RESEARCH ARTICLE Open Access
Free radicals produced by the oxidation of gallic
acid: An electron paramagnetic resonance study
Angelique C Eslami
1
, Wanvimol Pasanphan
2
, Brett A Wagner
1
, Garry R Buettner
1*
Abstract
Background: Gallic acid (3,4,5-trihydroxybenzoic acid) is found in a wide variety of plants; it is extensively used in
tanning, ink dyes, as well as in the manufacturing of paper. The gallate moiety is a key component of many
functional phytochemicals. In this work electron paramagnetic spectroscopy (EPR) was used to detect the free
radicals generated by the air-oxidation of gallic acid.
Results: We found that gallic acid produces two different radicals as a function of pH. In the pH range between
7-10, the spectrum of the gallate free radical is a doublet of triplets (a
H
= 1.00 G, a
H
= 0.23 G, a
H
= 0.28 G). This is
consistent with three hydrogens providing hyperfine splitting. However, in a more alkaline environment, pH >10,
the hyperfine splitting pattern transforms into a 1:2:1 pattern (a
H
(2) = 1.07 G). Using D
2
O as a solvent, we
demonstrate that the third hydrogen (i.e.a
H
= 0.28 G) at lower pH is a slowly exchanging hydron, participating in
hydrogen bonding with two oxygens in ortho position on the gallate ring. The pK
a
of this proton has been
determined to be 10.
Conclusions: This simple and novel approach permitted the understanding of the prototropic equilibrium of the
semiquinone radicals generated by gallic acid, a ubiquitous compound, allowing new insights into its oxidation
and subsequent reactions.
Background
Gallic acid (3,4,5-trihydroxybenzoic acid), found in a
variety of plants, is extensively used in tanning, ink dyes,
as well as in the manufacturing of paper [1]. In addition,
the gallate moiety is a key component of many foods
and drinks, e.g. there are two gallate moieties in the
important polyphenol, (-)- epi- gallocatechin-3-gallate
(EGCG); this and related polyphenols are responsible for
the antioxidant, anticarcinogenic, and antiviral proper-
ties of some of the most widely consumed beverages in
the world, such as green tea [2,3]. The three aromatic
phenoxyl groups of gallic acid are prone to oxidation
with the formation of hydrogen peroxide, quinones, and
semiquinones [4]. We have observed the formation of
two distinct semiquinones formed upon the oxidation
of gallic acid. Here we have investigated the nature of
these two different radicals.
Experimental
Gallic acid (3,4,5-trihydroxybenzoic acid, CAS No.: 149-
91-7) was obtained from Sigma, USA; sodium hydroxide
was from Fisher. All experiments were carried out in
100 mM potassium phosphate. The final concentration
of gallic acid was 1 mM, unless noted otherwise. All
solutions above neutral pH (alkaline solutions) were pre-
pared by adjusting with 1 M sodium hydroxide solution.
EPR spectroscopy was done using a Bruker EMX spec-
trometer equipped with a high-sensitivity cavity and an
Aqua-X sample holder. Spectra were obtained at room
temperature (24-27°C). Typical EPR parameters were as
follows: 3510 G center field; 10 G sweep width; 9.852
GHz microwave frequency; 20 mW power; receiver gain
varied as needed; modulation frequency of 100 kHz;
modulation amplitude of 0.10 G; conversion time of
40.96 ms; and time constant of 20.48 ms with 20
X-scans for each 1024 point spectrum. Spectral simula-
tions of EPR spectra were performed using the WinSim
program developed at the NIEHS by Duling [5].
In the experiments to determine the second pK
a
of the
gallate free radical 5.0 mL of 10 mM gallic acid (final
* Correspondence: garry-buettner@uiowa.edu
1
Free Radical and Radiation Biology, Med Labs B180, The University of Iowa,
Iowa City, IA 52242-1181, USA
Full list of author information is available at the end of the article
Eslami et al. Chemistry Central Journal 2010, 4:15
http://journal.chemistrycentral.com/content/4/1/15
© 2010 Eslami et al