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Experimental and Theoretical Investigation of Molybdenum Carbide and Nitride as Catalysts for Ammonia Decomposition

MPG-Autoren
http://pubman.mpdl.mpg.de/cone/persons/resource/persons22301

Zheng,  Weiqing
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

http://pubman.mpdl.mpg.de/cone/persons/resource/persons21440

Cotter,  Thomas Patric
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

http://pubman.mpdl.mpg.de/cone/persons/resource/persons21689

Kaghazchi,  Payam
Theory, Fritz Haber Institute, Max Planck Society;

http://pubman.mpdl.mpg.de/cone/persons/resource/persons27705

Jacob,  Timo
Theory, Fritz Haber Institute, Max Planck Society;

http://pubman.mpdl.mpg.de/cone/persons/resource/persons21519

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

http://pubman.mpdl.mpg.de/cone/persons/resource/persons58964

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

http://pubman.mpdl.mpg.de/cone/persons/resource/persons22294

Zhang,  Wei
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;
Shenyang National Laboratory for Materials Science Institute of Metal Research, Chinese Academy of Science;

http://pubman.mpdl.mpg.de/cone/persons/resource/persons22148

Su,  Dang Sheng
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;
Shenyang National Laboratory for Materials Science Institute of Metal Research, Chinese Academy of Science;

http://pubman.mpdl.mpg.de/cone/persons/resource/persons58985

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

http://pubman.mpdl.mpg.de/cone/persons/resource/persons22071

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

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Zitation

Zheng, W., Cotter, T. P., Kaghazchi, P., Jacob, T., Frank, B., Schlichte, K., et al. (2013). Experimental and Theoretical Investigation of Molybdenum Carbide and Nitride as Catalysts for Ammonia Decomposition. Journal of the American Chemical Society, 135(9), 3458-3464. doi:10.1021/ja309734u.


Zitierlink: http://hdl.handle.net/11858/00-001M-0000-000F-F0CE-3
Zusammenfassung
Constant COx-free H2 production from the catalytic decomposition of ammonia could be achieved over a high surface area molybdenum carbide catalyst prepared by a temperature programmed reduction-carburization method. The fresh and used catalyst was characterized by N2-adsorption/desorption, powder X-ray diffraction, scanning and transmission electron microscopes and electron energy-loss spectroscopy at different stages. Observed deactivation (in the first 15 hours) of the high surface area carbide during reaction was ascribed to considerable reduction of the specific surface area due to nitridation of the carbide under reaction condition. Theoretical calculations confirm that the N atoms tend to occupy subsurface sites, leading to the formation of nitride under NH3 atmosphere. The relatively high rate of reaction (30 mmol/gcat.min) observed for the catalytic decomposition of NH3 is ascribed to highly energetic sites (twin-boundaries, stacking faults, steps and defects) which are observed in both the molybdenum carbide and nitride samples. The prevalence of such sites in the as-synthesised material results in a much higher H2 production rate in comparison with previously reported Mo-based catalysts.