177
Original scientific paper
Journal of Microelectronics, 
Electronic Components and Materials
Vol. 54, No. 3(2024), 177 – 186
https://doi.org/10.33180/InfMIDEM2024.302
Aerosol-Deposition-Derived Graphite Thick Films 
for Electrochemical Sensors 
Matej Šadl
1+
, Barbara Repič
1,2,+
, Ivana Goričan
1,2
, Danjela Kuščer
1,2
 and Hana Uršič
1,2
1
Electronic Ceramics Department, Jožef Stefan Institute, Ljubljana, Slovenia
2
Jožef Stefan International Postgraduate School, Ljubljana, Slovenia
+
M.Š. and B.R. contributed equally
Abstract: Disposable electrochemical (EC) sensors are usually manufactured by screen printing and post-deposition temperature 
curing of the sensor’s components. However, complete removal of an organic vehicle requires curing at temperatures of a few 
hundred °C, which can lead to electrode-substrate incompatibilities and limit the choice of material. In this work, graphite thick-film 
electrodes without additives were deposited on polyimide substrates at room temperature using the aerosol-deposition method. 
The resulting thick films had good adhesion, a defect-free surface, a thickness of a few micrometers, a root-mean-square roughness of 
0.68 μm and sheet resistance of 27 Ω/sq. Scanning electron microscopy of the film surface revealed good particle compaction, while 
the X-ray diffraction analysis showed no peak broadening of the graphite thick films, which indicates a different deposition mechanism 
than that normally observed for ceramic powders. The EC properties of the graphite working electrodes were evaluated using cyclic 
voltammetry. The graphite films showed a low capacitive current of 0.114 mA, good reversibility of the redox process, a high EC active 
surface area of 1.44 cm
2
/cm
geo
2
 and a standard heterogeneous electron-transfer-rate constant of 0.0019 cm·s
–1
. The aerosol-deposited 
graphite thick-film electrodes show potential for the EC detection of a broad range of chemicals.
Keywords: graphite electrode; electrochemical detection; aerosol deposition; room-temperature process; polyimide foil
Debele plasti grafita nanešene v aerosolu za 
elektrokemijske senzorje
Izvleček: Elektrokemijski (EK) senzorji za enkratno uporabo se običajno izdelujejo tako, da komponente senzorja natisnemo s 
sitotiskom ter jih nato temperaturno obdelamo. Za popolno odstranitev organskega nosilca je plasti potrebno segreti do nekaj sto °C, 
kar lahko privede do nezdružljivosti med elektrodo in podlago ter omeji izbiro materiala. V tej raziskavi smo z metodo nanosa plasti 
v aerosolu pri sobni temperaturi pripravili debeloplastne grafitne elektrode brez dodatkov na poliimidne podlage. Tako pripravljene 
debele plasti se dobro držijo podlage, imajo površino brez vidnih defektov, debelino nekaj mikrometrov, hrapavost 0.68 μm in plastno 
upornost 27 Ω/sq. Z vrstično elektronsko mikroskopijo smo na površini plasti opazili kompaktno strukturo delcev. Pri rentgenski 
difrakciji debelih plasti grafita ne zaznamo širitve vrhov, kar nakazuje, da je mehanizem nanašanja pri grafitu drugačen kot je običajno 
za keramični prah. EK lastnosti grafitnih delovnih elektrod smo analizirali s ciklično voltametrijo. Grafitne plasti izkazujejo nizek 
kapacitivni tok z vrednostjo 0.114 mA, dobro reverzibilnost redoks procesa, veliko EK aktivno površino z vrednostjo 1.44 cm
2
/cm
geo
2
 in 
visok standardni koeficient heterogene reakcije z vrednostjo 0.0019 cm·s
–1
. Debeloplastne grafitne elektrode pripravljene z metodo 
nanosa plasti v aerosolu so primerne za EK detekcijo številnih kemikalij. 
Ključne besede: grafitna elektroda; elektrokemijska detekcija; metoda nanašanja plasti v aerosolu; priprava pri sobni temperaturi; 
poliimidna folija
* Corresponding Author’s e-mail: hana.ursic@ijs.si, danjela.kuscer@ijs.si
How to cite:
M. Šadl et al., “Aerosol-Deposition-Derived Graphite Thick Films for Electrochemical Sensors", Inf. Midem-J. Microelectron. Electron. Com-
pon. Mater., Vol. 54, No. 3(2024), pp. 177–186
1 Introduction
The amount of research on electrochemical (EC) sen-
sors is increasing owing to the requirement for the 
point-of-care and on-site detection of various com-
pounds such as pharmaceuticals, pesticides, toxins and 
heavy metals [1]–[8]. These are widely utilized in agri-

178
culture and the food industries as well as in environ-
mental and biomedical applications. The applications 
for disposable EC sensors dictate many requirements: 
good selectivity and sensitivity for a broad range of EC 
active species, reproducibility of the results, miniature 
and portable systems, ease of use and cost-effective 
production with easy scale-up possibilities [8]–[11]. 
The EC sensors consist of three electrodes, i.e., the 
counter, reference and working electrode (WE). In 
disposable EC sensors the electrodes are integrated 
on selected substrates, commonly by screen print-
ing and the subsequent firing of the deposited layers 
at elevated temperatures. The WE is a key component 
and should have high electrical conductivity and a high 
specific surface area.
Screen printing is the most commonly used method 
for depositing films that are typically a few tens of μm 
thick. It is a mature, commercially available technology, 
which offers patterning of the structures with good re-
producibility on laboratory and industrial scales [11]–
[14].
Although the screen-printing method is widely adopt-
ed, there are some challenges that need to be consid-
ered. In printing techniques, the ink or paste consists of 
a solid material dispersed in an organic vehicle. To ob-
tain good functional properties of the thick film, the or-
ganic vehicle must be removed during the processing. 
To remove the organic vehicle and to densify the thick 
film, a temperature of a few hundred °C is needed [14], 
[15]. Due to the degradation of carbon in air, annealing 
at higher temperatures requires an inert atmosphere 
[16]. However, high-temperature curing can lead to 
electrode-substrate incompatibilities, which signifi-
cantly limit the choice of substrate materials. To avoid 
this shortcoming, the EC active materials should be de-
posited at low temperature and without additives.
The aerosol deposition (AD) method, sometimes 
known as powder aerosol deposition, enables the di-
rect deposition of functional materials in the form of 
micrometre-sized dry powders without the use of ad-
ditives [17]. The deposition mechanism is based on 
the impact of the particles, and the film’s consolida-
tion occurs at room temperature, due to the high ki-
netic energy of the sprayed particles [18]–[21]. AD is a 
room-temperature process that enables the integra-
tion of functional materials on low-melting point and 
flexible substrates [22]–[25]. As a result, AD offers good 
material compatibility. It is generally used for the depo-
sition of ceramic films, but metals can also be depos-
ited. However, research on metal deposition is still in 
its beginnings. So far, the following materials have been 
deposited using AD: Cu [26], [27], Ag [28], [29], Al [30], 
M. Šadl et al.; Informacije Midem, Vol. 54, No. 3(2024), 177 – 186
[31], Fe [32] Fe-based amorphous alloys [33], (Bi,Sb)
2
Te
3
 
[34], [35], rare-earth magnets [36], [37] and graphite [38].
Carbon-based materials are commonly used as the WE 
in EC sensors. They are non-toxic, low-cost, have high 
electrical conductivity and allow the detection of vari-
ous compounds such as pharmaceuticals, pesticides, 
toxins and heavy metals [39]–[43].
In this study we processed a-few-μm-thick graphite 
films on a polyimide substrate by AD at room tem-
perature and without any post-deposition curing. The 
graphite thick films were structurally and microstruc-
turally characterized using contact profilometry, X-ray 
diffraction, atomic force microscopy and scanning 
electron microscopy. Their EC properties were investi-
gated by cyclic voltammetry. The purpose was to study 
the properties of graphite thick films prepared by a 
relatively new AD method and to assess the suitability 
of the aerosol-deposited thick films for use in EC ap-
plications.
2 Materials and methods
A commercially available graphite powder (graphite 
flake, 99.8 %, 043209, Alfa Aesar) was sieved through 
a mesh (with 80-μm openings) and vacuum dried at 
80 °C, before being aerosol deposited (AD) onto the 
substrate. A commercially available polyimide (PI) 
foil (Kapton HN, DuPont, DE, USA) with a thickness of 
125 μm was used as a substrate. The AD equipment 
was provided by InVerTech, Germany. A schematic of 
the AD setup is shown in [44]. During the AD the pro-
cess parameters (Table 1) were kept constant. After the 
film’s deposition the thick-film samples were cleaned 
by gently blowing them with air.
Table 1: Process parameters used during the AD.
Process parameter Value
Pressure in the deposition chamber 90 mbar
Pressure in aerosol chamber 0.6 mbar
Nozzle geometry (slit size) (0.5 ∙ 10) mm
2
Carrier gas species N
2
Gas flow rate 1 L·min
−1
Distance between nozzle 
and substrate
5 mm
Sweep speed 5 mm·s
−1
The particle size distribution of the initial graphite 
powder was determined in isopropanol using a light-
scattering laser granulometer (S3500, Microtrac, PA, 
USA). 

179
The X-ray diffraction (XRD) analysis was performed 
with a benchtop X-ray diffractometer (MiniFlex 600-C, 
Rigaku, Japan) using Cu-K
α
 radiation. Diffraction pat-
terns were recorded in the Bragg–Brentano geom-
etry using a silicon strip detector (D/teX Ultra) in a 2θ 
range of 10°–60° with a step of 0.01° and 0.06 s/step. 
The software X’Pert HighScore Plus 3.0e (PANalytical, 
Almelo, The Netherlands) was used to analyse the XRD 
patterns and strip the Cu-K
α2
 component.
The microstructures of the graphite powder and the 
surface of th graphite thick films were analysed using a 
field-emission scanning electron microscope (FE-SEM, 
JSM 7600F , Jeol, Japan), equipped with secondary elec-
tron and backscattered electron detectors. Before the 
analysis, the graphite powder was spread on the car-
bon tape.
The topography of the graphite thick films was ana-
lysed using contact stylus profilometry (DektakXT, 
Bruker, MA, USA) and atomic force microscopy (AFM, 
MFP-3D, Asylum Research, CA, USA). The thickness and 
root-mean-square surface roughness (R
q
) of the thick 
films were evaluated from a line profile measured with 
a contact profilometer using the software Vision64 
(Bruker, MA, USA). The thickness was evaluated from 
the step height of the film after curvature removal us-
ing a quadratic polynomial. R
q
 was evaluated from the 
2-mm roughness profile (length of 2 mm) obtained af-
ter filtering the total profile using Gaussian regression 
(cut off 0.8 mm). In the AFM analysis a Si tip on a Si/Al 
cantilever with a diameter of ~7 nm (AC240TSR3, Asy-
lum Research, CA, USA) was used for scanning in AC to-
pography mode. The root-mean-square surface rough-
ness R
q
AFM
 was also evaluated from the AFM map scans 
(with dimensions 80 μm x 80 μm).
The sheet resistance (R
s
) of the thick films was meas-
ured using the four-point probe technique, with the 
probes arranged equidistantly in a line. The R
s
 of the 
thick film was calculated from the measured voltage 
drop between the two inner probes and the current. A 
correction factor of 0.795 was used [45].
EC experiments were performed using a potentiostat-
galvanostat (Multi Autolab M 204, Methrom, The Neth-
erlands) controlled by Nova 2.1.5 software. A conven-
tional three-electrode cell configuration was used. The 
graphite thick films processed by AD were used as the 
WE, together with a conventional Ag/AgCl reference 
electrode and a platinum-sheet counter electrode 
(both from Methrom). The measurements were carried 
out in deaerated solutions at 25 °C. Cyclic voltammo-
grams were measured between –0.2 V and 0.6 V at a 
constant scan rate ( ν) of 20, 50, 100, 200 and 500 mV·s
–1
. 
The measurements were performed in a 0.1-M phos-
phate buffer solution (PBS) used as an electrolyte and 
in a 0.005-M equimolar solution of Fe(CN)
6
3-/4- 
(HCF) as 
a redox probe dissolved in the PBS. The voltammo-
grams measured at 100 mV·s
–1
 were characterized to 
determine the capacitive current (i
cap
) in the PBS, the 
peak-to-peak separation ( ∆E
pp
) and the cathodic-to-
anodic peak current ratio (i
pc
/i
pa
) in HCF . From the meas-
urements at different scan rates, the electrochemically 
active surface area was determined from the slope of 
the linear dependence of the peak current as a function 
of the square root of the scan rate using the Randles-
Ševćik equation. It was normalised using the geomet-
ric surface area to obtain a real electrochemically active 
surface area (A
ecsa
) [9]. Cyclic voltammograms recorded 
at different scan rates were also used to determine a 
standard heterogeneous electron-transfer-rate con-
stant (k
0
) using the Nicholson method [46], in which the 
k
0
 of a quasi-reversible reaction is related to a dimen-
sionless kinetic parameter (Ψ), calculated as a function 
of ∆E
pp
 at different scan rates. The electrodes were also 
used to determine operating potential window (OPW), 
which was assessed based on the qualitative inspec-
tion of a series of cyclic voltammograms, obtained by 
incrementally increasing or decreasing the vertex po-
tential of the sweep range in 0.05-V increments. The 
limits of the OPW are identified as the potential at 
which the current intensity was in the same range as 
the peak current of the redox probe.
The mechanical stability of the graphite thick films was 
additionally tested by immersing and rinsing them in 
organic solvents, i.e., methanol, ethanol and acetone.
3 Results
The graphite powder, which resulted in few-microme-
ter-thick films, was analysed using laser granulometry 
and SEM. The volumetric particle size distribution of 
the graphite powder measured by laser granulometry 
is shown in Figure 1(a). The distribution is monomod-
al with the particle size ranging between 1.6 μm and 
148 μm. The median (d
50
) particle size is 16.6 μm, rep-
resented by an orange vertical line. For the successful 
AD of ceramics, the typically reported particle size is 
between 0.2 μm and 2 μm [18]. Also for the AD of met-
als, the particle size window for a successful deposition 
is between 1 μm and 10 μm [30], [47]. However, in our 
case the AD of graphite powder was successful using 
much larger particles than typically used in AD. In the 
literature, there are not many reports that show a suc-
cessful AD using particles with d
50
 larger than 10 μm. 
These cases are limited to Nd-Fe-B magnets [37], MAX 
phase materials [48] and glass [49].
M. Šadl et al.; Informacije Midem, Vol. 54, No. 3(2024), 177 – 186

180
The SEM micrographs, taken with a secondary-elec-
tron detector in Figure 1(b, c), reveal the morphology 
of the graphite powder. Figure 1(b) shows large, ag-
glomerated particles with round-shaped surfaces. The 
agglomerates exceed 40  μm in diameter (red dashed 
circle). The agglomeration is in agreement with the la-
ser granulometry data (Figure 1(a)). On the other hand, 
Figure 1(c) shows particles that have an irregular shape, 
including plate-like surfaces that indicate the easy 
cleavage of the graphite flake-type particles. The small-
est particles are of the order of 1 μm.
The AD of the graphite powder on a PI substrate was 
successful, resulting in good adhesion of the film to 
the substrate and defect-free appearance of the film’s 
surface, as seen in Figure 2(a). A line scan across the de-
posited film is shown in Figure 2(b) and reveals an even 
film thickness of 4.4 μm. The root-mean-square rough-
ness (R
q
) reaches 0.68  μm, which is at least 3-times 
higher than reported for Al
2
O
3
 films and ceramic-metal 
(Al
2
O
3
-Al) multilayered thick films prepared by AD [18], 
[30]. A high surface roughness indicates a high specific 
surface area, which is advantageous in EC sensing ap-
plications. Note that after the AD the graphite film is 
still susceptible to abrasion. The sheet resistance (R
s
) of 
27 Ω/sq confirmed sufficient conductivity of the film 
for the EC measurement. The resistance is comparable 
to that of screen-printed conductive carbon films [50].
Figure 2: (a) Photograph of the deposited graphite 
thick film on a PI substrate. The orange line represents 
the position of the line scan. (b) Line profile measured 
by contact profilometry.
The XRD patterns of the graphite powder and depos-
ited thick films are shown in Figure 3. Both powder and 
film contain a graphite phase (PDF 075-2078) [51], with 
the most prominent reflection (002) at 2θ of 26.5°. Note 
that the powder also contains a trace amount of some 
other graphite phase, which overlaps with the (002) re-
flection. After the deposition, the peak position of the 
graphite phase does not change and the peak width 
does not increase. This shows that there is no crystal-
lite size reduction and build-up of microstrain due to 
the impacting particles, which is typically observed in 
the deposition of ceramic thick films [23], [52]. The XRD 
pattern of the graphite film also contains additional 
peaks and an increased background level arising from 
the PI substrate.
Figure 1: Analysis of the graphite powder. (a) Volu-
metric particle size distribution (grey) and cumulative 
curves (blue) evaluated from the laser granulometry. 
The vertical orange line represents the median (d
50
) 
particle size. The d
10
, d
50
 and d
90
 are also displayed in the 
inset table. (b, c) SEM images taken with a secondary-
electron detector. The red dashed circle with diameter 
of 40 μm marks a large agglomerate, while the smallest 
particles, around 1 μm, are marked with yellow arrows.
M. Šadl et al.; Informacije Midem, Vol. 54, No. 3(2024), 177 – 186

181
Figure 3: XRD patterns of the graphite powder (black), 
graphite thick film (blue) and blank PI substrate (or-
ange). (a) XRD patterns in 2θ range 10°–60°, (b) close-up 
view of the region of the most intense graphite peak.
The surface topography of the graphite thick films was 
analysed using AFM (Figure 4) and SEM (Figure 5). Fig-
ure 4(a, b, c) shows the AFM height, deflection and tap-
ping amplitude modes, respectively. The height image 
(Figure 4(a)) shows obvious craters, which contribute to 
the high R
q
AFM
, reaching 0.48 μm. Both the AFM and SEM 
images reveal irregularly shaped particles. An interest-
ing observation is the straight features (yellow arrows 
in Figure 4 and Figure 5(b)) that resemble sharp-edged 
particles, which indicates the flake-like nature of the 
deposited graphite film. From the SEM surface view, 
good particle compaction can be observed. In particu-
lar, the SEM image taken with a backscattered-electron 
detector (Figure 5(b)) reveals no clear pores or voids 
between the deposited particles. The backscattered-
electron detector is very appropriate for evaluating the 
film’s homogeneity as it gives a high contrast between 
the compact and porous regions.
An EC analysis of the graphite thick-film WE was made 
by cyclic voltammetry (Figure 6). The voltammogram 
measured in the PBS shows a low background with 
an i
cap
 of 0.114 mA, determined as the difference be-
tween cathodic and anodic currents at 0.2 V. For the 
characterization of the voltammogram recorded in 
HCF, we determined the anodic (i
pa
) and cathodic peak 
currents (i
pc
), which were corrected with capacitive 
currents measured in the PBS at the same potentials. 
The currents observed in both the PBS and HCF are 
higher than those observed for commercially available, 
screen-printed electrodes [9], or screen-printed graph-
ite-based WEs [53], [54]. From the i
pc
/i
pa
 ratio of 0.99, we 
can confirm the good reversibility of the redox process. 
From the anodic (E
pa
) and cathodic peak potentials (E
pc
), 
we determined an ∆E
pp
 of 176 mV as the absolute dif-
ference between the two values, indicating that this re-
dox couple exhibits a quasi-reversible behaviour at the 
graphite electrode prepared by AD [54].
The EC response of the WE at different scan rates is 
shown in Figure 7(a). According to the Randles-Ševčik 
equation, the peak current is proportional to A
ecsa
, 
which can in turn be calculated from the slope of the 
linear relationship between i
pc
 or i
pa
 and square root 
of the scan rate, shown in Figure 7(b). The data shows 
good linearity for both peak currents, but slightly dif-
ferent slopes. A
ecsa
 was calculated for both peaks, and 
their average value was 1.44 ± 0.06 cm
2
/cm
geo
2
. This val-
ue is higher than the screen-printed graphite electrode 
Figure 4: AFM map scans of the surface of graphite 
thick films. (a) height, (b) deflection, and (c) tapping 
amplitude. Yellow arrows designate sharp edges of the 
flake-like particles.
M. Šadl et al.; Informacije Midem, Vol. 54, No. 3(2024), 177 – 186

182
(0.79 cm
2
/cm
geo
2
) [54]. The increase in A
ecsa
 could be at-
tributed to the high surface roughness of the graphite 
thick films prepared by AD.
Since the ∆E
pp
 of the quasi-reversible process changes 
with the scan rate, we used cyclic voltammograms 
measured at different scan rates to plot how a dimen-
sionless kinetic parameter Ψ varies with the inverse 
square root of the scan rate, as shown in Figure 7(c). 
A k
0
 of 1.9·10
-3
  cm·s
–1
 was then calculated from the 
slope by the Nicholson method at ν = 20–500 mV·s
−1
 
(∆E
pp
 = 122–354 mV). Although the ∆E
pp
 at the high-
est scan rate used exceeds the range for which the Ni-
cholson method is valid, all points show good linearity. 
Compared to values reported by Trachioti et al. [54] for 
graphite screen-printed electrodes, we obtained simi-
lar k
0
 values. To determine in which potential range the 
Figure 5: The SEM images of the graphite thick film in 
surface view. The micrographs in (a) and (b) were taken 
with secondary-electron and backscattered-electron 
detector, respectively. Yellow arrows designate sharp 
edges of flake-like particles.
Figure 7: (a) Cyclic voltammograms of various scan 
rates of HCF for graphite thick-film WE, (b) plot of ca-
thodic and anodic peak currents of HCF as a function of 
the square root of the scan rate, (c) plot of Ψ vs. ν
-1/2
 for 
the reduction of HCF.
M. Šadl et al.; Informacije Midem, Vol. 54, No. 3(2024), 177 – 186
Figure 6: Cyclic voltammograms at 100 mV·s
–1
 of PBS 
(dotted line) and HCF (full line) at graphite thick-film 
WE.

183
electrode has a stable response, we also determined its 
OPW, which is from –0.9 V to 1.2 V. Electrode stability 
in the anodic direction makes it very suitable for the 
detection of phenolic compounds such as bisphenol A 
[6], dihydroxybenzene isomers such as hydroquinone, 
catechol and resorcinol [7], parabens [55], quinolone 
antibiotics [56], organohalides [57], as well as 4-nitro-
phenol and dopamine [58]. The graphite thick films 
were also mechanically stable and did not degrade or 
delaminate from the substrate when immersed in and 
rinsed with methanol, ethanol or acetone. Therefore, 
the films can also be used for the detection of analytes 
that require non-aqueous electrolytes. We can con-
clude that AD graphite thick films are applicable as 
working electrodes in EC sensors for the detection of 
various organic compounds. 
4 Conclusions
To avoid high temperatures in the fabrication of EC 
sensors, the AD method was used to process graphite 
thick films on PI substrates. The initial graphite powder 
consists of flake-type particles with an irregular shape 
that form large agglomerates. The powder particle size 
distribution shows a rather large d
50
 particle size of 
16.6 μm, which is rarely reported for the AD method. 
However, AD was successful and resulted in  ~4-μm-
thick films with a defect-free appearance and an R
q
 
of 0.68  μm. The SEM revealed good particle compac-
tion of the film surface. The XRD patterns showed no 
reduction in the crystallite size and no increase in the 
microstrain after deposition. The graphite is therefore 
not subjected to the same deposition mechanism that 
is typical for ceramics. An EC analysis by cyclic voltam-
metry showed good reversibility of the redox process 
for graphite working electrodes with a large, real A
ecsa
 
of 1.44 cm
2
/cm
geo
2
 and a k
0
 of 0.0019 cm s
–1
, compara-
ble to those reported for graphite in the literature. A 
reasonable OPW between –0.9 V and 1.2 V also enables 
their use as working electrodes for the EC detection of 
a broad range of chemicals.
5 Acknowledgments
This work was funded by the Slovenian Research and 
Innovation Agency (research project N2-0212, J2–3049, 
and research core funding P2-0105), Ministry of Higher 
Education, Science and Innovation of Republic Slo-
venia (C3360-23-252004, M-ERA.NET) and the Jožef 
Stefan Institute Director’s fund 2017-ULTRACOOL. The 
authors thank K. Spanou, N. Suban and V. Fišinger for 
assistance in the laboratory. 
6 Conflict of interest
The authors declare no conflict of interest. The found-
ing sponsors had no role in the design of the study; in 
the collection, analyses, or interpretation of data; in the 
writing of the manuscript, and in the decision to pub-
lish the results. 
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Arrived: 19. 04. 2024
Accepted: 18. 06. 2024
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