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Lab on a Chip c4lc00542b

Controlled splitting and focusing of a stream of
nanoparticles in a converging–diverging
microchannel
Ravi Kumar Arun, Kaustav Chaudhury, Moumita Ghosh,
Gautam Biswas, Nripen Chanda and Suman Chakraborty*
We Q3 demonstrate a converging–diverging channel design for
nanoparticle focusing that facilitates the interaction of
AgNPs with H
2
O
2
at an interface.
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Journal: Lab on a Chip
Paper: c4lc00542b
Title: Controlled splitting and focusing of a stream of nanoparticles in a converging–diverging microchannel
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Lab on a Chip
PAPER
Cite this: DOI: 10.1039/c4lc00542b
Received 8th May 2014,
Accepted 14th July 2014
DOI: 10.1039/c4lc00542b
www.rsc.org/loc
Q1 Controlled splitting and focusing of a stream of
nanoparticles in a converging–diverging
microchannel†
Q2 Ravi Kumar Arun,
a
Kaustav Chaudhury,
b
Moumita Ghosh,
a
Gautam Biswas,
cd
Nripen Chanda
a
and Suman Chakraborty*
b
We demonstrate the potential of a converging–diverging microchannel to split a stream of nanoparticles
towards the interfacial region of the dispersed and the carrier phases, introduced through the middle inlet
and through the remaining two inlets respectively, while maintaining a low Reynolds number limit (<10) for
the flow of both phases. In addition to the splitting of passive tracer particles, such as polystyrene beads as
used herein, the present setup has the potential to be utilized for a controlled reaction and thereby the
separation of products towards an intended location, as observed from the experimentation with
silver-nanoparticles and hydrogen–peroxide solution. Moreover, the microscale dimension of the channel
allows controlled deposition of the reaction product over the bottom surface of the channel, allowing the
possibility of bottom-up fabrication of microscale features. We unveil the underlying hydrodynamics that
lead to such behaviours through numerical simulations, which are consistent with the experimental
observations. The phenomenological features are found to be guided by the splitting of the intrinsic
streamlines conforming to the flow geometry under consideration.
Introduction
The potential of nanoparticle laden flow has been utilized,
traditionally, for augmentation in heat and mass transport.
1–4
Q4 In microscale devices, one may bring into play a plethora of
additional attributes with nanoparticle dispersions, which will
have an immense impact on biomedical and industrial
applications.
5–8
This can be primarily attributed to the micro-
scale dimension and different types of channel geometries,
9,10
which have essentially been guided by the quest to make com-
pact and effective miniaturized devices for offering smart
solutions to practical problems.
11
With these motivations in
the background, here we demonstrate, through experiments
and simulations, the potential of a periodically-repeated,
converging–diverging microchannel to split and focus a
stream of nanoparticles, carried by an aqueous medium. In
contrast to the traditional straight channels and microchannels
with sudden contraction–expansion zones,
12,13
the present
design, with a smoothly varying cross section, seems to offer
better control towards splitting and focusing the nanoparticles,
without sacrificing the very laminar nature of the inherent
flow field.
We conducted experiments with coloured dye, polystyrene
beads, and silver nanoparticles, as the dispersed phase. In all
the mentioned cases, we observed the accumulation of parti-
cles over the interfacial regions between the dispersed and
carrier phases. This demonstrates the focusing ability of the
present device for a wide range of particles, ranging from par-
ticles with similar dimensions to that of the carrier fluid, to
particles with dimensions as large as 500 nanometres. The
inherent hydrodynamics associated with the present setup
that leads towards the splitting of the stream of particles is
unveiled through numerical simulation, which is consistent
with the experimental observations.
The distribution of the coloured dye and the polystyrene
beads can be hypothesized by the theory of passive tracer
particles, at least for the present scenario. While using a
stream of silver nanoparticles, we use an aqueous solution of
hydrogen–peroxide as the carrier phase; thus, they participate
actively to form precipitates of silver oxides which also accu-
mulate over the two fluid interfacial regions, as shown here.
Therefore, there is potential for the present micro-device to
have wide ranging applications in micro total analysis
Lab Chip, 2014, 00, 1–9 | 1 This journal is © The Royal Society of Chemistry 2014
a
Micro System Technology Laboratory, CSIR-Central Mechanical Engineering
Research Institute, MG Avenue, Durgapur, India
b
Department of Mechanical Engineering, Indian Institute of Technology
Kharagpur, Kharagpur 721302, India. E-mail: suman@mech.iitkgp.ernet.in
c
Department of Mechanical Engineering, Indian Institute of Technology Kanpur,
Uttar Pradesh 208016, India
d
Department of Mechanical Engineering, Indian Institute of Technology
Guwahati, Guwahati 781039, India
† Electronic supplementary information (ESI) available: Details of silver
nanoparticles (AgNPs) and silver ion precipitate characterizations and their
microfluidic studies. See DOI: 10.1039/c4lc00542b
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systems (μTAS), medical diagnosis and in bottom-up fabrica-
tion processes, where the primary requirement is to maintain
controlled reactions and thereby separate specific products.
14–16
It is important to mention in the present context that a lot
of attempts have been made to split streams of micro or
nano sized particles,
13,17–21
mainly by utilizing microchannels
with different geometries.
22–24
However, the end results are
mostly confined to the achievement of augmented mixing,
separation and reaction. On the other hand, the intrinsic
microscale dimension of the channels can be potentially uti-
lized for focusing the nanoparticle stream over a particular
region, by allowing the controlled deposition of particles over
the channel surface in and around the targeted location.
25–27
This may eventually provide a useful means for the fabrica-
tion of microscale features with finer resolutions.
28
Our study
focuses on utilizing the potential of both the channel geome-
try and the microscale dimensions, in tandem. Additionally,
our approach can enable one to maintain control over the
extent of splitting along the transverse direction.
Materials and methods
Q5 Problem description with schematic
Fig. 1 illustrates the schematic of the present converging–
diverging microchannel, with three inlet systems.
We used the middle inlet to introduce the dispersed
phases (i.e. the nanoparticle laden solution), and the other
two inlets were utilized to supply the carrier phase. We
maintained the channel height, (H) = 0.15 mm, and length,
(L) = 25 mm.
29
The widths (W) of the converging and diverg-
ing zones were maintained at 3.3 and 0.8 mm, respectively.
Throughout the entire study, we maintained the flow rate of
the nanoparticle laden solution at 25 μL min
−1
, and the flow
rates of the carrier phase were varied as 25, 50, 100 and
250 μL min
−1
. We defined the Reynolds number for a particu-
lar entity as Re = D
eq
vρ/μ, where D
eq
is the hydraulic diameter
of the flow cross section, v = Q/A (A is the cross-sectional area
of the expansion region and Q is the flow rate), μ is dynamic
viscosity and ρ is the density of the solution. With the various
possible combinations of the flow rates, as obtained from the
mentioned data, we maintained a low Reynolds number limit
(<10) for the flow of both the dispersed and the carrier
phases, in order to maintain laminar flow conditions. We
maintained this limit of the Reynolds number, strictly, to
avoid the formation of unwanted eddies, which might have
disturbed the focusing ability of the present device by pro-
moting mixing over the entire cross section. The essential
features were demonstrated through rigorous experimenta-
tion. To unveil the underlying physics, we also conducted
numerical simulations, which were consistent with the exper-
imental observations.
Channel preparation and the experimental procedure
The experiments were conducted with an alternate converg-
ing–diverging poly-dimethylsiloxane (PDMS) microchannel.
Each wall of the channel consisted of 10 repeated structures.
The microchannel was fabricated using a single-step soft-
lithography technique. To obtain the negative template we
used a carbon dioxide laser (VLS-2.30, Universal Laser Inc.,
USA) engraving onto an 80 μm thick polystyrene sheet, pasted
on a double sided tape (thickness = 40 μm). The prepared
template was then pasted on a clean glass slide. The PDMS
elastomer (Dow Corning, USA), mixed with a cross-linking
agent at a 10 : 1 ratio (w/w), was stirred and degassed under a
vacuum system and then poured over the well-closed negative
template and kept at 60 °C in a hot-air oven for 30 min for
curing. After curing, the PDMS replica was removed from the
template mould and attached to a plasma (Harrick Plasma
Cleaner) oxidized glass slide, already cleaned with piranha
solution, to form a closed structure.
We conducted experiments with dye, polystyrene beads,
and silver nanoparticles as the dispersed phases. As carrier
phases, we used de-ionized water (DI) for the first two cases,
and an aqueous solution of hydrogen–peroxide for the third
one. Both the carrier and the dispersed phases were driven
by syringe pumps (Harvard Apparatus PHD 2000, USA), and
for visualization purposes we used an inverted optical micro-
scope (Leica DMI-4000B). To observe the phenomenological
features along the complete length of the channel, we took
pictures at different sections of the channel and then super-
imposed them to get the full details.
Experimentation with dye
Q6 We have chosen aqueous fruit dye (1.0 mg mL
−1
), for
experimentation with coloured dye. While conducting the
experiment with the mentioned flow rates, we obtained a
controlled divergence of the dye stream, along the entire
length of the channel. Upon further increasing the flow rates,
we observed rapid mixing of the dye; thus, we restricted our
focus to the mentioned flow rates only. We further executed
colorimetric intensity analysis to obtain the distribution of
the particles. With this primary idea, we then move towards
the experimentation with polystyrene beads, with a specific
objective which was to obtain the splitting of particle stream.
Experimentation with polystyrene beads
The fluorescent polystyrene beads (Sigma Aldrich, Saint Louis,
MO, USA), 30 nm and 500 nm in size, were suspended in DI
water with a particle concentration of 1.2 × 10
7
particles mL
−1
,
Fig. 1 A schematic representation of the nanoparticle distribution at
fluid–fluid interfaces in a converging–diverging microchannel.
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and used as the nanoparticle suspension for the present
study. The movements of the nanoparticles were monitored
under a LED fluorescence microscope (Leica DMI 4000B,
Germany) at a fixed wavelength of 470 nm and 530 nm, for
the 30 nm and 500 nm size particles, respectively. Here Q7 we
also observed the controlled divergence of the nanoparticle
stream, albeit to a further lateral extent than that of the for-
mer case. Subsequent quantitative colorimetric intensity anal-
ysis was used to demonstrate the controlled accumulation of
the polystyrene beads over the interfacial regions of the two
fluids. With the quantitative evidence in support of this, we
then moved towards exploiting the potential of the present
setup in maintaining a controlled reaction and allowing
the separation of products towards a specific location, as
endeavoured in the subsequent experimentation with the
silver nanoparticles and hydrogen–peroxide solution.
Experimentation with silver nanoparticles
Firstly, we prepared the silver-nanoparticle (AgNP) laden solu-
tion, following the reported chemical reduction method.
Briefly, 10 mg of AgNO
3
was added to 1 ml of DI water and
used as the stock solution. Subsequently, 20 mg of NaBH
4
was added to 1 ml of DI water and kept in a refrigerator to
avoid decomposition. Then, 20 mg of sodium dodecyl sul-
phate (SDS, Sigma Aldrich, Saint Louis, MO, USA) was mixed
with 20 ml of DI water and stirred for 10–15 min. During stir-
ring, 100 μl of AgNO
3
from the stock solution was added to
the SDS solution; the SDS solution was used to stabilize the
silver nanoparticles. Immediately, 300 μl of cooled NaBH
4
was added to the mixture and stirred for 10 min to achieve
the yellow colored AgNP solution. Finally, the nanoparticles
were characterized by UV-absorption spectroscopy and size
analysis (Fig. S1†). The size of the AgNPs was measured using
a NANOSIGHT particle size analyzer (NS500), and was found
to be in the range of 45 nm. In this case, the movements of
the nanoparticles were also monitored under a LED fluores-
cence microscope (Lieca DMI 4000B, Germany). The AgNP
solution was introduced through the middle inlet, whereas
the H
2
O
2
solution was introduced through the other two
inlets. Under the mentioned flow conditions, we observed the
accumulation of the reaction products in situ over the interfa-
cial region of the two fluids. We also found that the microscale
dimension of the channel allowed controlled precipitation
of the reaction products over the bottom glass surface of
the channel. The microscale features were then observed
using scanning electron microscopy (SEM) operated at 5 kV
(Hitachi S-3000N).
Results
We began our observation with the coloured dye; the charac-
teristic features are shown in Fig. 2. This behaviour was
observed under the flow of the carrier phase at 25, 50, 100
and 250 μL min
−1
and the dispersed phase at 25 μL min
−1
.
The first noteworthy fact is that we observed a divergence of
the dye stream; the distribution is earmarked by the
distribution of the coloured dye with the expansion–contraction
zone, as shown in Fig. 2. Under the mentioned flow rates, the
Reynolds numbers for the carrier and the dispersed phases
are found to be 0.58–5.8 and 1.12–3.64 respectively. When we
progressively increased the flow rates of the carrier phase
from 25 (Re
DI
= 0.58) to 250 μL min
−1
(Re
DI
= 5.80), we
observed a similar behaviour in the dye distribution, as
shown in Fig. 3. From the figure it is evident that with an
increase in the flow rate of the carrier phase, the width of the
dye distribution decreases. From the mentioned observations,
it is indicative that the present setup could be utilized to
focus the stream of particles by controlling the expansion–
contraction of the dye distribution.
However, it was imperative to investigate whether the
mentioned behaviours are associated with the channel geometry
or something else. To investigate this, we also conducted
experiments with three inlet straight microchannels, with the
same width as that of the expanded section of the present
converging–diverging channel. The results are shown in
Fig. S2.† With the various combinations of the flow rates of
the carrier and the dispersed phases, we found that none of
the combinations yield the expansion–contraction type dye
distribution. Thus, by comparing Fig. 2 and S2,† we can
proclaim that the typical expansion–contraction type dye
distribution in the converging–diverging channel is inherent
to the intrinsic geometry of the channel. However, with the
change in the combinations of the flow rates, the width of
the dye distribution changed within the straight channel as
Fig. 2 Superimposed microscope image of a converging–diverging
PDMS microchannel showing the characteristic feature of dye
distribution in DI water.
Fig. 3 Dye solution distribution under the flow rates of the carrier
phase at 25, 50, 100, 250 μL min
−1
, keeping the central dye flow rate at
25 μL min
−1
.
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4 | Lab Chip, 2014, 00, 1–9 This journal is © The Royal Society of Chemistry 2014
well. Thus, the controllability of the system seems to stem,
mainly, from the flow rate control.
An important inference that can be drawn from the above
observations is that the converging–diverging microchannel
can cause expansion–contraction of the dye stream. However,
the size of the dye molecules is typically of the order of the
size of the water molecules, acting as the carrier phase. Thus,
it is difficult to analyse the ability of the present setup to split
the stream of particles. Therefore, to investigate this ability
we have conducted experiments with the dispersed phase,
composed of an aqueous solution of polystyrene beads; the
results are shown in Fig. 4 for the dispersed phase containing
the nanoparticles with dimensions of the order of 30 nm. In
this case we also maintained the flow rate of the dispersed
phase at 25 μL min
−1
, while the flow rates of the carrier
phase varied from 25 to 250 μL min
−1
(along Fig. 4a–d). For
the sake of quantitative estimation, we also conducted a
colorimetric intensity analysis by measuring the fluorescence
intensity of the particles, as shown in the graphs along with
the corresponding images. From these graphs we can identify
that the intensities show a deepening tendency around the
channel centreline (specifically see Fig. 4f and g), while
showing peaks near the interfacial region of the two fluids.
This estimation suggests the localized distribution of the sub-
merged nanoparticles, specifically near the interfacial region,
in contrast to the homogenous distribution all over the dis-
persed phase region. However, from Fig. 4h, the fluorescence
intensity based estimation does not confirm the preferential
splitting of the transported nanoparticles; this may be attrib-
uted to issues with the resolution.
For the sake of further verification, we also conducted
experiments with nanoparticles with dimensions of the order
of 500 nm; the essential features are shown in Fig. 5. We
obtained approximately similar interfacial distances for the
500 nm particles with better focusing as compared to the
30 nm fluorescent particles (compare Fig. 4 and 5). Thus, the
results confirm that the present setup can be potentially
utilized for the splitting of streams of nanoparticles and to
focus them towards the interfacial region of the two fluids.
We performed similar experiments with the straight micro-
channel (Fig. S3†). We can clearly see that the focusing of the
nanoparticles is almost absent at all of the flow rate ratios.
Thus, with the experimental results in hand, it is suggestive
that the inherent geometry of the channel allows such typical
splitting of the streams of particles and makes them settle
over the interfacial region.
After gaining knowledge about the splitting and focusing
ability of the present setup, we explored the possibility of
achieving a controlled reaction and the subsequent separa-
tion of products, as it is one of the primary requirements in
micro-total-analysis systems. We explored the distribution of
metallic silver nanoparticles, 45 ± 4 nm in size, upon chemi-
cal reaction with H
2
O
2
in the present microchannel; shown
in the Fig. 6. We introduced dilute H
2
O
2
(0.9 M) as the carrier
fluid which reacts with the AgNPs at the interfaces to form
silver microstructures along the interfacial planes. Being an
oxidizing agent, H
2
O
2
oxidizes the AgNPs to silver ions, at an
alkaline pH (pH ~ 8.5) of the medium, that are spontaneously
precipitated as micron-size structures at the interfaces. The
interaction performance of the AgNPs and H
2
O
2
in the micro-
channel, as shown in Fig. 6, was recorded under an inverted
microscope for 30 min. We determined this 30 min reaction
time by monitoring the amount of reaction precipitate at dif-
ferent time intervals (Fig. S4†). At the beginning, there was
no precipitate at the interfaces, indicating the absence of the
reaction products from the interaction between the AgNPs
and H
2
O
2
. However, as the flow of the fluids continued, the
AgNPs started focusing at the interfaces and the formation of
Fig. 4 Hydrodynamic focusing of fluorescent nanoparticles (30 nm) in
the converging–diverging microchannel. (a–d) Microscopic
fluorescence images at 470 nm wavelength at different flow ratios of
the nanoparticle solution and DI water (25: 25, 25: 50, 25: 100 and 25: 250
respectively). (e–h) Plots of the fluorescence intensity versus distance along
the width of the channel showing particle distribution at the interfaces.
Note, that the maximum concentrations of the nanoparticles are observed
at two interfacial zones with a separation width of 100 μm at the flow ratio
of 25: 50.
Fig. 5 Hydrodynamic focusing of fluorescent nanoparticles (500 nm)
in a converging–diverging microchannel. (a) Fluorescent nanoparticles
are systematically focused at both of the interfaces while flowing
through the channel at a flow rate ratio of nanoparticles : DI of 25 : 50.
(b) The particle distribution in terms of the fluorescence intensity
versus distance along the width of the channel.
Fig. 6 Superimposed microscope image demonstrating the interaction
of the AgNPs and H
2
O
2
throughout the patterned micro-channel. A
gray coloured precipitate can be seen at the interfaces indicating the
in situ formation of silver microstructures as a product of the reaction.
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Lab Chip, 2014, 00, 1–9 | 5 This journal is © The Royal Society of Chemistry 2014
the products in the presence of co-flowing H
2
O
2
was seen at
10 min and gradually increased to a visible level at 30 min.
From the outset, we stated that the microscale dimension
of the channel can allow controlled deposition over the
bottom surface of the channel. Fig. 7 shows the precipitation
of the silver ions over the channel surface, after reaction; this
was confirmed by introducing aqueous NH
3
to the channel
after the reaction (Fig. S5†). Aqueous NH
3
dissolves the
precipitate by forming a soluble diamine–silver complex
([Ag(NH
3
)
2
]
+
) and confirms the existence of the Ag
+
ions.
30,31
The gray coloured silver ion precipitate remains at the inter-
facial planes; this can be attributed to the strong absorption
of the silver ions onto the PDMS and glass substrate. Upon
producing silver ions, the oxygen atoms of both of the
substrates are bound with Ag
+
ions in such way that the
surface-bound Ag
+
ions can subsequently function as seeds
for the growth of silver microstructures on glass and PDMS
substrates.
In order to investigate the growth mechanism of the silver
ion precipitate at the interfaces, we used SEM and EDS to
observe the material at different flow rates. Fig. 7(a–d) shows
the SEM images of the silver ion precipitate formed at the
interface due to the interaction between the AgNP and H
2
O
2
solutions at different flow rates after 30 min. The precipitate
appears as three-dimensional (3-D) agglomerates or irregu-
larly shaped micron-size structures. At a higher magnifica-
tion, the topography of these structures was revealed to be
formed by flower-like silver ion precipitates arranged at the
micrometre scale (Fig. 8a). The EDS spectrum shows the pres-
ence of elemental Ag in the precipitate (Fig. 8b). The peaks of
the Si and O elements are due to the Si substrate.
The reaction of AgNPs with H
2
O
2
was performed by
varying the flow rates of the carrier fluid (Q
H
2
O
2
= 25, 50, 100
and 250 μL min
−1
) while keeping the nanoparticle solution
flow rate, Q
AgNPs
, constant at 25 μL min
−1
. The applied
flow rates and corresponding Reynolds numbers (Re) are
shown in Table 1. At low Re
AgNP
(<1.15), the formation of the
precipitate from the AgNP and H
2
O
2
reaction was not seen
distinctly even after 10 min of flowing in the channel. As the
Re
AgNP
increased from 1.15 to 1.88 and then to 2.35, a thin
layer of silver ion precipitate was observed within 5 min. At
higher Re
AgNP
(>3.72), the precipitate started forming after
5 min, but the amount was less at the interface compared to
all lower Re
AgNP
(1.15, 1.88 and 2.35). This indicates that
Re
AgNP
in between 1.15–2.35 is the optimum for the nano-
particles to be distributed in a controlled manner at the
interfaces and to increase the contact area for accelerating
the interaction process with H
2
O
2
in a controlled manner
throughout the channel, as further confirmed by the SEM
and EDS studies (Fig. 7(a–c) and 8).
From the experimental results we can see that the con-
verging–diverging microchannel is capable of splitting and
subsequently focusing a stream of nanoparticles. Further
cross examination reveals that it is the very geometry of the
channel that makes this splitting possible. Therefore, it is
now imperative to analyze the inherent physics leading
towards these characteristic features. We discuss this issue in
the perspective of our numerical simulation studies.
Discussions
In order to unveil the underlying physics leading to particle
focusing, we conducted 3D numerical simulations for a
converging–diverging channel with the same dimensions as
those used in the experiments (see the ESI† for details).
Essentially, the velocity field, assuming incompressible flow,
is divergence free and is obtained by solving the Navier–
Stokes equation. Subsequently, the particle distributions were
obtained from Lagrangian tracking. Owing to the periodic
repetition of the channel geometry, we conducted a simula-
tion over a domain which was periodic along the direction of
the mean flow. Then the imposed flow rate was maintained
Fig. 7 Scanning electron microscopy images of the Ag ion precipitate
formed at the interfaces due to the interaction between the AgNP and
H
2
O
2
solutions at different flow rates of the carrier phase at (a) 25 μL min
−1
,
(b) 50 μL min
−1
, (c) 100 μL min
−1
and (d) 250 μL min
−1
for 30 min. The AgNP
solution flow rate was kept constant at 25 μL min
−1
. The insets show
the magnified images of the silver ion precipitate.
Fig. 8 (a) Magnified SEM image of the silver ion precipitates which
appear as flower-like structures. (b) The EDS spectrum of Ag ion
precipitates showing the presence of Ag. The peaks of the Si and O
elements are due to the Si substrate.
Table 1 Flow ratio and corresponding Reynolds number of the AgNP
and H
2
O
2
solutions
Flow ratio Q = 25 : 25 Q = 25 : 50 Q = 25 : 100 Q = 25 : 250
Re
H
2
O
2
0.58 1.16 2.32 5.79
Re
AgNP
1.15 1.88 2.35 3.72
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as the sum of the flow rates of the carrier and the dispersed
phases. In Fig. 9, we show the 3D simulation results of the
distributions of the 45 nm particles, with 10 500 kg m
−3
density (resembling the density of silver), at a flow rate of
25 μL min
−1
for both the carrier and the dispersed phases.
The figure shows that the observation from the present simu-
lation is in close agreement with the experimental results
(compared with Fig. 7a).
Initially, the particles were distributed in and around the
central axis of the channel. In response to the flow field, the
distribution of the particles was then obtained by solving the
kinetics equation for each particle
d
d
and
d
d
p
D g M S
p
p
u
f f f f
x
u
t t
= + + + = (1)
where x
p
and u
p
represent, respectively, the position and
velocity of the particle (in vector form), measured with
respect to a fixed-to-the-lab Cartesian reference frame, as
indicated in Fig. 9. The forces (per unit mass of the particle),
as shown in eqn (1), are the hydrodynamic drag force (f
D
),
force due to gravity (f
g
), virtual mass force (f
M
) and the
Saffman lift force (f
S
). They are estimated as
32–35
f u u
f g
f u u
D
p p
D p
p
g
p
M
p
p
Re
d
d
= ÷
( )
= ÷
|
\

|
.
|
|
= ÷
18
24
1
1
2
2
µ
µ
µ
µ
µ
µ
d
C
t
,
,
(( )
=
( )
÷
( )
¹
`
¦
¦
¦
¦
¦
¦
)
¦
¦
¦
¦
¦
¦
,
.
:
.
and
S
p p
p
f
D
D D
u u 5 188
1 2
1 4
µ
µ
v
d
(2)
Here g denotes the acceleration due to gravity (acting
along the −z direction), C
D
being the drag coefficient, and ρ,
μ and ν are the density, dynamic viscosity and kinematic
viscosity of the carrier phase (aqueous medium). Accordingly,
ρ
p
and d
p
denote the density and the diameter of the particle.
In eqn (2), the velocity vectors for the carrier phase and the
particle are denoted by u and u
p
. Accordingly, the strain rate
tensor is defined as D = ∇u + (∇u)
T
. Note that here the parti-
cle based Reynolds number is defined as Re
p
= d
p
|u − u
p
|/ν.
It is worth mentioning that for the simulation purpose, we
considered the contributions from all of the mentioned
forces.
During the tracking of particles, we considered the particle–
particle and particle–wall interactions to be elastic type. To the
present level of approximation, we did not take into account
the implication of any electrostatic interaction between the par-
ticles. In fact, any implication due to its accounting can be con-
sidered to be significant where the length scale over which the
characteristic changes in the particle distribution can be
observed, approaches the nanoscale regime.
36
Pertaining to the
present situation, the characteristic dimension of the zone of
the particles' divergence is well above this limit. However, in
our model we consider the two way coupling between the parti-
cles and the continuous phase. Specifically, that the gain (loss)
in momentum of a particle is accommodated as the loss (gain)
in momentum of the continuous phase.
It is now prudent to estimate the contribution of each of
the contributing forces in deciding the particle distribution
observed in mutually agreeing simulations and experiments.
First we note that studies have shown the influence of the
Saffman lift force on nanoparticle distribution.
25,26,36,37
However, their magnitudes are generally very small (~10
−14
N
to 10
−16
N, as estimated for the present experiments) and
there seems to be only a marginal change in the distribution
of the particles due to the accounting of this force. However,
for the sake of verification, we also conducted simulations
with and without the Saffman lift consideration in the model;
the comparison is shown in Fig. 10. From the figure, it is evi-
dent that the Saffman lift force does not induce any consider-
able change in particle distribution, at least for the present
setup. Subsequently, by comparing the order of magnitude
Fig. 9 3D simulation results of the distributions of 45 nm particles in a
converging diverging channel at a flow rate of 25 μL min
−1
, for both
the carrier and the dispersed phases. The flow was imposed along the
x direction and the particles were initially distributed axially around the
central axis of the channel.
Fig. 10 Splitting of the nanoparticle stream with d
p
= 45 nm and ρ
p
=
10500 kg m
−3
, with and without considering the Saffman lift force in
the converging–diverging channel at a flow rate of 25 μL min
−1
, for
both the carrier and the dispersed phases.
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contributions of the other forces, we found that f
g
and f
S
could be neglected as compared to f
D
. Thus, it seems that the
particles are basically dragged along the flow field. Addition-
ally from our simulation we found that u ~ u
p
. Thus, we can
consider that the particles move in the flow field as passive
tracer particles. Therefore, it is the inherent feature of the
intrinsic flow field that determines the distribution of the
particles. The dimension and the subsequent mass of each of
the nanoparticles are indicative of the fact that the particles
can be considered as passive tracer particles that are likely to
follow the streamlines closely at the steady state.
13,38
In search of the intrinsic flow features for the present
setup, in Fig. 11a we present the distribution of the stream-
lines, on an x–y plane passing through the central axis. From
the figure it is evident that the streamlines are compressed
and expanded in the converging and diverging sections,
respectively. The distribution of particles, therefore, follows a
similar pattern. For further verification, we performed simu-
lations in a straight channel with similar dimensions as
those used in the experiment; the particle distribution and
the streamlines are shown in Fig. 11b. The simulations were
also conducted with ρ
p
= 10 500 kg m
−3
and d
p
= 45 nm and
all the above mentioned forces were retained for Lagrangian
tracking of the particles. From Fig. 11b it is evident that the
particles with the given size closely follow the streamlines at
the given flow rate. Therefore, by comparing Fig. 11a and b
we can proclaim that the typical splitting of the nanoparticle
stream is a characteristic of the converging–diverging
channel geometry as considered in our work.
It is worth mentioning at this point that studies have
shown that even for flows with low Reynolds number,
secondary flows may exists specifically near the zones of
spatially varying curvatures of the channel geometry, and can
lead to some interesting features.
39–42
It is to be noted that
the cross section of the present device is also spatially vary-
ing. It is, therefore, imperative to unveil the possibility of the
influence of any such flow features. For this purpose, we
conducted simulations with different flow rates (Q). The flow
rate as maintained for presenting the results in Fig. 9, is con-
sidered as the base flow rate (Q
base
). Starting from Q/Q
base
=
1, we carried out simulations up to Q/Q
base
= 10; note that
this consideration is in tune with the present experimental
setup. As per our choice of reference frame, the central axis
was defined by the locus y = 0 and z = h/2, as shown in
Fig. 12a. In all the simulations, we then monitored the veloci-
ties at offsets y = δ (keeping z = h/2) as indicated in Fig. 12a.
In the left column of Fig. 12b we demonstrate the flow veloci-
ties u
x
, u
y
and u
z
, along the x, y and z directions respectively,
as obtained from the data monitored at δ = 5 × 10
−2
mm at
different x/L
ref
; here L
ref
was chosen as the width of the
expansion section. It needs to be emphasized that we
Fig. 11 (a) Distribution of the streamlines on an x–y plane passing
through the central axis, for (a) the converging–diverging channel and
(b) a straight channel. In both cases, the flow rates of both the carrier
and the dispersed phases were maintained at 25 μL min
−1
.
Fig. 12 (a) The description of the central axis and the offset δ. (b) The
variation of u
x
, u
y
and u
z
, (left column), measured along the x, y and z
directions respectively, and the corresponding u
x
/U
ref
, u
y
/U
ref
and
u
z
/U
ref
(right column), with x/L
ref
as obtained from the data monitored
at δ = 5 × 10
−2
mm.
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specifically focused our attention over the region around the
central axis where the particles are distributed. Specifically,
we endeavoured to scrutinize the hydrodynamic features
(namely the flow velocities) over this region so as to unveil
the essential physics of interest. Thus, we considered the
location at the mentioned offset around the central axis. The
gross flow feature at different zones within the channel is
already shown in Fig. 11a, through the distribution of the
streamlines. For distributions of u
x
and u
y
, here we only show
variations over a characteristic extent of x/L
ref
. The distribu-
tion over the entire extent of x/L
ref
is just the periodic repeti-
tion of those characteristic features. From the distributions
of u
x
in Fig. 12b, it is noteworthy that u
x
attains maxima at
the contraction zone. This is in tune with the continuity of
the flow rates across different cross sections. From the distri-
butions of u
z
in Fig. 12b, one can appreciate that at the con-
traction zone, it assumes magnitudes that are close to zero.
However, Q8 near the contraction zone, peaks of u
y
can be
observed at just upstream and downstream sides. Signifi-
cance of those optima were delineated Q9 post priory. Neverthe-
less, if we observe the variation of u
x
/U
ref
, u
y
/U
ref
and u
z
/U
ref
,
where U
ref
= Q/A (A is the cross-section area of the expansion
section), the corresponding curves collapse on each other, as
shown in the right column of Fig. 12b. The collapse indicates
that u
x
, u
y
and u
z
change proportionally with the imposed
flow rate. From this collapsing, we can also infer an impor-
tant fact: with the choice of a normalization scheme (using
the chosen L
ref
and U
ref
) it is possible to provide a generalized
depiction of the inherent hydrodynamics, so long as the
Reynolds number is kept low.
Among the u
x
/U
ref
, u
y
/U
ref
and u
z
/U
ref
distributions, as
shown in Fig. 12b, we found that u
x
/U
ref
and u
y
/U
ref
play
dominant roles in determining the inherent dynamics of the
present device, as can be appreciated from the negligible
order of magnitude of u
z
/U
ref
, in comparison to that of u
x
/U
ref
and u
y
/U
ref
. Q10 It is worth mentioning that the distribution of
both u
z
(Fig. 12b left column) and u
z
/U
ref
(Fig. 12b right
column) appear as noises. However, the ranges of the abso-
lute values within which their variations occur implicate that
the apparent fluctuations in u
z
and u
z
/U
ref
are not likely to
make any significant contribution in comparison to the veloc-
ity components along the other directions. Here the varia-
tions of u
z
and u
z
/U
ref
are presented to highlight the issue
that u
z
≪ u
x
and u
z
≪ u
y
. Thus, the essential physics is
primarily decided by u
x
and u
y
(subsequently by u
x
/U
ref
and
u
y
/U
ref
respectively).
In Fig. 13 we have compared the distributions of u
x
/U
ref
and u
y
/U
ref
for δ = ±5 × 10
−2
mm. From the figure it is evident
that in both cases, u
x
/U
ref
remains same. However, from
the distribution of u
y
/U
ref
one can appreciate that at a given
x/L
ref
, the u
y
/U
ref
distributions are the same in magnitude but
with a different sign. When the particles are approaching
the contraction zone, they experience symmetrically opposite
u
y
/U
ref
that endorses the squeezing of the distribution zone
of the particles. Subsequently, after coming out of the con-
traction zone, the u
y
/U
ref
distribution aides the expansion of
the distribution zone. The symmetrically opposite features
explain the symmetric distribution of the particles around
the central axis. With the above mentioned considerations
and the contrasting observations concerning the particle dis-
tributions in straight channels and converging–diverging
channels, we infer that the present splitting behaviour of
particles, in the present setup, is primarily due to the inher-
ent flow field, as realized from the geometrical features of
the confining domain. The very geometry of the channel
endorses periodic divergence and expansion of the stream-
lines, thereby causing the nanoparticles to trail along.
This type of distribution of nano-sized particles can be
beneficial to fabricate various microstructures inside the con-
fined channels for numerous applications. In the present
study, for example, the focused silver nanoparticles formed a
precipitate after reacting with H
2
O
2
at the interfaces thus
containing highly active Ag
+
ions and can directly be involved
in specific chemical or biological reactions for catalytic
purposes.
43
In the reported literature, silver is deposited at
the interfaces of microfluidic channels to encounter many
practical settings.
28,44
However, their fabrication processes
follow expensive and multi-step methods including multi-
stage photolithography, etching, accurate alignment and so
on. Moreover, there is little information known about the
morphological features of the precipitate formed inside
microchannels. In the present study, we have utilized a pro-
cess for the controlled synthesis of silver microstructures
throughout its interfacial length in a wavy fashion which will
provide a large surface area as compared to the straight
microchannel. The micro-structured silver ion precipitate
may have potential use in microelectronics and catalysis and
we may utilize this precipitate as microcatalysts for various
catalytic reactions in microchannels.
29
Conclusions
Our observations reveal that in a converging–diverging micro-
channel, with a smoothly varying cross-section, a stream of
nanoparticles can be split into two halves, and can be made
Fig. 13 The distributions of u
x
/U
ref
and u
y
/U
ref
at δ =
±
5 × 10
−2
mm to
show the particle distribution at the near contraction and near
expansion zones.
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to remain focused over a particular region, specifically over
the interfacial region of the dispersed and carrier phases.
Moving a step ahead, one can conduct a controlled reaction,
and thereby separate the reaction-product over the targeted
location, using the present setup. Moreover the reaction
product is found to be deposited over the bottom surface of
the channel along a track parallel to the interfacial region of
the two fluids. The splitting and subsequent focusing ability
of the present setup primarily stems from the geometry
assisted convergence and divergence of the streamlines, and
thereby induces the dispersed particles to trail along. The
controlled deposition, on the other hand, endorses a simple
strategy for bottom-up fabrication of microscale features.
Acknowledgements
The authors are thankful to the CSIR-CMERI, India, for the
financial support through the projects OLP-190312 and OLP-
101512. The authors also acknowledge the help of the insti-
tute CRF facility for conducting SEM studies.
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