ELECTRICAL CONTROL OF PARTICULATE P O L L U T A N T S

FROM FLAMES
D. R. HARDESTY* AND F. J. WEINBERG

Department of Chemical Engineering and Chemical Technology, Imperial College, London, England
Following the demonstration that growth and deposition of flame carbon can be controlled
by applied electric fields, the object of the present study is to extend this principle to particulate
pollutants from flames in general. The aim is to use suitable field configurations, so as to cause
the fl'ee charges produced during chemi-ionization to attach to particles, even in the absence
of any other spontaneous charging mechanism. The abundance of chemi-ions in hydrocarbon
flames, prevented from recombination by the applied field, replaces the corona discharge of
"electrostatic" precipitation which is so wasteful of power. The optimum charging conditions
are investigated theoretically. Since the trajectories in fields of particles of known size and
charge (and, hence, mobility) are accurately predictable, these parameters are measured experimentally. In addition to drawing on previous results for flame carbon, particles of Si02
from hexamethyl disiloxane and the products of tetraethyl lead, both injected into premixed
methane/air flames, are studied. Allowing for the difference that, unlike carbon, these particles
cannot be made to burn up, their behavior is generally similar. In particular, their deposition
in fields and decrease in particle size, brought about by field-induced shortening of residence
times, allow a similar degree of electrical control to be exercised. In the case of lead oxide,
difficulties arise when the flame temperature exceeds its low boiling point, because it is then
present as a vapor in the zone in which charges usually attach. This leads to the proposal and
testing of an alternative system in which a second flame is used as an ion source in a cooler
part of the product stream. This may prove of practical use, particularly where a second-stage
flame is used to combat incomplete combustion. The theory of charge acquisition is generalized
1o allow prediction of performance and optimization of design.
Principles

that the entire process of burning sprays and

particulate dispersions can be controlled electrically, all the way from electrical dispersion
and charging, over mixing with air inducted by
ion pumps, to burning controlled by fields.
Such methods obviously have great scope for
controlling particulate pollutants. The trajectory of a particle of radius (rp) carrying (Ne)
charges in a field (E) is accurately predictable1
in terms of its mobility (kp). For all the conditions relevant here a quasi-steady state analysis
will accurately describe the particle motion. The
instantaneous field-induced velocity (vp) is
therefore simply related to the local applied field
intensity by

The application of electric fields to charged

dispersions makes it possible to alter particle
trajectories. I n this way, fully formed particles
may be caused to deposit in specified places or
to burn up if they are combustible, while, by
applying fields to the region in which they are
formed, their rate of formation, their size, or
concentration may be modified. Examples of
manipulating particles electrically range from
established industrial practice to laboratory
curiosities. The best knowI1 are probably electrostatic precipitation and paint spraying under
the influence of electric fields. More-recent developments include control of carbon formation
in flames, as regards its amount, particle size,
and deposition. ~,2 Very recently, 3 it was shown

vp----kpE.

(1)

The "small ion" theory 4 (Knudsen Number,

* Present address: Sandia Corp., Albuquerque,
New Mexico.

hp/r~>>l), in which the free molecular path

regime is perturbed by dipole forces induced in
907

908

POLLUTANT FORMATION AND DESTRUCTION IN FLAMES

colliding gas molecules by the charge-carriers:

kp= [-0.235/(Do-- 1 )0.5][-(M+Mp)/MMp]O.5

(oo/o),

(2)

is applicable to ions, but not to the particles

here considered. Even for the smallest of these
aggregates, the effects of divergence of the field
induced around them by their own charge is
negligible and application4 of classical kinetic
theory gives
kp= [-0.75 (Ne)/Mup'][-l+ ( M / M p ) ] .5. (3)
For the case where particles are large and
massive, compared to individual gas molecules,
but smaller than their mean free path, Eq. (3)
becomes

lop= (0.75Ne/lrhp ) (I/rp ~)

= (0.75Ne/p) (k T/S~rm )o.5 (1/r~).

(4)

For particles large in comparison to the mean

free path, the gas is no longer sensed in terms of
individual collisions. Particle motion is determined principally by the balance of electrical
and drag forces. Depending upon the Reynolds
Number, based on particle diameter, the relevant
gas properties become the viscosity (7) and the
density (p). In the Stokes regime, where Re<3,
the mobility becomes

kp = Ne/6~r~r~.

(5)

In the Newton regime, where 700< R e < 2 X 105,

the mobility is given by

lop= (Ne/O.22~rpE).5(1/rp).

(6)

The appropriate expression for the transition

regime, where 3_<Re<700 is not obvious. The
relationship,

kp = O.12 (Ne)o.71/r p ( Ep )o.29(~?)0.43,

(7)

based on linear interpolation of the drag law,

has been proposed.5
A complete specification of particle trajectories
under any set of conditions follows from combining the predictions of mobility, taking into
account the time rate of change of particle size
and charge, the distribution of field intensity,
and consideration of convective effects. The

velocities so predicted have recently been verified for electrically sprayed fuel droplets, using
both photographic particle tracking and Doppler
velocimetry techniques. 6
The main object of this paper is to explore
methods by which particulate pollutants can be
caused to acquire charge most efficiently, in
flame systems. For the purpose of the subsequent
discussion; the wide variety of mechanisms by
which charge can be acquired (e.g., see Ref. 1 )
may be roughly subdivided into spontaneous
charging (e.g., thermionic electron emission) and
attachment, by one of several mechanisms, of
free ions or electrons.
Although the spontaneous processes (i.e.,
those occurring in the absence of fields) can produce a charged cloud---e.g, of soot particles7 they are less amenable to direct control. For
particles for which they are significant, they
can always be assisted by those mechanisms
which are controllable by fields.
In terms of minimizing the wastage of charge
deliberately provided, dispersion in a field (but
in the absence of breakdown) is ideally efficient.
In this, the particulate phase may be regarded
as the fragments of an initially continuous
charged capacitor. This principle has been used
in combustion, ~ but is applicable only to systems
in which the particles are available as an initially
continuous phase. "Electrostatic" precipitation,
on the other hand, is very inefficient due to
its wastage of the charge generated. A great deal
of power is required to ionize the gas in a corona
discharge, following which the majority of the
free charges created flow to the opposite electrode
without attaching, their great velocity being a
necessary consequence of the high fields required
to achieve breakdown. (A limited amount of
slowing down can be arranged by causing the
field lines to diverge.)
In the presence of flame, there is a very advantageous and much neglected alternative--the
use of free charges produced during chemiionization and separated by an applied field.
Although here again there is no way of ensuring
that all the free charges will attach to particles,
at least no additional power is expended in
breaking down the gas. In the absence of a
sufficient field, the chemi-ions simply recombine
and the free charge is lost. The maximum power
dissipated is, indeed, limited by the avoidance of
breakdown in the presence of unipolar space
charge. It is very small--e.g., ir~ a unidimensional system, it is always less than 0.1 Watts/
cm2.1 In what follows, the optimum methods of
using flame ions to charge any particles present
are investigated. Any spontaneous charging is

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POLLUTANT FORMATION AND DESTRUCTION IN FLAMES

910

becomes

20
-

~t)th~
r~'--= 47rrp~b/e.

(rE) i /e i

-----

"I; : t d i f f / t b O m b

/;/

1.6

~ ..

CURVE

T (K)

300

~ooo

2000

1.2

2-~ 0.8

2. Relative Importance of Different Mechanisms

The most immediately obvious form of comparison is in terms of the time required to
acquire a specified charge for a particle of known
size (see Fig. 2). A very striking consequence of
the above-mentioned simplification is that, for
all regimes,

,,~5> /

- -

~-~>

""",,//
~v'~"

(19)

tN ~ 1 / M ,

(2o)

where tN is the time required by a particle of

radius rp to acquire a charge Ne. The inverse
square dependence of charging time on rp for
all these mechanisms is a consequence of the
circumstance, further discussed below, that, for
combustion systems subjected to large fields,
I

~0
20
E (kvl cm.)

(Edi f ft, %ombt, ethert) < 1,

30

FIG. 1. Ratios of field-induced ion velocity,

(vE)~=k~E, to ion mean thermal speed (~0, and
characteristic diffusion and bombardment charging
times (tdiu/tbo~b) as functions of electric field intensity (E) and temperature (T) for H30 + ion.
kH~o+=3.2(T/3OO)(cm2/sec V).

and in its strong dependence on work function

which makes it specific to certain substances
(some of which, however, are very important in
combustion--e.g., carbon). Nevertheless, the
equivalent simplification again applies here (see
Fig. 2). The rate of charge acquisition by
thermionic emission is
~ ) t h ~ = (4~r%:/e) exp(--Ne2/%]cT),

(16)

so that the number of charges per particle at

any given time becomes
Nth: = (r~kT/e 2) ln(l+ethe, t),

(17)

~th~,=47rerp@/k T,

(18)

where

and ~ b = A T 2 e x p ( - - e / k T ) is the thermionic

emission current density (amp/cm2), an empirically determined quantity, like the work
function ~. The relevant charging law here

(21 )

and Eqs. (10), (13), and (17) reduce to

Ndlf f---- (Ircini)r~t,

(22)

Nbomb= (37rEnikl)rp2t,

(23)

N,~hor=(4~/e)Mt.

(24)

In order to compare the relative effectiveness of

the two attachment mechanisms, the ratio of
times to acquire a given charge by diffusion and
bombardment becomes
r = tdiff/tbon, b = 3kiE/hi= 3[ (v~)i/5i],

(25)

where (vE)i is the field-induced ion velocity, and

6i the ion mean thermal speed.
It is immediately obvious that bombardment
is potentially dominant, since the maximum
value of E occurs at breakdown (Eb) (see
Fig. 1). It must be borne in mind that breakdowu sets ill at the electrode (see Ref. 1 ), for
which 2000K is not a very realistic temperature.
However, an appreciable proportion of the distance between electrodes enclosing a flame must
be at field intensities well below Eb--particularly
at sub-saturation conditions, 1 and there will be
regions in which diffusion charging dominates.
The relative importance of thermionic emission
and attachment processes, follows similarly from
comparison of the characteristic thermionic
time, tthe, to the appropriate limiting attachment
time. Assuming that bombardment charging is

ELECTRICAL CONTROL OF PARTICULATE POLLUTANTS

the dominant attachment process, Eqs.
and (24) for Nbo~b= Nther give

(23)

= tt~/tbomb = 0.75 (e/~b) Enlki

= 0.75

(j/~).

(26)

In view of the exponential dependence of the

thermionic emission current density on temperature, thermionie emission will be of increasing
importance at high temperatures, for materials
of low work function (carbon and high-boilingpoint metal oxides). It wilI be seen (Fig. 2) that,
at 2000K, for example, carbon particles become
charged by thermionic emission in a much
shorter time than can be achieved by bombardment under optimum conditions. Yet a drop of
temperature of 200K makes bombardment
absolutely dominant.
3. Optimization

As regards thermionic emission, it follows from

the above that this cannot be influenced by
modifying the electrical structure, but only the
thermal one, and is significant only for a few
materials. For these, it is important to make the
electrode on the hot side the cathode, in order
not to oppose the thermionic effect.
As regards bombardment charging, Eq. (15)
yields the maximum rate of charging as
[31rr~(jm~/e)-]. Put in this form, numerical
values can be assessed immediately, the maximization of .]~ having been extensively analyzed
(see Ref. 1 for summary), because it underlies
the optimization of most other electrical effects.
Thus, for plane electrodes maintained at STP
5 mm from a flame, j ~ - - 0 . 2 5 mA/cm 2= 1.6X
10~ electron charges/era 2, which gives the maximum rate of bombardment charging as 1.5X
1016rp2 electron charges/sec. This is shown as
the curve in Fig. 2 which lies below all but the
high-temperature thermionic charging of carbon
and barium oxide.
Optimization of diffusion charging is less immediately obvious, since very small fields allow
opposite charges to co-exist and to recombine,
while very large fields diminish (ni). Since
bombardment is dominant over all, the problem
resolves into calculating the distribution of
(ni) under conditions which optimize bombardment--i.e., ji. The relevant relationship is
ni = Iji/kie[Eo2+ (8~-jix/ki)].5},

(27)

the suffix 0 denoting conditions at the ion source,

x = 0, where diffusion charging peaks.

911

So far, we have concerned ourselves only with

the rate of charging. To maximize final charge,
the time of residence should also be optimized.
This is assisted by divergent flow, which decreases flow velocity, particularly in the regions
of high field intensity. Association of this with
a divergent field geometry further improves the
distribution of electrical parameters. As regards
bombardment charging, jm~ is increased, because of the more gradual buildup of space
charge. The maximum current density at the
flame is increased by factors of up to 2 and
1.48, in the cases of cylindrical and spherical
geometries, respectively} As regards diffusion
charging, whereas in one dimension,

fo

~nldx = (Eb/4~re)~f(x),

(28)

(that is, as long as the maximum

current density
is drawn at each position the net acquired
charge depends only on the breakdown field
strength, and there is no advantage in varying
the electrode separation distance), very considerable improvements
can result from field
divergence. For spherical geometry,
under
optimum conditions
f xo+. . . . nldx= (Eb/4~re)[lOx .... ~12--1]

(29)

O+ e

where xo, xo+e, and Xo+X .... are the positions of

the burner, flame, and second electrode, and
e/xo and xo/x .... <<1.
A further improvement results from rapid
cooling of the products. This serves not only to
decrease the linear velocity at constant massflow rate, but also increases the breakdown field
strength, which is inversely proportional to
absolute temperature ~ at the electrode and,
hence, the maximum current which can be
drawn. Another circumstance in which early
cooling is particularly beneficial occurs when
the particulate product has a boiling point
lower than the flame temperature (see "Experimental Results"). In that ease, no charge is
attached by the product prior to condensation,
unless condensation takes place on charged
nuclei or the molecule has a low ionization
potential. Cooling here promotes early condensation, which is important because the
maintenance of a unipolar ion cloud over large
distances minimizes the charging current obtainable.
Lastly, it may be advisable, in special eases,
to separate the flow geometry from that of the
lines of field altogether. This, of course, always
happens to some extent, since the particulates

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ELECTRICAL CONTROL OF PARTICULATE POLLUTANTS

are ultimately collected on some electrode which
is by-passed by the flow lines. At the flame,
however, we have so far thought in terms of
lines of field along those of flow, both being
orthogonal to the flame front. An extreme case
of separating the two systems would be the use
of a second flame as an ion source for a precipitator remote from the main flame. This would
allow electrical and flow parameters to be
optimized separately; thus, the ion flow could be
everywhere perpendicular to the gas flow, distance to the (cool) collecting electrode could be
minimized, and flow expansion could be arranged
perpendicular to the lines of field. From the point
of view of charge attachment, it can be shown
that such a system is more efficient than conventional "electrostatic" precipitators, because the
latter cannot be operated at field strengths ~ust
below breakdown at the collector electrode without secondary ionization, and therefore production of charges of opposite polarity, all over the
inter-electrode space. Of course, the over-all
efficiency, in terms of power input, plunges
steeply when a second flame is introduced as the
ion-source--instead of using the chemi-ions inevitably present in the first. However, special
circumstances are likely to arise in which such
a second source of ions may be present anyhow.
Thus, in systems such as internal combustion
engines, the use of secondary air injection to
burn up products of incomplete combustion is
becoming increasingly common. Since, in such ~/
system, it would be all but impossible to apply
electric fields to the primary stage and, furthermore, since some of the particulate pollutants
do not condense out until after some cooling of
the products, the use of such a second stage as
an ion source for a precipitator may prove to be
of practical interest.

4. Quantitative Prediction
Although the theory of calculating charging
rates follows from the above sections, space does
not permit analytical solutions to be set down
for all the systems advocated above. However,
it is possible--and remarkably straightforward
as a result of the above-mentioned simplificat i o n s - t o set up a single nomogram, such as
Fig. 2, which makes quantitative prediction
possible for any system of known particle
growth rate, field, flow, and temperature distribution. It is important to stress that, while
the full theory is completely general, this approximation is confined to the case of large
fields applied to flames. The calculation is based
on ions, not only because positive ions are used
to reinforce thermionic emission, but also be-

913

cause the mobility of electrons is so high that,

at any appreciable field intensity, their space
charge becomes insignificant (see Ref. 1). Thus,
the simplification which leads to these curves
being parallel straight lines would break down
for very small particles if N ever became appreciable (the deviation is indicated by the
single dotted curve representing thermionic
charging of barium oxide for the acquisition of a
second charge). However, this does not occur
under the circumstances considered, for the
following reasons. The smallest particles detectable in flames take an appreciable time (on
the scale of their residence time) to acquire their
first charge--for which the theory is, of course,
exact. Thereafter, their mobility is so high
(unless they grow so rapidly that the restriction
disappears) that they are removed before they
have time to acquire further charges. The
manner in which the detailed theory deviates
from our approximation actually helps to maintain the latter valid; it will be seen that it serves
to delay the acquisition of subsequent charges.
The data for thermionic emission and its
sources are as follows:
Specie
C
SiO~
BaO

A (amp/cm 2) K~
48
12.3
2.88

~ (eV) Ref.
4.4
4.75
1.68

8
9
9

where, ~b= A T 2 exp (--e/k T), amp/cm 2.

The relevance of carbon is obvious, SiO2 was
used as an example of a chemically inert particulate in the present work, while barium salts
are used as smoke suppressants.
The lowest bombardment charging curve corresponds to the maximum charging current
(plane electrodes at STP). The higher curves
correspond to 1/2 and 1/10 that current.
The diffusion charging lines are loci of particular ion concentrations, the lowest curve
corresponding to the highest ion concentration
deemed relevant to flames subjected to fields,
101/cm a. The others are fractions of 1/10 and
1/100 (ni) .....
The graphs are used in combination with a
model of particle growth, usually from initially
uncharged nucleates. It now appears likely that,
even in the presence of strong electric field intensities, initial particle growth by coalescence
and agglomeration can occur prior to the attainment of the first charge3 ,~,1 By modeling the
time dependence of particle size and, hence, the
number of particles for a constant mass system,
the growth history can be followed through the
flame zone until the time and place of acquisition

914

POLLUTANT FORMATION AND DESTRUCTION IN FLAMES

(~)

MIXING
CH4 , 26rnl/sec.
CHAMBER
r - - ~
J AIR, 320 mt/sec.
/
TVAp
l
/
,
,Ir---

.~

ru

, ~

l~,

rU

rU

2~

c.,

~,.

PYREX

HOOD \ I I

SUCTION
~
PUMP
\
LGLASS WOOL
-FILiER

~/

BLEEE

01L

L . ~

L~__ C O O U N G ~ ~ r

I MEKER

AOD,T,VE

FLOWMETERS

E/

OON..RF.OW
--

# ' ~
"--'~- - -~--'~
FLAT@ ~ i ,

I
r'~

.L
(~

COUNTERFLOW SYSTEM
FOR MOBILITY MEASUREMENT

L~

ELECTRICAL

AIR

/oRY,.GANDTOWERS

CCiklpl~l=C:qf3~SURGE TANK
...........

f
/' ~
/I
|J

,/

/-FLAT FLAME
(STOICH TOWN GAS/AlE

..,

_c_ RECIPIIAI:OR[ !?;:;';)'.;?.

"
BURNER 31:m: ":;:!,::
~ 1 ~ -

FLAME PRECIPITATOR

FIG. 3. Experimental systems.

of the first charge. Thereafter (or right from the

beginning, in the case of growth on charged
nuclei), the particle history is modified but still
predictable. The size and acquired charge define
the mobility [-see Eqs. (4)-(7)] which, together with the local field intensity, determines
the modified velocity and residence time to the
acquisition of the next charge, and so on. Any
known situation can thus be quantified by a
numerical procedure.

Experimental Results
Measurements were carried out initially on
SiO2 particles formed from hexamethyl disiloxane, as an example of a chemically inert
particulate product generated in a flame, and
then extended to products of Pb(C2Hs)t. Results for carbon were extracted from previous
work. 2 The flames were stabilized on a Mekertype burner (see Fig. 3), situated between two
parallel-plate electrodes such that electric-field
and gas-stream lines were nearly coincident. To
this end, the upper electrode was steam cooled
and designed to provide minimum obstruction
to products flow. Particulate-forming substances

in small controlled amounts were added to premixed methane/air flames by using an air bypass
through a temperature-controlled bubbler.
For predetermined flame and field conditions,
and fixed additive flow rate, total rates of particulate mass deposition were determined by
brushing the deposit collected on the electrodes
during each experiment into a pre-weighed
filter connected to a suction pump. Particles
carried by the product gases were similarly
collected during the experiment by a filter in
the exhaust manifold.
In addition to mass-deposition rates, the
current and mean particle size were determined
as a function of applied potential. Particulate
samples were obtained directly on electronmicroscope carbon grids, passed through the
stream of product gases at several distances
from the flame front. The mean particle size
was estimated from numerous electron micrographs at magnifications of 20,000 to 65,000 by
averaging over 30 to 50 particles.
The mobility of positive and negative charge
carriers in the hot product gases was determined
from the slope of the curve of (current density) tm
vs (applied potential) for the additive-free ease.
In order to determine ion and particle mobility

ELECTRICAL CONTROL OF PARTICULATE POLLUTANTS

at a controlled temperature, a counterflow technique was employed, see Fig. 3 (b). The charged
species were induced to pass through the coarse
grid in the central electrode by the variable
control field Ed, and to drift against the uniform
air eounterflow. The mobility was simultaneously determined from the threshold value of
voltage at which current appears in the counterflow circuit, and from the linear slope of (ja) '/2
vs Vd above the threshold voltage, when space
charge becomes limiting.
Results for the case of Si02 formation are
compared to previously obtained data for
carbon deposition in Fig. 4. All data apply to the
case of positive-ion flux through the particulateladen product gases. Figure 5(a, b, e) shows
representative electron mierographs of Si02
particles obtained at x = 5 cm from the flame,
which were used to deduce the dependence of
mean particle size on applied potential. As in
the case of carbon formation, it is apparent that
all SiO~ particles are, in fact, charged positively
for the ease of positive-ion flux. In contrast to
fame carbon, 1,2 these particles cannot, of course,
be made to burn up. Their total yield, therefore,
remains unchanged. However, their acquisition
of charge, mobility, consequent controllability
by field, and size decreasing with increasing
field intensity, are very similar. Particle size is
reduced by a factor of 3 (i.e. particle mass by a
factor of ~-~30) with increasing applied potential,
due to simultaneous particle charging and rapid
removal to the electrode with subsequent decrease ir~ residence time in the product gas.
With increasing applied potential, the mass
fraction of Si02 removed from the product exhaust is more than doubled. Note that, even in
the absence of applied fields, up to 30% of the
particulate is deposited on the electrode, due to
finite obstruction to product flow.
In the absence of added siloxane, the positiveion mobility in the product gas was measured
from the slope of the current-potential characteristic curve below saturation, and found to be
kl = 21.0:E 1.0 (cm2/see V) at Tb= 2000K,
which compares quite favorably with the calculated value of 21.2 cm2/sec V for the H~O+ ion,
and thus confirms the validity of the numerical
calculations leading to Figs. 1 and 2. Using the
counterflow technique, the SiO~ particle mobility
was found to vary by less than 30% about a
mean of 0.13 cm2/sec V at 300K.
From the measured particle mobility and size,
the charge per particle can be estimated by
applicatio~ of the appropriate mobility law
FEqs. (4)-(7)~. From Fig. 4(c), it is clear that

915

3O0

~/

//c

C ( POSITIVE FLUX)

,NET,E FLX,

200
X=
X=

9cm.
2cm.

Si 0 z. POSITIVE FLUX

.< ,oo

2
3
4
5
6
APPLIED POTENTIAL( kv )
a) PARTICLE SIZE FOR C AND S~ O= AS A
FUNCTION OF APPLIED POTENTIAL
1

~ C , ELECTRODE

100

~ C, EXHAUST

/j

~C~ FLANGE

!FLAME

~ 4

,c

$i O=
30

o~
60
ELECTRODE

FLAME

40

/i
z

2i

us~

2o

' ~

~"~l
BURNER 0
2
3
&
5
6
APPLIED POTENTIAL ( k v )
b} MASS FRACTION DEPOSITED AND FLAME CURRENT
WITH POSITIVE FLUX FOR C AND Si O= FORMA?ON

L
u 1' 0 ~ " , , ~

;I

- ,o-'1-~
-

,641
10

.CARBON

RANGE

" ~

r N

\T

:2~ ,=,oo,

I00
1000
PARTICE RADIUS (A )

c} MOBILITY AS A FUNCTION OF
RADIUS FOR
SIOL AND C

PARTICLE

FZG. 4. Experimental results for SiO2 and carbon

deposition.

the particles are likely to be singly charged, as

was observed in the case of carbon deposition. 2
Since, at the above mobility, the particles respond to fields of the order of 104 V/cm with
velocities of the order 10~ cm/s, residence times
for the acquisition of second and subsequent
charges are greatly reduced. By the same token,
the singly charged particles are adequately controllable at combustion-flow velocities.
Particle charges derived from rp and kp can be
compared with the predictions of Fig. 2. The
data for Si02 were obtained for an oxidizer-rich
mixture with Tb=2000K, and rather long residence times. From Fig. 2 and the measured
particle sizes, it is to be expected that thermionic

916

POLLUTANT FORMATION AND DESTRUCTION IN FLAMES

Fro. 5. Electron micrographs of SiO2 and PbO particulates sampled from products at 5 cm from flame
for positive flux case. (Magnification 56,000 for SiO2.) (a) (Upper left) SiO.2, no field; (b) SiO2, 1 kV; (c)
SiO2, 6 kV; (d) PbO, 2 kV, magnification 16,000.

emission will contribute to the net acquisition of

positive charge. Indeed, even in the absence of
applied fields, there is evidence that, for Tb=
1800K, SiO2 is charged.
The results for lead oxide were qualitatively
similar in their evidence of charging and the
consequent change in deposition pattern. There
were, however, two major differences. The
particles grew to a much larger size--with a
much wider statistical variation--and their
mobility in fields was very small. Investigations
of their physical properties revealed a boiling
point very considerably below that of either
Si02 or C, and below the temperature of most
of the flames. (Neither this nor the thermionic
emission of SiO2 was appreciated when the
additives were chosen.) This would account for
all the observations, since the pollutant would
be present as vapor in the region in which
particles usually acquire their charge, and
would condense rapidly and irregularly where
the gas cools. A typical electron micrograph is
shown ia Fig. 5(d). Evidence of melting and
coalescence was observed even on solid surfaces
which had been placed too close to the flame.
This is a case in which a separate second flame
as an ion source for a precipitator could be used

beyond the point at which the products have

cooled sufficiently for lead oxide particles to
have formed. A system designed to explore the
novel principle is shown as an insert to Fig. 3 (c).
It was tested on SiO2 because lead oxide is a poor
thermionic emitter, and it was of interest to investigate to what extent such a device could be
used to neutralize any charge already present
on the particle.
The results confirmed the practical utility of
the concept. When the products were cooled
above the flame (to allow neutralization of
thermionically charged particles by electron reattachment) a negative flux was more effective
by a factor of 2, in terms of mass deposition per
unit of electrode area, than a positive flux. This
indicates a higher attachment cross section for
electrons or negative ions than positive ions.
When the precipitator current was caused to
pass through the high-temperature post-flame
zone, in which positively charged SiO2 particles
are expected, virtually all the Si02 formed was
caused to deposit at the negative electrode, with
no deposit at the anode for a positive ion flux
(reinforcement of thermionic charging). A negative flux was not as effective although a substantial deposit at the anode indicated successful

ELECTRICAL CONTROL OF PARTICULATE POLLUTANTS

attachment of a negative charge in excess of the
original positive charge. A smaller deposit was
collected at the cathode, with a loss of "neutralized" particles to the exhaust stream. In the
absence of applied fields to the precipitator
flame, virtually no Si02 deposited on the electrodes.
Conclusions
The attachment of flame ions, which would
otherwise recombine unprofitably, to particulate
pollutants to allow their subsequent manipulation by electric fields, has b e e r demonstrated.
This appears possible for all particulates; in the
case of thermionic emittors, attachment is used
to reinforce their tendency to become positively
charged. For species whose boiling point lies below the flame temperature, the use of a second
flame as an ion source in a cooler part of the
stream is advocated. The theory of predicting
rates of charging and, hence, particle traiectories
in fields, in terms of their growth histories, is
established and leads to the prediction of optimum conditions.

v
p
~b
~b

917

collision frequency
mass density
thermionic work function
thermionie emission current density

Subscripts
b
burned gases, break-down
bomb bombardment mechanism
d
conditions during mobility measurement
b y counter flow between two upper
electrodes
diff
diffusion mechanism
i
ion
max maximum
p
particle
0
conditions at STP; at ion source
s
saturation condition
ther thermionie mechanism

Acknowledgments
We are indebted to Mr. E. R. Place for helpful
comments, to the Associated Octel Co., Ltd., for a
financial contribution to our research costs, and to
the N.S.F. for a Post-Doctoral Fellowship to one of
us (D.R.H.).

Nomenclature
g
D
E
e
j
k

kl
kp

21I
m
N
n
p
Re
rp
T
t
v
x
X

mean thermM velocity

dielectric constant
electric field intensity
electron charge
current density
Boltzmann constant
ion mobility
particle mobility
molecular weight (of neutral species)

REFERENCES
1. LAWTON, J. AND WEINBERG, F. J.: Electrical
Aspects of Combustion, Clarendon Press, 1969.
2. MAYO, P. J. AND WEINBERG, F. J.: Proc. Roy.
Soc. A319, 351 (1970).
3. THONG, K. C. AND WEINBERG, F. J. : Proc. Roy.
Soc. A324, 201 (1971).
4. LANGEVIN,P.: Annal. Chim. Phys. 5, 245 (1905).
5. GUGAN,K., LAWTON,J., AND WEINBERG, F. J.:

mass

Tenth Symposium (International) on Combustion,

number of electron charges per particle

number density
pressure
Reynolds Number
particle radius
absolute temperature
time
velocity
distance coordinate
viscosity
mean free path

p. 709, The Combustion Institute, 1965.

6. SCHWAR, M. J. R., THONG, .

C., AND WEIN-

BERG, F. J.: J. Phys. D. 3, 1962 (1970).

7. BALL, R. T. AND HOWARD, J. B.: Thirteenth

Symposium (International)

on Combustion, p.

353, The Combustion Institute, 1971.

8. VON ENGEL, A.: Ionized Gases, Clarendon

Press, 1965.
9. International Critical Tables 6, 53 (1929).
10. ULICTCH, G. D.: Combust. Sci. Technol. 4, 47
(1971).

COMMENTS
A. K. Oppenheim, University of California,
Berkeley, Cal. Since the application of an appreciable electric potential at low current can
have great iidluence on the burning rate, are
such devices currently being considered for

industrial applications? If so, what particular

areas of application should be, in the authors'
opinion, most profitable? I presume that they
should be quite effective in the abatement of
smoke from industrial plants.

918

POLLUTANT FORMATION AND DESTRUCTION IN FLAMES

Gail D. Ulrich, University of New Hampshire,

Durham, N.H. I am interested in flames containing large concentrations of particles. What
do you consider the maximum concentrations of
charged particles that can be realized in both
carbon-containing and non-carbon-containing
flames, in the presence and absence of applied
electric fields?

S. Way, Westinghouse Research Labs., Pittsburgh, Pa. Would the authors have reason to
believe that electrical control of soot particles
might be feasible under the conditions that
exist in gas-turbine combustion systems? Our
own feeling in this matter is that the prospect is
not promising. Calculations were made of
charge acquired by the particles, assuming the
bombardment mechanism, and with appropriate
calculated values of particle mobility (Cunningham correction to viscosity, etc.), we found
that lateral deflection of the charged soot
particles, in highest practical electric fields,
would be only a few millimeters, as the sooty
gas stream flowed from the combustor toward
the turbine. While prospects do not appear
promising for control of soot emission from the
exhaust stream by electrical means, might it be
possible to effect control, to some degree, of
unwanted carbon deposits in the flame tube?

Authors' Reply. We certainly do expect that

this work will prove to have a variety of practical
applications, even though they may have to be
taken up in establishments better suited to their
exploitation than is our academic environment.
My own feeling is that the association of combustion with electric fields--and indeed with
arcs, complex heat exchangers, and other systems we are studying--would continue to appear too elaborate only in a world of unlimited
sources of inexpensive fuel and of unlimited
sinks for undesirable products. We are rapidly
coming to the end of an era in which combustion
was thought of in this way.

As regards the questions concerning limitations of the application of electric fields, these
are detailed in Chap. 8 of Ref. 1. Oversimplifying
somewhat, the restrictions are most severe (except for ionic wind effects) where it is necessary
to have a large distance between the electrodes.
This tends to minimize the field which can be
applied at the thin central ion source--the
flame--without inducing secondary ionization in
the electrode spaces.
This theory gives the following answer to
Dr. Ulrich's question: under optimum conditions (cold electrodes, 5 mm from flame) in a
unidimensional system, 1 sq. cm. of flame provides a current sufficient to give one electronic
charge to each of 1.6X 1015 particles per second.
This numer is inversely proportional to both
the electrode separation and its temperature,
but can be increased by changes in geometry. 1
I agree with Dr. Way that existing gasturbine combustion systems make it difficult to
arrange for small electrode spacings without
increasing pressure losses. However, the displacements he calculates (a few mm) may be
quite sufficient to remove particles from the
pyrolysis zones of diffusion flames in which they
grow--which has been shown2 to result in great
decreases of total carbon produced. The prevention of deposition on particular surfaces also
seems perfectly feasible, since there is no difficulty about maintaining large fields adjacent to
relatively cool surfaces. Afterburners, where
used, may provide a convenient alternative site
for simple experiments.

REFERENCES
1. LAWTON, J. AND WEINBERG, F. J.: Electrical
.~pects of Combustion, Clarendon Press, Oxford, 1969.
2. PLACE, E. R. AND WEINBERG, F. J.: Proc. Roy.
Soc. A289, 192 (1965).