C02 – Catalytic Monoliths with Narrow Particle Size Distribution in Washcoats with Well-Defined Gradients

This project aims at developing highly active and selective structured catalysts, bridging the gap between model catalysts and more realistic reactor systems. The best candidates for both the supports and noble metal clusters/particles are used for washcoating monoliths. This requires the scale-up of promising cluster / nanoparticle preparation routes with narrow size distribution, targeted washcoat preparation and zone and dual layer coating along with online / in situ monitoring of their formation processes. They are used for X-ray microscopy, spatially resolved catalytic/structural studies and transient lab bench tests as well as for correlating the properties to the manufacturing process.

Project-related publications by participating researchers

Project- and subject-related list of publications
J. Becher, D.F. Sanchez, D. E. 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. Nat. Catal. 2021, 4 (1), 46-53. DOI: 10.1038/s41929-020-0552-3.
S. Chen, X. Huang, D. Schild, D. Wang, C. Kübel, S. Behrens, Pd–In intermetallic nanoparticles with high catalytic selectivity for liquid-phase semi-hydrogenation of diphenylacetylene. Nanoscale 2022, 14 (47), 17661-17669. DOI: 10.1039/D2NR03674F.
D. Eggart, A. Zimina, G. Cavusoglu, M. Casapu, D. E. Doronkin, K. A. Lomachenko, J.-D. Grunwaldt, Versatile and high temperature spectroscopic cell for operando fluorescence and transmission x-ray absorption spectroscopic studies of heterogeneous catalysts. Rev. Sci. Instrum. 2021, 92 (2), 023106. DOI: 10.1063/5.0038428.
F. Eichner, E. Turan, J. Sauer, M. Bender, S. Behrens, Supported silver and copper catalysts in the oxidative dehydrogenation of methanol to formaldehyde: a comparative study under industrially relevant conditions. Catal. Sci. Technol. 2023, 13, 2349-2359. DOI: 10.1039/D2CY01405J.
F. Eichner, J. Sauer, M. Bender, S. Behrens, The titania-catalyzed oxidative dehydrogenation of methanol to formaldehyde. Appl. Catal. A. 2023, 663, 119305. DOI: 10.1016/j.apcata.2023.119305.
F. Maurer, A. M. 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 (18), 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. 2023, 123 (1), 379-444. DOI: 10.1021/acs.chemrev.2c00495.
D. I. Sharapa, D. E. Doronkin, F. Studt, J.-D. Grunwaldt, S. Behrens, Moving Frontiers in Transition Metal Catalysis: Synthesis, Characterization and Modeling. Adv. Mat. 2019, 31 (26), 1807381. DOI: 10.1002/adma.201807381.
C. Schmitt, N. Da Roit, M. Neumaier, C. Maliakkal, D. Wang, T. Henrich, C. Kübel, M. Kappes, S. Behrens Continuous flow synthesis of atom-precise platinum clusters. Nanoscale Adv. 2024. DOI: 10.1039/D4NA00074A.
G. Tofighi, H. Lichtenberg, A. Gaur, W. Wang, S. Wild, K. Herrera Delgado, S. Pitter, R. Dittmeyer, J.-D. Grunwaldt, D. E. Doronkin, Continuous synthesis of Cu/ZnO/Al₂O₃ nanoparticles in a co-precipitation reaction using a silicon based microfluidic reactor. React. Chem. Eng. 2022, 7 (3), 730-740. DOI: 10.1039/D1RE00499A.

Project- and subject-related list of publications

J. Becher, D.F. Sanchez, D. E. 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. Nat. Catal. 2021, 4 (1), 46-53.

DOI: 10.1038/s41929-020-0552-3.

S. Chen, X. Huang, D. Schild, D. Wang, C. Kübel, S. Behrens, Pd–In intermetallic nanoparticles with high catalytic selectivity for liquid-phase semi-hydrogenation of diphenylacetylene. Nanoscale 2022, 14 (47), 17661-17669.

DOI: 10.1039/D2NR03674F.

D. Eggart, A. Zimina, G. Cavusoglu, M. Casapu, D. E. Doronkin, K. A. Lomachenko, J.-D. Grunwaldt, Versatile and high temperature spectroscopic cell for operando fluorescence and transmission x-ray absorption spectroscopic studies of heterogeneous catalysts. Rev. Sci. Instrum. 2021, 92 (2), 023106.

DOI: 10.1063/5.0038428.

F. Eichner, E. Turan, J. Sauer, M. Bender, S. Behrens, Supported silver and copper catalysts in the oxidative dehydrogenation of methanol to formaldehyde: a comparative study under industrially relevant conditions. Catal. Sci. Technol. 2023, 13, 2349-2359.

DOI: 10.1039/D2CY01405J.

F. Eichner, J. Sauer, M. Bender, S. Behrens, The titania-catalyzed oxidative dehydrogenation of methanol to formaldehyde. Appl. Catal. A. 2023, 663, 119305.

DOI: 10.1016/j.apcata.2023.119305.

F. Maurer, A. M. 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 (18), 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. 2023, 123 (1), 379-444.

DOI: 10.1021/acs.chemrev.2c00495.

D. I. Sharapa, D. E. Doronkin, F. Studt, J.-D. Grunwaldt, S. Behrens, Moving Frontiers in Transition Metal Catalysis: Synthesis, Characterization and Modeling. Adv. Mat. 2019, 31 (26), 1807381.

DOI: 10.1002/adma.201807381.

C. Schmitt, N. Da Roit, M. Neumaier, C. Maliakkal, D. Wang, T. Henrich, C. Kübel, M. Kappes, S. Behrens Continuous flow synthesis of atom-precise platinum clusters. Nanoscale Adv. 2024.

DOI: 10.1039/D4NA00074A.

G. Tofighi, H. Lichtenberg, A. Gaur, W. Wang, S. Wild, K. Herrera Delgado, S. Pitter, R. Dittmeyer, J.-D. Grunwaldt, D. E. Doronkin, Continuous synthesis of Cu/ZnO/Al₂O₃ nanoparticles in a co-precipitation reaction using a silicon based microfluidic reactor. React. Chem. Eng. 2022, 7 (3), 730-740.

DOI: 10.1039/D1RE00499A.

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

Project Area C - Catalytic reactors