1 s2.0 S0003267012007295 Main

Analytica Chimica Acta 734 (2012) 3144
Contents lists available at SciVerse ScienceDirect
Analytica Chimica Acta

journal homepage: www.elsevier.com/locate/aca
Review
Recent developments and applications of screen-printed electrodes in

environmental assaysA review
Meng Li, Yuan-Ting Li, Da-Wei Li, Yi-Tao Long
State Key Laboratory of Bioreactor Engineering & Department of Chemistry, East China University of Science and Technology, 130 Meilong Road, Shanghai, 200237, PR China
h i g h l i g h t s
g r a p h i c a l
! Screen-printed electrodes (SPEs) are

economical substrates that attract
interests.
! SPEs have been utilised for the rapid
in situ analysis of environmental pollutants.
! The configuration designs and printing materials of SPEs are developed a
lot.
! Some pretreatment techniques of
surfaces are especially addressed.
The configuration designs and printing materials of screen-printed electrodes (SPEs) are developed ov
the past decades and the applications of SPEs in environmental analysis are reviewed in this article.
a r t i c l e
a b s t r a c t
i n f o
Article history:
Received 9 March 2012
Received in revised form 4 May 2012
Accepted 12 May 2012
Available online 20 May 2012
Keywords:
Screen-printed electrodes
Electrochemistry
Environmental analysis
Recent developments
a b s t r a c t
Screen-printed electrodes (SPEs), which are used as economical electrochemical substrates, have go
through significant improvements over the past few decades with respect to both their format and th
printing materials. Because of their advantageous material properties, such as disposability, simplici
and rapid responses, SPEs have been successfully utilised for the rapid in situ analysis of environmen
pollutants. This critical review describes the basic fabrication principles, the configuration designs
SPEs and the hybrid analytical techniques based on SPEs. We mainly overview the electrochemical app
cations of SPEs in environmental analysis over the past 3 years, including the determination of orga
compounds, heavy metals and gas pollutants.
2012 Elsevier B.V. All rights reserv
Abbreviations: AChE, acetylcholinesterase; AuNPs, gold nanoparticles; ASV, anodic stripping voltammetry; BChE, butyrylcholinesterase; BOD, biochemical oxyg
demand; BiSPEs, bismuth-modified SPEs; !BSPEs, screen-printed microband electrodes; CB, carbon black; CC, catechol; CNTs, carbon nanotubes; CO, carbon monoxid
COD, chemical oxygen demand; CoPC, cobalt-phthalocyanine; CTAB, cetyltrimethylammonium bromide; CTS, Chitosan, poly-["-1-4]-2-amino-2-deoxy-d-glucopyrano
CV, cyclic voltammetry; DAB, 1,2-diaminobenzene; DPV, differential pulse voltammetry; ECL, electrochemiluminescence; FIA, flow injection analysis; Fe3 O4 /Au, Au-collo
coated Fe3 O4 ; GCE, glassy carbon electrode; GO, graphene oxide; HQ, hydroquinone; HRP, horseradish peroxidase; ISEs, ion-selective electrodes; ITO, tin-doped indium oxid
Lac, laccase; LPG, liquefied petroleum gas; LSM, strontium-doped lanthanum manganite; MnOx , manganese oxide; MWCNTs, multi-walled carbon nanotubes; NOx , nitrog
oxide; 1-OHP, 1-hydroxypyrene; Ops, organophosphate pesticides; OPH, OP hydrolase; PAHs, polyaromatic hydrocarbons; PANI, polyaniline; PANI-MB, plyaniline-methyle
blue; PANI-PDTDA, plyaniline-poly(2,2 -dithiodianiline); PAP, polyazetidineprepolymer; PASE, 1-pyrenebutanoic acid, succinimidyl ester; PPO, polyphenol oxidase enzym
SAMs, self-assembled monolayers; SERS, surface-enhanced Raman scattering; SPBE, screen-printed bismuth electrode; SPCE, screen-printed carbon electrode; SPEs, scree
printed electrodes; SPUMEs, screen-printed edge band ultramicroelectrodes; Tyr, tyrosinase; VOCs, volatile organic compounds; YSZ, yttria-stabilised zirconia.
Corresponding author. Tel.: +86 21 642 50032; fax: +86 21 642 50032.
E-mail address: ytlong@ecust.edu.cn (Y.-T. Long).
0003-2670/$ see front matter 2012 Elsevier B.V. All rights reserved.
http://dx.doi.org/10.1016/j.aca.2012.05.018
32
M. Li et al. / Analytica Chimica Acta 734 (2012) 3144
Contents
1.
2.
3.
4.
Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .
Fabrication . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .
2.1.
Principles . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .
2.2.
Printing materials and pretreatments . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .
2.3.
Novel designs . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .
Applications for environmental analysis . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .
3.1.
Routine water quality tests . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .
3.1.1.
pH and dissolved oxygen . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .
3.1.2.
Nitrite and phosphate . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .
3.2.
Organic compounds . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .
3.2.1.
Phenolic compounds . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .
3.2.2.
Pesticides . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .
3.2.3.
Herbicides. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .
3.2.4.
Polyaromatic hydrocarbons . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .
3.2.5.
Antibiotic residues . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .
3.3.
Heavy metals . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .
3.3.1.
Pb(II) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .
3.3.2.
Cd(II) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .
3.3.3.
Hg(II) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .
3.3.4.
As(III) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .
3.3.5.
Simultaneous detection of several different metals . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .
3.4.
Gas pollutants . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .
3.4.1.
Carbon monoxide . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .
3.4.2.
Nitrogen oxide . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .
3.4.3.
Volatile organic compounds . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .
3.5.
Bacteria . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .
3.6.
Radioelements . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .
Concluding remarks and future perspectives . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .
Acknowledgement . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .
Meng Li received the B.S. degree in 2010 from East

China Normal University. She is currently a Ph.D. student under the supervision of Prof. Yi-Tao Long in the
Department of Chemistry at East China University of
Science and Technology, Shanghai, China. Her current
research interests focus on spectroelectrochemistry
and environmental analysis.
Yuan-Ting Li received the B.S. degree in 2009 from

Shanghai University, Shanghai, China. She is currently
working towards the Ph.D. degree in analytical chemistry under the supervision of Prof. Yi-Tao Long at
the East China University of Science and Technology,
Shanghai, China. Her current research interests focus
on biosensor and environmental monitoring technology.
1. Introduction
The advent of screen-printing technology has opened new
exciting opportunity to apply electrochemical techniques for
environmental analyses outside a centralised laboratory. Using
screen-printing technology, the mass production makes screenprinted electrodes (SPEs) with consistent chemical performance.
Besides the need for controlling the chemical nature of the measure
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Da-Wei Li received the Ph.D. degree in environmental

science from Dalian University of Technology, Dalian,
China, in 2008. He is currently working as a research
associate in Prof. Yi-Tao Longs group at the East
China University of Science and Technology, Shanghai,
China. His research interests mainly focus on environmental monitoring technology and electroanalytical
chemistry.
Yi-Tao Long received Ph.D. degree (1998) in analytical chemistry under the supervision of Prof. Hongyuan
Chen from Nanjing University. He worked as a
Research Scientist in University of Saskatchewan and
University of Alberta, Canada for 5 years. From 2006
to 2007, he worked as an Associate Specialist in the
Berkeley Sensor and Actuator Center, University of
California, Berkeley. He was appointed as the Professor of ECUST, Shanghai to start his independent
research since 2008. His research interests include
nanopore single molecule detection, biointerface
analysis, biosensors, bioelectrochemistry, impedance
spectroscopy, in situ nano spectroelectrochemistry,
engineered molecular assemble, nanomaterial chemistry, and biomimetic coenzyme Qs.
media, SPEs may be the most appropriate electrochemical sensors for in situ analysis because of their linear output, low power
requirement, quick response, high sensitivity and ability to operate
at room temperature [1,2].
Many commercial sources of SPEs in different configurations
exist, and it is very convenient to fabricate homemade ones in small
batches with screen-printing machines. The formats of SPEs are
changeable with respect to the requirements for a specific analyte.
In addition, the surface of SPEs can be easily modified to fit multiple

purposes related to different pollutants and to achieve a variety of
improvements. Many kinds of modifiers of SPEs exist for environmental analysis, including noble metals, inorganic nanomaterials,
enzymes, and DNA sequences. SPEs combine ease of use and portability with simple, inexpensive analytical methods. Consequently,
SPEs can be successfully applied to in situ environmental analysis
and achieve improvements in detection, as has been shown over
the past several years.
This review addresses the advances in SPE fabrication and
applications in environmental monitoring from 2009 to 2011.
More published accounts of groundbreaking work with SPEs have
appeared than those covered here. This review is a small sampling
of the available literature and is not intended to cover all advancements reported over the past 3 years. This paper focuses on novel
designs, methods and materials of SPEs as well as their applications
in environmental analysis.
2. Fabrication
2.1. Principles
As a traditional and ancient technique, screen printing was
introduced worldwide over a thousand years ago and exists today in
fields such as art, textiles, and advertising. Researchers have utilised
the screen printing technique to create electrode devices on various substrates to fulfil the demand for reproducible, stable and
disposable devices that are suitable for mass production. Therefore, electrodes manufactured using the screen-printing technique
have attracted wide interest and the related SPEs fabrications have
been reviewed [3]. In addition, the extensive range of modifications to SPEs opens numerous fields of application in environmental
analysis.
The screen-printing technique uses a woven mesh to support
an ink-blocking stencil, and a roller or squeegee is moved across
the screen stencil to force or pump ink or other printable materials
past the threads of the woven mesh in the open areas. In general,
a series of woven meshes is prepared to print the different parts
of the electrode. Between printing two ink layers on a substrate,
the ink needs to first be solidified through a thermal treatment.
Finally, a protective ink coating is used to insulate the conductive
track from the electrodes.
2.2. Printing materials and pretreatments
During the printing process of SPEs, the pastes most commonly
used are silver ink and carbon ink. Silver ink is printed as a conductive track, whereas the working electrodes are mostly printed
using carbon ink or gold ink. Carbon paste is a widespread material
because it is relatively inexpensive, easy to modify and chemically inert. Gold paste is also employed in SPEs but less so than
carbon because of its higher cost. However, the generation of selfassembled monolayers (SAMs) through strong Au S bonds [4] is
creating an increased interest for gold to be employed in SPEs.
The screen-printed gold electrodes are applied as electrochemical
biosensors, including enzymatic, immune-, or genosensors [58].
The printing inks for SPEs contain some mineral binders or
insulating polymers to improve adhesion onto the substrate. The
existence of polymers in inks for working electrodes might shelter the electrochemically active carbon particles and increase the
electron transfer resistance, which would result in slower kinetics of heterogeneous reaction, and quasi-reversible or irreversible
redox processes might therefore occur at the SPEs [9]. To improve
the slow electron transfer of bare SPEs, one can modify the printing
paste with certain materials. Currently, noble metals show the best
overall catalytic performance and play a dominating role as ele

trocatalysts. However, their high cost is a serious impediment
commercial applications, so less expensive materials, such as ma
ganese oxide (MnOx ), are used to replace the noble metal materia
The commercial manganese oxide particles were efficiently mix
into the carbon ink formulation prior to screen printing [10]. As
result, the prepared MnOx SPCE exhibited good performance as
electro-catalyst for the sensing of nitrite ions and ascorbic acid wi
low detection limits. Bismuth oxide [1113] and bismuth nanopa
ticles [14] have also been successfully mixed with the carbon pas
to prepare SPBEs.
Pretreatment is another method to enhance the electrochem
ical properties of SPEs. The main purpose of pretreatment for
SPE is to remove the organic ink constituents and contaminan
and to increase the surface roughness and functionalities. Ther
fore, various researchers have proposed a short electrochemic
pre-anodisation method, a potential cycling method [15], and
two-step pretreatment approach that combines chemical trea
ments (soaked in a high-concentration solution of NaOH) a
electrochemical treatments (anodisation in a mild NaOH solutio
[16]. Moreover, plasma treatment has been introduced to clean a
modify the surface of SPCEs. For example, Ar, O2 , SF6 and CHF3 pla
mas have been used to improve the sensitivity and reproducibil
of SPCEs [1720].
2.3. Novel designs
The forms of the SPEs can vary and could be contrived accor
ing to the demands for analysis where common forms include
disc, a ring, and a band. Compared with common SPEs, the SP
in the micrometre-scale range can exhibit advantageous featur
attributed to microelectrodes, such as improved signal-to-noi
ratios, independence of forced convection, a low ohmic drop [21,2
and a faster mass-transport rate than conventional electrodes [2
However, micrometre-scale SPEs are considered difficult to pr
duce and are not very reproducible. To overcome this obstac
some researchers print the normal-sized working electrodes on t
polymer substrates. After the plate has been cut perpendicular
the conductive track with a scalpel, the formed transversal surfa
could work as a microelectrode [24,25]. Moreover, a carbon-in
based micro-tubular band electrode inside a well was developed v
screen printing [26]. The purpose of the well is to provide a know
volume for enzymatic reactions and other reactions of interest.
create the well-like electrodes, holes were mechanically punch
Fig. 1. Schemes of (a) side view illustrating the method for manufacturing well SP
(b) image of a well electrode strip, and (c) a vertical section cut through the cen
of the well containing the coordinate system used for the well electrode simulati
Adapted with permission from Ref. [26].
2009 Springer.
34
Fig. 2. Configurations of electrochemical microarray: (a) photos of a complete 96-well microplate (left) and the printed 96 carbon and Ag/AgCl electrodes with comb-type
connections (right). Reprinted with permission from Ref. [27]. Copyright 2007 Elsevier. (b) Schematic representation of the screen-printed array for direct electro-addressing
of antibodies at the surface of carbon SP microarray. CMA: 4-carboxymethylaniline. Reprinted with permission from Ref. [28]. Copyright 2007 Elsevier. (c) Scheme of assembled
screen-printed electrode array into a holder to produce 16 sealed microwells.
Reprinted with permission from Ref. [29].
2008 American Chemical Society.
or laser-drilled through the four carbon pads to create four well

electrodes on one strip. The fabrication process is shown in Fig. 1.
The application of screen-printed electrode arrays offers
the advantages of rapidity and the possibility to perform the
calibration and the analysis of several unknown samples simultaneously. A disposable sensor array was constructed that consisted
of a 96-well plate whose bottom has been modified with an array
of 96 screen-printed sensors, each of which was composed of a
Fig. 3. Novel design of SPEs: photos of (a) three eight-electrode carbon ink-based arrays stamped on the epidermis and (b) three-electrode contingent on a stress ball. Adapted
with permission from Ref. [31]. Copyright 2012 Royal Society of Chemistry. (c) Photo of SPE on an underwater garment (left) and a red indicative LED (right) when pollutant
content in seawater exceeds a certain level. (For interpretation of the references to colour in this figure legend, the reader is referred to the web version of the article.)
2011 Royal Society of Chemistry.
carbon working electrode and an Ag/AgCl pseudo-reference electrode (shown in Fig. 2a below). The array, which was connected
to a multichannel readout, could perform virtually simultaneous
determinations [27]. There are several different types of screenprinted microarrays, such as a biochip composed of eight working
electrodes, one ring-shaped pseudo-reference electrode and one
central auxiliary electrode (shown in Fig. 2b) [28]. Another type
of array was sandwiched between insulating layers to produce
microwells, as shown in Fig. 2c. Each array consisted of 16 working
electrodes and rested on a foam pad stabilised by a Teflon block
[29].
In spite of the attractive merits of SPEs, one limitation of
fabrication methodology still hampers its incompatibility with
non-planar substrates. Therefore, particular attention is paid to the
SPEs directly printed on some rigid and flexible substrates (shown
in Fig. 3a and b) [30,31]. Recently, first example of wearable screenprinted electrochemical sensor was reported (shown in Fig. 3c)
[32]. By printing the electrodes on neoprene substrates, this sensorpotentiostat microsystem could provide a visual indication and
real-time monitor the levels of marine contaminants if they have
exceeded a pre-defined threshold.
3. Applications for environmental analysis
SPEs have been used as a support to produce portable electrochemical sensors that offer exciting opportunities to perform
environmental analyses, such as routine water quality tests for
organic contaminants and heavy metals, amongst other species.
3.1. Routine water quality tests
3.1.1. pH and dissolved oxygen
An increasing need exists for reliable sensors to monitor the
variation in pH in harsh environments. The concept of screen printing is interesting because it can simplify the electronic sensing
components for in-the-field testing and replace the traditional
glass electrode that requires frequent re-calibration and is unstable. pH sensors with one electrode (with both the reference and
the measurement electrode) were attempted to be printed based
on this concept [33]. This research resulted in one printing process being capable of printing pH sensors with different pastes onto
one substrate. Almost simultaneously, a three-electrode integrated
system was successfully fabricated for pH sensing, which simplified the electronic components and increased the sensitivity vs.
the two-electrode system [34] (which has also been expanded for
the electroanalytical sensing of hydroxide ions using a nickel oxide
bulk modified SPE [35]).
The dissolved oxygen concentration is also an important parameter to evaluate water quality. A disposable CdS-modified SPE has
been utilised to determine the dissolved oxygen concentration in
water by a hot electron-induced cathodic electrochemiluminescence (ECL) method [36]. The excellent luminescent properties of
semiconductor nanocrystals allow CdS-modified SPEs to be operated at a lower potential without a dramatic evolution of hydrogen
due to the electrolysis of water. Moreover, because the common
thin film in an Al/Al2 O3 electrode is unstable in strongly acidic or
basic media, CdS-modified SPEs could be used as an alternative
because some insulating polymers or mineral binders in carbon
paste could form a thin insulating layer for cathodic ECL. This developed method has the potential to detect chemical oxygen demand
(COD) and biochemical oxygen demand (BOD).
3.1.2. Nitrite and phosphate
A sensitive and simplified method for the determination of
nitrite and phosphate ions at low levels is critically important
because of their ubiquitous nature and toxicity. Some designs based
on the advantages of SPEs have been fabricated and are feasible f

the sensing of nitrate. Because nitrite is difficult to detect on co
ventional electrodes by direct electrochemical oxidation becau
of the required large overpotential, a MnO2 SPE was fabricat
to lower the operating potentials for nitrite sensing [10]. Micr
electrodes combined with screen-printing technology have be
utilised to fabricate sensitive sensors for nitrite, which has adva
tages that include the minimisation of the iR drop (even witho
a supporting electrolyte), an increased mass transport to the ele
trode surface, and the facilitation of a rapid response with a stea
current potential [37]. A screen-printed shallow recessed graph
microelectrode array was designed without modification, whi
permitted the sensing of nitrite at low micromolar levels in riv
water samples [38]. Furthermore, a low-cost electrochemical c
was specifically designed for screen-printed edge band ultramicr
electrodes (SPUMEs) for the detection of nitrite by flow injecti
analysis (FIA) [37]. The SPUMEs were built in a three-electro
pattern, where the edge of the films could serve as a band-ty
ultramicroelectrode. The SPUMEs combined with FIA were su
cessfully applied in the determination of nitrite in the absence o
supporting electrolyte in ground and lake waters, which drama
cally simplified the detection process.
Ion-selective electrodes (ISEs) are often used for routine wat
analysis, especially because they have the ability to measure va
ous species in turbid or coloured samples. For phosphate ions, th
strongly hydrophilic character makes them challenging to dete
mine. Therefore, three types of electrodes (screen-printed, carb
paste and the conventional PVC membrane electrodes) were co
structed as the substrates for phosphate ion-selective electrod
[39]. Among them, the SPE-based ISEs worked satisfactorily with
detection limit of 4.0 !mol L1 for phosphate ion and showed a fa
response of approximately 2 s.
3.2. Organic compounds
3.2.1. Phenolic compounds

The rapid in situ determination of phenolic compounds and th
derivatives is an important environmental challenge because
the easy penetration of such species through membranes or ski
of plants, animals and humans, with toxic side effects [15]. SP
based electrochemical biosensors have led to a low-cost, simp
and sensitive analytical method for phenolic compounds.
The direct electrochemical behaviour of individual pheno
compounds at non-pretreated SPEs has been previously discusse
thereby simplifying the procedures for electrode treatment [40,4
In certain cases, the electro-oxidation products of phenol wou
passivate the surface of SPEs and hinder the electron transf
process. The use of surfactants with antifouling properties in co
junction with preconcentration is an effective way to solve t
problem. One research studied the usage of SPEs in the presence
a cationic surfactant, cetyltrimethylammonium bromide (CTAB),
determine bisphenol A in river water and sewage samples [41].
Phenolic isomers usually coexist in environmental sample
therefore, methodologies to spontaneously determine pheno
isomers are of great interest. The challenge in isomer analy
is the overlapping peak potentials in untreated SPEs that ex
as a result of similar structures and properties. Electrochemic
pretreatment has been used because of its simplicity. After pr
treatment, the organic binder within the surfaces of SPEs w
removed, and graphite particles in the micrometre-size range we
exposed, which increased the specific surface area of the SP
A simultaneous method for the determination of hydroquino
(HQ) and catechol (CC) was applied at anodically pretreated SP
in river water samples and yielded a good peak separation of H
and CC [42]. Another study reported that an electrochemically pr
treated SPE was employed for the simultaneous determination
36
aminophenol isomers in river water [15]. Three well-defined oxidation peaks of aminophenol in the isomer mixture could be achieved
using derivative techniques.
Further studies have been performed at chemically modified
SPEs, especially nanomaterial-modified SPEs, because the modifying substances can dramatically increase the sensitivity and
selectivity of detection because of their unique electronic, catalytic and chemical properties [43]. A nanocomposite-modified
SPE coated with multi-walled carbon nanotubes (MWCNTs) and
electrodeposited gold nanoparticles (AuNPs) was fabricated to
determine the three types of dihydroxybenzene isomers in water
samples [44]. Compared with a nontreated SPE, the fabricated
SPE displayed significantly greater electrocatalytic activity for
the oxidation of dihydroxybenzenes because AuNPs supported
on the conducting MWCNTs enhanced the sensitivity remarkably. Using differential pulse voltammetry (DPV), the authors
simultaneously determined three kinds of isomers at the modified SPE. In addition, multielectrode arrays have recently received
considerable attention because of their ability to provide multicomponent, simultaneous and high-throughput analyses. For example,
an MWCNT-modified screen-printed multielectrode array was
designed for the determination of dihydroxybenzene isomers [45].
This strategy was also demonstrated to have the potential for
detecting other organic isomers.
SPE-based electrochemical biosensors appear to be an attractive
and suitable option for the more sensitive and selective determinations of phenolic compounds. Enzymes have been widely used
in the preparation of biosensors for the analysis of phenolic compounds and have allowed the measurement to be performed at
a low applied potential to significantly reduce the interference
[46]. Two important types of polyphenol oxidase enzyme (PPO),
tyrosinase (Tyr) and laccase (Lac), can catalyse the oxidation of benzenediols and phenols to quinones or to radical species by reaction
with oxygen in solution [47].
One of the most important aspects that affects the performances
of enzymatic biosensors is their effective immobilisation on the
electrode surface. Hence, most research in this area has focused on
the development of approaches that retain the biochemical activity of an enzyme whilst minimising the enzymes denaturation and
leakage into solution. One approach is to immobilise the enzyme
through the entrapment method. As immobilising agents, polyazetidineprepolymer (PAP) and polyvinyl alcohol photopolymer have
been successfully used to immobilise Lac on surfaces of SPEs. The
efficiency of the constructed SPEs was confirmed using phenolic
analysis [4850].
Electrodeposition is another simple method to immobilise an
enzyme onto an electrode surface. One biosensor for phenol detection was achieved through the electrodeposition of PPO with the aid
of a Bi3+ precursor onto the MWCNT-modified SPE without the use
of any matrix or binder [51]. Other research reported a biosensor
for the detection of 1,2-diaminobenzene (DAB) by electropolymerisation of PPO, DAB and a mediator complex on a screen-printed Pt
electrode [52]. The analytical results for DAB demonstrated that the
mediator-modified enzymes displayed improved electron-transfer
rates compared to that of the native enzyme.
Other efficient immobilisation methods have been recently
developed. The combination of magnetic nanoparticles with bioimmobilisation, separation and detection could provide unique
capabilities and improve the performance of biosensors. Magnetic
nickel nanoparticles were utilised as an immobilisation platform
to construct disposable biosensors, with the highest performance
for determination of bisphenol A compared with biosensors based
on Fe3 O4 and AuNPs [53]. Moreover, some simple and versatile
noncovalent methods through supermolecular interactions could
also be utilised to construct biosensors. One biosensor based on
the immobilisation of Tyr-protected AuNPs onto 1-pyrenebutanoic
acid, succinimidyl ester (PASE) functional graphene oxide (GO)

modified SPE was fabricated for the determination of CC [54]. PASE
is a bi-functional molecule that was assembled onto GO sheets
through noncovalent ## interactions. Using this approach, Tyr
could be assembled onto SPEs with a high degree of control and
specificity, which led to good stability and a high sensitivity for the
determination of CC. Silver-electrodeposited screen-printed electrodes (Ag-SPEs) were introduced as portable surface-enhanced
Raman scattering (SERS) substrates to detect phenolic compounds
[55]. These SERS-active substrates are easily prepared and stored,
and they are better suited for in situ determinations than silver colloids. Combing with the electrostatic preconcentration technique,
Ag-SPEs based SERS sensors could be qualitatively and quantitatively to analyse polar organic pollutants with detection limits of
0.1 nmol L1 .
3.2.2. Pesticides
Pesticides, especially organophosphate pesticides (OPs), can
lead to cholinergic dysfunction, which disrupts the health of
both humans and animals. Monitoring the amount of pesticides
in water and soil is an effective way to detect the abuse of
pesticides in agriculture [56]. Because pesticides can inhibit the
activity of many enzymes, such as acetylcholinesterase (AChE),
butyrylcholinesterase (BChE), OP hydrolase (OPH), and Tyr, various inhibition biosensor systems based on SPEs have emerged in
recent years as promising alternatives for in-the-field detection
of pesticides (Table 1). When an enzyme immobilised on an SPE
interacts with the substrate, the electroactive species are produced.
After the enzyme is exposed to the inhibitor, the decreased enzyme
activity leads to a decrease in the current intensity. Hence, the general quantitative principle of pesticides is primarily based on the
amperometric measurement of the decreased enzyme activity [57].
The performance of biosensors depends considerably on the
method used to immobilise the enzymes. Cross-linking [5759],
physical entrapment [60] and solgel [61] approaches are the traditional chosen strategies. However, the utilisation of these types of
immobilisation methods, the non-renewability of the sensing surface and the aggressive detection environment, which could lead
to enzyme denaturation, are problems that need to be addressed.
Recently, enzyme immobilisation using magnetic materials has
been explored for the construction of biosensors for pesticides.
The magnetic feature of magnetic materials enables enzymatic
reactions to occur close to the transducer, a rapid separation of
the immobilised enzyme in the magnetic field for the renewability of the sensitive surface, and a good microenvironment for
retaining the bioactivity of the enzyme. Hybrid core/shell biomagnetic glasses, which consist of a Fe3 O4 inorganic core and a
mesoporous silica shell, were synthesised as a platform for AChE
immobilisation [61]. SPEs with AChE-biomagnetic glasses were
employed to construct a paraoxon biosensor with a detection limit
in the nanomolar range. Another magnetic nanoparticle species,
Au-colloid-coated Fe3 O4 (Fe3 O4 /Au), where Au improves the stability of magnetic Fe3 O4 cores, was selected for the immobilisation
of AChE on composite membrane-based SPEs using an external
magnetic field [62]. When the magnet is removed, the SPE surface
can be easily renewed. In addition, to eliminate the mass-transfer
problems commonly associated with immobilisation, whole cells
could be directly used for immobilisation without permeabilisation. Whole cells of Escherichia coli were successfully immobilised
on SPEs through a cross-linking agent for methyl parathion analysis, and only a small sample volume was required for detection
[63].
During the amperometric measurement, the modification of
SPEs with mediators is necessary to reduce the relatively high
working potential, which causes interference from other electroactive compounds. Prussian blue [57,62], carbon nanotubes [59,62],

Table 1
Pesticide sensors based on SPEs dedicated to environmental analysis applications.
SPE configuration
Analyte
Sensor characteristic
LOD (ppb)
Reference
Nanometre-sized titania/SPE
BChE-based Prussian Blue/SPE
0.63
2
0.5
12
25
10b
19b
5b
6b
4
1.3
[60]
[61]
AChE-based MWCNT-cellulose/SPE
AChE-based PEDOT:PSSa /SPE
Dichlofenthion
Paraoxon
Chlorpyrifos-methyl oxon
Aldicarb
Carbaryl
Carbaryl
Diazinon
Carbofuran
Methyl parathion
Carbaryl
Chlorpyrifosoxon
AChE-biomagnetic glasses/SPE
AChE-based magnetic composite/SPE
recombinant Escherichia coli/SPE
Molecularly imprinted polymer/SPE
Paraoxon
Dimethoate
Methylparathion
Fenitrothion
14
5.6 104
131.6
222
[65]
[66]
[67]
[69]
AChE-based Prussian Blue/SPE

Tyr-based CoPc-cellulose-graphite/SPE
a
b
[62]
[63]
[64]
PEDOT:PSS-poly(3,4-ethylenedioxythiophene):poly(styrenesulphonate).
The minimum value of the linear range.
cobalt-phthalocyanine (CoPC) [64] and conductive polymer [60]

have been successfully used to lower the working potential of pesticide biosensors. These electronic mediators are typically deposited
on the surface of SPEs using a drop-coating method or screenprinting technology using a conductive paste.
Furthermore, to provide a rapid response and signal for the
existence of complex pesticides within samples, a screen-printed,
amperometric biosensor array that consisted of 12 CoPC-modified
SPEs was used for the simultaneous determination of OPs [64]. Six
different AChE enzymes were immobilised on different SPE surfaces
to achieve the inhibition data in a sample solution.
Enzyme-based biosensors can only provide the total toxicity
of a mixed sample without the possibility of selectively quantifying different pesticides. To avoid the utilisation of enzymes,
molecular imprint and photoelectrochemical technologies with
high selectivities towards specific pesticide species have been used
to analyse pesticides in environmental samples (Table 1). A molecularly imprinted polymer was obtained by the electropolymerisation
of Ni(II)-p as an SPE coating for the selective and in-the-field
determination of fenitrothion through cyclic voltammetry [65].
Another group has described a simple photoelectrochemical
SPE sensor for dichlofenthion based on a nanometre-sized TiO2
photocatalytic degradation mechanism [56]. This sensor creates
new opportunities for the monitoring of other non-electroactive
pesticides.
3.2.3. Herbicides
The increasing use of herbicides impacts drinking water and
affects crop safety, resulting in contamination of the water and
soil system. One common approach for the selective detection
of herbicides is the immunoassay method. Combined with SPEs,
the immunoassay approach allows for a single shot determination
of herbicides, thereby avoiding the cleaning and reuse of active
components. An enzyme-linked screen-printed immunoassay was
fabricated for isoproturon based on a horseradish peroxidase
(HRP)-labelled polyclonal antibody [66]. This sensing platform
incorporated a membrane into the working electrode allowing
for the covalent immobilisation of assay reagents and fast signal transduction. With respect to the simplification of procedures
and improvements in sensitivity, an AuNPs-assisted ultra-sensitive
non-enzyme electrochemical immunoassay has been reported [67].
The sensitivity detection achieved sub-nanomole levels for chlorsulphuron using anodic stripping voltammetry. This strategy could
also be readily utilised for the simultaneous screening of different
analyte arrays of environmental importance.
However, the immunoassay procedure faces some drawbac

such as the time-consuming antibody generation process a
the possibility of cross-reactivity of the antibody with simi
compounds [68]. Hence, many researchers have focused th
investigations on the development of biosensors for alternati
uses. The use of photosynthesis biosensors for this purpose th
employ natural photosynthesis machinery has been well doc
mented. The entrapment of photosynthetic materials is challengi
with respect to the construction of photosynthesis biosenso
Screen-printing and self-assembly technologies are common
utilised to immobilise photosynthetic materials. A screen-print
algal biosensor was fabricated by mixing unicellular microal
cells into an algal ink for evaluation of the toxicity of herbicid
which yielded a shorter assay time [69]. Another example report
recently is the immobilisation of photosynthetic-reaction reporte
onto gold SPEs using a self-assembled monolayer for the develo
ment of a unique biointerface [68]. The biosensor displayed go
performance with respect to achieving effective mediator tran
fer to the SPEs, with a detection limit of 1.15 nmol L1 for atrazin
Moreover, the development of whole-cell biosensors has draw
attention because the living cells can function as bioreporters th
offer a fast and effective assessment of the overall toxicity of a wat
system. A whole-cell triazine herbicide biosensor based on ma
netic nanoparticles functionalised living cells has been report
(Fig. 4) [70]. This methodology allowed for efficient cell immobi
sation and did not affect the cellular metabolism.
3.2.4. Polyaromatic hydrocarbons

Polyaromatic hydrocarbons (PAHs), which contain two or mo
fused aromatic rings, often require complex preconcentration pr
cedures during detection because of their low solubility in wat
Therefore, SPEs could be an effective extraction and absorpti
tool for PAHs because aromatic compounds could interact with t
graphite walls and stack onto carbon materials through noncov
lent bonding [71].
The electrochemical oxidation behaviour and the oxidati
mechanism for 1-hydroxypyrene (1-OHP) has been investigat
at a disposable SPE [72]. In particular, PAHs are always found
a mixture of individual compounds with similar molecular stru
ture, similar electron density and a lack of side groups. Therefo
an immunosensor based on SPEs was developed for PAH detecti
using a co-exposure competition assay. The immunosensor d
played cross-reactivities of varying degrees towards 16 importa
PAH compounds [73]. Nevertheless, the production of antibodi
specific for only one PAH is difficult. Future approaches may invol
38
Fig. 4. A sketch of the biosensor setup based on a screen-printed electrode, a

tetrafluoroethylene support with the embedded permanent magnet and magnetically functionalised microalgae cells. The arrow indicates the order of assembly.
The inset shows a typical optical microscopy image of the MNP-functionalised C.
pyrenoidosa cells.
2011 Royal Society of Chemistry.
the use of various antibodies within a single sensor to produce

different signals and deliver more information regarding the PAH
mixture.
Fig. 5. (a) Schematic representation of a disposable screen-printed array based

on eight graphite round-shaped working electrodes, each one with a silver
pseudo-reference electrode and a graphite counter electrode. (b) A disposable
screen-printed array, the magnet holding block, and the two components assembled
in the proper position.
3.2.5. Antibiotic residues

The detection of antibiotic residues in environmental samples
through the combination of disposable electrochemical sensors
has achieved significant attention for fast, low-cost and sensitive detection. Tetracyclines, as an important class of antibiotics,
were investigated on gold SPEs using cyclic voltammetry and FIA
[74]. A screen-printed eight-electrode-based immunoarray for the
detection of sulfonamide antibiotics was developed using magnetic
beads as a solid phase, which allowed the rapid extraction of sulfonamides in complex matrices (Fig. 5) [75]. The combination of
the antibody-based assays, magnetic bead separation and screenprinted array transduction is an attractive aspect of this research
that has the potential to be used in the development of a highsample-throughput screening system.

2010 John Wiley and Sons.
3.3. Heavy metals

In developing countries, rapid economic development often
occurs at the expense of the environment. The environmental damage from heavy metals has only begun to be remedied. Therefore,
simple and inexpensive sensing devices are needed for in situ monitoring. In recent decades, heavy metals have been persistently
monitored all over the world because of their toxicity, even at low
concentrations [76]. Common toxic metal ions, such as Pb(II), Cd(II),
Hg(II), and As(III), are especially important because they are neurotoxic (e.g., Pb(II) [77] and Hg(II)), easily absorbed by the human
body and accumulate within the environment and living organisms
[78]. Historically, electrochemical stripping analysis, commonly
using anodic stripping voltammetry (ASV), has been widely recognised as a powerful technique for heavy-metal detection because
of the simplicity of the instrument as well as its moderate cost and
portability. Moreover, the ASV technique combined with SPEs can
handle all scenarios that require rapid, inexpensive, sensitive and
accurate determination [79] in the field of environmental monitoring. Most studies of heavy-metal determination using SPEs show
that mercury, gold, silver, bismuth or other materials modified on
the surface of SPEs can improve selectivity or sensitivity [24,7983].
A number of reviews have provided an in-depth analysis of specific areas. Therefore, we have reviewed and listed the recent
developments in heavy-metal-ion detection using different modified SPEs with some optimised analytical parameters in Table 2.
3.3.1. Pb(II)
According to a recent review [84], sensors for Pb(II) detection are
usually modified with carbon, bismuth, gold or other materials to
improve sensitivity. These modifiers can be transplanted onto the
surface of SPEs to allow detection to be more convenient. The most
widely used modifier of SPEs for electroanalysis is bismuth because
of its good analytical performance and its environment-friendly
characteristics. Since the pioneering report in 2000 [81], bismuthmodified SPEs (BiSPEs) have been broadly applied to the field of
environmental [85] monitoring. Advantages, such as not requiring the removal of dissolved oxygen during stripping analysis and
characterisation over a wide negative-potential window [8587],
make testing convenient. Moreover, the bismuth-modified SPEs
can improve sensitivity; for example, the detection limits of Pb(II)
can reach the ppb level or lower [88].
In general, bismuth is in situ or ex situ electroplated onto the
surface of working electrodes to form a Bi film on SPEs. Based on
this observation, a novel sensor was developed for the one-step
sensing of Pb(II) [82,89] by covering a paper disk impregnated with
buffer and reagents (including an internal standard of Zn(II) and
a plating solution of Bi(III)) on a screen-printed carbon electrode.
After the sample was added to the surface of the electrode, it could
be applied to run a single-step assay for Pb(II) detection (Table 2).
The performance of the electrode was satisfactory (550 ppb Pb(II)
detected), and only a final, small volume of the sample (10 !L) was
needed to be placed on the surface of the paper for running one
assay. In addition, an internal standard with a known concentration
was added to improve the accuracy and precision [90,91]. Hg-free
screen-printed microband electrodes (!BSPEs), which are easily
manufactured with the option to renew the electrode surface, was
used to detect Pb(II) and a theoretical detection limit of 2.3 ng mL1
was calculated based on a signal-to-noise ratio of three [92].

Table 2
Application examples of SPEs for metal ion detection.
Metal ion
Modification
Stripping
technique
Limit of
detection
(LOD) (ppb)
Time (s)
Potential (vs. Ag/AgCl)
Pb(II)
None/!BSPEs
Bi
LSASV
SWASV
2.3 ng mL1
<5
1500
120
Hg thin film/micro-well
SWASV
ex situ deposited Hg (5 !g)

AuNPs amalgam
Microelectrode array/Hg
SWASV
DPASV
SWASV
2 109 mol L1
(0.2 ppb)
0.2
2.6
1.3
Hg(II)
SPGEs
Thiol compound
SPCE/PANI + PDTDA
SPCE/PANI + MB
SWASV
it
DPASV
DPASV
As(III)
PtNPs
AuNPs
AcH
Cd(II)
Practical application
Reference
1.3 V
1.4 V
Surface water
[99]
[89]
60
1.0 V
Soil solution
[103]
60
100
300
1.0 V
1.1 V
1 V
River water
River/tap water
River water
[100]
[102]
[90]
1.1
1
56
54
60
120
120
+0.3 V
0.3 V
0.3 V
Waste water
Drinking water
Ultra pure water
[112]
[113]
[116]
[117]
CV
LSV
it
5.68
0.4
0.8
160
0.4 V (vs. SCE)
Tap water
Canal water
Tap water
[120]
[121]
[125]
BiNPs
SWASV
Pb(II): 0.9
Cd(II): 1.2
Zn(II): 2.6
120
1.4 V
Waste water
Tap water
[18]
Au film
SWASV
1.0 V
+0.3 V
1.0 V
+0.3 V
[133]
SWASV
120
120
120
120
Tap water
Preconcentrated with
thiol-modified Fe3 O4
Pb(II): 0.5
Hg(II): 1.5
Pb(II): 0.02
Hg(II): 0.08
Tap water
[133]
Crown-ether/Hg film
LSASV
Pb(II): 1.65
Cd(II): 0.67
120
1.0 V
River water
Soil solution
[134]
CTS/SPCE
DPASV
Pb(II): 3.4
Cu(II): 5
Cd(II): 5
Hg(II): 2
30
1.0 V
Tap water
[137]
Hg/MWCNTs-CTS/SPE
SWASV
Pb(II): 4.8
Cd(II): 1.3
Cu(II): 1.3
300
1.3 V
River water
[138]
Pb(II), Cd(II), Zn(II)
Pb(II), Hg(II)
Pb(II)
Cd(II)
Pb(II), Cu(II), Cd(II),
Hg(II)
Pb(II), Cd(II), Cu(II)
Deposition
SWASV, square wave anodic stripping voltammetry; DPASV, differential pulse anodic stripping voltammetry; LSASV, linear sweep anodic stripping voltammetry; CV, cy
voltammetry; LSV, linear sweep voltammetry.
3.3.2. Cd(II)
Although bismuth is widely used to modify SPEs for the detection of heavy metals, this approach exhibits shortcomings. For
example, acidic or highly alkaline working media may be necessary for in situ plating of Bi film, because of the Bi(III) hydrolysis in
neutral and alkaline media [86]. In contrast, the quasi-noble-metal
behaviour of mercury allows analyses over a wide pH range [93].
Because of the high affinity of mercury for metals associated with
the analytical performance of stripping voltammetry, low detection
limits can be achieved with relatively short analysis times without degassing [94]. Mercury is therefore still used as the modifier
for trace metal detection [93,95]. However, because of the toxicity
of mercury, researchers are actively pursuing ways to reduce the
amount that is needed for modification of SPEs.
A thin-film mercury screen-printed working electrode was combined with a micro-well to detect Cd (II) (see Fig. 6) [96]. The use of
a micro-well reduced the volume of the sample to 200 !L without stirring, which minimised the loss of sensitivity. Moreover,
this working electrode was used for direct analysis in raw samples of soil solution without pretreatment, which provides a useful
method for the in situ determination of heavy metals.
Some researchers have also printed auxiliary electrodes with
the working electrode on the same polymer plates [93]. This
screen-printed sensor was ex situ electrodeposited with a small
quantity (approximately 5 !g) of mercury at 0.1 V (vs. Ag/AgCl).
However, when this sensor was used, an additional commercial
reference electrode or counter electrode was needed to compose
a 3-electrode system for detection. Therefore, a screen-printed

electrode system on the same substrate would be more convenie
A 3-electrode device with a standard USB port conveniently co
nected to a PC or laptop computer was designed [95].
Microelectrodes provide new tools for environmental analys
however, the difficulty of recording very low currents using micr
electrodes needs to be overcome [97]. Therefore, microelectro
arrays have been consequently developed to obtain a higher cu
rent output [98]. Based on femtosecond laser ablation technologi
square arrays of 64 microelectrodes (8 8) were made in a pol
mer substrate and then screen-printed carbon ink (see Fig. 7) [8
Because of the small overall surface of SP!EA, only a low quant
of mercury (less than 1 !g) was ex situ deposited, and the devic
were sufficient to perform a trace analysis of river water close to
zinc mine.
3.3.3. Hg(II)
Mercury is also one of the most problematic heavy-me
pollutants in environmental monitoring and its organic form
bioaccumulative and toxic. Moreover, the accumulation of mercu
in the human body can cause severe disease, such as kidney a
respiratory failure, and damage to the gastrointestinal and nervo
systems [99].
Bare gold electrodes or modified gold electrodes are usually ch
sen for inorganic Hg(II) detection because the high affinity for Hg(
enhances preconcentration [100]. However, the major drawbac
of the use of a gold electrode are structural changes at the surfa
40
Fig. 6. Schemes of (a) a screen-printed sensor and (b) a screen-printed sensor adds with a microwell.
Adapted with permission from Ref. [96].
caused by amalgam formation. For this reason, time-consuming

cleaning treatments are necessary to achieve reproducibility [101].
Alternatively, commercial screen-printed gold electrodes make
routine measurements of Hg(II) in water samples simpler and more
attractive because preplating steps are unnecessary. Commercial
screen-printed gold electrodes (SPGEs, DropSens, Spain) have been
successfully used for the measurement of Hg(II) in ambient water
[102].
Some researchers have detected Hg(II) using SPEs based on the
electrochemical behaviour of a Hg-complex. A thiol-probe based
on SPEs modified with a film of nanostructured carbon black (CB)
is highly sensitive to thiocholine and cysteine. After the Hg(II) is
added, a non-electroactive complex is formed, which leads to a
diminished signal [103]. This sensor is a promising replacement for
the traditional gold electrode. The application of polyaniline (PANI)
has been investigated for the preconcentration and speciation of
inorganic Hg(II) and methyl mercury, [CH3 Hg]+ , in various water
samples [104,105]. Other researchers have modified bare SPCEs
with a conducting polymer layer of PANI, polyanilinepoly(2,2 dithiodianiline) (PANI-PDTDA) [106] or polyaniline-methylene
blue (PANI-MB) [107], and these SPCE/polymer sensors could be
used as alternative transducers for the voltammetric stripping and
analysis of inorganic Hg(II). Moreover, this electrochemical sensor has been utilised for the simultaneous determination of Hg(II),
Pb(II), Ni(II) and Cd(II) [108,109].
3.3.4. As(III)
Arsenic, also a kind of toxic element, can dissolve from minerals
to contaminate groundwater under certain geochemical conditions
and upon microbiological activity. Drinking water rich in arsenic
over a long period of time leads to arsenic poisoning or arsenicosis.
Some researchers have prepared PtNPs/SPCEs by electrochemically depositing K2 PtCl6 to detect As(III) [110]. PtNPs/SPCEs makes
no interference from Cu(II) towards the oxidation of As(III) during detection. Usually, the sensitivity of CV is lower than that of
ASV, which includes a preconcentration step under the same conditions. With the use of SPCEs modified with citrate-capped AuNPs,
As(III) was determined with no interference from Cu(II) [111].
These metallic nanomaterials provided a new means for multiple
modifications of SPEs and the replacement of traditional preciousmetal electrodes.
Recently, enzymatic biosensors have also been used for the
determination of hazardous metals because some metals can act as
enzyme inhibitors, which lead to sensitive and specific detection
[112,113]. For this reason, acetylcholinesterase (AchE) was immobilised by covalent linkage on the surface of SPCEs to detect As (III)
[114]. However, the interference of Hg(II), Ni(II) and Cu(II) species
cannot be neglected. Thus, an enzyme that is more specific and
sensitive to As(III) might be selected for future detection.
3.3.5. Simultaneous detection of several different metals
SPEs designed for the simultaneous determination of different metals are more interesting for time and cost reasons. SPEs
modified with Hg and Bi, either in situ [115] or ex situ [116,117],
are commonly used to determine Pb(II) and Cd(II) concentrations. Otherwise, Bi could be deposited on SPEs in many forms,
such as bismuth oxide [1113], bismuth nanoparticles [14], bismuth co-deposited with metal ions in solution [118] and bismuth
pre-deposited as a film [119]. As far as we can determine, Bi
nanoparticles plated on SPEs using the SWASV technique exhibited the lowest detection limits of Pb(II), Cd(II) and Zn(II). When
combined with a flow cell, the detection limits could be lower [14].
Fig. 7. Side and top views of different steps for microelectrode array fabrication: (a) membrane of mylar, (b) membrane after laser ablation; (c) ablated membrane after
screen-printing; and (d) side of the screen-printed membrane after the application of the insulation.
2009 Elsevier.
The normal Au-film-coated SPEs displayed excellent linear

behaviour. Moreover, the researchers improved the preconcentration technique by modifying the magnetic particles (superparamagnetic iron oxide (Fe3 O4 ) nanoparticles [120,121]) with thiols to
preconcentrate heavy metals from samples whose concentrations
were lower than 1 !g L1 [122].
Because crown-ethers can form complexes by fitting metal
cations into the cage of the crown structure, some researchers
have modified crown-ether-based membranes on a thin-film of Hgcoated SPCE to achieve a selective uptake of Pb(II) and Cd(II) [123].
In addition, the crown-ethers can protect the working surface from
interferences during analysis. Without deoxygenation and stirring,
this device was successfully used to detect Pb(II) and Cd(II) Also,
this device was utilised in raw samples and in the semicontinuous
monitoring of Pb(II) and Cd(II) for 42 h in tap water [94].
Chitosan,
poly-["-1-4]-2-amino-2-deoxy-d-glucopyranose
(CTS), can form stable chelates with many transition-metal ions
through hydroxyl and amino groups. CTS and its derivatives have
been used for the electrochemical determination of metal ions with
glassy carbon electrode (GCE) [124]. Some researchers modified
CTS on the surface of SPCEs for the simultaneous determination of
Pb(II), Cu(II), Cd(II) and Hg(II) with preconcentration time of only
30 s [125]. In addition, CTS could be used for the homogeneous
dispersion of MWCNTs [126] and the CTS-MWCNTs composite
film exhibited significant improvements in tensile modulus and
strength [127]. A small amount of mercury was subsequently
deposited in situ, and a random array of mercury nano-droplets
formed on the surface of the MWCNTs-CHIT/SPE. This sensor
was used for the simultaneous determination of Pb(II), Cd(II) and
Cu(II). Moreover, a hybrid analytical method, which combined
electrochemical adsorptiondesorption with colourimetric
analyses, was developed to detect heavy-metal ions [128]. The
electrochemical adsorptiondesorption procedure, which is more
convenient and less time-consuming, was used as a pretreatment
process for the colourimetric analysis. The colourimetric approach
used for quantitative analysis may avoid errors that arise from the
instability of the electroanalytical method.
3.4. Gas pollutants
Many analytical instruments, such as those based on colour
reactions, chemical luminescence, or IR absorption, have been used
for measuring the concentration levels of toxic gases. Comparing
with these instruments, the electrochemical gas sensors prepared
using a screen-printing method were low in cost, simple in construction, and small in size. Such screen-printed gas sensors have
gradually been applied in environmental analysis.
3.4.1. Carbon monoxide
Carbon monoxide (CO) is a colourless, odourless, tasteless and
poisonous gas that is commonly produced by the incomplete combustion of fossil fuels. It combines with haemoglobin to produce
carboxyhaemoglobin, which is ineffective for delivering oxygen to
body tissues, and a level of 50% carboxyhaemoglobin may result in
seizure, coma, or death.
Because of its excellent stability and ion-conducting behaviour
over a wide range of oxygen partial pressures and temperatures,
yttria-stabilised zirconia (YSZ) was utilised as an electrolyte to
detect CO. Whereas strontium-doped lanthanum manganite (LSM)
was used as the counter electrode, and Au was used as the sensing electrode [129]. This film was fabricated by the screen-printing
technique, which allowed the implementation of a compact planar
device in an easy, fast and highly economical manner. The excellent
performance and fast response time to CO molecules were corroborated at relatively low temperatures without a cross-sensitivity to
NO2 . Otherwise, the sensor signal showed long-term stability.
Another CO sensor was based on the deposition of Pt nanopar

cles on a SPUME with Nafion as the solid polymer electrolyte (Fig.
[130]. The sensor scheme requires no supporting electrolyte, a
the catalytic activity is enhanced substantially because of the
nanoparticles deposited homogeneously on the electrode. In th
study, Pt is employed as the working electrode because it is high
catalytic to CO oxidation and is chemically stable [131]. The Nafi
thin-film solid polymer electrolyte is hygroscopic, which allow
the conduction of protons and permits the gases to access t
electrodes [132]. The developed gas sensor has a good cataly
oxidative activity regarding the determination of CO or gaseo
formaldehyde [133]. This device could be used for in situ measur
ments and for continuous monitoring.
A CO gas sensor has been reported that was based on a scree
printed SnO2 film on an alumina substrate [134]. SnO2 is an n-ty
semiconductor, and a screen-printed porous SnO2 thin film cou
interact with oxygen by transferring electrons from the condu
tion band to adsorbed oxygen atoms, which would result in t
formation of ionic species such as O2 or O . When the SnO2 fi
is exposed to a reducing gas, such as CO, the adsorbed oxygen
removed by oxidation of the gas, and the captured electrons a
injected into the conduction band. The screen-printed SnO2 fi
exhibited excellent selectivity towards CO gas against LPG (li
uefied petroleum gas), CH4 and H2 , high sensitivity and reliab
correlation over the range of 2575 ppm.
3.4.2. Nitrogen oxide

Nitrogen oxide (NOx ) refers to NO and NO2 that are produc
during combustion, especially at high temperatures. NO in the
may convert to nitric acid, which has been implicated in the form
tion of acid rain. NO2 , a reddish-brown toxic gas, has a characteris
sharp, biting odour and is a prominent air pollutant; symptoms
poisoning (lung edema) may appear several hours after inhalati
of a low but potentially fatal dose. Also, low concentrations (4 ppm
will anesthetise the nose, thus creating a potential for overexp
sure. Furthermore, both NO and NO2 participate in depletion of t
ozone layer.
Various types of solid-state NOx sensors have been dev
oped, as reviewed previously [135]. Sensors that incorpora
solid electrolytes can operate at high temperatures and are t
most promising sensors for monitoring NOx in high-temperatu
combustion exhausts or in the environment. A decade aft
that, solid-electrolyte-based sensors were developed [136]. Som
researchers fabricated screen-printed tin-doped indium oxi
(ITO) thin films on glass substrates to detect NOx gases [137]. T
transparent and conductive ITO thin films were obtained from
organometallic-based paste fired in an infrared furnace. Moreov
the specific morphology of the screen-printed ITO film (granu
and porous) was highly suitable for the development of stable a
efficient NOx gas sensors.
3.4.3. Volatile organic compounds

Volatile organic compounds (VOCs), which are numerou
varied, and ubiquitous, are organic chemicals with a hi
vapour pressure under ambient conditions. Many VOCs, inclu
ing formaldehyde, acetone, and methanol, are dangerous to hum
health or cause harm to the environment. VOCs are present in ne
furnishings, wall coverings, and office equipment such as phot
copy machines, which can off-gas VOCs into the air and result
long-term health problems.
A gas sensor based on WO3 thick films, which have good ele
trical and optical properties, exhibited excellent acetone vapo
sensing properties. The sensitivity of this sensor could reach abo
456% at 300 C with fast response and recovery times [138]. In add
tion, the conductivity of the carbon nanotubes (CNTs) has be
found to be sensitive to various gases, and CNT-based gas senso
42
Fig. 8. Schemes of (a) the structure of the screen printed edge band ultramicroelectrodes (SPUME) assembly with a built-in three-electrode configuration, (b) an SEM image
of Pt nanoparticles deposited on the surface of a carbon working electrode and (c) a representation of the electrode structure.
have been reported [139,140]. Thus, a screen-printed nanocomposite film composed of MWCNTs and a silicon dioxide binder has
been reported to detect organic gases, including acetone, ethanol,
formaldehyde and methanol. The conductivity of the film decreases
when the film is exposed to organic gases. The existence of micropores in the composite provides channels for gas molecules to
absorb onto CNTs and increase the resistance of the CNT composite.
3.5. Bacteria
SPEs provide excellent platforms for the rapid detection of
bacteria to lower the risks of infection and prevent enteric diseases and economic losses. An indirect sandwich enzyme-linked
immunosensing strip was fabricated for the specific detection of
E. coli O157:H7 because of the use of double-specific antibodies
[141]. Another example of the selective detection of E. coli was
based on an impedimetric immunosensor developed using selfassembled monolayer-modified gold SPEs [142]. It was used for
the rapid analysis of E. coli in river and tap water samples without preconcentration steps. It is noteworthy that the SPEs involved
in these research efforts act primarily as functional components.
Thus, a screen-printed integrated microsystem for the detection of
pathogens was developed in which the SPEs served as both functional and structural components, which improved the simplicity
and ease of fabrication [143]. This research intends to be an outline
for a series of methodological procedures, immobilisation, lysis and
detection, integrated within a low-cost microsystem. In addition,
the study of bacteria species immobilised or adsorbed on electrode
surfaces is interesting for sensor applications. A simple method
with the application of a disposable SPE was used to study the
direct electron-transfer reaction at Shewanella sp. bacteria without the aid of a redox mediator [144]. The SPE was modified with
bacteria using an easy drop-coating procedure, which avoided the
laborious and time-consuming step of growing a bacterial biofilm
on the electrode.
3.6. Radioelements
Radioelements are radiologically and chemically toxic, and the
application of SPEs has contributed to the monitoring of trace
radioelements in the aquatic ecosystem. Dedicated efforts to monitor uranium (U) have been reported. Among these efforts, the
electroanalytical strategy appears to be one of the most promising

methods because of the low power requirement and the utility of
portable instrumentation. Recently, a 4-carboxyphenyl-grafted SPE
has been reported for sub-nanomolar U(VI) analysis using squarewave voltammetry [145]. This approach increased the electrode
selectivity, and Cd(II), Pb(II) and Zn(II) caused no significant interference. Another sensor for U(VI) detection in aqueous solutions
was based on electrochemically induced, non-modified SPEs, with
a detection limit of 4.5 nmol L1 [146].
4. Concluding remarks and future perspectives
Screen-printed electrodes provide a crucial analytical tool to satisfy the increasing demand for the rapid, sensitive and selective
determination of environmental pollutants. The SPEs can be easily
adapted to detect a wide range of analytes and are inexpensive. In
addition, they can be easily combined with other techniques to fit
particular applications.
In this review, we summarised the published novel designs
of SPEs and their application in environmental analysis over
the past 3 years. Two branches of SPE development are underway: devices with specificity and devices capable of simultaneous
determinations. Various materials used to modify the working system, including nanomaterials, enzymes, and noble metals, were
discussed. Moreover, the changeable format of SPEs and screenprinted electrode arrays can be applied for the simultaneous
detection of environmental pollutants. Certain hybrid techniques
based on SPEs are introduced herein for more sensitive and rapid
determinations.
Considerable selective and sensitive SPEs have already been
developed for environmental analysis, which provides a variety of
tools that may be utilised for in situ determinations. This review
may provide the appropriate background for the development of
novel analytical tools for the determination of environment pollutants. The field of SPEs, however, continues to grow and find
new areas of application. We believe that this field will focus
more on unique materials and multiple analytical methods over
the coming years. Furthermore, miniaturisation via microchip format may decrease the analysis time, sample volumes and reagent
consumption and enhance portability for in situ determinations.
Miniaturisation will force researchers to solve problems associated
with integrated, small devices and multichannel readout devices.
Acknowledgement
This research was supported by the National Science Fund for
Distinguished Young Scholars (no. 21125522), the Natural Science Foundation of China (grant no. 21007015), the Fundamental
Research Funds for the Central Universities (no. WK1013002) and
the Open Project Program of the State Key Laboratory of Chemical
Engineering (ECUST, SKL-ChE-11C01).
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Analytica Chimica Acta 734 (2012) 3144

Contents lists available at SciVerse ScienceDirect

Analytica Chimica Acta

Recent developments and applications of screen-printed electrodes in

! Screen-printed electrodes (SPEs) are

M. Li et al. / Analytica Chimica Acta 734 (2012) 3144

Meng Li received the B.S. degree in 2010 from East

Yuan-Ting Li received the B.S. degree in 2009 from

Da-Wei Li received the Ph.D. degree in environmental

M. Li et al. / Analytica Chimica Acta 734 (2012) 3144

In addition, the surface of SPEs can be easily modified to fit multiple

overall catalytic performance and play a dominating role as ele

M. Li et al. / Analytica Chimica Acta 734 (2012) 3144

or laser-drilled through the four carbon pads to create four well

M. Li et al. / Analytica Chimica Acta 734 (2012) 3144

on the advantages of SPEs have been fabricated and are feasible f

3.2.1. Phenolic compounds

M. Li et al. / Analytica Chimica Acta 734 (2012) 3144

acid, succinimidyl ester (PASE) functional graphene oxide (GO)

M. Li et al. / Analytica Chimica Acta 734 (2012) 3144

AChE-based Prussian Blue/SPE

cobalt-phthalocyanine (CoPC) [64] and conductive polymer [60]

However, the immunoassay procedure faces some drawbac

3.2.4. Polyaromatic hydrocarbons

M. Li et al. / Analytica Chimica Acta 734 (2012) 3144

Fig. 4. A sketch of the biosensor setup based on a screen-printed electrode, a

the use of various antibodies within a single sensor to produce

Fig. 5. (a) Schematic representation of a disposable screen-printed array based

3.2.5. Antibiotic residues

Reprinted with permission from Ref. [75].

3.3. Heavy metals

M. Li et al. / Analytica Chimica Acta 734 (2012) 3144

Potential (vs. Ag/AgCl)

ex situ deposited Hg (5 !g)

Ultra pure water

0.4 V (vs. SCE)

Pb(II), Cd(II), Zn(II)

Pb(II), Cd(II), Cu(II)

a 3-electrode system for detection. Therefore, a screen-printed

M. Li et al. / Analytica Chimica Acta 734 (2012) 3144

caused by amalgam formation. For this reason, time-consuming

M. Li et al. / Analytica Chimica Acta 734 (2012) 3144

The normal Au-film-coated SPEs displayed excellent linear

Another CO sensor was based on the deposition of Pt nanopar

3.4.2. Nitrogen oxide

3.4.3. Volatile organic compounds

M. Li et al. / Analytica Chimica Acta 734 (2012) 3144

electroanalytical strategy appears to be one of the most promising

M. Li et al. / Analytica Chimica Acta 734 (2012) 3144

[48] M.D. Fusco, C. Tortolini, D. Deriu, F. Mazzei, Talanta 81 (2010) 235240.

M. Li et al. / Analytica Chimica Acta 734 (2012) 3144

[123] C. Parat, S. Betelu, L. Authier, M. Potin-Gautier, Anal. Chim. Acta 14 (2006)

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