C2 - Catalytic monoliths with narrow particle size distribution in washcoats with well-defined gradients

Objective

This project aims at developing advanced washcoated monoliths as catalysts for studies under transient operating conditions, bridging the gap between model catalysts and more realistic reactor systems. The best candidates for both the supports (with defined morphology) and noble metal clusters/particles are used for the preparation of the washcoat of monoliths. This requires the scaling-up of promising nanoparticle preparation routes with narrow size distribution, targeted washcoat preparation and zone and dual layer coating. The resulting coated monoliths serve as basis for X-ray microscopy, spatially resolved catalytic and structural studies and transient lab and engine bench tests.

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/s41929-020-00552-3
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 coprecipitation 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/s41929-020-00552-3

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 coprecipitation reaction using a silicon based microfluidic reactor. React. Chem. Eng. 2022, 7 (3), 730-740.

DOI: 10.1039/D1RE00499A

Project Area C - Catalytic reactors