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Shape-Controlled CeO2 Nanoparticles: Stability and Activity in the Catalyzed HCl Oxidation Reaction
journal contribution
posted on 2017-08-11, 00:00 authored by Chenwei Li, Yu Sun, Igor Djerdj, Pascal Voepel, Carl-Christian Sack, Tobias Weller, Rüdiger Ellinghaus, Joachim Sann, Yanglong Guo, Bernd M. Smarsly, Herbert OverCeO2 is a promising catalyst for the HCl oxidation (Deacon
process) in order to recover Cl2. Employing shape-controlled
CeO2 nanoparticles (cubes, octahedrons, rods) with facets
of preferential orientations ((100), (111), (110)), we studied the
activity and stability under two reaction conditions (harsh: Ar:HCl:O2 = 6:2:2 and mild: Ar:HCl:O2 = 7:1:2). It turns
out that both activity and stability are structure-sensitive. In terms
of space time yield (STY), the rods are the most active particles,
followed by the cubes and finally the octahedrons. This very same
trend is reconciled with the complete oxygen storage capacity (OSCc),
indicating a correlation between the observed activity STY and the
OSCc. The apparent activation energies are about 50 kJ/mol for cubes
and rods, while the octahedrons reveal an apparent activation energy
of 65 kJ/mol. The reaction order in O2 is positive (0.26–0.32).
Under mild reaction conditions, all three morphologies are stable,
consistent with corresponding studies of CeO2 powders and
CeO2 nanofibers. Under harsh reaction conditions, however,
cubes and octahedrons are both instable, forming hydrated CeCl3, while rods are still stable. The present stability and activity
experiments in the catalytic HCl oxidation reaction over shape-controlled
CeO2 nanoparticles may serve as benchmarks for future ab
initio studies of the catalyzed HCl oxidation reaction over well-defined
CeO2 surfaces.
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stabilityshape-controlled CeO 2 nanoparticlescubeCatalyzed HCl Oxidation Reaction CeO 2HCl oxidation reactionCeO 2 surfacesfuture ab initio studiesreaction conditionsShape-Controlled CeO 2 NanoparticlesCeO 2 powdersoxygen storage capacityoctahedronCeO 2 nanofibersSTYEmploying shape-controlled CeO 2 nanoparticles
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