www.elsevier.com/locate/ces
Abstract
A systematic engineering study on continuous synthesis of bismuth metal nanoparticles by vapor condensation in tube $ows is presented.
Simulations of aerosol nucleation, condensation and coagulation are cast in a design diagram format to guide experimental studies on
the e4ect of process parameters on product nanoparticle characteristics. Flow visualization, tracer gas analysis and computational $uid
dynamics are used to unravel the e4ect of particle residence time distribution on product morphology during evaluation of alternate
quenching designs for the metal vapor. Bismuth nanoparticles of average diameter 12–37 nm, as determined by nitrogen adsorption and
X-ray di4raction, were made by controlling the quenching gas $ow rate, carrier gas $ow rate and process pressure. ? 2002 Elsevier
Science Ltd. All rights reserved.
Keywords: Design; Nanostructure; Particle formation; Fluid mechanics; Bismuth; Inert gas condensation
0009-2509/02/$ - see front matter ? 2002 Elsevier Science Ltd. All rights reserved.
PII: S 0 0 0 9 - 2 5 0 9 ( 0 2 ) 0 0 0 6 4 - 7
1754 K. Wegner et al. / Chemical Engineering Science 57 (2002) 1753–1762
the heated crucible. The particle transport by forced convec- 2:2 mm i.d. Inconel tube. This inlet tube is supported by a
tion resulted in a reduction of number concentration and res- stainless steel $ange which also closes the feed side of the
idence time of the nuclei so that smaller nanosize powders pipe and contains connectors for pressure and temperature
could be produced. Konrad, Haubold, Birringer, and Gleiter sensors.
(1996) applied continuous gas $ow also for the synthesis of On the other side of the Inconel pipe a stainless steel lance
nanosize copper–bismuth alloys by co-evaporation. Copper consisting of a center tube and three annular tubes forms a
crystallites with up to 10% bismuth could be synthesized by diluter, heat exchanger and condenser outlet (Fig. 1). The
directing the gas $ux over Crst the copper and then the bis- 16:5 mm i.d. center tube of this lance (diluter-tube) carries
muth melt. The jet aerosol $ow condenser was investigated the product aerosol to a glass Cber Clter (Whatman GF=A) in
further by Haas, Birrringer, Gleiter, and Pratsinis (1997) for a stainless steel Clter holder with the help of a vacuum pump
the synthesis of palladium nanoparticles with primary par- (Vacuubrand RZ 16). Cooling water of 5◦ C $ows through
ticle median diameters of 2–11 nm. Compared to IGC pro- the Crst and third annulus of the lance at a $ow rate of 60 l=h.
cesses relying on free convection, an 80% reduction in the An argon stream (Pan Gas 99.999%) is introduced into the
primary particle median diameter and a 17% reduction in condenser through the second annulus between the cooling
the geometric standard deviation of the primary particle size water shell as quenching gas. This quenching gas discharges
distribution could be achieved with this aerosol $ow con- in counter$ow to the aerosol jet through 12 equally sized
denser. Tsantilis, Pratsinis, and Haas (1999) combined com- nozzles with an inner diameter of 2:5 mm which are uni-
putational $uid and monodisperse particle dynamics to de- formly arranged at the front side of the lance as shown in
scribe the $ow pattern and particle formation in this aerosol the photograph in Fig. 1 (cap-free diluter). The schematic
$ow condenser. in Fig. 1 shows a stainless steel gas return cap which can be
Here, the synthesis of metal nanoparticles by vapor con- mounted on the diluter to guide the quenching gas perpen-
densation is systematically investigated. Aerosol process de- dicularly to the Bi-laden carrier gas stream, thus forming a
sign is used, for the Crst time to our knowledge, to guide T-mixer. This cap can separate the evaporation zone from
experimental studies on the e4ect of process parameters (va- the condensation (quenching and particle formation) zone
por quenching rate, temperature and pressure) on product of the unit (cap-diluter). Here, the performance of the two
metal nanoparticle characteristics. Hence, synthesis of bis- diluter (or quenching gas) conCgurations in gas cooling and
muth nanoparticles is investigated as these particles are used mixing is investigated for their e4ect on particle formation.
for dry phototools in the production of printed circuit boards An additional water-cooled heat exchanger is connected
(Eickmans et al., 1996). The 200 nm-thin bismuth imaging with a gate valve to the outlet of the diluter and cools the
layer of these phototools must be uniform and requires parti- aerosol to a temperature of 30◦ C at the Clter. This temper-
cles to have average diameters of 50 nm or less, a low degree ature is recorded at the center of the Clter with a type K
of agglomeration and a reasonably narrow primary particle thermocouple and controls the cooling water $ow rate. A
size distribution (Eickmans et al., 1996). Here, bismuth va- precision needle valve $ow controller (Bronkhorst EL-Flow
por is produced in an externally heated tube $ow condenser 201 A) connected to the gas-side inlet of the heat exchanger
containing a crucible with the Bi melt. Transport of the va- (10 cm after the diluter and 30 cm before the Clter) allows
por in an argon carrier gas jet is followed by rapid quench- the addition of trace amounts of oxygen (Pan Gas, 99.999%)
ing with a second argon stream (in a diluter) and by particle to the aerosol stream. All tube connections are made with
collection on a Clter. This experimental design is selected vacuum $anges (Balzers KF-series) to allow gas-tight op-
as it separates the evaporation from the particle formation eration at subatmospheric pressure. The carrier and quench-
zone (during quenching) allowing to systematically study ing gas streams are controlled by calibrated mass $ow
the in$uence of cooling rate and quenching conCguration controllers (Bronkhorst EL-Flow 201 A and AC). The
on product particle characteristics using nitrogen adsorption, pressure in the condenser is measured by a capacitative
transmission electron microscopy and X-ray di4raction. pressure sensor (MKS Baratron) and is controlled by a
butter$y valve (MKS 653B) at the inlet side of the vacuum
pump.
2. Experimental
Fig. 1 shows a schematic of the jet aerosol $ow con- Prior to heating the unit, the ceramic crucible was loaded
denser unit. The middle section of an Inconel pipe (length with about 5 g of bismuth granules (Fluka, 99.9995%) and
1000 mm, inner diameter 52:5 mm) is heated to the desired placed at the appropriate position in the $ow condenser.
process temperature by a tubular furnace (Carbolite CFM The condenser was closed air-tight, purged with argon to
14=1) to evaporate bismuth from an alumina crucible (Alsint a pressure of 1500 mbar and evacuated to 0:1 mbar after-
99.7). From the pipe inlet (feed side) argon carrier gas (Pan wards. This procedure was repeated three times to remove
Gas, 99.999%) is introduced above the crucible through a air from the system. The condenser was then closed with
K. Wegner et al. / Chemical Engineering Science 57 (2002) 1753–1762 1755
Fig. 1. Schematic of the aerosol $ow condenser with its Inconel pipe (1), the crucible containing the bismuth melt (2), the furnace (3), the evaporation
zone (4), and the cap-free diluter (5). An inset schematic shows the diluter conCguration with gas return cap (6) used to introduce the quenching gas
perpendicular to the Bi-laden carrier gas jet.
the gate valve, Clled with argon to atmospheric pressure (Micromeritics Gemini 2306) employing the BET isotherm.
and heated at a rate of 25◦ C=min to the operating temper- Assuming all particles to be monodisperse spheres,
ature of 1000◦ C. After the set temperature was reached, the BET-equivalent particle diameter was calculated as
the gate valve was opened slowly and the argon $ow rates dp = 6=(Bi SSA), with the density of bismuth at room
and system pressure were adjusted to the desired operating temperature being Bi = 9790 kg=m3 (Lide, 1997). Trans-
conditions. The oxygen concentration in the particle col- mission electron microscopy (Hitachi H600, operated at
lection region was set to 1000 ppm with the needle valve 100 kV) was employed to determine the morphology of the
$ow controller in order to form a passivating oxide layer bismuth nanoparticles. Therefore, 0:2 mg of powder was
at the surface of the freshly produced bismuth particles suspended in 1 ml of toluene (Fluka, ¿ 99:5%) and 0:1 ml
(Russell, 1967; Uchikoshi, Sakka, Yoshitake, & Yoshihara, of the surfactant octyltrimethoxysilane (Fluka, ¿ 97%) be-
1994). Without oxygen, bismuth nanoparticles with diame- fore it was applied to a TEM grid. X-ray di4raction analysis
ters smaller than 18 nm rapidly oxidized after exposure to (XRD, Siemens D 5000, Cu K radiation) was performed
ambient air. In a standard experiment the furnace temper- over an angle of 20◦ ¡ 2 ¡ 60◦ in steps of 0:02◦ . Care
ature was 1000◦ C, the pressure 1000 mbar, while the oxy- was taken that all characterization methods were carried out
gen, carrier and quenching gas $ow rates were 11:5 × 10−3 , right after synthesis since bismuth nanoparticles slowly oxi-
1.5 and 10 l=min, respectively. Experiments were carried dize in air and can completely transform into bismuth oxide
out from 200 to 1000 mbar, carrier gas $ow rates of 0.75 after a few weeks, as was observed in the course of this
–3:0 l=min and quenching gas $ow rates of 5 –20 l=min. All work.
volumetric $ow rates are reported at 25◦ C and 1013 mbar. Centerline temperatures in the $ow condenser were
After each experimental run the gate valve was closed and recorded at 1000 mbar and a furnace set temperature of
the Clter was changed in ambient air. If no further exper- 1000◦ C for quenching gas $ow rates of 5, 10, 15 and
iments were performed, the condenser was slowly cooled 20 l=min and a carrier gas $ow rate of 1:5 l=min. Therefore,
down to room temperature. Each experiment was performed a 750 mm long S-type thermocouple with a 0:5 mm bead
twice and found to be reproducible within 5% of the product supported by an alumina tube (o:d: = 4 mm) was introduced
speciCc surface area (SSA). from the unit outlet. The thermocouple was mounted on an
xy-positioning table allowing precise positioning inside the
2.3. Measurements condenser. Temperatures were recorded every 2 cm inside
the evaporation zone and every 1 cm in the quenching zone.
The average speciCc surface area (SSA) of the pow- Measurements were performed for both the cap-free and
ders was determined by nitrogen adsorption at 77 K the cap-diluter.
1756 K. Wegner et al. / Chemical Engineering Science 57 (2002) 1753–1762
2.4. Flow characterization jet at an outlet temperature of 1000◦ C is about 400 for an
argon $ow rate of 1:5 l=min, indicating that the $ow in the
Cold $ow visualization experiments were carried out in a condenser is in the transition regime (Bejan, 1984). There-
transparent (quartz glass) unit of similar dimensions at room fore, the simulations were performed using the RNG k–
temperature and pressure in order to visually study the in$u- model (Yakhot & Orszag, 1986) provided by FLUENTTM
ence of the diluter cap on the $ow pattern of particles inside for $ows in the transient regime (Fluent Inc., 1998) ac-
the condenser. Therefore, the crucible was Clled with am- counting for low Reynolds number e4ects. The tempera-
monia solution (NH3; aq , Aldrich 24%) while the carrier gas tures at the condenser walls were measured and set as con-
was saturated with hydrochloric acid (HClaq , Aldrich 25%) stant boundary conditions for the simulations. At a furnace
in a bubbler prior to introduction into the unit, leading to the set point of 1000◦ C, the plate supporting the carrier gas
formation of ammonium chloride particles above the cru- nozzle, the nozzle itself and the carrier gas had a temper-
cible (Dahlin, Su, & Peters, 1981). A vertical plane through ature of about 980◦ C. A temperature of 680◦ C was mea-
the center axis of the condenser was illuminated with a laser sured for the walls of the cap, while the temperature of the
sheet created by an argon laser (Lexel 95, operated at 2:5 W) diluter-tube and the quenching gas was 5◦ C. The outer walls
and a plano-concave cylindrical lens (Newport CKV513-C). of the evaporation chamber exhibited a temperature proCle
The laser light was scattered by the ammonium chloride par- which could by approximated with the parabolic function
ticles (corresponding to the bismuth particles of the present T (◦ C) = −2:58x2 − 1:50x + 980, where x (cm) is the dis-
experiment) and made the $ow pattern in the unit visible. tance from the condenser inlet. The wall temperatures did
Photographs of $ow patterns were taken with a digital cam- not vary for di4erent operating conditions.
era (Minolta RD 175) for carrier and quenching gas $ow A monodisperse particle dynamics model accounting
rates of 1.5 and 10 l=min, respectively. for simultaneous nucleation, condensation and coagulation
The residence time distribution of the carrier gas in the (Panda & Pratsinis, 1995) was employed to derive a de-
$ow condenser was investigated by introducing CO2 (Pan sign diagram for synthesis of bismuth nanoparticles in a jet
Gas 99.995%) as a tracer into the carrier gas stream at the aerosol $ow condenser (Tsantilis, Pratsinis, & Haas, 1999).
unit inlet and detecting the CO2 concentration at the unit out- SpeciCcally, the e4ects of the evaporation temperature Tv
let with a mass spectrometer (Balzers GSD 300 O). There- (K) and the inert gas $ow rate Qr (l=min) on bismuth aver-
fore, a sampling loop was loaded with 3 ml CO2 and in- age particle diameters were investigated. The Bi properties
stantly discharged into the argon carrier gas stream with the of importance were surface tension (Frurip & Bauer, 1977):
help of a GC valve (C. Erba S.A. 40541), thus creating a
Dirac peak. The time between the discharge of the sampling (J=m2 ) = (418 − 0:07 × T )=1000 (1)
loop and the drop of the CO2 concentration in the outlet gas
to its initial value was recorded along with the CO2 concen- and vapor pressure (Hultgren, Desai, Hawkins, Gleiser, &
tration. Kelley, 1973)
Temperature and velocity proCles inside the $ow con- Furthermore, the nucleation rate was given by Girshick and
denser were simulated using the commercially available Chiu (1990), while the collision frequency coeTcient for
computational $uid dynamics (CFD) software FLUENTTM Brownian coagulation was based on the Fuchs interpolation
5.2. The geometry of the condenser can be taken as axisym- function from the free molecular to the continuum regime
metric if the in$uence of the crucible on the $ow is neg- (Seinfeld, 1986). The design calculations were carried out
ligible and the 12 outlet nozzles of the quenching gas are for a tubular aerosol $ow condenser with dimensions con-
modeled as an annular slit providing the same average gas sistent with those of the diluter (quenching zone) of the ac-
outlet velocity. The in$uence of these simpliCcations on the tual experimental setup (i:d: = 16:5 mm). In addition, it is
$ow characteristics inside the unit was evaluated by carry- assumed that the argon carrier gas is saturated with bismuth
ing out a three-dimensional (3-D) simulation for the actual vapor and enters the condenser at evaporation temperature
geometry at a system temperature of 1000◦ C, a pressure of TV (ranging from 1000 to 1150 K) and $ow rate Qr (quench-
1000 mbar and a carrier gas $ow of 1:5 l=min and compar- ing and carrier gas, ranging from 5 to 20 l=min) at 1 atm. For
ing it to the two-dimensional (2-D) axisymmetric conCgura- every set gas $ow rate, the temperature was assumed to drop
tion without crucible. The time-consuming 3-D simulation linearly with a constant gradient of (TV − TL )=L = 50 K=cm
revealed only a minor de$ection of the carrier gas jet by the over the investigated length of L = 10 cm. Therefore, the
crucible presence which was negligible for the study of the cooling rate at the exit of the condenser was calculated as
overall $ow pattern in the condenser. Thus, all CFD simu-
TV − T L 4Qr TL
lations here were made for the 2-D axisymmetric geometry C (K=s) = (3)
described above. The Reynolds number of the carrier gas L D2 Tr
K. Wegner et al. / Chemical Engineering Science 57 (2002) 1753–1762 1757
The formation of dead volumes shown in the $ow simu- 4.2.2. Temperature
lation was veriCed by measuring the residence time distri- Fig. 7 shows the condenser temperature along the center-
bution (RTD) of carrier gas, following the CO2 tracer gas line with the corresponding saturation ratio S =p=ps for both
concentration. Fig. 6 shows the response signal to a Dirac the cap-free and the cap-diluter, where p is the partial pres-
peak of CO2 that is inserted at t = 0 into the carrier gas sure of bismuth calculated with the evaporation rate from the
stream for each diluter conCguration. For the cap-free di- crucible and ps is the saturation vapor pressure of bismuth
luter (Fig. 6a) most of the tracer leaves the unit after about (Eq. (2)). The temperature in the unit with cap-free diluter
3:5 s, creating a sharp peak with a small shoulder toward decreases almost linearly with the distance from the carrier
longer residence times, which indicates that only a small gas nozzle (925◦ C) and reaches 570◦ C at the entrance of the
fraction of the gas is trapped in dead volumes, as was pre- diluter-tube, 11 cm from the nozzle exit. This rather steep
dicted by the $ow simulation (Fig. 5a). After 10 s, all CO2 temperature decrease is due to the dilution of the Bi-laden
has left the unit. Placing the cap on the diluter drastically carrier gas with cold quenching gas, as is shown in Figs. 4
alters the residence time distribution, as can be seen by com- and 5. The temperature gradient remains unchanged inside
paring Fig. 6a with Fig. 6b. The maximum of the response the diluter-tube and a temperature of 380◦ C is reached after
still exits the unit after about 3:5 s, the height of the peak 19 cm from the nozzle exit. Temperatures are much higher
representing a normalized CO2 concentration, however, is in the evaporation zone with the cap-diluter since quenching
only about half the value of the one detected before. The gas does not enter this region (Figs. 4 and 5). A tempera-
RTD exhibits a distinct shoulder for t ¿ 4 s, indicating that ture of 780◦ C is obtained at the cap face, 10 cm from the
a considerable fraction of the tracer gas is trapped in dead carrier gas nozzle. With the cap-diluter a steep temperature
volume and is slowly released over a period of about 20 s. gradient results inside the diluter-tube, giving a temperature
This di4erence in RTD can be explained by the visualization of 260◦ C after 19 cm from the inlet nozzle. This is about
and simulation of the $ow patterns shown in Figs. 4 and 5. 120◦ C lower than for the cap-free diluter and shows the su-
In the cap-free diluter conCguration, carrier gas which does perior performance of this conCguration in gas quenching
not directly exit the condenser is transported back to the in agreement with literature (Chilton & Genereaux, 1930;
upstream region by the counter-$owing quenching gas and Forney, NaCa, & Vo, 1996).
1760 K. Wegner et al. / Chemical Engineering Science 57 (2002) 1753–1762
Fig. 9. Axial centerline temperatures for the cap-diluter and four quenching
gas $ow rates (carrier gas $ow rate: 1:5 l=min, pressure: 1000 mbar, fur-
nace set temperature: 1000◦ C). Steeper temperature gradients are achieved
at higher quenching gas $ow rates.
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