Available online at www.sciencedirect.
com Current Opinion in
ScienceDirect
Review Article
Recent advances in voltammetric, amperometric and
ion-selective (bio)sensors fabricated by
microengineering manufacturing approaches
Christos Kokkinos and Anastasios Economou
Summary
Over the last few years, microengineering fabrication ap-
proaches, originating from the semiconductor manufacturing
technology, have been increasingly used for the development
of electrochemical (bio)sensors and analytical devices. The
application of various microengineering technologies en-
ables the rapid mass fabrication of low-cost and disposable
sensors of small size with uniform and strictly controlled
geometry and surface properties and provides wide scope for
device miniaturization and integration. This work will focus on
the latest developments of microfabricated voltammetric,
amperometric and ion-selective sensors with representative
applications to organic/gas analysis, ion detection, bio-
sensing/wearable devices and electrochemical imaging/in-
vivo sensing.
Addresses
Laboratory of Analytical Chemistry, Department of Chemistry, National
and Kapodistrian University of Athens, 157 71, Athens, Greece
Corresponding author: Economou Anastasios (aeconomo@chem.
uoa.gr)
Current Opinion in Electrochemistry 2020, 23:21–25
This review comes from a themed issue on Sensors and Biosensors
Edited by Zbigniew Stojek
For a complete overview see the Issue and the Editorial
Available online 2 March 2020
https://doi.org/10.1016/j.coelec.2020.02.020
2451-9103/© 2020 Published by Elsevier B.V.
Keywords
Microengineering, Microfabrication, Electrochemical sensors, Elec-
trodes, Ion-selective sensors, Voltammetry, Lithography, Electro-
chemical imaging, Trace metal analysis, In-vivo analysis, Biosensors.
Introduction
Nowadays, standard microengineering thinefilm pro-
cesses, borrowed from the semiconductor and inte-
grated circuit manufacturing industry, are increasingly
being used to fabricate chemical sensors, biosensors
and integrated analytical devices. Key advantages of
(bio)sensors and devices fabricated by means of
microengineering-based approaches include [1,2]:
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Electrochemistry
i) Amenability to batch processing (i.e. the fabrication
of many devices in parallel), a practice which ac-
celerates the manufacturing output rate and reduces
the manufacturing cost.
ii) High reproducibility in the sensors’ dimensions,
properties and performance, a direct consequence of
the strict control of the fabrication process.
iii) Potential for size reduction, thereby minimizing the
sample volume.
iv) Flexibility in the selection of the geometrical char-
acteristics and dimensions of the sensors.
v) Scope for on-chip integration of several components
(several sensors, electronics etc.) and various
detection approaches in lab-on-a-chip devices.
vi) Possibility to improve the sensors’ characteristics or
to add new functionalities by chemical or physical
modification.
On the other hand, the drawbacks of the micro-
engineering processes for the fabrication of (bio)sensors
are related to the requirements for specific masks for
lithography, for specialized equipment and for access to
special laboratory facilities. As a result, the
manufacturing cost of limited-production prototypes is
relatively high when compared to alternative sensor
fabrication technologies (e.g. screen-printing). Howev-
er, the production cost is significantly reduced when
mass-production of these devices is envisaged, so that
the realization of single-use disposable or semi-
disposable sensors at a reasonable cost is feasible.
Although there are countless variations in the fabrication
processes depending on the sensor requirements,
configuration and availability of equipment, a typical
sequence for the microfabrication of a (bio)sensor con-
sists of four main steps [1,2]:
i) Deposition: typically, a thin layer of the appropriate
conductive electrode material is deposited on an
insulating substrate using chemical vapor deposition
or physical vapor deposition approaches.
ii) Patterning: a light-sensitive photoresist layer is then
deposited on top of the conductive material and
patterned, commonly using photolithography.
Current Opinion in Electrochemistry 2020, 23:21–25
22 Sensors and biosensors
iii) Etching: the pattern is transferred from the photo-
resist layer to the conductive film by an etching or
lift-off process. Additional conductive layers (elec-
trodes) can be deposited and structured by
repeating the processes (i)-(iii) as required.
iv) Insulation: finally, an insulating material is depos-
ited on top of the patterned conductive film.
This review will focus on the development of voltam-
metric, amperometric and ion-selective (bio)sensors
microfabricated using integrated circuit manufacturing
approaches with emphasis on recent applications to
organic/gas analysis, ion detection, biosensors/wearable
devices and electrochemical imaging/in-vivo sensing.
Organic and gas analysis
Several microfabricated electrochemical sensors have
been reported in the literature for the detection and
quantitation of the important neurotransmitter dopa-
mine using: microengineered 3D carbon electrodes with
nanoporous sponge-like networks decorated with gold
particles with dendritic nanostructures [3]; a three-
electrode chip with a working electrode consisting of
three-dimensional suspended pyrolytic carbon micro-
electrodes [4]; interdigitated electrodes with dense
carbon nanotube forests [5]; a cylindrical Au nano-
electrode array [6]; and an array of recessed Au nano-
electrodes, which allows simultaneous voltammetric
detection of dopamine ascorbic acid and uric acid [7].
Other noteworthy applications of microengineered
sensors to organic analysis and bioanalysis include the
following: a three-in-one boron-doped diamond sensor
for the detection of isatin [8]; three-electrode sensors
with a flexible and highly ordered Au or Ag nanopillar
array working electrode for the detection of DNA of
foodborne pathogens [9]; a flexible microfluidic on-chip
electrochemical cell to monitor the adhesion of murine
3T3 fibroblasts [10]; and a non-enzymatic flexible field-
effect transistor (FET) glucose sensor using NiO
quantum dots-modified ZnO nanorods [11].
Another interesting application area, to which micro-
fabrication technologies are well suited, is the devel-
opment of miniaturized Clark-type oxygen sensors.
Representative examples include a batch three-elec-
trode oxygen monitor [12] and a microfluidic device
coupled to an oxygen macroelectrode to measure the
bactericidal activity of cells [13].
Ion detection
Heavy metals and semi-metals [Hg(II), Pb(II), As(III),
Cu(II), Cd(II), Ni(II), Co(II)] can be quantified pre-
dominantly by stripping analysis. There are several re-
ports of single working electrodes manufactured via
thin-film approaches for trace metal analysis: an Au-
Current Opinion in Electrochemistry 2020, 23:21–25
film electrode for the determination of Pb(II), As(III)
and Hg(II) by anodic stripping voltammetry (ASV) [14];
an indium tin oxide (ITO) electrode for the determi-
nation of Mn(II) by cathodic stripping voltamme-
try [15]; an Au nanoring electrode patterned on an Si
micropillar for the determination of Pb(II) by ASV [16];
a flow-through cell incorporating a microfabricated Au
working electrode for the determination of As(III) by
stripping coulometry [17]; and boron-doped diamond
film electrodes for ASV detection of Zn(II), Cd(II) and
Pb(II) after in situ Bi deposition [18].
Microelectrode arrays can be readily fabricated by
microengineering approaches and possess distinct ad-
vantages over macroelectrodes and single microelec-
trodes such as improved S/N ratios, enhanced mass-
transfer and lower iR drop. Examples include an Au
microelectrode array for the ultrasensitive detection of
As(III) by ASV [19] as well as a sputtered Bi micro-
electrode array applied to the detection of Co(II) by
adsorptive stripping voltammetry [20].
Different types of disposable integrated three-electrode
cell-on-a-chip devices have been reported that are
particularly suitable for on-site monitoring of several
heavy metals and As using different types of working
electrodes such as Au/reduced graphene oxide/carbon
nanotubes in situ plated with Bi [21], a micropillar array
plated in situ with Bi [22] and sputtered Bi [23], Cu [24]
and Au [25] electrodes.
Microfabrication technologies have also found their way
into paper-based devices [as demonstrated by an inte-
grated paper-based device with a sputtered Sn-film
electrode for the voltammetric determination of
Cd(II) and Zn(II) [26]] as well as fluidic devices [27].
In addition, different microfabricated ion-selective de-
vices have been reported based on ion-selective mem-
branes or FET operation principles. Potentiometric
microengineered sensors include a pH sensor for bio-
fluids based on a CeTixOy sensing membrane [28], a
disposable Naþ-sensing microfabricated device [29], an
Si nanowire FET for pH measurements [30], a solution-
gated graphene transistor device for measuring Cl
concentration in water [31], a lab-on-a-chip platform for
potentiometric NHþ 4 detection in sewage water [32]
and an on-chip ion-selective electrode array for multi-
plex detection of heavy metals [Pb(II), Cd(II), As(V)
and Hg(II)] [33].
Biosensing and wearable devices
Enzymatic biosensors using thin-layer approaches have
been developed mainly for glucose sensing after modi-
fication with glucose oxidase. Typical examples are a
carbon interdigitated nanoelectrode array decorated
with Au nanoparticles for amperometric enzymatic
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 Microfabricated voltammetric, amperometric and ion-selective (bio)sensors Kokkinos and Economou
redox-cycling detection [34], a miniaturized glucose
biosensor consisting of an Au-carbon quantum dots-Au
nanoparticles microelectrode array [35] and a glucose
monitor with conducting micropillar polymer patterns
[36]. Finally, Gao et al. [37] have reported a flexible
microneedle electrode array-based biosensor for the
simultaneous enzymatic detection of glucose, uric
acid and cholesterol.
Various types of DNA biosensors manufactured by
microengineering approaches have been also described.
Representative examples are a miniaturized electro-
chemical platform for the label-free detection of DNA
hybridization with an Au nanoparticle-modified working
electrode [38] and an electrochemical paper-based
device for the determination of DNA via ASV detec-
tion of Cd(II) released from CdSe quantum dot labels at
an Sn-film working electrode [39].
Microfabricated immunosensors have also found wide-
spread applicability for protein assays: a portable mini-
aturized device with a three Au-electrode system was
developed for the aptamer-based detection of ochra-
toxin A [40]; three-Pt electrode cells were used for the
detection of Salmonella after modification of the working
electrode with ZnO nanorods and functionalization with
Salmonella antibodies [41]; a multiplexed miniaturized
microfluidic biosensor was developed to simultaneously
detect four pulmonary hypertension biomarkers [42].
Finally, an electrochemical redox cycling-based immu-
nosensor was developed for cardiac myoglobin sensing
based on a 3D sub-micrometer-sized mesh suspended
above an interdigitated nanoelectrode array [43].
Over the last years, wearable devices are increasingly
gaining the attention of the scientific community for (bio)
chemical and physiological on-line monitoring directly on
the body and various microfabrication technologies are
exploited for this purpose. For example, the development
of flexible and fully integrated microfabricated sensor
arrays for on-body simultaneous monitoring of pH and
electrolytes (Naþ, Kþ, Cl) [44] and multiplexed in situ
perspiration monitoring of sweat metabolites (glucose,
lactate) and Naþ, Kþ [45] have been reported. In
addition, a wound dressing system was implemented
based on flexible pH sensors that can monitor the infec-
tion of a wounded area by tracking its pH value [46].
Electrochemical imaging/in-vivo
electroanalysis
The detection of the release of oxidizable neurotrans-
mitters from single vesicles and single cells using elec-
trochemical microfabricated devices and microchips
offers the possibility of probing exocytosis with subcel-
lular spatial resolution.
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23
Large-scale integration (LSI)-based amperometric de-
vices have been recently described for duplex differen-
tial electrochemical imaging [47] and for monitoring the
activity of enzymes in cells and the respiration activity
of cells [48,49]. In addition, microfabricated LSI devices
[50], diamond-based multi-electrode arrays [51] and
movable thin-film microelectrode array probes [52] have
been developed for one-dimensional and two-
dimensional electrochemical imaging of single exocy-
tosis events related to neurotransmitters release with
high spatiotemporal resolution.
Measurement of oxygen consumption of isolated cells
has been demonstrated using microfabricated devices.
Chips composed of microwell arrays integrating
nanoelectrodes were developed to achieve dual optical
and electrochemical detection on isolated mitochondria
via monitoring of oxygen consumption [53] and a device
to measure single-cell oxygen consumption rate has
been demonstrated for cell metabolism evaluation [54].
In addition, a microfabricated on-chip device was pro-
posed enabling the noninvasive measurement of oxygen
consumption rates of single embryos [55].
Finally, Ribet et al. [56] have proposed a continuous
glucose monitoring sensing system, for in-situ sensing in
the dermal interstitial fluid; the device is based on the
integration of an ultraminiaturized, three-electrode
electrochemical enzymatic sensing probe in the lumen
of a single hollow microneedle.
Conclusions and outlook
Microengineering technologies, adopted from the
semiconductor manufacturing industry, have found
widespread applications in the fabrication of electro-
chemical (bio)sensors. According to the authors’
opinion, the following areas are expected to have the
highest potential impact in the near future:
i) Disposable three-electrode heavy metal sensors
based on ‘green’ metal films (Bi, Sn, Cu, Au) for on-
site environmental trace analysis in conjunction
with ASV detection.
ii) Integrated microengineered electrochemical cells,
combined with microfluidic devices, enabling
convenient sample introduction for monitoring of
oxygen concentration, environmental analysis and
bioanalysis.
iii) Microfabricated electrochemical sensors for multi-
plexed enzymatic, DNA and protein assays as well as
for monitoring vital electrolytes, with particular
emphasis on wearable devices.
iv) LSI-based devices and electrode arrays for electro-
chemical imaging and amperometric real-time
evaluation of the quantal release of neurotransmit-
ters from single cells.
Current Opinion in Electrochemistry 2020, 23:21–25
24 Sensors and biosensors
Conflict of interest statement
Nothing declared.
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