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Supported palladium nanoparticles on hybrid mesoporous silica: Structure/activity-relationship in the aerobic alcohol oxidation using supercritical carbon dioxide

MPS-Authors
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Hou,  Zhenshan
Service Department Theyssen (Technical Labs), Max-Planck-Institut für Kohlenforschung, Max Planck Society;

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Theyssen,  Nils
Service Department Theyssen (Technical Labs), Max-Planck-Institut für Kohlenforschung, Max Planck Society;

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Brinkmann,  Axel
Service Department Theyssen (Technical Labs), Max-Planck-Institut für Kohlenforschung, Max Planck Society;

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Bühl,  Michael
Research Department Thiel, Max-Planck-Institut für Kohlenforschung, Max Planck Society;

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

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Spliethoff,  Bernd
Service Department Tesche (EM), Max-Planck-Institut für Kohlenforschung, Max Planck Society;

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Tesche,  Bernd
Service Department Tesche (EM), Max-Planck-Institut für Kohlenforschung, Max Planck Society;

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

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Leitner,  Walter
Service Department Leitner (Technical Labs), Max-Planck-Institut für Kohlenforschung, Max Planck Society;
Institut für Technische und Makromolekulare Chemie, Lehrstuhl für Technische Chemie und Petrolchemie, RWTH Aachen;

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Citation

Hou, Z., Theyssen, N., Brinkmann, A., Klementiev, K. V., Grünert, W., Bühl, M., et al. (2008). Supported palladium nanoparticles on hybrid mesoporous silica: Structure/activity-relationship in the aerobic alcohol oxidation using supercritical carbon dioxide. Journal of Catalysis, 258(2), 315-323. doi:10.1016/j.jcat.2008.07.002.


Cite as: http://hdl.handle.net/11858/00-001M-0000-000F-9027-2
Abstract
The preparation, characterization, and catalytic properties of Pd nanoparticles supported on mesoporous organic–inorganic hybrid materials are described for continuous-flow aerobic oxidation of alcohols using supercritical carbon dioxide (scCO2) as a mobile phase. The nanoparticles were generated “bottom-up” from molecular precursors that were precoordinated to the support through suitable anchor units. The most active material allows high single-pass conversions in scCO2 at temperatures as low as 60 °C. This high activity may be associated with the presence of small primary crystallites (approx. 2 nm) that conglomerate to ensembles about 25 nm in size, leading to a larger number of high-indexed planes in small volume units. These findings may provide useful guidelines for further catalyst design on the nanoscale for green oxidation methods.