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DOI 10.1007/s10404-016-1726-1
RESEARCH PAPER
Received: 21 November 2015 / Accepted: 3 March 2016 / Published online: 30 March 2016
Springer-Verlag Berlin Heidelberg 2016
Abstract This paper describes two methods for controlling capillary-driven liquid flow on microfluidic channels.
Unlike flow driven by external forces, capillary-driven flow
is dominated by interfacial phenomena and, therefore, is
sensitive to the channel geometry and chemical composition (surface energy) along the channel. The first method
to control fluid flow is based on altering surface energy
along the channel through regulation of UV irradiation
time, which enables adjusting the contact angle along the
fluid path. The slowing down (delay) of the liquid flow
depends on the stripe length and its position in the channel.
Using this technique, we generated flow delays spanning
from a second to over 3min. In the second approach, we
manipulated the flow velocity by introducing contractions
and expansions in the channel. The methods used herein
are inexpensive and can be incorporated to the microfluidic
channel fabrication step. They are capable of controlling
liquid flow with precise time delays without introducing
the foreign matter in the fluidic device.
Keywords Capillary forces Paper-based microfluidics
Surface flow Control
1Introduction
Recently, paper has attracted interest as a possible substitute for conventional microfluidics substrates because it is
cost-effective, user-friendly, environmentally friendly, and
simple to produce and dispose off. Paper-based microfluidic devices (PADs) enable precise transport of microliter volumes of liquid without pumps driven by capillary
action. Accordingly, it has great potential for point-of-care
(POC) diagnostics in resource-limited and home care settings (Hitzbleck etal. 2012; Von Lode 2005). PADs can
perform fluid handling and quantitative analysis, and
numerous applications have already been demonstrated in
healthcare, veterinary medicine, environmental monitoring,
and food safety: recent reviews detail specific applications
(Ballerini etal. 2012; Cate etal. 2015; He etal. 2015; Li
etal. 2012; Sackmann etal. 2014; Santhiago etal. 2014;
Yetisen etal. 2013). Controlled liquid transport in devices
is crucial for obtaining reproducible results and consistent
sensitivity (Yetisen etal. 2013). Active metering techniques
such as mechanical pumping, electro-wetting, magnetic
field, and electro-osmotic force provide rapid and precise
manipulation of microliter volumes of liquid. However,
they require additional energy sources or equipment (e.g.,
voltage amplifier, pump, power supplier) hence leading to
increased size, cost and complexity of microfluidic device.
The development of ways to control, and particularly delay
the fluid flow would enable greater functionalities to be
implemented on paper-based microfluidic devices. For
instance, the introduction of control over liquid transport
could enable sequential delivery of samples to perform
multiple timed analytical steps in a single step.
Several ways, including photolithography (Martinez
etal. 2008), laser techniques (Fu etal. 2010a, b), plasma
oxidation (Li etal. 2008), and different printing techniques,
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Page 2 of 9
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2Materials andmethods
Commercially available pigment-coated paperboard
(200g/m2, Stora Enso, Sweden) was coated with TiO2
nanoparticles in a roll-to-roll process using the liquid
flame spray (LFS) method. The LFS coating was carried out in the pilot scale paper converting line at Tampere University of Technology. A detailed description of
the process has been presented previously (Mkel etal.
2011; Teisala etal. 2010). The TiO2-coated paper was then
exposed to ultraviolet irradiation (320390nm) (Bluepoint
4 ecocure, Hnle UV technology, DE) via a photomask.
Figure 1 below shows the LFS coating process, a SEM
cross-sectional image of the coated paper and UV irradiation step. Fast and less-expensive photomask was made by
cutting office paper, and for high resolution a photomask
Page 3 of 9 63
O
H
Liquid
precursor
TiO nanoparticles
2
Pigment
coating
UV- irradiation
Photomask
Paper
2 mm
1 m
Base paper
2 m
Fig. 1a Liquid flame spray setup, b UV irradiation setup, c cross-sectional and top SEM images showing TiO2 LFS nanoparticles on paperboard and d the two types of photomasks used to block UV irradiation: silver ink printed on glass (top) and cut office paper (bottom)
3Results anddiscussion
3.1Paper surface treatment
Superhydrophobic paper surface was created by LFS coating of TiO2 nanoparticles. Figure2 shows the shift in the
water contact angle of paperboard from nearly 70 to 150
after TiO2 deposition. The rise in the contact angle is due
to a combination of the nanoparticle surface chemistry
and the complex surface structure that incorporates both
nano- and microscale roughness to enhance the water
repellency (Teisala etal. 2010, 2013). Exposure to UV
light transformed the surface wettability from superhydrophobic to hydrophilic regime. Depending on the exposure
time, the water contact angle of TiO2-coated paperboard
dropped from 150 to nearly 70, 30, and 10 after 5,
10, and 20min UV irradiation. This conversion has been
5 min
20 min
180
160
10 min
Paper board
140
120
100
80
60
40
20
0
10
15
20
25
30
35
Time [s]
Fig.2Water contact angle of paperboard as a function of UV-irradiation time. Reference paperboard (filled squares), paperboard coated
with TiO2 nanoparticles (X) and TiO2-coated paper after UV exposure for 5min (filled diamonds), 10min (filled triangles) and 20min
(filled circles). Inserted are pictures of a water droplet levelling 30s
after it was placed on paper with 0, 5, 10 and 20min UV exposure
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63
Page 4 of 9
under UV irradiaon
carbonaceous layer
16
Length[mm]
100
12
80
8
60
40
20
0
10
20
30
40
50
60
Mean CA []
120
Time, [s]
Fig.4Contact angle and base length over time as a 10l droplet
spreads on a low surface energy region (irradiation time 2min) of
channel to a higher surface energy region (irradiation time 20min).
Inserted are images of the droplet at the start, before, and after it
crosses from one region to the other
13
OH
UV irradiation
TiO2
TiO2
OH
Page 5 of 9 63
y = 0.01x3.31
y = 4E-3x3.39
Distance, mm
Distance, mm
y = 3.03x3.20
10
1
0.01
0.5mm@5mm
2mm@5mm
0.1
1mm@5 mm
uniform channel
10
10
y = 6x0.12
y = 24x0.82
1
0.01
100
y = 5x0.09
0.5mm@5mm
2mm@5mm
0.1
y = 5x0.04
1mm@5 mm
uniform channel
10
100
Time, s
Time, s
Fig. 5a Flow delay caused by changing the length of a stripe of low wettability and b piecewise power law fits to the liquid front movement
y = 0.01x3.31
10
1mm@5 mm
1mm@10mm
Distance, mm
Distance, mm
y = 13x0.02
10
y = 9x0.02
y = 28x0.81
y = 5x0.09
1mm@15mm
1
0.01
uniform channel
1mm@10mm
uniform channel
0.1
Time, s
10
100
1
0.01
0.1
1mm@5 mm
1mm@15mm
10
100
Time, s
Fig. 6a Delay of the liquid front obtained at different stripe locations along the channel and b piecewise power law fits to the liquid front
movement
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Page 6 of 9
80
70
60
50
40
10 mm away
30
20
15 mm away
0
Time, s
F = (cos A cos B )
where F is the driving force, liquid surface tension, and
A and B are the contact angles at receding and advancing angles as illustrated in Fig.7 inset. The stripe closer to
reference point, located 10mm away, shows a high receding contact angle (A) because of higher volume of the liquid leading to a high driving force. In conclusion, surface
energy differences can be used to regulate flow in a specific microfluidic application by changing the thickness of
the barrier stripe as well as the location of the stripe along
the channel. Similar to flow delays created by dissolving
sugar or erodible solvent, liquid flows continuously once
passing the delay barrier. Delay times over 60s may be
2mm channel
50
2->3@1cm
2->3@2cm
The surface flow control was achieved by creating channels with expansions and constrictions. Figure8 shows
different channel designs: a 2-mm constant width channel
that acts as reference, stripes with two different constant
widths with a narrow channel connected to a wider channel at a distance 10 and 20mm lengths from the liquid
source inlet and an expansion along the channel. The position of meniscus over time is plotted for the different channels. Initially, at time t=0, the liquid meniscus position in
the channel was set as 5mm in the analysis. The constant
width channel shows a steady velocity in the liquid front
before slowing down. This decrease in velocity is attributed to finite liquid supply in addition to viscous resistance
(Songok etal. 2014). The liquid front reached a distance
40mm in nearly 5s. This can be compared to liquid flow
through the paper matrix (Grade 1 chromatography paper),
where a liquid front reached 35mm in 50s in the experiment conducted by Zhong etal. with the constant width
paper fluidic channels fabricated by wax printing (Zhong
etal. 2012). To control the flow, the channel widths were
varied. The channel width was increased by 50% (2mm
to 3mm at 10 and 20mm away from the channel inlet)
and decreased by 50% (21mm at 10mm). The results
show similar flow characteristics before the point at which
the channel width was changed. At the transition point
from narrow to a wide channel, i.e., at 5 and 15mm, the
liquid front velocity decreased significantly. In accordance
to mass conservation, increasing the width of the channel
means increasing the area thus results in decrease of liquid
front velocity. However, moving from the wider channel to
2->1 contr
2 mm uniform channel
Meniscus position, mm
2 mm
40
20
2 mm
10
30
0
20
0.5
1
Time, s
1.5
2 mm
3 mm
20 mm
10
0
3 mm
10 mm
Time, s
10
1 mm
15
Fig. 8a Position of the liquid front plotted as a function of time when the channel width was increased or decreased. b Channel geometries.
The inset shows results close to origin
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Page 7 of 9 63
60
Meniscus position, mm
2 mm
50
40
2 mm
1 mm
30
20
2 mm
2mm channel
1 mm long constriction
2 mm long constriction
5 mm Bulb
10
0
uniform channel
10
15
Time, s
20
25
1 mm
30
2 mm
5 mm
1s
1s
2s
2s
25 s
14 s
180 s
180 s
Fig.10Sequential images showing different liquid arriving at different time into the channel and the subsequent mixing of the liquids. Scale
bar of 10mm. a Shows a straight channel and b a zigzag channel
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4Conclusion
In this work, we report two methods with which a flow
delay can be achieved in surface flow-based paper-based
fluidic devices without additional fabrication steps or user
action requirement. The first method we have shown takes
advantage of the surface energy contrast to cause a flow
delay. The surface energy difference along a channel was
accomplished by varying the UV exposure time of TiO2coated paper. The flow retardation is achieved as the liquid
flows over a higher contact angle stripe. Parameters to control the delay include the length and position of the stripe
along the channel. This broadens the time range in which
timed fluidic delivery may be achieved. We have also
demonstrated flow delay through changing the geometry
(width) of the channel. These approaches effectively control the flow without increasing the required liquid volume.
A combination of surface wettability gradient and varying
the channel geometry has been used to show sequential
delivery can be achieved without using external source of
energy. We have also shown that homogeneous mixing can
be achieved in capillary-driven surface flow. The mixing is
fostered by the back flow and flow recirculation because
it induces transversal flow. Potential shortcomings of the
proposed liquid flow control system are related to possible interactions between the TiO2 nanoparticles and the
reagents used in a device. Furthermore, the open channels
proposed herein are not suitable for assays requiring very
13
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