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Культура Документы
DOI 10.1007/s00216-013-7013-z
REVIEW
Received: 7 March 2013 / Revised: 19 April 2013 / Accepted: 23 April 2013 / Published online: 16 May 2013
# Springer-Verlag Berlin Heidelberg 2013
Abstract Inkjet printing has evolved from an office printing application to become an important tool in industrial
mass fabrication. In parallel, this technology is increasingly
used in research laboratories around the world for the fabrication of entire (bio)chemical sensing devices or single
functional elements of such devices. Regularly stated characteristics of inkjet printing making it attractive to replace an
alternative material deposition method are low cost, simplicity, high resolution, speed, reproducibility, flexibility, noncontact, and low amount of waste generated. With this
review, we give an overview over areas of (bio)chemical
sensing device development profiting from inkjet printing
applications. A variety of printable functional sensor elements are introduced by examples, and the advantages and
challenges of the inkjet method are pointed out. It is demonstrated that inkjet printing is already a routine tool for the
fabrication of some (bio)chemical sensing devices, but also
that novel applications are being continuously developed.
Finally, some inherent limitations of the method and challenges for the further exploitation of this technology are
pointed out.
Keywords Inkjet printing . Screen printing . Electrodes .
Conducting polymers . Microfluidic paper-based analytical
devices
Abbreviations
DBSA
Dodecylbenzenesulfonic acid
DOD
Drop-on-demand
Nobutoshi Komuro and Shunsuke Takaki have equally contributed to
this work.
N. Komuro : S. Takaki : K. Suzuki : D. Citterio (*)
Department of Applied Chemistry, Keio University,
3-14-1 Hiyoshi, Kohoku-ku,
223-8522 Yokohama, Japan
e-mail: citterio@applc.keio.ac.jp
HRP
LbL
LED
LOD
ODF
PANI
PEDOT-PSS
SERS
Horseradish peroxidase
Layer-by-layer
Light emitting diode
Limit of detection
Oligodeoxyfluoroside
Polyaniline
Poly(3,4-ethylene
dioxythiophene)-poly(styrenesulfonate)
Surface enhanced Raman
scattering
Introduction
The application of inkjet printing technology is by far no
longer limited to the printing of text or graphical data onto
paper, films, or three-dimensional objects. The probably
earliest report on the application of inkjet printing for
(bio)sensor fabrication was published in 1988 [1]. The authors of that work looked at inkjet technology to tackle the
challenge of selectively depositing an active sensing layer
onto a small area of a field effect transistor. Over the past
years, inkjet printing has evolved into a general industrial
fabrication tool for depositing controlled small amounts of
liquids onto a user-selected, well-defined area. Inkjet printing technology has grown up to industrial-scale mass production, where it is, for example, nowadays used in the
fabrication of color filters for light-emitting diodes and
full-color high-resolution flat panel displays [2]. The application of inkjet printing technology for material deposition
and device fabrication has been regularly reviewed in the
past [36]. Promoted by the rapid expansion of application
areas and the technical progress in printing equipment,
inkjet printing technology has relatively early found its role
as a tool supporting the mass production of (bio)analytical
devices. Probably among the earliest routine applications
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N. Komuro et al.
Fig. 2 Ink droplets (10 pL nominal droplet size) ejected from an array
of nozzles with 21 m diameterdiameter; the distance between the blue
lines is 100 m
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additive character makes those methods comparably economical in terms of material use. In contrast, photolithography [16]
is based on a subtractive approach, resulting in the creation of
waste. While photolithographic methods are superior to inkjet
printing in terms of achievable resolution, their subtractive
character calls for a larger number of processing steps and the
selective removal of pre-deposited material requires a specific
mask for every pattern, resulting in lower flexibility.
Material deposition methods featuring even higher resolution and patterning densities, such as for example soft lithography approaches [16, 17] and dip-pen nanolithography [16, 18],
are not discussed here, although they are increasingly applied,
in particular in the fabrication of bioanalytical devices.
However, their processing throughput and their cost efficiency
are at present not competitive to inkjet printing.
Dimatix DMP-2811
Optical / colorimetric
Optical / absorbance
Electrochemical /
conductometric
Electrochemical /
chromoamperometric
Electrochemical /
resistance
Piezo
Epson R230
NH3 gas
Organic vapors
CO2
Alcohol vapor
H2O2, NADHe,
Salbutamol
Chemical O2 demand
(COD)
Ascorbic acid
Triglycerides
Epinephrine,
norepinephrine,
dopamine
Glucose, H2O2
Piezo
Dimatix DMP-2800
Au electrode array
(nanoparticles)
Au electrode precursor
(nanoparticles)
Polyaniline nanoparticle
sensing layer
Ammonium persulfate oxidant
for vapor phase polymerization
of polyaniline electrodes
PEDOT-PSSd film
Aqueous NH3
Piezo
Dimatix DMP-2800
Au electrodes (nanoparticles)
HP Deskjet D2360
Dimatix DMP-2831
Dimatix DMP-2811
HP Deskjet 693C
Epson C46/C48
Dimatix DMP-2800
HP 4250
Dimatix DMP-2800
HP Deskjet 690C
Thermal
Piezo
Piezo
Thermal
Piezo
Piezo
Thermal
Piezo
Thermal
Piezo
Piezo
Epson R290
Dimatix DMP-2800
Piezo
Dimatix DMP-2800
Piezo
Thermal
Olivetti
Dimatix DMP-2800
Thermal
Piezo
Piezo
Dimatix DMP-2800
Au and Ag electrodes
(nanoparticles)
Type
pH, glucose
Printerb
Electrochemical /
potentiometric,
amperometric
Electrochemical /
impedimetric
Electrochemical /
amperometric
Sensing applications
Transduction mechanisma
Copy paper
Polyester film
Silver electrodesc on PET film
Si/SiO2 substrates with
lithographically defined
Ti/Pt electrodes
LED lens surface
PET transparency
PET film
Screen-printed carbon
electrodes on filter paper
PET sheets
Carbon electrodesc
Carbon electrodesc
[50]
Carbon electrodesc
on PET film
PET film
[62, 63]
[60]
[59]
[57]
[49]
[10]
[46]
[56]
[45]
[104]
[58]
[54, 55]
[53]
[20, 21]
[52]
[42]
[41]
[40]
[31]
Ref
Polyimide
Coated paper
Coated paper
Substrate
Table 1 (Bio)chemical sensing devices fabricated by inkjet printing. Table items are grouped according to the sensor transduction mechanism, which is not necessarily the same order as in the main text
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N. Komuro et al.
pH
Optical / fluorescence
Mechanical / mass
Optical / colorimetric
Malathion, heroin,
cocain
pH, DNA, gas
Nitrite ions
Streptavidin
NO2 gas
Rhodamine 6G
Optical / SERS
Carbohydrate-binding proteins
Food spoilage
and ripening
Ricin
BSA, glucose
HRP activity
Malaria antigen
ATP, IgG
Phenolic compounds
Neurotoxins,
organophosphate
pesticides, bacteria
in food samples
Phosphate
Sensing applications
Optical / colorimetric
(fluorescence-based)
Transduction mechanisma
Table 1 (continued)
PicoJet-2000
PicoJet-2000
Dimatix DMP-2831
Hewlett-Packard
Autodrop MD-P-705-L
Epson Workforce 30
Thermal
Piezo
Piezo
Piezo
Thermal
Piezo
Piezo
Piezo
Piezo
Scienion S3 Flexarrayer
Epson Workforce 30
Piezo
Thermal
Piezo
Epson R280
Not-specified
research-type printer
Autodrop MD-P-705-L
Thermal
Thermal
Thermal
HP LaserJet 1000
Canon Pixma ip4500
HP Deskjet F4280
Piezo
Piezo
Thermal
Piezo
Piezo
Type
Scienion
Dimatix DMP-2800
Canon iP4700
Dimatix DMP-2800
Dimatix DMP-2800
Printerb
Filter paper
Filter paper
Filter paper
Silicon cantilevers
QCM
Silicon cantilevers
Chromatography paper
Chromatography paper
Microfluidic chip
(Si/ polydimethylsiloxane)
Silicon microring resonators
Chromatography paper
Cotton paper
Filter paper
Filter paper
Nitrocellulose strips
Filter paper
Filter paper
Filter paper
Substrate
[85, 86]
[84]
[15]
[76]
[107]
[75]
[74]
[73]
[72]
[71]
[70]
[69]
[68]
[106]
[23]
[93]
[105]
[89]
[6567]
[64]
Ref
Glucose
pH
IgG
Electrochemical / resistance
Optical / reflectometry
Photonic crystals
Antibody spots
Blocking solution
Microfluidic structure
Italic font indicates the application of a research-use material printer, whereas plain font indicates the use of a consumer desktop printer.
2-(Dibutylamino)ethanol.
The actual pattern is drawn with a wax-pen, following the inkjet printed pattern outline.
Poly(methyl methacrylate).
Piezo
Piezo
Dimatix DMP-2800
PicoSpot Jet
Dispensing System
Thermal
Piezo
Piezo
Type
Dimatix DMP-2800
Epson PX-101
Printerb
Bold face indicates an all inkjet printed approach, where all major sensor fabrication steps were achieved with an inkjet printer.
DBAEi, NADHe
Optical / electrochemiluminescence
Optical / colorimetric
Heavy metals
pH, H2O2
Sensing applications
Optical / colorimetric
Transduction mechanisma
Table 1 (continued)
Hydrophobically
coated glass slides
Filter paper
Filter paper
Filter paper
Substrate
[108]
[91]
[90]
[92]
[87, 88]
Ref
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N. Komuro et al.
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N. Komuro et al.
Fig. 3 Different types of inkjet printing devices for laboratory use: (a) research-use material printer accommodating a multiple nozzle single-use
print head; (b) research-use inkjet dispenser with single nozzle print head; (c) piezoelectric consumer desktop printer
salt, onto paper or plastic substrates precoated with a positively charged polymer, poly(diallyldimethyl ammonium chloride). The induced charge neutralization results in a
spontaneous sintering of the silver nanoparticles at room
temperature, leading to metallic silver traces with 20% the
conductivity of bulk silver, a value otherwise only achieved
by extended sintering at high temperatures. Perelaer et al. have
demonstrated a time reduced sintering method for electrodes
printed with a commercial silver nanopaste ink (piezoelectric
research-type printer) resulting in 40% of bulk silver conductivity [36]. The method relies on a combination of photonicand microwave-induced sintering that can be completed in
less than 15 s, making it suitable for a continuous roll-to-roll
fabrication process. In another approach chosen by Tobjrk et
al., conductivities corresponding to 10%20 % of that of bulk
silver have been obtained by exposing electrodes printed with
a commercial Ag nanopaste ink (piezoelectric research-type
printer) for 15 s to an IR lamp [37]. This method was also
successfully applied to electrodes printed from gold nanoparticle inks (piezoelectric research-type printer) [38]. The same
research group has finally combined inkjet printed gold working and counter electrodes with an inkjet printed silver electrode, electrochemically converted into an Ag/AgCl reference
electrode, to obtain an amperometric three-electrode paper
sensing device for glucose [31]. This low-cost inkjet printed
three-electrode paper chip platform, which can be obtained
through a roll-to-roll process, performs equally well to a more
costly conventional electrochemical sensor setup. Nie et al.
have demonstrated the possibility to achieve highly conductive silver lines on PET substrates (50% the conductivity of
bulk silver) from a particle free metal precursor solution
(silver citrate) [39]. The approach is based on the thermal
reduction of the inkjet deposited silver citrate (piezoelectric
desktop printer) in the presence of 1,2-diaminopropane. The
formation of a silver-amine complex results in a decreased
redox potential, allowing the thermal reduction of Ag+ at
relatively low temperatures (50 min at 230 C). By reducing
the heat treatment temperature to 150 C, which allows the use
of more heat-sensitive substrates, still 10% of bulk silver
conductivity can be achieved.
In many applications, the use of gold electrodes is preferable over silver electrodes because of the chemical inertness of
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the electrode conductivity. These are examples of applications where the inkjet deposited electrode material simultaneously acts as the active sensing layer.
Inkjet printing of active sensing layers for electrochemical
sensors
It has been shown in the previous section that inkjet printing
can be a great tool for the very simple and rapid fabrication
of electrodes, in some cases requiring nothing more than an
off-the-shelf consumer desktop printer. Another important
application of inkjet printing technology is the coating of
electrodes with an active sensing layer. Frequently, that
layer consists of a film of a conducting polymer with the
purpose of fabricating an electrochemical gas sensor
whereby, in some cases, the polymer simultaneously
acts as electrode and active sensing layer without the
requirement of a separate underlying electrode substrate.
Weng et al. have reviewed the printing of conducting polymers in general [47].
Widely inkjet printed conductive polymers include
polypyrrole, polyaniline (PANI), and poly(3,4-ethylene
dioxythiophene)-poly(styrenesulfonate) (PEDOT-PSS).
One problem encountered with PANI is the fact that it is
insoluble in water and even in many common organic solvents, which makes the straightforward formulation of
inkjet printable inks challenging. When the use of an offthe-shelf desktop printer is targeted, the inks have to be
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N. Komuro et al.
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technique, which lacked in reproducibility. They used a piezoelectric consumer inkjet printer to deposit an aqueous colloidal TiO2 particle (6 wt%) ink containing 1.8 wt% of
carbowax as viscosity modifier onto indium tin oxide glass.
The inkjet printed sensing layers were directly compared with
those deposited by the conventional dip coating method.
Figure 7 shows a comparison of inkjet printed and dip coated
TiO2 electrodes. A more homogenous film formation is clearly confirmed for the inkjet printed electrode. As in other cases
of depositing an active sensing layer by inkjet printing, film
thickness control was easily achieved by varying the number
of printed layers. The sensing results revealed that inkjet
printed TiO2 films have good fabrication reproducibility and
that the relative standard deviations for independently fabricated electrodes are smaller compared with commonly used
dip coated sensors.
Research on optical (bio)chemical sensors has been very intensive over the past decades and continues to increase. The
essential part of any optical sensor is the active sensing layer
incorporating the signal transducing molecules. Major issues
with mass production of optical sensors are reproducible,
speedy, and controlled deposition of the active sensing layer.
Regarded as being rapid, reproducible, controllable (e.g., size,
shape, position of deposited material), contamination-free, and
Optical sensors
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Fig. 7 Comparison of an inkjet printed TiO2 electrode (left) and dipcoated electrode (right). Reprinted from Reference [58] Yang M; Li L.H.;
Zhang S.Q.; Li G.Y.; Zhao H.J. (2010) Preparation, characterization, and sensing application of inkjet printed nanostructured TiO2
photoanode. Sens Actuators B 147:622628, Copyright (2010), with
permission from Elsevier
N. Komuro et al.
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Fig. 10 Highly precise deposition of biotinylated bovine serum albumin on individual microcantilevers (45 m width, 300 m length) by
piezoelectric inkjet printing. Adapted from Reference [76] Ness SJ,
Kim S, Woolley AT, Nordin GP (2012) Single-sided inkjet
functionalization of silicon photonic microcantilevers. Sens Actuators
B 161:8087, Copyright (2012), with permission from Elsevier
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Jayawardane et al. used the microfluidic patterning process developed by Li et al. described above [85] in the
preparation of a low cost PAD for the detection of reactive
phosphate in water [89]. The sensing reagents for the
phosphomolybdenum blue-based phosphate determination
were deposited by manual pipetting.
Delaney et al. relied on the same alkenyl ketene dimer inkjet
printing method for microfluidic patterning to create PADS
for the electrochemiluminescence-based (ECL) sensing of
2-(dibutylamino)-ethanol and nicotinamide adenine dinucleotide (NADH) [90]. The inkjet patterned paper sections were
loaded with a ruthenium(II) complex ECL-transducer by manual pipetting and laminated onto screen printed carbon electrodes to assemble the final sensing devices.
In a report on an all-printed glucose sensor for diagnostics,
Mttnen et al. compared the performance of inkjet printing
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Final remarks
Of course, inkjet printing is not a universally applicable technology. One major limitation comes from the requirement for
N. Komuro et al.
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