Microimaging by IR microscopy is applied to the recording of the evolution of the concentration profiles of reactant and product molecules during catalytic reaction, notably during the hydrogenation of benzene to cyclohexane by nickel dispersed within a nanoporous glass. Being defined as the ratio between the reaction rate in the presence of and without diffusion limitation, the effectiveness factors of catalytic reactions were previously determined by deliberately varying the extent of transport limitation by changing a suitably chosen system parameter, such as the particle size and by comparison of the respective reaction rates. With the novel options of microimaging, effectiveness factors become accessible in a single measurement by simply monitoring the distribution of the reactant molecules over the catalyst particles.
The remarkable differences in the guest diffusivities in nanoporous materials commonly found with the application of different measuring techniques are usually ascribed to the existence of a hierarchy of transport resistances in addition to the diffusional resistance of the pore system and their differing influence due to the differing diffusion path lengths covered by the different measuring techniques. We report diffusion measurements with nanoporous glasses where the existence of such resistances could be avoided. Molecular propagation over diffusion path lengths from hundreds of nanometers up to millimeters was thus found to be controlled by a uniform mechanism, appearing in coinciding results of microscopic and macroscopic diffusion measurement.
Enhancing the activity
and stability of catalysts is a major challenge
in scientific research nowadays. Previous studies showed that the
generation of an additional pore system can influence the catalytic
performance of porous catalysts regarding activity, selectivity, and
stability. This study focuses on the epoxide-mediated sol–gel
synthesis of mixed metal oxides, NiAl
2
O
4
and
CoAl
2
O
4
, with a spinel phase structure, a hierarchical
pore structure, and Ni and Co contents of 3 to 33 mol % with respect
to the total metal content. The sol–gel process is accompanied
by a polymerization-induced phase separation to introduce an additional
pore system. The obtained mixed metal oxides were characterized with
regard to pore morphology, surface area, and formation of the spinel
phase. The Brunauer–Emmett–Teller surface area ranges
from 74 to 138 m
2
·g
–1
and 25 to
94 m
2
·g
–1
for Ni and Co, respectively.
Diameters of the phase separation-based macropores were between 500
and 2000 nm, and the mesopore diameters were 10 nm for the Ni-based
system and between 20 and 25 nm for the cobalt spinels. Furthermore,
Ni–Al spinels with 4, 5, and 6 mol % Ni were investigated in
the dry reforming of CH
4
(DRM) with CO
2
to produce
H
2
and CO. CH
4
conversions near the thermodynamic
equilibrium were observed depending on the Ni content and reaction
temperature. The Ni catalysts were further compared to a noble metal-containing
catalyst based on a spinel system showing comparable CH
4
conversion and carbon selectivity in the DRM.
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