Development and optimization of the BDD-electrochemical oxidation of the
antibiotic trimethoprim in aqueous solution
Teresa González
a
, Joaquín R. Domínguez
a,
⁎, Patricia Palo
a
,
Jesús Sánchez-Martín
a
, Eduardo M. Cuerda-Correa
b
a
Department of Chemical Engineering and Physical Chemistry, Area of Chemical Engineering, Faculty of Sciences, University of Extremadura, Avda. de Elvas, s/n, E-06006 Badajoz, Spain
b
Department of Organic and Inorganic Chemistry, Faculty of Sciences, University of Extremadura, Avda. de Elvas, s/n, E-06071 Badajoz, Spain
abstract article info
Article history:
Received 16 September 2010
Received in revised form 2 June 2011
Accepted 3 July 2011
Available online 3 September 2011
Keywords:
Electrochemical advanced oxidation
processes
Electro-oxidation
Anodic oxidation
Boron-doped diamond electrodes
Pharmaceuticals
Trimethoprim
The occurrence of antibiotics in the aquatic environment has led to an increasing concern about the potential
environmental risks and the maintenance and spread of antibacterial resistance among microorganisms.
Electrochemical oxidation processes are promising technologies to treat low contents of toxic and
biorefractory pollutants in water. Anodic oxidation of Trimethoprim, the most frequently detected antibiotic
in surface waters, was carried out using boron-doped diamond electrodes at galvanostatic mode. A statistical
design of experiments has been used to study the influence of the different operating variables: pH (in the
range 3–11), current intensity (from 0 to 320 mA cm
-2
), supporting electrolyte concentration Na
2
SO
4
in the
range 0–0.5 mol L
-1
, and solution flow rate between 1.25 and 10.80 cm
3
min
-1
. Response Surface
Methodology technique was used to optimize Trimethoprim degradation. Current intensity resulted to be
the main variable influencing Trimethoprim degradation, followed by salt concentration and pH. ANOVA test
reported significance for five of the fourteen involved variables. An optimum Trimethoprim degradation of
100% was found at pH 3, under a flow rate equal to 1.25 cm
3
min
-1
, and with a current density equal to
207 mA cm
-2
, using a supporting electrolyte concentration equal to 0.49 mol L
-1
.
© 2011 Elsevier B.V. All rights reserved.
1. Introduction
Considering the wide variety and different applications of
antibiotics and the ever increasing tendency to use them, it is no
surprise that these drugs are among the most ubiquitous environ-
mental contaminants [1,2]. The occurrence of antibiotics in the
aquatic environment has led to an increasing concern about the
potential environmental risks as well as about the maintenance and
spread of antibacterial resistance among microorganisms. Develop-
ment of antibiotic resistance of bacteria was demonstrated in surface
and groundwater affected by the sewage treatment plant effluent [3].
Whether antibiotics transported in the environment from human and
livestock sources lead to increased antibiotic resistant bacteria or have
deleterious effects on water quality is an important but largely
unresolved issue. The use of antibiotics may also accelerate the
development of antibiotic resistance genes and bacteria, which shade
health risks to humans and animals [4].
The main source of antibiotics in the environment is the excretion
of incompletely metabolized drugs by humans and animals. Other
sources may include the disposal of unused antibiotics and waste
from pharmaceutical manufacturing processes [5]. Residential care
facilities and hospitals are known contributors of antibiotics to
municipal wastewater [6]. Other contributors to surface and
groundwater are effluent from wastewater treatment plants [6]
and industrial facilities (including pharmaceutical plants), and
surface run-off from concentrated animal feeding operations [1].
Recently, scientists have raised concerns about pharmaceutical
residues detected in surface waters and wastewaters and their
potential to cause adverse effects in humans and aquatic species
[7,8]. Wastewater typically contains a number of medications and
antibiotics that people have either used or discarded. Many of these
chemical compounds remain biologically active and some of them,
especially antibiotics, stimulate the development of antibiotic
resistant bacteria.
Recent studies have confirmed the presence of low levels of
pharmaceuticals in estuaries, rivers, streams, and ground water as
well as in sediments [9,10]. The ecological effects of these contaminants
in coastal waters are largely unknown. However, there is growing
evidence that some of these chemicals may have negative effects on
reproduction in aquatic species.
Trimethoprim (TMP) [2,4-diamino-5-(3′,4′,5′-trimethoxybenzyl-
pyrimidine)] (molecular formula C
14
H
18
N
4
O
3
, molecular weight
290.32, CAS Number 738-70-5, pKa = 7.2) is a very good antifolate
drug. It selectively inhibits the bacterial form of the dihydrofolate
reductase enzyme [11,12]. TMP is among the most important
synthetic antibiotics used worldwide in human and veterinary
Desalination 280 (2011) 197–202
⁎ Corresponding author. Tel.: + 34 924289300x86888; fax: + 34 924289385.
E-mail address: jrdoming@unex.es (J.R. Domínguez).
0011-9164/$ – see front matter © 2011 Elsevier B.V. All rights reserved.
doi:10.1016/j.desal.2011.07.012
Contents lists available at ScienceDirect
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