Arbeitsgruppe Kleist

Forschung

von Prof. Dr. Wolfgang Kleist

Forschung

Katalysatorentwicklung

Unsere Arbeitsgruppe beschäftigt sich mit dem Design von neuartigen Heterogenkatalysatoren. Ein Schwerpunkt liegt dabei auf der Entwicklung von hochdefinierten Single-Site-Katalysatoren auf Basis von Metall-organischen Gerüstverbindungen (MOFs) sowie Zeolithen. Außerdem werden über klassische und innovative Präparationsmethoden geträgerte Übergangsmetallkatalysatoren hergestellt.

Katalytische Anwendungen

Unsere Heterogenkatalysatoren werden in verschiedenen Flüssig- und Gasphasenreaktionen eingesetzt. Hier werden relevante Reaktionsparameter gezielt variiert, um Umsätze, Ausbeuten und Selektivitäten zu optimieren. Kinetische und mechanistische Studien werden durchgeführt, um die Reaktionsmechanismen der katalytischen Umsetzungen besser zu verstehen und Struktur-Aktivitäts-Korrelationen zu bestimmen.

Zu den aktuell untersuchten Prozessen gehören insbesondere Power-to-X-Reaktionen (Methanisierung von CO2, Fischer-Tropsch, Alkoholsynthese), selektive Oxidationsreaktionen und C-C-Kupplungsreaktionen in flüssiger Phase.

Röntgenbasierte Charakterisierungsmethoden

Neben verschiedenen Standardcharakterisierungsmethoden setzen wir insbesondere röntgenbasierte Charakterisierungsmethoden ein, um die Strukturen unserer Katalysatorsysteme auf molekularer Ebene zu anlaysieren. Zur Strukturaufklärung der Materialien und der Identifizierung von strukturellen Veränderungen während der Katalyse werden Strukturverfeinerungen in Kombination mit hochauflösenden Röntgenpulverdiffraktometriemessungen durchgeführt. Die lokale chemische Umgebung und die Oxidationszustände der Übergangsmetallzentren werden mittels Röntgenabsorptionsspektroskopie analysiert.

Publikationsliste

Buchbeiträge


4. Hydrodeoxygenation of lignocellulose-derived platform molecules,
K. Hengst, M. Schubert, W. Kleist, J.-D. Grunwaldt, in Catalytic Hydrogenation for Biomass Valorization (R. Rinaldi, Editor), RSC Energy and Environment Series No.13, The Royal Society of Chemistry, 2015, p. 125-150.

3. High output catalyst development in heterogeneous gas phase catalysis,
W. Kleist, J.-D. Grunwaldt, in Modern Applications of High Throughput R&D in Heterogeneous Catalysis (A. Hagemeyer, A.F. Volpe Jr., Eds.), Bentham Science Publishers, 2014, p. 357-371.

2. Global challenges in chemicals and energies - Standardization and acceleration of catalysis R+D,
M. Schneider, B. Alston, S. Higgins, H. Davies, A. Creeth, R.J. Nichols, A.I. Cooper, F. Dumeignil, L. Montagne, R. Froidevaux, S. Heyte, S. Junwen, J. Xiaomei, S. Min, M. Xuhong, W. Kleist, J.-D. Grunwaldt, in Modern Applications of High Throughput R&D in Heterogeneous Catalysis (A. Hagemeyer, A.F. Volpe Jr., Eds.), Bentham Science Publishers, 2014, p. 310-316.

1. Amination reactions,
T. Mallat, A. Baiker, W. Kleist, K. Köhler, in Handbook of Heterogeneous Catalysis, 2nd Edition (G. Ertl, H. Knözinger, F. Schüth, J. Weitkamp, Eds.), Wiley-VCH, Weinheim, 2008, p. 3548-3564.

Patente


2. Process for the preparation of a mixed oxide catalysts by flame spray pyrolysis,
P. Sprenger, J.-D. Grunwaldt, W. Kleist, A. Fischer, EP3323510 (A1), 2018.

1. Method for the hydrothermal preparation of molybdenum-bismuth-cobalt-iron-based mixed oxide catalysts,
P. Sprenger, J.-D. Grunwaldt, W. Kleist, A. Fischer, WO2017157837 (A1), 2017.

Wissenschaftliche Journale


55. One-step synthesis of core-shell-structured mixed-metal CPO-27(Cu,Co) and investigations on its controlled thermal transformation,
J. Bitzer, C. Göbel, A. Muhamad Ismail, Q. Fu, M. Muhler, W. Kleist, Eur. J. Inorg. Chem.2021, accepted for publication, doi: 10.1002/ejic.202100227.

54. Formic acid-assisted selective hydrogenolysis of 5-hydroxymethylfurfural to 2,5-dimethylfuran over bifunctional Pd nanoparticles supported on N-doped mesoporous carbon,
B. Hu, L. Warczinski, X. Li, M. Lu, J. Bitzer, M. Heidelmann, T. Eckhard, Q. Fu, J. Schulwitz, M. Merko, M. Li, W. Kleist, C. Hättig, M. Muhler, B. Peng, Angew. Chem. Int. Ed.2021, 60, 6807-6815; Angew. Chem.2021, 133, 6882-6891.

53. Increasing the complexity in the MIL-53 structure: The combination of the mixed-metal and the mixed-linker concepts,
J. Bitzer, Teubnerová, W. Kleist, Chem. Eur. J.2021, 27, 1724-1735.

52. Hard X-ray-based techniques for structural investigations of CO2 methanation catalysts prepared by MOF decomposition,
N. Prinz, L. Schwensow, S. Wendholt, A. Jentys, M. Bauer, W. Kleist, M. Zobel, Nanoscale2020, 12, 15800-15813.

51. The introduction of functional side groups and the application of the mixed-linker concept in divalent MIL-53(Ni) materials,
J. Bitzer, A. Titze-Alonso, A. Roshdy, W. Kleist, Dalton Trans.2020, 49, 9148-9154.

50. Tailoring the breathing behavior of functionalized MIL-53(Al,M)-NH2 materials by using the mixed-metal concept,
J. Bitzer, S.-L. Heck, W. Kleist, Microporous Mesoporous Mater.2020, 308, 110329.

49. Experimental evidence for the incorporation of two metals at equivalent lattice positions in mixed-metal metal-organic frameworks,
J. Bitzer, S. Otterbach, K. Thangavel, A. Kultaeva, R. Schmid, A. Pöppl, W. Kleist, Chem. Eur. J.2020, 26, 5667-5675.

48. Post-synthetic modification of DUT-5-based metal-organic frameworks for the generation of single-site catalysts and their application in selective epoxidation reactions,
C. Yildiz, K. Kutonova, S. Oßwald, A. Titze-Alonso, J. Bitzer, S. Bräse, W. Kleist, ChemCatChem2020, 12, 1134-1142.

47. Continuous production of higher alcohols from synthesis gas and ethanol using Cs-modified CuO/ZnO/Al2O3 catalysts,
K.M. Walter, M.-A. Serrer, W. Kleist, J.-D. Grunwaldt, Appl. Catal. A - Gen.2019, 585, 117150.

46. Regulating the size and spatial distribution of Pd nanoparticles supported by the defect engineered metal-organic framework HKUST-1 and applied in the aerobic oxidation of cinnamyl alcohol,
P. Guo, Q. Fu, C. Yildiz, Y.-T. Chen, K. Ollegott, C. Froese, W. Kleist, R.A. Fischer, Y. Wang, M. Muhler, B. Peng, Catal. Sci. Technol.2019, 9, 3703-3710.

45. Enhancing the water splitting performance of cryptomelane-type α-(K)MnO2,
H. Antoni, D.M. Morales, J. Bitzer, Q. Fu, Y.-T. Chen, J. Masa, W. Kleist, W. Schuhmann, M. Muhler, J. Catal.2019, 374, 335-344.

44. Synthesis strategies and structural arrangements of isoreticular mixed-component metal-organic frameworks,
J. Bitzer, W. Kleist, Chem. Eur. J.2019, 25, 1866-1882.

43. CuPd mixed-metal HKUST-1 as a catalyst for aerobic alcohol oxidation,
P. Guo, C. Froese, Q. Fu, Y.-T. Chen, B. Peng, W. Kleist, R.A. Fischer, M. Muhler, Y. Wang, J. Phys. Chem. C2018, 122, 21433-21440.

42. Supported gold- and silver-based catalysts for the selective aerobic oxidation of 5-(hydroxymethyl)furfural to 2,5-furandicarboxylic acid and 5-hydroxymethyl-2-furancarboxylic acid,
O.R. Schade, K.F. Kalz, D. Neukum, W. Kleist, J.-D. Grunwaldt, Green Chem.2018, 20, 3530-3541.

41. Reactivity of bismuth molybdates for selective oxidation of propylene probed by correlative operando spectroscopies,
P. Sprenger, M. Stehle, A. Gaur, A.M. Gänzler, D. Gashnikova, W. Kleist, J.-D. Grunwaldt, ACS Catal.2018, 8, 6462-6475.

40. Operando Raman spectroscopy on CO2 methanation over alumina-supported Ni, Ni3Fe and NiRh0.1 catalysts: role of carbon formation as possible deactivation pathway,
B. Mutz, P. Sprenger, W. Wang, D. Wang, W. Kleist, J.-D. Grunwaldt, Appl. Catal. A - Gen.2018, 556, 160-171.

39. Surface oxidation of supported Ni particles and its impact on the catalytic performance during dynamically operated methanation of CO2,
B. Mutz, A.M. Gänzler, M. Nachtegaal, O. Müller, R. Frahm, W. Kleist, J.-D. Grunwaldt, Catalysts2017, 7, 279.

38. Potential of an alumina supported Ni3Fe catalyst in the methanation of CO2: impact of alloy formation on activity and stability,
B. Mutz, M. Belimov, W. Wang, P. Sprenger, M.-A. Serrer, P. Pfeifer, W. Kleist, J.-D. Grunwaldt, ACS Catal.2017, 7, 6802–6814.

37. Aerobic oxidation of α-pinene catalyzed by homogeneous and MOF-based Mn catalysts,
Y.S. Raupp, C. Yildiz, W. Kleist, M.A.R. Meier, Appl. Catal. A - Gen.2017, 546, 1-6.

36. Recent advances in selective propylene oxidation over bismuth molybdate based catalysts: Novel synthetic, spectroscopic and theoretical approaches,
P. Sprenger, W. Kleist, J.-D. Grunwaldt, ACS Catal.2017, 7, 5628-5642.

35. Continuous synthesis of γ–valerolactone in a trickle-bed reactor over supported nickel catalysts,
K. Hengst, D.A.J.M. Ligthart, D.E. Doronkin, K.M. Walter, W. Kleist, E.J.M. Hensen, J.-D. Grunwaldt, Ind. Eng. Chem. Res.2017, 56, 2680-2689.

34. Dynamic transformation of small Ni particles during methanation of CO2 under fluctuating reaction conditions monitored by operando X-ray absorption spectroscopy,
B. Mutz, H.W.P. Carvalho, W. Kleist, J.-D. Grunwaldt, J. Phys. Conf. Ser.2016, 712, 012050.

33. Bismuth molybdate catalysts prepared by mild hydrothermal synthesis: Influence of pH on the selective oxidation of propylene,
K. Schuh, W. Kleist, M. Høj, V. Trouillet, P. Beato, A.D. Jensen, J.-D. Grunwaldt, Catalysts2015, 5, 1554-1573.

32. Synthesis and post‐synthetic modification of amine‐, alkyne‐, azide‐ and nitro‐functionalized metal-organic frameworks based on DUT‐5,
M.A. Gotthardt, S. Grosjean, T.S. Brunner, J. Kotzel, A.M. Gänzler, S. Wolf, S. Bräse, W. Kleist, Dalton Trans.2015, 44, 16802-16809.

31. Continuous catalytic hydrodeoxygenation of guaiacol over Pt/SiO2 and Pt/H-MFI-90,
M. Hellinger, S. Baier, P.M. Mortensen, W. Kleist, A.D. Jensen, J.-D. Grunwaldt, Catalysts2015, 5, 1152-1166.

30. Synthesis of γ-valerolactone by hydrogenation of levulinic acid over supported nickel catalysts,
K. Hengst, M. Schubert, H.W.P. Carvalho, C. Lu, W. Kleist, J.-D. Grunwaldt, Appl. Catal. A - Gen.2015, 502, 18-26.

29. Systematic study on the influence of the morphology of α-MoO3 on the selective oxidation of propylene,
K. Schuh, W. Kleist, M. Høj, A.D. Jensen, P. Beato, G.R. Patzke, J.-D. Grunwaldt, J. Solid State Chem.2015, 228, 42-52.

28. Methanation of CO2: Structural response of a Ni-based catalyst under fluctuating reaction conditions unraveled by operando spectroscopy,
B. Mutz, H.W.P. Carvalho, S. Mangold, W. Kleist, J.-D. Grunwaldt, J. Catal.2015, 327, 48-53.

27. Effect of the addition of ethanol to synthesis gas on the production of higher alcohols over Cs and Ru modified Cu/ZnO catalysts,
K.M. Walter, M. Schubert, W. Kleist, J.-D. Grunwaldt, Ind. Eng. Chem. Res.2015, 54, 1452-1463.

26. Synthesis and characterization of bimetallic metal-organic framework Cu-Ru-BTC with HKUST-1 structure,
M.A. Gotthardt, R. Schoch, S. Wolf, M. Bauer, W. Kleist, Dalton Trans.2015, 44, 2052-2056.

25. Design of highly porous single-site catalysts through two-step postsynthetic modification of mixed-linker MIL-53(Al),
M.A. Gotthardt, R. Schoch, T.S. Brunner, M. Bauer, W. Kleist, ChemPlusChem2015, 80, 188-195.

24. Catalytic hydrodeoxygenation of guaiacol over platinum supported on metal oxides and zeolites,
M. Hellinger, H.W. Pereira de Carvalho, S. Baier, D. Wang, W. Kleist, J.-D. Grunwaldt, Appl. Catal. A - Gen.2015, 490, 181-192.

23. One-step synthesis of bismuth molybdate catalysts via flame spray pyrolysis for the selective oxidation of propylene,
K. Schuh, W. Kleist, M. Høj, V. Trouillet, A.D. Jensen, J.-D. Grunwaldt, Chem. Commun.2014, 50, 15404-15406.

22. Selective oxidation of propylene to acrolein by hydrothermally synthesized bismuth molybdates,
K. Schuh, W. Kleist, M. Høj, V. Trouillet, P. Beato, A.D. Jensen, G.R. Patzke, J.-D. Grunwaldt, Appl. Catal. A - Gen.2014, 482, 145-156.

21. Post-synthetic immobilization of palladium complexes on metal-organic frameworks - A new concept for the design of heterogeneous catalysts for Heck reactions,
M.A. Gotthardt, A. Beilmann, R. Schoch, J. Engelke, W. Kleist, RSC Adv.2013, 3, 10676-10679.

20. Salen-based coordination polymers of manganese and the rare earth elements - Synthesis and catalytic aerobic epoxidation of olefins,
A. Bhunia, M.A. Gotthardt, M. Yadav, M.T. Gamer, A. Eichhöfer, W. Kleist, P.W. Roesky, Chem. Eur. J.2013, 19, 1986-1995.

19. Aerobic epoxidation of olefins catalyzed by the metal-organic framework STA-12(Co),
M.J. Beier, W. Kleist, M.T. Wharmby, R. Kissner, B. Kimmerle, P.A. Wright, J.-D. Grunwaldt, A. Baiker, Chem. Eur. J.2012, 18, 887-898.

18. Synthesis, structural properties and catalytic behavior of Cu-BTC and mixed-linker Cu-BTC-PyDC in the oxidation of benzene derivatives,
S. Marx, W. Kleist, A. Baiker, J. Catal.2011, 281, 76-87.

17. Identification of the active species generated from supported Pd catalysts in Heck reactions: An in situ quick scanning EXAFS investigation,
S. Reimann, J. Stötzel, R. Frahm, W. Kleist, J.-D. Grunwaldt, A. Baiker, J. Am. Chem. Soc.2011, 133, 3921-3930.

16. Effect of dehydration on the local structure of framework aluminum atoms in mixed-linker MIL-53(Al) materials studied by solid-state NMR spectroscopy,
Y. Jiang, J. Huang, S. Marx, W. Kleist, M. Hunger, A. Baiker, J. Phys. Chem. Lett.2010, 1, 2886-2890.

15. Flame-made MgAl2−xMxO4 (M= Mn, Fe, Co) mixed oxides: Structural properties and catalytic behavior in methane combustion,
N. van Vegten, T. Baidya, F. Krumeich, W. Kleist, A. Baiker, Appl. Catal., B2010, 97, 398-406.

14. Tuning functional sites and thermal stability of mixed-linker MOFs based on MIL-53(Al),
S. Marx, W. Kleist, J. Huang, M. Maciejewski, A. Baiker, Dalton Trans.2010, 39, 3795-3798.

13. Platinum nanoparticles: Crucial role of crystal face and colloid stabilizer in the diastereoselective hydrogenation of cinchonidine,
E. Schmidt, W. Kleist, F. Krumeich, T. Mallat, A. Baiker, Chem. Eur. J.2010, 16, 2181-2192.

12. MOF-5 based mixed-linker metal-organic framework: Synthesis, thermal stability and catalytic application,
W. Kleist, M. Maciejewski, A. Baiker, Thermochim. Acta2010, 499, 71-78.

11. Mixed-linker metal-organic frameworks as catalysts for the synthesis of propylene carbonate from propylene oxide and CO2,
W. Kleist, F. Jutz, M. Maciejewski, A. Baiker, Eur. J. Inorg. Chem.2009, 3552-3561.

10. Amination of aryl chlorides and fluorides toward the synthesis of aromatic amines by palladium catalyzed route or transition metal free way: Scopes and limitations,
W. Kleist, S.S. Pröckl, M. Drees, L. Djakovitch, K. Köhler, J. Mol. Catal. A: Chem.2009, 303, 15-22.

9. Pd/MOx materials synthesized by sol-gel co-precipitation as catalysts for carbon-carbon coupling reactions of aryl bromides and chlorides,
W. Kleist, J.-K. Lee, K. Köhler, Eur. J. Inorg. Chem.2009, 261-266.

8. Heck reactions of aryl chlorides catalyzed by ligand free palladium salts,
W. Kleist, S.S. Pröckl, K. Köhler, Catal. Lett.2008, 125, 197-200.

7. Gold-catalyzed aerobic oxidation of benzyl alcohol: Effect of gold particle size on activity and selectivity in different solvents,
P. Haider, B. Kimmerle, F. Krumeich, W. Kleist, J.-D. Grunwaldt, A. Baiker, Catal. Lett.2008, 125, 169-176.

6. Genesis of coordinatively unsaturated palladium complexes dissolved from solid precursors during Heck coupling reactions and their role as catalytically active species,
K. Köhler, W. Kleist, S.S. Pröckl, Inorg. Chem.2007, 46, 1873-1883.

5. A simple aqueous phase synthesis of high surface area aluminum fluoride and its bulk and surface structure,
W. Kleist, C. Haeßner, O. Storcheva, K. Köhler, Inorg. Chim. Acta2006, 359, 4851-4854.

4. Supported palladium catalysts in Heck coupling reactions - Problems, potential and recent advances,
K. Köhler, S.S. Pröckl, W. Kleist, Curr. Org. Chem.2006, 10, 1585-1601.

3. Copper-free heterogeneous catalysts for the Sonogashira cross-coupling reaction: Preparation, characterisation, activity and applications for organic synthesis,
P. Rollet, W. Kleist, V. Dufaud, L. Djakovitch, J. Mol. Catal. A: Chem.2005, 241, 39-51.

2. Design of highly active heterogeneous palladium catalysts for the activation of aryl chlorides in Heck reactions,
S.S. Pröckl, W. Kleist, K. Köhler, Tetrahedron2005, 61, 9855-9859.

1. In-situ generation of molecular Pd species from solid catalysts - A new successful concept for the activation of aryl chlorides in the Heck reaction,
S.S. Pröckl, W. Kleist, M. A. Gruber, K. Köhler, Angew. Chem. Int. Ed.2004, 43, 1881-1882; Angew. Chem.2004, 116, 1917-1918.

Akademische Schriften


3. Novel concepts for the design of single-site catalysts based on metal-organic frameworks,
W. Kleist, Habilitationsschrift, Karlsruher Institut für Technologie (KIT), 2014.

2. The understanding of the reaction mechanism as the basis for the design of highly active heterogeneous palladium catalysts and optimized reaction conditions for coupling reactions in organic synthesis,
W. Kleist, Dissertation, Technische Universität München, 2006.

1. Palladium-Metalloxid-Katalysatoren für Heck-Reaktionen mit Brom- und Chloraromaten - Neuartige Präparationsmethoden durch Sol-Gel-Verfahren
W. Kleist, Diplomarbeit, Technische Universität München, 2003.

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