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Redox Properties of Manganese-Containing Zirconia Solid Solution Catalysts Analyzed by In Situ UV–Vis Spectroscopy and Crystal Field Theory

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Klokishner,  Sophia
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;
Institute of Applied Physics of the Academy of Sciences of Moldova;

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Reu,  Oleg
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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Chan-Thaw,  Carine E.
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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Jentoft,  Friederike C.
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;
Chemical, Biological, and Materials Engineering, University of Oklahoma School;

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Schlögl,  Robert
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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Citation

Klokishner, S., Reu, O., Chan-Thaw, C. E., Jentoft, F. C., & Schlögl, R. (2011). Redox Properties of Manganese-Containing Zirconia Solid Solution Catalysts Analyzed by In Situ UV–Vis Spectroscopy and Crystal Field Theory. The Journal of Physical Chemistry A, 115(28), 8100-8112. doi:10.1021/jp2034054.


Cite as: http://hdl.handle.net/11858/00-001M-0000-0012-1BF9-F
Abstract
The optical absorption spectra of manganesepromoted sulfated zirconia, a highly active alkane isomerization catalyst, were found to be characterized by oxygen-to-manganese charge-transfer transitions at 300-320 nm and d-d transitions of manganese ions at 580 and 680 nm. The latter were attributed toMn4þ and Mn3þ ions, which are known to be incorporated in the zirconia lattice. The oxygen surroundings of these ions were modeled assuming a substitutional solid solution. The crystal field splittings, vibronic coupling constants, and oscillator strengths of the manganese ions were calculated on the basis of a cluster model that considers the manganese center as a complex with the adjacent ions of the lattice as ligands. The ratio of Mn3þ to Mn4þ ions was determined using the spectra and the model, and the relative concentrations of Mn2þ, Mn3þ, and Mn4þ ions were determined with the help of the average valence known from X-ray absorption data in the literature. The redox behavior of manganese-promoted sulfated zirconia in oxidizing and inert atmosphere was elucidated at temperatures ranging from 323 to 773 K.