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Journal Article

Hydrothermal synthesis of bi-functional nanostructured manganese tungstate catalysts for selective oxidation

MPS-Authors
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Li,  Xuan
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;
UniCat-BASF Joint Lab, Technische Universität Berlin;

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Lunkenbein,  Thomas
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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Kröhnert,  Jutta
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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Pfeifer,  Verena
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;
Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, Elektronenspeicherring BESSY II;

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Girgsdies,  Frank
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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

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Trunschke,  Annette
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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Fulltext (public)

c5fd00191a.pdf
(Publisher version), 2MB

Supplementary Material (public)

SI_Faraday151123_final.pdf
(Supplementary material), 2MB

Citation

Li, X., Lunkenbein, T., Kröhnert, J., Pfeifer, V., Girgsdies, F., Rosowski, F., et al. (2016). Hydrothermal synthesis of bi-functional nanostructured manganese tungstate catalysts for selective oxidation. Faraday Discussions, 188, 99-113. doi:10.1039/C5FD00191A.


Cite as: http://hdl.handle.net/11858/00-001M-0000-0029-31A4-8
Abstract
The mechanism of C-H activation in selective oxidation reactions of short-chain alkane molecules over transition metal oxides is critically affected by the balance of acid-base and redox sites at the surface of the catalyst. Using the example of manganese tungstate we discuss how the relative abundance of these sites can be controlled via synthetic techniques. Phase-pure catalysts composed of the thermodynamic stable monoclinic MnWO4 phase have been prepared by hydrothermal synthesis. Variation of the initial pH value resulted in rod-shaped nano-crystalline MnWO4 catalysts composed of particles with varying aspect ratio. The synthesis products have been analysed by transmission elecron microscopy, X-ray diffraction, infrared, and photoelectron spectroscopy. In-situ Raman spectroscopy was used to investigate the dissolution-re-crystallization processes occuring under hydrothermal conditions. Ethanol oxidation was applied to probe the surface functionalities in terms of acid-base and redox properties. Changes in the aspect ratio of the primary catalyst particles are reflected in the product distribution induced by altering the fraction of acid-base and redox sites exposed at the surface of the catalysts in agreement with the proposed mechanism of particle growth by re-crystallization during ageing under hydrothermal conditions.