De. Giblin et al., INCORPORATION OF HELIUM INTO ENDOHEDRAL COMPLEXES OF C-60 AND C-70 CONTAINING NOBLE-GAS ATOMS - A TANDEM MASS-SPECTROMETRY STUDY, Journal of the American Chemical Society, 119(41), 1997, pp. 9883-9890
Endohedral complexes of fullerenes and noble-gas atoms were originally
prepared by a mass spectrometric method involving high-energy collisi
ons of fullerene ions and noble-gas targets and, following that, by a
high-pressure, high-temperature method involving neutral fullerenes an
d a noble gas as reactants. The latter method has made available suffi
cient quantities of the endohedral complexes of C-60 and C-70 with the
various noble gases (He, Ne, Ar, and Kr) that the tandem mass spectro
metric method can be used to test the possibility of preparing a new c
lass of endohedral complexes that contain two noble-gas atoms. These n
ew capture complexes do indeed form upon activation of the radical cat
ion of the noble-gas endohedral complex by high-energy collisions with
helium atoms. These complexes then decompose to give equivalent paral
lel losses of C-2 units accompanied by expulsion of none, one, or both
of the captured noble-gas atoms. The capture event causes the gain in
excess of 34 eV of additional internal energy, but the capture comple
xes survive on the time scale (similar to 50 mu s) for the transit thr
ough the tandem mass spectrometer. Their survival, along with their fr
agmentation characteristics, is consistent with formation of an endohe
dral complex containing both noble-gas atoms although the fullerene ca
ge may now be distorted especially when the fullerene is C-60. By anal
ogy with the properties of empty fullerene and endohedral metallofulle
rene complexes, end points exist for the equivalent number of C-2 unit
s that can be expelled to give a closed-structure product that contain
s either one or two noble-gas atoms. These end points correlate direct
ly with the sizes of the fullerene and the noble-gas atom(s), giving s
upport to our conclusion that endohedral complexes containing two nobl
e gases can be prepared.