Fast mixing by lamination.

Jens Branebjerg, Peter Gravesen, Jens Peter Krog and Claus Rye Nielsen
Danfoss AIS, DK-6430 Nordborg, Denmark
Phone: (+45)74 88 24 39, Fax: (+45) 74 88 40 00, E-Mail: dktlfowqx@ibmmail.com

ABSTRACT macroscopic wsrld, such as stirring or creation of

A micro mixer based on multistage multi-layer
lamination is presented. The micro mixer has been
designed as an integrated part of a micromachined
chemical analysis system. The fabrication technology is
based on wet chemical etching of PYREX-glass and
Silicon substrates which are subsequently bonded
anodically ,
The micro mixer is designed to work in the flow
range 1 - 10 pl/min with a Reynolds number less than 1
and an undisturbed lamina1 flow pattern.
Comprehensive theoretical studies and computer
simulations have been carried out in order to understand
the detailed flow behaviour and diffusion in the mixer,
and to set up design criteria needed to obtain perfect or
near perfect multi-layer lamination.
As a result of the study of a generic type of micro
mixer and flow simulations, the need of a "separation
plate" inside each mixer stage is revealed.
The performance of micro machined single stage
mixers has been verified by mixing experiments using the
fast reaction of phenol-red and an acid. The experimental
set-up takes advantage of the transparent PYREX-glass
plate offering the possibility to study mixing phenomena
by video microscopy.
INTRODUCTION
Effective mixing is important in many
miniaturised flow systems. In Micro Total Analysis
Systems (pTAS) fast mixing can reduce the analysing
time and improve process control in industrial
applications [I]. In miniaturised chemical synthesis
reactors fast and effective mixing combined with good
conditions for temperature control in micro reactors give
new possibilities in control of exothermic processes [2].
Further, subsecond mixing will improve research in
kinetic events in flow injection and cytometric analysis
~31.
Mixing in general follows a two-step sequence.
First segmentation where a heterogenous miixture of
substantially homogenous domains of the two fluids is lamination, and ways of realizing such a lamination in a
formed by convection, and secondly interdiffusion of micro fabricated device have been proposed by at least
molecules between nearby domains.
Segmentation procedures, well known from the Ilmenau [7].
turbulent flow cannot be scaled down to mini or micro
systems with dimensions so small, that Reynolds numbers
exceeding 2000 (the limit for turbulent flow) are not
feasible.
In miniaturized flow systems with Reynolds
numbers in the range from 2 to 100 it is possible to
design flow-structures which will take advantage of inertia
forces to assist segmentation. Segmentation by shear
forces was utilised in a coaxial mixer which had an inner
core liquid stream at a low flow rate and an outer flow
stream at a higher flow rate [3]. The measured mixing
time in the coaxial mixer was 55 ms at a Reynolds
number of 5. Another example of mixing by inertia forces
was demonstrated in a zigzag formed channel. The two
liquid streams flowed along each other in a 300 pm x 600
p m x 100 mni clhannel including 80 zigzags, and mixed
in 1 second at a Reynolds Number of 33 [l].
In microfluidic structures with Reynolds numbers
below 1 segmentation is only possible by the way in
which the two fluids are merged, and the mixing time is
dominated by diffusion. One way to obtain segmentation
is to inject one liquid into another through micro nozzles
[4]. An alternative way of decreasing the mixing time is
to stack the two flow streams in one channel as thin
layers, thus increasing the contact area as well as reducing
the diffusion length.
The miicro mixer presented in this paper works on
the principle of multi-stage multi-layer lamination of two
liquid streams. The mixer was developed for a pTAS
application for an industrial chemical sensor and was
fabricated in the same process sequence as all other liquid
handling components of the pTAS. Detailed simulations
were developed for the flow through the mixer and for
lamination and mixing of the two flow streams after the
mixer. Mixing times of 100 - 300 ms were measured for
a single stage mixer, which is in good agreement with
theory.
CONCEPT OF LAMINATION
The idea of mixing two fluids by multi-layer
two research groups: IMM [5,6], and University of

0-7803-2985-6196 $5.00 0 1996 IEEE 441

 Perfect lamination can be obtained in a flow with
a sufficiently low Reynolds number provided that the
channel system guiding the fluid is designed in such a
way that the pressure gradients in the flow channels will
force the two fluids to laminate.

Fig.2: Lamination and splitting in a planar two input two

output mixer, using a Separation plate (white) to force the
fluid f l o w s to laminate.

THEORY O F LAMINATION

A detailed theoretical description of flow and

diffusion phenomena in the laminar regime is very useful
during design and testing of mixers for microsystems. In
this section we present results on flow and diffusion for
an idealized and general geometry.
The fully developed velocity profile for laminar
flow in a straight channel of rectangular cross section of
Fig. 1: A generic two input - two output mixer including
dimensions W x H is easily found by numerical methods.
laminution and splitting shown in free 3 - 0 space.
For channels having W significantly larger than H the
Top: horizontal lam ination, bottom: vertical lamination.
velocity profile turns out to be very close to parabolic in
the direction of the short dimension and almost constant
If it is possible also to split a laminate flow in two
in the other direction except within a distance similar to
channels without disturbing its laminar nature, a cascade
H from the channel walls. This is also expected
of n subsequent mixers can be used to interlace two fluids
intuitively, as the distance to the nearest walls is the only
into one stream laminated in 2" layers.
physically important parameter for laminar flow. From
Shown in Fig.1 is a generic channel arrangement
laid out in a free 3D space. When considering symmetry our solution we find that the peak velocity (vF*) in the
middle of the channel is related to the average velocity
it is obvious that a perfect lamination and split into two
(v,,,,,~~) (as calculated from the volume flow rate) as
channels is obtained. It is even so, that depending on the
flow direction, either horizontal or vertical lamination will
be the result. In the present case, using wet etching
technology and wide channels, we prefer horizontal vpeak (' 2 1-0. 6l2 H / W )vaverage
lamination. In a LIGA-like technology with narrow, deep
channels one would prefer vertical lamination.
However, in a practical micro system it is difficult to within 1.5 % when W 2 3 H .
When solving the diffusion problem for a
realize a channel system without any limitations in 3D
laminated structure, it is useful to consider the Fourier
space. For the ease of fabrication one would prefer to
realize the structure in planar technology by surface expansion of the initial concentration profile, as it is well
known [SI that the time evolution of the concentration
structuring and bonding.
The generic channel structure shown in Fig.1 can profile is given by the time evolution of each of the
be transformed into a planar technology on one important Fourier components. Each Fourier component k decays
exponentially during the diffusion process with a time
condition: That the two fluids are kept physically
separated in all parts of the channel system where they constant 2, given by
are not flowing in the same direction. This implies the
inclusion of a thin separation plate into the planar version
Lk2
of the laminating mixer, as shown in Fig.2. Tk = ( 2 7 r - 2 -
In the following we present the fabrication, simulation
D'
and experimental results proving the feasibly of a micro
mixer including a separation plate. where L , is the "wavelength" of the Fourier component
and D is the diffusivity.
This explains concisely what is also expected from
qualitative arguments that a 2"-layer structure can mix 4"-'
442
times faster than a 2-layer structure, as the wavelength of
the Fourier component of longest wavelength and thus
slowest decay rate scales with the layer thickness.
Fig.3: Calculated time evolutions of the concentration
profile of a dijfusing species in a laminated liquid
structure (x being the coordinate along the direction of
lamination). (a): Symmetric lamination, FZO f l o w . ( 6 ) :
Asymmetric lamination, no f l o w . ( c ) : Symmetric
lamination, f l o w . (d): Asymmetric lamination, f l o w .
Different line types correspond to different times (in units
of H2/D): full line: t=O, dashed line: t=0.005, dot-dashed
line: t=0.01, dot-dash-dashed line: t=0.02. In the case of
flowing liquid, times are sojoum times f o r the central part
of the structure.
minor benefit is obtained by lamination. The qualitative
counterpart of this argument is, that unless the outermost
layers are of half thickness, half of their content of the
diffusing species has to be distributed over all of the inner
layers before full mixing is achieved. When being of only
half thickness, they are balanced by their neighbouring
layer like all the other layers are.
However, a simple cascade of two-input two-
output mixers results in an asymmetric lamination.
Symmetric lamination can be obtained with a
modification of the first mixer into a three-input two-
output mixer which build up a (Hl4,H/2,Hl4) type of
laminate. This initial mixer can be followed by as many
regular two input two output mixers as desired for the
particular application.
In F i g 3 we have illustrated this aspect by the time
evolution of the concentration profile of the diffusing
species in the symmetric and the asymmetric case. The
time evolutions have been calculated both for a stationary
and a flowing liquid (the former being intuitively simpler
to understand). For the flowing liquid the geometric layer
thickness will decrease towards the centre of the channel
due to the parabolic velocity profile in a cascade mixer
structure; each layer still represents the same amount of
material as the corresponding layer do in the stationary
case. In the calculations all significant diffusion and
convection teirms have been taken into account (Details of
the calculations will be published elsewhere). The figure
clearly illustrates the strong effect of the slowly decaying
asymmetric component.

FABRICATION
For example, in the case of a stationary,
symmetric multi-layer lamination of initial amplitude,,C
,
The micro mixer is designed to fit in a system
the concentration profile C(x,t) being the solution to the
concept for micro liquid handling [l].In the same process
diffusion equation, can be written:
sequence it is possiblle to produce valves, pumps, filters
and mixers connected with flow channels.
The system is realised in a bonded silicon/glass
sandwich, as shown in Fig. 4. Membranes are etched from
the back side of the silicon wafer towards an etchstop
layer on the component side, filters are defined as holes
in the etchstop layer and liquid channels are etched into
the glass.
The micro mixer structure is realized by the
Here the fundamental "wavelength" L equals H/2"-', 2"
overlay of one channel etched into glass over another
being the number of layers, and (0 < x < H ) .
channel etched in silicon. In the region where the two
At the same time, the Fourier argument makes a
channels overlap, they are separated by a plate defined in
small but important detail of mixing by lamination very
the etchstop layer. The channel covered by the separation
clear: The lamination has to be symmetric, i.e. the top and
plate is constructed by underetching in the <loo>
bottom most layer should be of only half thickness
direction through slits in the plate.
compared to the other layers. Otherwise, i.e. if the
lamination is asymmetric, the Fourier expansion of the
initial profile will contain a component with a wavelength
twice the channel dimension, no matter how thin the
laminated layers are. This component will sooner or later
become dominant because of its slow decay, and only a
443
Fig.4: A cross section of the bonded silicon/glass vafer showing a sequence of system components, f r o m left to right:
inlet with filter, inlet valve, p u m p membrane, outlet valve, 2:l switching valve, mixer, outlet with filter.

mixing was complete.

Fig.5: SEM-micrograph of three under-etched silicon
plates f o r 3 micro mixers coupled in a cascade. The plates
have been underetched through slits parallel to the <I OO>
direction.
The liquid flow into the micro mixer was
controlled by differential hydrostatic pressures ranging
from 0.2 to 5 kPa resulting in flow rates from 0.5 to 12
pl/min which were measured by weighing the output
liquid. The mixing process in the micro mixer was studied
with a video microscope having a spatial resolution of 5
pm and recorded on tape with a time resolution of 40 ms.
The mixing time was determined by measuring the
distances from the mixing point to the point of complete
mixing, the knowledge of the flow rates, and the flow
profiles in the outlet channel.

The liquid channels in the system are 300 pm

wide and 30 ym high; only in the inlet branches to the
micro mixer the channels are 150 pm wide. The
separation plate is 5 ym thick and has 15 pm wide slits.

EXPERIMENTAL CHARACTERISATION
The purpose of the experimental characterisation
was to measure the time for complete mixing of two
liquids in the micro mixer and to study inhomogenety in
the mixing across the outlet channel. The reaction of a
pH-indicating phenol-red and an acid was chosen to
visualize the mixing process by studying the colors of the
liquids through the glass wafer. The chemical reaction
between phenol-red and an acid benefits from being
extremely fast and therefore the time for lamination of the the range of 100 - 300 ms. The measured mixing times
two input liquids and complete formation of the resulting
color reaction product was practically identical to the
mixing time. The color of the reaction product was
yellow and transparent compared to the dark red color of
unreacted phenol-red. Therefore, when the color all
through the liquid stream had changed to clear yellow the
' #
Fig.6: A video microscope print of the mixing process in
the micro mixer. The dark liquid entering f r o m the upper
left is phenol-red, it laminates in the mixer with an acid
coming f r o m the lower left. The outlet towards the right
is evenly yellow at the picture frame, and thus fully
mixed.
At equal input flow rates the mixing time was in
did not correlate with the flow rate, and the variation in
the measured mixing times may be a result of our criteria
of complete mixing, which were based on human
judgement of when the color was homogenously changed
to yellow all across the outlet channel.
Based on the theory presented above, one can

444
 ~

calculate a mixing time ( tmix= 3 ~ = , 274 ms ), noting sufficient length to fulfil its purpose
that ( L, = 2H = 60 pm ) and using a value of ( D = I I
mm2/s ).
In the mixing process shown in Fig.6 the red
(dark) pH-indicator and the clear acid flow into the micro
mixer from the left. Incompletely mixed zones are seen in
the micro mixer to the right of the separation plate and in
the centre of the outlet channel. The last part of the outlet
channel has clear yellow zones with complete mixing.
The dark zones in one of the input channels and on the
right side of the outlet channel are caused by
imperfections in the glass. The incomplete mixing zones
in the centre and left side of the micro mixer and in the
outlet channel are a result of an uneven thickness of the
laminated liquid layers due to flow of the red pH-
indicator through the slits in the separation plate. 100 micrometer
+ - i I

Fig.7: Simulated cross-flow in the separation plate (see

DISCUSSION OF UNEVEN LAMINATION
text f o r details). The plate is indicated by U coarse gray
color. Other gray colors are contours of the velocity
When the mixer is produced by the technique
perpendicular to the plate (directed up through the plate
described above, uneven lamination caused by flow
everywhere above the dashed symmetry line and vice
through the slits in the separation plate is a potential
versa). The entrance channel above the symmetry line
problem. The magnitude and possible effects of this cross-
goes beneath the separation plate and vice versa.
flow have been addressed theoretically in addition to the
experimental work described.
Fluid dynamic simulations based on standard
In a single step mixer uneven lamination is a
finite-volume methods [SI as implemented in the Star-CD
serious problem as the uneven lamination is counteracted
software have been applied to estimate the cross-flow
only by diffusion over a length scale of the order of the
under typical operational conditions. The simulations are
channel width. If several mixers are used in a cascade,
based on the real geometry with only minor
alternating lefb'right inversion of the mixer geometries
simplifications: The shape of the slits near the edge and
will reduce the effect of uneven lamination in two ways:
the centre line is simplified (see Fig.7), the separation
In each of the earlier mixers where the lamination is still
plate is taken to be infinitely thin, and the steps in the
coarse compared to the cross-flow, the net displacement
"lower" channel at the transition from the glass plate to
of one liquid will be in the opposite direction compared
the silicon wafer several times the channel height away
to the previous mixer step due to the left/right inversion.
from the region of interest have been neglected. A flow
In later mixer steps where the lamination is fine compared
of water (at 20°C) of 0.50 pWmin in each input channel
to the cross-flow, the unevenness is diluted away. Locally
is assumed (Details of the simulations will be published
uneven layer thickness along the short dimension of the
elsewhere). The calculated flow velocity perpendicular to
channel is of minor importance as diffusion in this
the separation plate in the plane of the plate is shown in
direction is fast. It should be pointed out that the problem
Fig.7. From these velocities, the total cross-flow in either
of uneven lamination is not a fundamental problem of the
side of the channel is obtained by integration over the slit
present design: The whole idea of the separation plate is
areas
to avoid cross-flows and the slits which are needed only
As it is expected from qualitative arguments valid
for the fabrication process can easily be optimized further.
when the flow is governed by pressure gradients rather
A reduction of slit width from 15 to 5 pm will reduce the
than kinetic energy, the direction of the cross-flow is so
cross-flow by nearly one order of magnitude [IO] or to
that the liquids tend to remain in the side of the mixer
about 4% of Ihe main flow. A 4% cross-flow will not
structure where they initially entered. The magnitude of
influence the lamination process significantly, and 5 pm
the cross-flow is estimated to 0.088 pL/min on either side
slits are thus regarded as a reasonable trade off between
of the symmetry line corresponding to 35 % of the fluid
performance and ease of fabrication.
otherwise flowing in a quarter of the total channel defined
by the symmetry line and the separation plate. It should
be noticed that 83 % of the cross-flow go through the
first slit, 15 % through the second, and only 2 % through
the third, confirming that the separation plate has

445
 CONCLUSIONS
A micro mixer for fast mixing in laminar flow has
been developed. In the mixer two liquids are guided on
top of each other and kept separated by a plate until they
are forced to laminate. The fast mixing is a result of the
increased contact area and decreased diffusion length,
when the two liquids were stacked in a rectangular
channel.
The micro mixer structure was fabricated in a
process sequence together with pumps, valves, filters and
fluid connections, in a liquid handling system of a Micro
Total Analysis System (pTAS). The micro mixer was
designed to be coupled in a cascade to obtain multi-layer
lamination, and the small size of the micro mixer with its
dead volume of less than 10 nl, ensured fast mixing even
at low flow rates.
The performance of the micro mixer was verified
by video microscope investigation making it possible to
detect complete mixing across the whole outlet channel of
the micro mixer and in its full depth. Complete mixing in
the hole cross section of the outlet channel was obtained
in 100 - 300 ms. Prior to complete mixing, zones were
observed with incompleted mixing due to liquid flow
through the slits in the separation plate of the mixer.
The consequences of the cross-flow through the
separation plate were verified by 3D-flow simulations of
the micro mixer. Furthermore, the simulations showed
that a reduction of the width of the slits to 5 pm in future
designs will reduce the undesired cross-flow through the
separation plate by nearly one order of magnitude, and in
practice make the micro mixer perform as if the plate was
without slits.
A fluidic theory was derived to describe the time
for mixing in a single mixer as well as in a cascade
coupled mixers after multi-layer lamination. Cascading n
mixers will, when done in the right way, reduce the
mixing time by a factor of 4w1and counteract a possible
uneven lamination in a single mixer.
The developed micro mixer ensures sufficient
mixing in the pTAS for process control in industrial
applications, which was the primary goal of this work.
Implementation of the described improvements in the
design of the micro mixer is predicted to result in mixing
times of a few milliseconds, which will be attractive in
more demanding applications like in micro reactors and
studies of kinetic events.
446
ACKNOWLEDGEMENTS
This work was performed as part of the Materials
Centre for Microelectronics (MCM) program, supported
by the Danish Agency for Trade and Industry, The Danish
Natural Science Research Foundation, and the Danish
Technical Science Research Foundation under the
Materials Development Program.
We would like to thank the staff of the
Mikroelektronik Centret, at The Technical University of
Denmark, for supporting our work. Especially Gert
Blankenstein is thanked for his support and help in the
experimental characterisation of the micro mixers.
Michael Skovgaard, Danfoss Compressors GmbH,
Flensburg, is acknowledged for inspiring discussions of
flow phenomena and careful and professional help with
the fluid dynamics simulations.
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