B2 - Project title: Systematic Synthesis and Catalytic Performance Tests of Defined Noble Metal Species on Powder Supports

Objective

This project addresses the influence of noble metal particle size/composition and morphology of the support on the catalyst performance and its activation/deactivation/reactivation behavior under model and realistic reaction conditions. Model catalysts will be prepared following the ‘precursor concept’, i.e. mono- and bimetallic clusters or particles of defined size are synthesized by new chemical procedures in solution, and anchored on support oxide. Light-off/light-out profiles (CH₄/CO/NO oxidation and NO reduction) under model reaction conditions and advanced performance tests and kinetic studies during rapid gas mixture and temperature variations will be systematically conducted.

Project-related publications by participating researchers

Prof. Dr. Silke Behrens
D. I. Sharapa, D. E. Doronkin, F. Studt, J.‐D. Grunwaldt, S. Behrens, Moving frontiers in transition metal catalysis: Synthesis, characterization and modeling, Adv. Mater. 2019, 31, 1807381 DOI: 10.1002/adma.201807381
M. Gentzen, D. E. Doronkin, T. L. Sheppard, A. Zimina, H. Li, J. Jelic, F. Studt, J.-D. Grunwaldt, J. Sauer, S. Behrens, Supported intermetallic PdZn nanoparticles as bifunctional catalysts for the direct synthesis of dimethyl ether from CO-rich synthesis gas, Angew. Chem. Int. Ed. 2019, 58, 15655-15659 DOI: 10.1002/anie.201906256
M. Gentzen, D.E. Doronkin, T.L. Sheppard, J.-D. Grunwaldt, J. Sauer, S. Behrens, An intermetallic Pd₂Ga nanoparticle catalyst for the single step conversion of CO-rich synthesis gas to dimethyl ether, Appl. Catal.A, 2018, 562, 206-214 DOI: 10.1016/j.apcata.2018.04.018
A. Llevot, B. Monney, A. Sehlinger, S. Behrens, M. A. R. Meier, Highly efficient Tsuji–Trost allylation in water catalyzed by Pd-nanoparticles, Chem. Commun. 2017, 53, 5175-5178 DOI: 10.1039/C7CC02380D
S. Behrens, G. Spittel, A new palladium nanoparticle catalyst on mesoporous silica prepared from a molecular cluster precursor, Dalton Trans. 2005, 868-873 DOI: 10.1039/B415665J

Prof. Dr. Silke Behrens

D. I. Sharapa, D. E. Doronkin, F. Studt, J.‐D. Grunwaldt, S. Behrens, Moving frontiers in transition metal catalysis: Synthesis, characterization and modeling, Adv. Mater. 2019, 31, 1807381

DOI: 10.1002/adma.201807381

M. Gentzen, D. E. Doronkin, T. L. Sheppard, A. Zimina, H. Li, J. Jelic, F. Studt, J.-D. Grunwaldt, J. Sauer, S. Behrens, Supported intermetallic PdZn nanoparticles as bifunctional catalysts for the direct synthesis of dimethyl ether from CO-rich synthesis gas, Angew. Chem. Int. Ed. 2019, 58, 15655-15659

DOI: 10.1002/anie.201906256

M. Gentzen, D.E. Doronkin, T.L. Sheppard, J.-D. Grunwaldt, J. Sauer, S. Behrens, An intermetallic Pd₂Ga nanoparticle catalyst for the single step conversion of CO-rich synthesis gas to dimethyl ether, Appl. Catal.A, 2018, 562, 206-214

DOI: 10.1016/j.apcata.2018.04.018

A. Llevot, B. Monney, A. Sehlinger, S. Behrens, M. A. R. Meier, Highly efficient Tsuji–Trost allylation in water catalyzed by Pd-nanoparticles, Chem. Commun. 2017, 53, 5175-5178

DOI: 10.1039/C7CC02380D

S. Behrens, G. Spittel, A new palladium nanoparticle catalyst on mesoporous silica prepared from a molecular cluster precursor, Dalton Trans. 2005, 868-873

DOI: 10.1039/B415665J

Dr. Maria Casapu
E. Ogel, M. Casapu, D. E. Doronkin, R. Popescu, H. Störmer, C. Mechler, G. Marzun, S. Barcikowski, M. Türk, J.-D. Grunwaldt, Impact of preparation method and hydrothermal aging on particle size distribution of Pt/γ-Al₂O₃ and its performance in CO and NO oxidation, J. Phys. Chem. C, 2019, 123, 9, 5433-5446 DOI: 10.1021/acs.jpcc.8b11065
A.M. Gänzler, M. Casapu, F. Maurer, H. Störmer, D. Gerthsen, G. Ferré, P. Vernoux, B. Bornmann, R. Frahm, V. Murzin, Tuning the Pt/CeO₂ interface by in situ variation of the Pt particle size, ACS Catal. 2018, 8, 4800-4811 DOI: 10.1021/acscatal.8b00330
M. Casapu, A. Bernhard, D. Peitz, M. Mehring, M. Elsener, O. Kröcher, A Niobia-Ceria based multi-purpose catalyst for soot oxidation, urea hydrolysis, and selective catalytic reduction of NOx in diesel exhaust, Appl. Catal. B, 2011, 103, 79-84 DOI: 10.1016/j.apcatb.2011.01.011
M. Casapu, A. Fischer, A.M. Gänzler, R. Popescu, M. Crone, D. Gerthsen, M. Türk, J.-D. Grunwaldt, Origin of the normal and inverse hysteresis behavior during CO oxidation over Pt/Al₂O₃, ACS Catal. 2017, 7, 343-355 DOI: 10.1021/acscatal.6b02709
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

Dr. Maria Casapu

E. Ogel, M. Casapu, D. E. Doronkin, R. Popescu, H. Störmer, C. Mechler, G. Marzun, S. Barcikowski, M. Türk, J.-D. Grunwaldt, Impact of preparation method and hydrothermal aging on particle size distribution of Pt/γ-Al₂O₃ and its performance in CO and NO oxidation, J. Phys. Chem. C, 2019, 123, 9, 5433-5446

DOI: 10.1021/acs.jpcc.8b11065

A.M. Gänzler, M. Casapu, F. Maurer, H. Störmer, D. Gerthsen, G. Ferré, P. Vernoux, B. Bornmann, R. Frahm, V. Murzin, Tuning the Pt/CeO₂ interface by in situ variation of the Pt particle size, ACS Catal. 2018, 8, 4800-4811

DOI: 10.1021/acscatal.8b00330

M. Casapu, A. Bernhard, D. Peitz, M. Mehring, M. Elsener, O. Kröcher, A Niobia-Ceria based multi-purpose catalyst for soot oxidation, urea hydrolysis, and selective catalytic reduction of NOx in diesel exhaust, Appl. Catal. B, 2011, 103, 79-84

DOI: 10.1016/j.apcatb.2011.01.011

M. Casapu, A. Fischer, A.M. Gänzler, R. Popescu, M. Crone, D. Gerthsen, M. Türk, J.-D. Grunwaldt, Origin of the normal and inverse hysteresis behavior during CO oxidation over Pt/Al₂O₃, ACS Catal. 2017, 7, 343-355

DOI: 10.1021/acscatal.6b02709

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 B - Porous catalysts