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2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim wileyonlinelibrary.com (1 of 6) 1605744
Lactate Detection in Tumor Cell Cultures Using Organic
Transistor Circuits
Marcel Braendlein, Anna-Maria Pappa, Marc Ferro, Alexia Lopresti, Claire Acquaviva,
Emilie Mamessier, George G. Malliaras, and Róisín M. Owens*
M. Braendlein, A.-M. Pappa, M. Ferro,
Prof. G. G. Malliaras, Prof. R. M. Owens
Department of Bioelectronics
Ecole Nationale Supérieure des Mines
CMP-EMSE, MOC
Gardanne 13541, France
E-mail: owens@emse.fr
A. Lopresti, Dr. C. Acquaviva, Dr. E. Mamessier
INSERM U1068
Institut Paoli-Calmettes
CRCM, CNRS
Aix Marseille Université
Marseille 13009, France
DOI: 10.1002/adma.201605744
However, some key issues still impede their practical imple-
mentation in a clinical setting. These issues include signal drift
due to environmental changes (e.g., electrolyte evaporation,
temperature changes, instability of transducer), as well as signal
misinterpretation due to interference (e.g., charged species or
oxidizable compounds in complex media).
[13]
Sensor circuits
represent an elegant alternative solution, departing from a
single sensor and focusing on a more complete system that can
be readily intercepted with simple acquisition tools, as demon-
strated by Svensson et al.
[14]
Recently, the organic electrochemical transistor (OECT) has
drawn considerable attention as a sensing element.
[15–17]
In a
three-terminal configuration, the active material, being com-
prised of an organic semiconductor, can be electrochemically
doped or dedoped through an ionic current from the electro-
lyte into the polymer, thereby changing its conductivity.
[18]
The possibility for low voltage gating provides devices sen-
sitive to biological signals that may consist of minute ionic
currents.
[19]
OECTs have proven to outperform state-of-the-
art devices such as electrodes,
[20]
and have been used in a
wide variety of biological applications, including metabolite
sensing.
[21–23]
Bearing in mind the complex issues related to sensitive and
specific detection of metabolites of interest in pathologies such
as cancer, in this article, we present an in vitro electronic plat-
form for sensitive and accurate metabolite sensing in highly
interfering samples, such as cell culture media. In particular,
we developed a reference-based sensor circuit, by integrating
two differently functionalized OECTs, comprised of the well-
known organic p-type semiconductor poly(3,4-ethylenedioxythi-
ophene):poly(styrene sulfonate) (PEDOT:PSS),
[24]
into a Wheat-
stone bridge layout. The planar all-PEDOT:PSS configuration of
the channel and the gate (Figure 1a) facilitates the device bio-
functionalization
[23]
and also allows for future integration with
microfluidics. For the device fabrication, a new lithographic
approach based on a fluorinated photoresist, that allows for
direct patterning of spun-cast PEDOT:PSS, was employed in
this work (Figure S1, Supporting Information). Starting from
a homogeneously coated PEDOT:PSS film and ablatively pat-
terning the active areas,
[25,26]
a greater device homogeneity can
be achieved (Figure 1b and Figure S2c, Supporting Informa-
tion), contrary to the conventional Parylene-C peel-off tech-
nique.
[27]
According to the output and transfer characteristics
of the OECTs (Figure S2a,b, Supporting Information), the max-
imum transconductance
[28]
g
m
= ΔI
D
/ΔV
GS
of 6.4 mS is obtained
at V
GS
= 200 mV, which coincides with the sensor’s working
potential, to ensure maximum sensitivity. By adding a drain
load resistor in series with the OECT, a floating voltage point
Rapid and early diagnosis of disease is known to be a significant
factor in treatment and improved prognosis, notably in cancer.
From the first commercialized device based on the “enzyme
electrode,” introduced by Clark and Lyons, able to measure
accurately glucose concentrations in whole blood samples,
[1,2]
to research prototypes of miniaturized epidermal sensor chips
able to measure real-time multiple analytes,
[3]
biosensors have
evolved significantly and become invaluable tools for diag-
nosis of many pathologies from infections to heart disease.
Remarkably, little of the progress in the field of biosensing has
translated to improved diagnosis of cancer.
[4]
Use of biosensors in diagnostic applications requires iden-
tification of a biomarker (to confer specificity) while the sen-
sitivity is mostly related to the intimate coupling of a reaction
involving the biomarker with a transducer. In cancer diag-
nostics, clinicians are highly dependent on the identification
of biomarkers that will reliably predict occurrence and recur-
rence of cancerous cell populations, however such reliable bio-
markers are few and far between, perhaps explaining the dearth
of cancer biosensing devices.
[5,6]
One marked feature of cancer
however, is the increased glycolytic activity associated with
highly proliferative aggressive cell growth.
[7]
In recent years,
increased metabolic activity has been suggested as a biomarker
for cancer. This idea is not new, having been introduced over
60 years ago by Warburg, who predicted enhanced uptake and
usage of glucose and thus production of lactate.
[8]
Lactate has
proven to be a prognostic indicator of the degree of malignancy
in primary tumors as well as of the probability of metastasis.
[9]
Electrical, label-free biosensing of metabolites such as glucose
and lactate is known to be advantageous with regards to speed
and sensitivity, and indeed the integration of biosensors with
microelectronic devices has brought about multiplexed capabili-
ties as well as enabling miniaturization and automation.
[10–12]
Adv. Mater. 2017, 29, 1605744
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