Original research article
Synergism between anodic oxidation with diamond anodes and
heterogeneous catalytic photolysis for the treatment of
pharmaceutical pollutants
Juan M. Peralta-Hern
andez
a, *
, Catalina de la Rosa-Ju
arez
b
, Vianey Buzo-Mu
~
noz
b
,
Javier Paramo-Vargas
b
, Pablo Ca
~
nizares-Ca
~
nizares
c
, Manuel A. Rodrigo-Rodrigo
c
a
Department of Chemistry, University of Guanajuato, Guanajuato 36040, Mexico
b
Department of Research and Graduate Studies, Center for Applied Innovation in Competitive Technologies, Le on 37545, Mexico
c
Department of Chemical Engineering, University of Castilla-La Mancha, Ciudad Real 13071, Spain
article info
Article history:
Received 27 February 2015
Received in revised form
10 September 2015
Accepted 5 November 2015
Available online 12 April 2016
Keywords:
Anodic oxidation
Heterogeneous catalytic photolysis
Diclofenac
Acetaminophen
Boron-doped diamond
Titanium dioxide
abstract
The mineralization of diclofenac and acetaminophen has been studied by single anodic oxidation with
boron-doped diamond (AO-BDD) using an undivided electrolysis cell, by single heterogeneous catalytic
photolysis with titanium dioxide (HCP-TiO
2
) and by the combination of both advanced oxidation pro-
cesses. The results show that mineralization can be obtained with either single technology. The type of
functional groups of the pollutant does not influence the results of the single AO-BDD process, but it has
a significant influence on the results obtained with HCP-TiO
2
. A clear synergistic effect appears when
both processes are combined showing improvements in the oxidation rate of more than 50% for diclo-
fenac and nearly 200% for acetaminophen at the highest current exerted. Results obtained are explained
in terms of the production of oxidants on the surface of BDD (primarily peroxodisulfate) and the later
homogeneous catalytic light decomposition of these oxidants in the bulk. This mechanism is consistent
with the larger improvement observed at higher current densities, for which the production of oxidants
is promoted.
© 2016 Chinese Institute of Environmental Engineering, Taiwan. Production and hosting by
Elsevier B.V. This is an open access article under the CC BY-NC-ND license (http://
creativecommons.org/licenses/by-nc-nd/4.0/).
1. Introduction
In recent years, a large number of research groups around the
world have conducted investigations on the detection and removal
of pharmaceutical compounds, such as analgesics, anti-
inflammatories, anti-microbials, antiepileptics, beta-blockers, es-
trogens and lipid regulators, typically found as emerging pollutants
in surface water, ground water (including drinking water) and in-
dustrial wastewaters at concentrations ranging from a few mgL
1
to
several mg L
1
[1e3]. In developing countries, such as Mexico, the
management of these pollutants is not regulated and, therefore,
they are continuously discharged into the environment without
any treatment. Consequently, they do not undergo any significant
degradation in industrial wastewater treatment facilities or in
conventional urban wastewater treatment plants.
Diclofenac and acetaminophen are two common drugs used to
treat various diseases in human beings. Diclofenac (sodium salt (2-
[2-(2,6-dichlorophenyl) aminophenyl] acetate ion)), is one of the
most common non-steroidal anti-inflammatory drugs. It is widely
used for controlling renal colic and protecting against recurrent
urinary calculi, and it is also present in numerous pharmaceutical
preparations to treat other various diseases. As a result of its
resistance to biodegradation, it is one of the pollutants most
frequently detected in groundwater, rivers and lakes around the
world with concentrations in the environment as high as 4.4 mgL
1
[4e6]. Acetaminophen (paracetamol), N-(4-hydroxyphenyl) acet-
amide is a drug with analgesic properties. It inhibits the synthesis
of prostaglandins, cellular mediators responsible for the onset of
pain. It also has antipyretic effects. It is usually presented in the
form of capsules, tablets, suppositories or oral drops.
In the search for efficient ways to remove these pollutants,
several technologies have been used, highlighting the electro-
chemical processes, such as electro-oxidation, also known as
* Corresponding author.
E-mail address: juan.peralta@ugto.mx (J.M. Peralta-Hern andez).
Peer review under responsibility of Chinese Institute of Environmental
Engineering.
Contents lists available at ScienceDirect
Sustainable Environment Research
journal homepage: www.journals.elsevier.com/sustainable-
environment-research/
http://dx.doi.org/10.1016/j.serj.2015.11.003
2468-2039/© 2016 Chinese Institute of Environmental Engineering, Taiwan. Production and hosting by Elsevier B.V. This is an open access article under the CC BY-NC-ND
license (http://creativecommons.org/licenses/by-nc-nd/4.0/).
Sustainable Environment Research 26 (2016) 70e75