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Platinum Group Metal-Doped Tungsten Phosphates for Selective C-H Activation of Lower Alkanes

MPG-Autoren
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Dimitrakopoulou,  Maria
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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

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Skorupska,  Katarzyna
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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Tarasov,  Andrey
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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Zitation

Machado, R., Dimitrakopoulou, M., Girgsdies, F., Löser, P., Xie, J., Wittich, K., et al. (2022). Platinum Group Metal-Doped Tungsten Phosphates for Selective C-H Activation of Lower Alkanes. ACS Catalysis, 12, 13116-13130. doi:10.1021/acscatal.2c02645.


Zitierlink: https://hdl.handle.net/21.11116/0000-000B-4801-3
Zusammenfassung
Platinum group metal (PGM)-based catalysts are known to be highly active in the total combustion of lower hydrocarbons. However, through an alternative catalyst design reported in this paper by isolating PGM-based active sites in a tungsten phosphate matrix, we present a class of catalysts for selective oxidation of n-butane, propane, and propylene that do not contain Mo or V as redox-active elements. Two different catalyst concepts have been pursued. Concept A: isolating Ru-based active sites in a tungsten phosphate matrix coming upon as ReO3-type structure. Concept B: dilution of PGM-based active sites through the synthesis of X-ray amorphous Ru tungsten phosphates supported on SiO2. Using a high-throughput screening approach, model catalysts over a wide compositional range were evaluated for C3 and C4 partial oxidation. Bulk crystalline and supported XRD amorphous phases with similar Ru/W/P compositions showed comparable performance. Hence, for these materials, composition is more crucial than the degree of crystallinity. Further studies for optimization on second-generation supported systems revealed even better results. High selectivity for n-butane oxidation to maleic anhydride and propane oxidation to an acrolein/acrylic acid has been achieved.