimensional spatial resolution of concentration profiles in catalytic reactors by planar laser-induced fluorescence: NO reduction over Diesel oxidation catalysts. Angew. Chem. Int. Ed. 2015, 54, 2653-2655 DOI: 10.1002/anie.201410324
S. Wan, T. Häber, R. Suntz, O. Deutschmann, Investigation of HCHO catalytic oxidation over Platinum using planar laser-induced fluorescence. Appl. Catal. B, 2020, 264, 118473 DOI: 10.1016/j.apcatb.2019.118473

Prof. Dr. Olaf Deutschmann

O. Deutschmann, J.-D.Grunwaldt, Exhaust gas aftertreatment in mobile systems: status, challenge, and perspectives. Chem. Ing. Tech. 2013, 85, 595-617

DOI: 10.1002/cite.201200188

D. Chan, S. Tischer, J. Heck, C. Diehm, O. Deutschmann, Correlation between catalytic activity and catalytic surface area of Pt/Al₂O₃ DOC: An experimental and microkinetic modeling study. Appl. Catal. B. 2014, 165, 153-165

DOI: 10.1016/j.apcatb.2014.03.009

S. Kannepalli, A. Gremminger, S. Tischer, O. Deutschmann, Optimization of axial catalyst loading in transient-operated zone-structured monoliths: Reduction of cumulative emissions in automotive oxidation catalysts. Chem. Eng. Sci. 2017, 174, 189-202

DOI: 10.1016/j.ces.2017.09.013

A. Zellner, R. Suntz, O. Deutschmann, Two dimensional spatial resolution of concentration profiles in catalytic reactors by planar laser-induced fluorescence: NO reduction over Diesel oxidation catalysts. Angew. Chem. Int. Ed. 2015, 54, 2653-2655

DOI: 10.1002/anie.201410324

S. Wan, T. Häber, R. Suntz, O. Deutschmann, Investigation of HCHO catalytic oxidation over Platinum using planar laser-induced fluorescence. Appl. Catal. B, 2020, 264, 118473

DOI: 10.1016/j.apcatb.2019.118473

Prof. Dr. Jan-Dierk Grunwaldt
J.-D.Grunwaldt, J. B. Wagner, R. E. Dunin-Borkowski, Imaging catalysts at work: A hierarchical approach from the macro- to the meso- and nano-scale. ChemCatChem, 2012, 5, 62-80 DOI: 10.1002/cctc.201200356
A. M. Gänzler, M. Casapu, D. E. Doronkin, F. Maurer, P. Lott, P. Glatzel, M. Votsmeier, O. Deutschmann, J.-D.Grunwaldt, Unravelling the different reaction pathways for low temperature CO oxidation on Pt/CeO₂ and Pt/Al₂O₃ by spatially resolved structure-activity correlations. J. Phys. Chem. Lett. 2019, 10, 7698-7705 DOI: 10.1021/acs.jpclett.9b02768
B. Kimmerle, J.-D.Grunwaldt, A. Baiker, P. Glatzel, P. Boye, S. Stephan, C. G. Schroer, Visualizing a catalyst at work during the ignition of the catalytic partial oxidation of methane. J. Phys. Chem. C, 2009, 113, 3037-3040 DOI: 10.1021/jp810319v
A. M. Gänzler, M. Casapu, A. Boubnov, O. Müller, S. Conrad, H. Lichtenberg, R. Frahm, J.-D.Grunwaldt, Operando spatially and time-resolved X-ray absorption spectroscopy and infrared thermography during oscillatory CO oxidation. J. Catal. 2015, 328, 216-224 DOI: 10.1016/j.jcat.2015.01.002
A. M. Gänzler, M. Casapu, P. Vernoux, S. Loridant, F. J. Cadete Santos Aires, T. Epicier, B. Betz, R. Hoyer, J.-D.Grunwaldt, Tuning the structure of Platinum particles on ceria in situ for enhancing the catalytic performance of exhaust gas catalysts. Angew. Chem. Int. Ed. 2017, 56, 13078-13082 DOI: 10.1002/anie.201707842

Prof. Dr. Jan-Dierk Grunwaldt

J.-D.Grunwaldt, J. B. Wagner, R. E. Dunin-Borkowski, Imaging catalysts at work: A hierarchical approach from the macro- to the meso- and nano-scale. ChemCatChem, 2012, 5, 62-80

DOI: 10.1002/cctc.201200356

A. M. Gänzler, M. Casapu, D. E. Doronkin, F. Maurer, P. Lott, P. Glatzel, M. Votsmeier, O. Deutschmann, J.-D.Grunwaldt, Unravelling the different reaction pathways for low temperature CO oxidation on Pt/CeO₂ and Pt/Al₂O₃ by spatially resolved structure-activity correlations. J. Phys. Chem. Lett. 2019, 10, 7698-7705

DOI: 10.1021/acs.jpclett.9b02768

B. Kimmerle, J.-D.Grunwaldt, A. Baiker, P. Glatzel, P. Boye, S. Stephan, C. G. Schroer, Visualizing a catalyst at work during the ignition of the catalytic partial oxidation of methane. J. Phys. Chem. C, 2009, 113, 3037-3040

DOI: 10.1021/jp810319v

A. M. Gänzler, M. Casapu, A. Boubnov, O. Müller, S. Conrad, H. Lichtenberg, R. Frahm, J.-D.Grunwaldt, Operando spatially and time-resolved X-ray absorption spectroscopy and infrared thermography during oscillatory CO oxidation. J. Catal. 2015, 328, 216-224

DOI: 10.1016/j.jcat.2015.01.002

A. M. Gänzler, M. Casapu, P. Vernoux, S. Loridant, F. J. Cadete Santos Aires, T. Epicier, B. Betz, R. Hoyer, J.-D.Grunwaldt, Tuning the structure of Platinum particles on ceria in situ for enhancing the catalytic performance of exhaust gas catalysts. Angew. Chem. Int. Ed. 2017, 56, 13078-13082

DOI: 10.1002/anie.201707842

Project Area C - Catalytic reactors