TECHNICAL REPORTS
822
Adsorption of antibiotics on the surfaces of common mineral
sorbents plays a major role in determining their fate in soils and
sediments. he mechanisms of these reactions are, therefore,
important for understanding and predicting the environmental
fate of antibiotics. We used in situ attenuated total relectance
Fourier-transform infrared spectroscopy to elucidate the binding
mechanisms of oxytetracycline (OTC) onto the surface of magnetite
[Fe
3
O
4(s)
], a common Fe oxide mineral in soils and sediments, as
a function of pH (3–9) and aqueous OTC concentration (5–
150 μmol L
-1
). Comparison of dissolved OTC spectra to those of
OTC–magnetite surface complexes indicated strong interactions
of OTC molecules with the Fe
3
O
4(s)
surface via carbonyl (C=O)
and amine (–NH
2
) moieties of the amide group (–CONH
2
) and
the N atom of the dimethyl amino group [–N(CH
3
)
2
]. Increasing
the aqueous OTC concentration led to increased OTC adsorption
but did not notably alter the OTC binding mode at the magnetite
surface. he results of this study would help to assess the importance
of Fe oxide minerals in determining the environmental fate of OTC
in soils and sediments.
In Situ Attenuated Total Relectance Fourier-Transform Infrared Study of
Oxytetracycline Sorption on Magnetite
Sudipta Rakshit, Evert J. Elzinga, Rupali Datta, and Dibyendu Sarkar*
O
xytetracycline, which belongs to the tetracy-
cline (TC) group of antibiotics, is widely used in live-
stock production as a therapeutic agent and growth
promoter (Arikan et al., 2007; Kümmerer, 2009a, 2009b). Due
to low absorption in the animal gut, a large portion of antibi-
otics is excreted through feces and urine (Kumar et al., 2005).
Application of untreated animal manure onto agricultural land
is one of the most common pathways of entry for antibiotics into
the environment (Kong et al., 2012). Reported adverse efects of
OTC include growth of antibiotic-resistant microbial strains,
inhibition of microbial soil respiration, Fe(III) reduction, and
nitriication (Halling-Sørensen, 2001; Boleas et al., 2005; hiele-
Bruhn and Beck, 2005; Aristilde et al., 2010; Knapp et al., 2010).
Adsorption of antibiotics on minerals in soils has been found
to decrease their adverse environmental efects (Chander et al.,
2005). A thorough knowledge of the eiciency and mechanisms
of antibiotic retention on clay and oxide minerals is required
to provide guidance on risk assessment criteria in soils and
sediments (Aristilde et al., 2010). Hence, many studies have
been performed to investigate the adsorption of antibiotics
onto common clay and oxide minerals (Kulshrestha et al., 2004;
Figueroa and MacKay, 2005; Gu and Karthikeyan, 2005; Trivedi
and Vasudevan, 2007; Aristilde et al., 2010; Rakshit et al., 2010;
Zhao et al., 2012). Macroscopic sorption studies have shown that
Fe oxides such as goethite, hematite, and magnetite have a high
ainity for OTC, exhibiting strongly pH-dependent sorption
behavior (Figueroa and MacKay, 2005; Rakshit et al., 2010). For
OTC adsorption on goethite and hematite, maximum adsorption
occurs around pH 8, consistent with the mineral surface charge
(i.e., goethite and hematite point of zero net proton charge is
close to 8) and OTC speciation (-log acid dissociation constant
pK
a
values 3.57, 7.49, and 9.44), and adsorption decreases at
both lower and higher pH values, resulting in a bell-shaped
pH envelope (Figueroa and MacKay, 2005). For magnetite,
OTC adsorption is highest (approximately 90%) at low pH
values and decreases with increasing pH >5.5 to 60% (at pH
9.4) (Supplemental Fig. S1). Macroscopic adsorption trends of
OTC onto goethite and hematite surfaces have been described
using surface complexation models (Figueroa and MacKay,
2005); however, studies providing direct characterization of
Abbreviations: ATR, attenuated total relectance; FTIR, Fourier-transform infrared;
IR, infrared; OTC, oxytetracycline.
S. Rakshit and D. Sarkar, Earth and Environmental Studies Dep., Montclair State
Univ., Montclair, NJ 07043; E.J. Elzinga, Dep. of Earth and Environmental Sciences,
Rutgers Univ., Newark, NJ 07102; and R. Datta, Dep. of Biological Sciences,
Michigan Technological Univ., 1400 Townsend Drive, Houghton, MI 49931.
Copyright © American Society of Agronomy, Crop Science Society of America,
and Soil Science Society of America. 5585 Guilford Rd., Madison, WI 53711 USA.
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writing from the publisher.
J. Environ. Qual. 42:822–827 (2013)
doi:10.2134/jeq2012.0412
Supplemental data ile is available online for this article.
Received 25 Oct. 2012.
*Corresponding author (sarkard@mail.montclair.edu).
Journal of Environmental Quality
ORGANIC COMPOUNDS IN THE ENVIRONMENT
TECHNICAL REPORTS