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  In Situ Observations of Phase Transitions in Metastable Nickel (Carbide)/Carbon Nanocomposites

Bayer, B. C., Bosworth, D. A., Michaelis, F. B., Blume, R., Habler, G., Abart, R., et al. (2016). In Situ Observations of Phase Transitions in Metastable Nickel (Carbide)/Carbon Nanocomposites. The Journal of Physical Chemistry C, 120(39), 22571-22584. doi:10.1021/acs.jpcc.6b01555.

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Bayer et al - in-situ Ni-C nanocomposites_SI.pdf (Supplementary material), 168KB
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 Creators:
Bayer, Bernhard C.1, 2, Author
Bosworth, David A.3, Author
Michaelis, F. Benjamin1, Author
Blume, Raoul4, Author
Habler, Gerlinde5, Author
Abart, Rainer5, Author
Weatherup, Robert S.1, Author
Kidambi, Piran R.1, Author
Baumberg, Jeremy J.6, Author
Knop-Gericke, Axel7, Author           
Schlögl, Robert7, Author           
Baehtz, Carsten8, Author
Barber, Zoe H.3, Author
Meyer, Jannik C.2, Author
Hofmann, Stephan1, Author
Affiliations:
1Department of Engineering, University of Cambridge, Cambridge, UK, ou_persistent22              
2Faculty of Physics, University of Vienna, Vienna, Austria, ou_persistent22              
3Department of Materials Science and Metallurgy, University of Cambridge , Cambridge, UK, ou_persistent22              
4Helmholtz-Zentrum Berlin für Materialien und Energie, Berlin, Germany, ou_persistent22              
5Department of Lithospheric Research, University of Vienna, Althanstrasse 14, Vienna, Austria, ou_persistent22              
6Cavendish Laboratory, University of Cambridge, Cambridge, U.K, ou_persistent22              
7Inorganic Chemistry, Fritz Haber Institute, Max Planck Society, ou_24023              
8Institue of Radiation Physics, Helmholtz-Zentrum Dresden-Rossendorf, Dresden, German, ou_persistent22              

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 Abstract: Nanocomposite thin films comprised of metastable metal-carbides in a carbon matrix have a wide variety of applications ranging from hard coatings to magnetics and energy storage and conversion. While their deposition using non-equilibrium techniques is established, the understanding of the dynamic evolution of such metastable nanocomposites under thermal equilibrium conditions at elevated temperatures during processing and during device operation remains limited. Here, we investigate sputter deposited nanocomposites of metastable Ni carbide (Ni3C) nanocrystals in an amorphous carbon (a-C) matrix during thermal post-deposition processing via complementary in-situ X-ray diffractometry, in-situ Raman spectroscopy and in-situ X-ray photoelectron spectroscopy. At low annealing temperatures (300 °C) we observe isothermal Ni3C decomposition into face-centered-cubic Ni and amorphous carbon, however, without changes to the initial finely structured nanocomposite morphology. Only for higher temperatures (400-800 °C) Ni-catalyzed isothermal graphitization of the amorphous carbon matrix sets in, which we link to bulk-diffusion-mediated phase separation of the nanocomposite into coarser Ni and graphite grains. Upon natural cooling, only minimal precipitation of additional carbon from the Ni is observed, showing that even for highly carbon saturated systems precipitation upon cooling can be kinetically quenched. Our findings demonstrate that phase transformations of the filler and morphology modifications of the nanocomposite can be decoupled which is advantageous from a manufacturing perspective. Our in-situ study also identifies the high carbon content of the Ni filler crystallites at all stages of processing as the key hallmark feature of such metal-carbon nanocomposites that governs their entire thermal evolution. In a wider context, we also discuss our findings with regard to the much debated potential role of metastable Ni3C as a catalyst phase in graphene and carbon nanotube growth.

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 Dates: 2016-02-152016-09-022016-10-06
 Publication Status: Issued
 Pages: 36
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1021/acs.jpcc.6b01555
 Degree: -

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Title: The Journal of Physical Chemistry C
  Abbreviation : J. Phys. Chem. C
Source Genre: Journal
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Publ. Info: Washington DC : American Chemical Society
Pages: 14 Volume / Issue: 120 (39) Sequence Number: - Start / End Page: 22571 - 22584 Identifier: ISSN: 1932-7447
CoNE: https://pure.mpg.de/cone/journals/resource/954926947766