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

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

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

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

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

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

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

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

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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;

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

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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: https://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.