Heterogeneous
catalysts are
essential for the majority of all chemical processes in industry. In
addition, they find numerous applications in refineries and in energy
conversion, and they help to protect the environment.
Nevertheless, their discovery and their optimization has often been
based on trial
and error, and there are only a few cases, in which a complete
understanding on the atomic level was achieved.
The Laboratory of Industrial Chemistry performs fundamental research in
the area of heterogeneous catalysis and aims to develop catalysts based
on mechanistic insight. The scientific challenge is the elucidation of
the reactions on the atomic level and
their interplay with the complex surface chemistry of heterogeneous
catalysts, which usually consist of many phases and components, often
present as nanoparticles or as X-ray amorphous layers.
The examined reactions belong to industrial redox chemistry.
Reduction catalysis comprises methanol synthesis, Fischer-Tropsch
synthesis, or the synthesis of higher alcohols. Oxidation catalysis
focuses on the selective oxidation of propene and methanol, the
oxidative dehydrogenation of hydrocarbons, or the selective oxidation
of alcohols in the gas phase and in the liquid phase. Recently, we
entered the fields of
electrocatalysis and heterogeneous photocatalysis.
Liquid-phase
oxidation and electrocatalysis require a deeper understanding of
solvation-related phenomena.
For the synthesis of catalysts a large repertoire of methods
is
available including chemical vapor deposition, spray drying
and precipitation performed in a cascade of micromixers. In
recent
years
the catalytic growth and surface modification of multiwalled carbon
nanotubes (CNTs) has become a major topic due to the numerous
applications of CNTs in electrocatalysis. All the necessary
routine techniques for catalyst characterization are
available with a strong focus on sorption techniques.
For improving the catalysts we first of all
study steady-state kinetics. Numerous continuously operated
flow set-ups with
online analytics are available, which allow to screen the parameter
space efficiently under full computer control using LabVIEW. The role
of the various elementary steps is investigated by applying transient
kinetic methods such as temperature-programmed reactor operation,
dosing pulses
and concentration steps, and using isotopes including SSITKA. For these
methods we strongly rely on fast online mass spectrometry. In
addition,
we try to gain as much spectroscopic information as possible using
mainly FTIR and photoelectron spectroscopy. Recently, static and
dynamic microcalorimetry have been developed into versatile
tools to
probe the surface properties quantitatively.
Our research contributes to the Collaborative Research
Center SFB 558
"Metal-substrate interactions in heterogeneous catalysis", the
Research Departments Interfacial
Systems Chemistry (IFSC), Materials Research,
and Plasma,
the Center for
Electrochemical Sciences (CES), all at the
Ruhr-University Bochum, and to the Center
for Nanointegration Duisburg-Essen (CeNIDE).
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Stearate-based
Cu colloids in methanol synthesis: structrual changes driven by strong
metal-support interactions, S. Schimpf, A. Rittermeier, X.
Zhang, Z. Li, M. Spasova, M. van den Berg, M. Farle, Y. Wang, R.
Fischer, M. Muhler, ChemCatChem,
2010,
2, 214-222
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Electrocatalytic
activity and stability of nitrogen-containing carbon nanotubes in the
oxygen reduction reaction, S. Kundu, T. C. Nagaiah, W.
Xia, Y. Wang, S. van Dommele, J. H. Bitter, M. Santa, G. Grundmeier, M.
Bron, W. Schuhmann, M.
Muhler, J. Phys. Chem. C,
2009,
113, 14302-14310
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A
highly efficient gas-phase route for the oxygen-functionalization of
carbon nanotubes based on nitric acid vapor, W. Xia, C.
Jin, S. Kundu, M. Muhler, Carbon,
2009,
47, 919-922
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High
surface area ZnO nanoparticles via a novel continuous precipitation
route, S. Kaluza, M. K. Schröter, R. Naumann
d'Alnoncourt, T. Reinecke, M. Muhler, Adv. Funct. Mater.,
2008,
18, 3670-3677
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Consistent
approach
to adsorption thermodynamics on heterogeneous surfaces using different
empirical energy distribution models, X. Xia, S. Litvinov,
M.
Muhler, Langmuir,
2006,
22, 8063-8070
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The
influence of
strongly reducing conditions on strong metal-support interactions in
Cu/ZnO catalysts used for methanol synthesis, R. Naumann
d'
Alnoncourt, X. Xia, J. Strunk, E. Löffler, O. Hinrichsen, M.
Muhler, Phys. Chem.
Chem.
Phys., 2006,
8,
1556-1565
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On the
mechanism of
the oxidative amination of benzene with ammonia to aniline over NiO/ZrO2
as cataloreactant, N. Hoffmann, M. Muhler, Catal. Lett., 2005, 155-159
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The
two-step
chemical vapor deposition of Pd(allyl)Cp as an atom-efficient route to
synthesize highly dispersed palladium nanoparticles on carbon nanofibers,
C. Liang, W. Xia, H. Soltani-Ahmadi, O. F.-K. Schlüter, R. A.
Fischer, M. Muhler, Chem.
Commun, 2005,
282-284
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On the
nature of
the active state of supported ruthenium catalysts used for the
oxidation of carbon monoxide: Steady-state and transient kinetics
combined with in situ Infrared Spectroscopy, J.
Aßmann, V.
Narkhede, L. Khodeir, E. Löffler, O. Hinrichsen, A. Birkner,
H.
Over, M. Muhler, J.
Phys.
Chem. B, 108, 2004,
14634-14642
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Mechanistic
studies on
the oxidative dehydrogenation of methanol over polycrystalline silver
using the temporal-analysis-of-products approach, A. C.
van Veen, O. Hinrichsen, M. Muhler, J. Catal., 2002, 209, 501-514
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The
ammonia synthesis catalyst of the next generation: barium-promoted
ruthenium, H. Bielawa, O. Hinrichsen, A. Birkner, M.
Muhler, Angew. Chemie
Int. Ed., 2001,
40, 1061-1063
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On the
role of monomeric vanadyl species in toluene adsorption and oxidation
on V2O5/TiO2 catalysts: a Raman and in situ
DRIFTS study, S. Besselmann, E. Löffler, M.
Muhler, J. Mol. Catal.
A: Chem. 2000,
162 , 393-403
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