Cluster: Integrale Konzepte der Katalyse II (D1/E1, D2/E2)

D1: Chemical activation of methane
The chemical activation of methane is done within the framework of oxidative coupling of methane (OCM). We persue a multi-scale approach that combines con­cepts and methodologies of chemical syn­thesis, physical chemistry and surface sci­ence with chemical engineering.
Our first research package is devoted to the experimental and theoretical analysis of ho­mogeneous (gas phase) processes, extended over all relevant dimensions of transport, to achieve a comprehensive kinetic description based upon observables or theoretically verified input data.
The existing family of reaction models will be validated and combined with our second research package, dedicated to identi­fying the relevant surface reactions, determine the concomitantly released heat, and identify the species that are dissociated from the surface to activate the gas phase reaction.
D2: Dry reforming of methane (DRM)
Due to the low selectivity of methane activation, oxidative coupling of methane (OCM) is associated with a considerable pro­duction of CO2 which in turn requires costly separation procedures in industrial applications.
Thus, concomitant to the improvement of the OCM process, the studies in this research band aim at conversion routes of CO2 that may be combined with the OCM process, i.e., the dry reform­ing of methane (DRM):
CH4 + CO2 → 2 CO + 2 H2 (D2-1).
Here we follow the same multi-scale strategy as outlined for OCM. Cata­lytic model systems on ideal surfaces are systematically explored in terms of the adsorption behavior of reactants and putative intermediates and products. In a model approach the acti­vation of CO2 with basic and redox species will be studied over binary and ternary manganese oxo gas phase clusters and thin chromium oxide films with well-controlled defect chemistry.

Principal investigators
Sauer, Joachim Prof. Dr. rer. nat. Dr. h.c. (Details) (Theoretical Chemistry / Quantum Chemistry)

DFG-Exzellenzinitiative: Cluster

Duration of project
Start date: 11/2012
End date: 10/2017

M. Haertelt, A. Fielicke, G. Meijer,K. Kwapień, M. Sierka, J. Sauer, Structure determination of neutral MgO clusters - hexagonal nanotubes and cages, Phys. Chem. Chem. Phys. 14 (2012) 2849-2856.

R. Włodarczyk, M. Sierka, J. Sauer, D. Löffler, J. J. Uhlrich, X. Yu, B. Yang, I. M. N. Groot, S. Shaikhutdinov, H. J. Freund, Tuning the electronic structure of ultrathin crystalline silica films on Ru(0001), Phys. Rev. B 85 (2012) 085403.

B. Yang, Y. Pan, X. Lin, N. Nilius, H.-J. Freund, C. Hulot, A. Giraud, S. Blechert, S. Tosoni, J. Sauer, Stabilizing gold adatoms by thiophenyl derivates: A possible route towards metal redispersion, J. Am. Chem. Soc. 134 (2012) 11161-11167.

K. Sillar, J. Sauer, Ab initio prediction of adsorption isotherms for small molecules in metal-organic frameworks (MOFs). The effect of lateral interactions for methane/CPO-27-Mg,
J. Am. Chem. Soc. 134 (2012) 18354-18365.

S. Sicolo, J. Sauer, Interaction of CO with Electron-Rich Defects on MgO(100), J. Phys. Chem. C 117 (2013) 8365–8373.

J. Paier, C. Penschke, J. Sauer, Oxygen defects and the surface chemistry of ceria - quantum chemical studies compared to experiment, Chem. Rev.113 (2013) 3949–3985.

A. D. Boese, J. Sauer, Accurate adsorption energies of small molecules on oxide surfaces: CO–MgO(001), Phys. Chem. Chem. Phys. 15 (2013) 16481–16493.

Z.-C. Wang, J.-W. Liu, M. Schlangen, T. Weiske, D. Schröder, J. Sauer, H. Schwarz, Thermal Methane Activation by a Binary V-Nb Transition-Metal Oxide Cluster Cation: A Further Example for the Crucial Role of Oxygen-Centered Radicals, Chem. Eur. J. 19 (2013) 11496–11501.

T. Kropp. J. Paier. J. Sauer, Support Effect in Oxide Catalysis: Methanol Oxidation on
Vanadia/Ceria, J. Am. Chem. Soc. 136 (2014) 14616-14625.

G. Piccini, M. Alessio, J. Sauer, Y. Zhi, Y. Liu, R. Kolvenbach, A. Jentys, J. A. Lercher, Accurate Adsorption Thermodynamics of Small Alkanes in Zeolites. Ab initio Theory and Experiment for H- Chabazite, J. Phys. Chem. C 119 (2015) 6128-6137.

M. Ončák, R. Włodarczyk, J. Sauer, Water on the MgO(001) Surface: Surface Reconstruction and Ion Solvation, J. Phys. Chem. Lett. 6 (2015) 2310-2314.

C. Tuma, J. Sauer, Quantum chemical ab initio prediction of proton exchange barriers between CH4 and different H-zeolites, J. Chem. Phys. 143 (2015) 102810.

C. Yang, F. Bebensee, A. Nefedov, C. Wöll, T. Kropp, L. Komissarov, C. Penschke, R. Moerer, J. Paier, J. Sauer, Methanol Adsorption on Monocrystalline Ceria Surfaces, J. Catal. 336 (2016) 116-125.

B. Solis, J. Sauer, Y. Cui, S. Shaikhutdinov, H.-J. Freund, Oxygen Scrambling of CO2 Adsorbed on CaO(001), J. Phys. Chem. C 121 (2017) 18625-18634.

C. Yang, X. Yu, S. Heissler, P. Weidler, A. Nefedov, Y. Wang, C. Wöll. T. Kropp, J. Paier, J. Sauer,
O2 Activation on Ceria Catalysts - The Importance of Substrate Crystallographic Orientation, Ang. Chem. Int. Ed. 56 (2017) 16399 -16404
O2-Aktivierung an Cerdioxid-Katalysatoren - Zur Bedeutung der kristallographischen Orientierung des Substrats, Ang. Chem. 129 (2017) 16618-16623.

C. Penschke, J. Paier, J. Sauer, Vanadium Oxide Oligomers and Ordered Monolayers Supported on CeO2(111): Structure and Stability Studied by Density Funtional Theory, J. Phys. Chem. C 122 (2018) 9101-9110.

G. Feng, M. V. Ganduglia-Pirovano, C.-F. Huo, J. Sauer, Hydrogen Spillover to Copper Clusters on Hydroxylated y-Al2O3, J. Phys. Chem. C 122 (2018) 18445-18455.

Last updated on 2022-08-09 at 15:05