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

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.

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 Creators:
Zheng, Weiqing1, Author           
Cotter, Thomas Patric1, Author           
Kaghazchi, Payam2, Author           
Jacob, Timo2, Author           
Frank, Benjamin1, Author           
Schlichte, Klaus3, Author
Zhang, Wei1, 4, Author           
Su, Dang Sheng1, 4, Author           
Schüth, Ferdi3, Author
Schlögl, Robert1, Author           
Affiliations:
1Inorganic Chemistry, Fritz Haber Institute, Max Planck Society, ou_24023              
2Theory, Fritz Haber Institute, Max Planck Society, ou_634547              
3Research Department Schüth, Max-Planck-Institut für Kohlenforschung, Max Planck Society, ou_1445589              
4Shenyang National Laboratory for Materials Science Institute of Metal Research, Chinese Academy of Science, ou_persistent22              

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 Abstract: 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.

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Language(s): eng - English
 Dates: 2012-10-022013-01-272013-03-06
 Publication Status: Published in print
 Pages: -
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1021/ja309734u
 Degree: -

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Title: Journal of the American Chemical Society
  Other : J. Am. Chem. Soc.
Source Genre: Journal
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Publ. Info: American Chemical Society
Pages: 7 Volume / Issue: 135 (9) Sequence Number: - Start / End Page: 3458 - 3464 Identifier: ISSN: 0002-7863
CoNE: https://pure.mpg.de/cone/journals/resource/954925376870