DOI: 10.1007/s10967-007-0919-1 Journal of Radioanalytical and Nuclear Chemistry, Vol. 273, No.3 (2007) 609–614
0236–5731/USD 20.00 Akadémiai Kiadó, Budapest
© 2007 Akadémiai Kiadó, Budapest Springer, Dordrecht
ESR study of ascorbic acid irradiated with gamma-rays
H. Tuner,* M. Korkmaz
Hacettepe University, Department of Physics Engineering, Beytepe, 06800 Ankara, Turkey
(Received June 27, 2006)
The interest in application of high-energy ionizing radiation for sterilization of pharmaceutical products and foodstuffs has led a number of workers
to investigate the radiation sensitivity of vitamins. Aside from its use as a vitamin, ascorbic acid (AA) or some derivatives are employed as
antioxidants in foodstuffs. The effects of ionizing radiation on AA in simple solutions and in mixture of naturally occurring compounds have been
extensively reported in the literature. However, the effects of ionizing radiation on solid AA were reported in few works which described rather
dosimetric features of AA. No reports, except one, are available describing the characteristic features of the radiolytic intermediates produced after
irradiation of polycrystalline AA. Irradiation studies performed on single crystal of AA has led us to reinvestigate our previous work on the
radiolytic intermediates produced in irradiated polycrystalline AA. Three radical species, rather than two, having different characteristics were
decided contributing to the formation of experimental electron spin resonance (ESR) spectrum of γ-irradiated polycrystalline AA. Spectral
parameters of these species were calculated after exhaustive spectrum simulation calculations based on data derived from experimental microwave
saturation and dose-response studies.
Introduction
Ascorbic acid (AA) is a water-soluble vitamin and
most important free oxygen scavenger. AA is stable
when dry, but in solution it is readily oxidized to
dehydroascorbic acid (DHAA),
1
especially in the
presence of trace amounts of copper, iron and alkali. Its
molecular structure is given in Fig. 1. AA or some
derivatives are employed as antioxidants and radiation
protector in foodstuffs, to prevent rancidity, browning of
cut apples and other fruits and in meat curing.
2
AA is
noted for its complex multi-functional effects.
Depending on medium conditions, AA can act as an
antioxidant, pro-oxidant, metal cheaters, a reducing
agent or an oxygen scavenger. Radiosensitivity and
stability of AA in different in vitro systems and in
different matrices were the subject of different research
works using ESR spectroscopy and other methods.
3–9
Radiation damage produced in irradiated solid AA were
also reported in the literature using ESR spectroscopy,
but those investigations which considered only the
variations of the intensities of the resonance line of
doublet appearance, were rather oriented toward the
determination of AA dosimetric properties.
10,11
Spectroscopic parameters of the radicalic species
produced upon irradiation were not reported in none of
these works except the ESR work carried out in our
laboratory. Spectrum simulation calculations based on
the presence of two different radical species and on
signal intensity data derived from a room temperature
spectrum were performed in this work. However, our
later studies on irradiated single crystals of AA revealed
that ESR spectra of crystalline samples consist, in
general, more than nine resonance lines of different
* E-mail: htuner@hacettepe.edu.tr
intensities except some specific orientations. Hence, it
was concluded that such a spectrum cannot be explain
along with radical species with unpaired electrons
localized on carbon and oxygen atoms of five member
rings as advised in Reference 10. Therefore, it was
decided that species produced after the damage of the –
CHOHCH
2
OH molecular part of AA should also take
part in the formation of experimental ESR spectra of
irradiated solid AA. Consequently, in the present work,
simulation calculations performed in our previous work
were repeated adopting a model consisting of the
presence of three different radical species using, as
input, the data derived from experimental microwave
and dose-response studies carried out for irradiated
polycrystalline AA.
Experimental
AA fine powder was supplied by Vankim Ltd.
(Istanbul, Turkey). The AA samples, in polycarbonate
vials, were irradiated in the dose range 0.5–25 kGy. All
irradiations were performed at room temperature using a
60
Co ionizing radiation source at the Sarayköy
Establishment of the Turkish Atomic Energy Agency in
Ankara. The dose rate (1.6 kGy/h) was previously
calibrated using Fricke dosimetry.
The ESR spectra were recorded at room temperature
using a Bruker EMX 131 X-band spectrometer equipped
with a cylindrical cavity. Numbers were assigned to the
observed resonance peaks and intensity measurements
were performed with respect to the spectrum base line.
An unirradiated sample was kept as a reference.