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Synthesis and properties of open fullerenes encapsulating ammonia and methane

Bloodworth, Sally; Gräsvik, John; Alom, Shamim; Kouril,, Karel; Elliott, Stuart J.; Wells, Neil J.; Horsewill, Anthony J.; Mamone, Salvatore; Jimenez-Ruiz, Monica; Rols, Stéphane; Nagel, Urmas; Room, Toomas; Levitt, Malcolm H.; Whitby, Richard J.

Authors

Sally Bloodworth

John Gräsvik

Shamim Alom

Karel Kouril,

Stuart J. Elliott

Neil J. Wells

Anthony J. Horsewill a.horsewill@nottingham.ac.uk

Salvatore Mamone

Monica Jimenez-Ruiz

Stéphane Rols

Urmas Nagel

Toomas Room

Malcolm H. Levitt mhl@soton.ac.uk

Richard J. Whitby rjw1@soton.ac.uk



Abstract

We describe the synthesis and characterisation of open fullerene (1) and its reduced form (2) in which CH₄ and NH₃ are encapsulated, respectively. The ¹H NMR resonance of endohedral NH₃ is broadened by scalar coupling to the quadrupolar ¹⁴N nucleus, which relaxes rapidly. This broadening is absent for small satellite peaks, which are attributed to natural abundance ¹⁵N. The influence of the scalar relaxation mechanism on the linewidth of the ¹H ammonia resonance is probed by variable temperature NMR. A rotational correlation time of τc= 1.5 ps. is determined for endohedral NH₃, and of τc=57±5 ps. for the open fullerene, indicating free rotation of the encapsulated molecule. IR spectroscopy of NH3@2 at 5 K identifies three vibrations of NH₃ (ν₁, ν₃ and ν₄) redshifted in comparison with free NH₃, and temperature dependence of the IR peak intensity indicates the presence of a large number of excited translational/ rotational states. Variable temperature ¹H NMR spectra indicate that endohedral CH4 is also able to rotate freely at 223 K, on the NMR timescale. Inelastic neutron scattering (INS) spectra of CH₄@1 show both rotational and translational modes of CH₄. Energy of the first excited rotational state (J=1) of CH₄@1 is significantly lower than that of free CH₄.

Journal Article Type Article
Publication Date Feb 5, 2018
Journal ChemPhysChem
Print ISSN 1439-4235
Electronic ISSN 1439-7641
Publisher Wiley
Peer Reviewed Peer Reviewed
Volume 19
Issue 3
APA6 Citation Bloodworth, S., Gräsvik, J., Alom, S., Kouril,, K., Elliott, S. J., Wells, N. J., …Whitby, R. J. (2018). Synthesis and properties of open fullerenes encapsulating ammonia and methane. ChemPhysChem, 19(3), https://doi.org/10.1002/cphc.201701212
DOI https://doi.org/10.1002/cphc.201701212
Keywords endofullerenes; inelastic neutron scattering spectroscopy; infra-red spectroscopy; NMR spectroscopy; SpinDynamica
Publisher URL http://onlinelibrary.wiley.com/doi/10.1002/cphc.201701212/full
Copyright Statement Copyright information regarding this work can be found at the following address: http://creativecommons.org/licenses/by/4.0

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Copyright Statement
Copyright information regarding this work can be found at the following address: http://creativecommons.org/licenses/by/4.0





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