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Highly Ordered Mesoporous Cobalt-Containing Oxides: Structure, Catalytic Properties, and Active Sites in Oxidation of Carbon Monoxide

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Gu,  Dong
Research Department Schüth, Max-Planck-Institut für Kohlenforschung, Max Planck Society;

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Jia,  Chun-Jiang
Research Group Rinaldi, Max-Planck-Institut für Kohlenforschung, Max Planck Society;
Key Lab for Colloid and Interface Chemistry, School of Chemistry and Chemical Engineering, Shandong University, Jinan 250100, People’s Republic of China;

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Weidenthaler,  Claudia
Research Group Weidenthaler, Max-Planck-Institut für Kohlenforschung, Max Planck Society;

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Bongard,  Hans-Josef
Service Department Lehmann (EMR), Max-Planck-Institut für Kohlenforschung, Max Planck Society;

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Spliethoff,  Bernd
Service Department Lehmann (EMR), Max-Planck-Institut für Kohlenforschung, Max Planck Society;

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Schmidt,  Wolfgang
Research Group Schmidt, Max-Planck-Institut für Kohlenforschung, Max Planck Society;

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Schüth,  Ferdi
Research Department Schüth, Max-Planck-Institut für Kohlenforschung, Max Planck Society;

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Citation

Gu, D., Jia, C.-J., Weidenthaler, C., Bongard, H.-J., Spliethoff, B., Schmidt, W., et al. (2015). Highly Ordered Mesoporous Cobalt-Containing Oxides: Structure, Catalytic Properties, and Active Sites in Oxidation of Carbon Monoxide. Journal of the American Chemical Society, 137(35), 11407-11418. doi:10.1021/jacs.5b06336.


Cite as: http://hdl.handle.net/11858/00-001M-0000-0028-7E82-C
Abstract
Co3O4 with a spinel structure is a very active oxide catalyst for the oxidation of CO. In such catalysts, octahedrally coordinated Co3+ is considered to be the active site, while tetrahedrally coordinated Co2+ is assumed to be basically inactive. In this study, a highly ordered mesoporous CoO has been prepared by H2 reduction of nanocast Co3O4 at low temperature (250 °C). The as-prepared CoO material, which has a rock-salt structure with a single Co2+ octahedrally coordinated by lattice oxygen in Fm3̅m symmetry, exhibited unexpectedly high activity for CO oxidation. Careful investigation of the catalytic behavior of mesoporous CoO catalyst led to the conclusion that the oxidation of surface Co2+ to Co3+ causes the high activity. Other mesoporous spinels (CuCo2O4, CoCr2O4, and CoFe2O4) with different Co species substituted with non/low-active metal ions were also synthesized to investigate the catalytically active site of cobalt-based catalysts. The results show that not only is the octahedrally coordinated Co3+ highly active but also the octahedrally coordinated Co2+ species in CoFe2O4 with an inverse spinel structure shows some activity. These results suggest that the octahedrally coordinated Co2+ species is easily oxidized and shows high catalytic activity for CO oxidation.