E L S E VI E R

PIh S0016-2361(97)00045-8
Fuel Vol, 76, No. 8, pp. 801-805, 1997
1997 Elsevier Science Ltd. All rights reserved
Printed in Great Britain
0016-2361/97 $17.00+0.00
Dry tri boel ectrostati c beneficiation
of fl y ash
Heng Ban, Tian X. Li, James C. Hower, John L. Schaefer and
John M. Stencel
Center for Applied Energy Research, University of Kentucky, 3572 Iron Works Pike, Lexington,
KY 40571-8433, USA
(Received 1 February 1996; revised 10 January 1997)
A laboratory-scale triboelectrostatic separation system in conjunction with analytical techniques was used to study
fly ash beneficiation. Fly ash samples were characterized by size analysis and carbon content and then subjected to
dry triboelectrostatic separation. Due to differences in the surface physical and chemical properties of the carbon
and ash, particles of unburnt carbon and fly ash were triboelectrically charged to opposite polarity and then
separated by passing them through a static electric field. Ash fractions deposited on the positive and negative
electrodes were collected, analysed for carbon content and subjected to SEM and petrographic analyses. The
results indicate that the physical and chemical properties of the ash dictate the maximum carbon-ash separation
that would be possible. In addition, the potential of dry separation technology for removing unburnt carbon from
coal ash was demonstrated. 1 9 9 7 E l s e v i e r S c i e n c e Lt d.
( Ke y wo r d s : f l y a s h ; b e n e f i c i a t i o n ; t r i b o e l e c t r o s t a t i c s e p a r a t i o n )
Most coal combustion ash produced in the USA is
landfilled, the cost of which in some states has risen to
more than $30/ton. This financial burden, increased interest
in i mprovi ng the environmental and social impacts of coal
utilization, and the possibility of recovering constituents of
fly ash and/or using it for industrial applications (e.g.
cement, structural and paint/plastic fillers, cenospheres,
magnetite and specialty carbons) point to its future potential
as an important industrial commodi t y ~.
An important property of fly ash which limits its use is the
carbon content. However, reducing the carbon content to
meet Class F of the ASTM C618-89a and C311-90
specifications 2 for use of ash as a mineral admixture in
Portland cement concrete is not an easy task. For example,
the information given in T a b l e 1 shows that, even for high
carbon conversion efficiencies during coal combustion, the
carbon content of fly ash is difficult to reduce below the
6 wt% LOI (loss on ignition) C618 classification standard. It
may be possible to reduce the carbon content efficiently by
use of beneficiation technologies. Because > 90% of the fly
ash in the USA is handled in the dry state, dry beneficia-
t i o n - - o r triboelectrostatic separ at i on- - has been the recent
focus of research at CAER, some of which is discussed in
this paper.
Dry triboelectrostatic separation technology is just
beginning to be applied to recover purified ash from fly
ash streams which contain high concentrations of carbon.
Due to differences in the surface physical and chemical
properties of the carbon and ash, they can be electrically
charged to opposite polarity by particle-to-particle or by
particle-to-surface contact. By manipulating the polarity
and magnitude of this charge, the carbon and ash can be
separated by passing them through an external electric
field: see F i g u r e 1. The successful application of dry
separation technology to ash purification would be sig-
nificant because it would enable expanded utilization of a
mineral resource which otherwise is landfilled or not used to
its full potential.
A number of dry triboelectrostatic separation systems
have been designed for application to particle segregation,
one of t hem submitted for patenting as early as 19043,4 .
5 9 10 1 1 12 14
Ciccu e t a l . - , Inculet , Finseth e t a l . and Ban e t a l . -
exami ned the use of triboelectrostatic separation to purify
minerals and to separate mineral matter from coal. These
15
efforts and others have provided important fundamental
insight into particle surface electrical properties and
engineering parameters which allow charging of particles
to opposite polarities and their subsequent separation under
a static electric field. Coal fly ash could be considered a
direct analogue to coal, because in both cases the goal is to
separate a mi nor constituent from the maj or one, the
difference being that in coal the mineral matter is the mi nor
constituent and carbon the major, whereas in fly ash the
reverse is true. As a consequence of the groundbreaking
work by Ciccu e t a l . 5 - 9 and Finseth e t a l . 11 there is renewed
interest in the application of triboelectrostatic separation
systems. Already a relatively compl ex electrostatic separa-
16 17
tor has been constructed and operated ' at a scale of
- 1 8 t h -~. The operating differences between such units
primarily relate to the met hod by which fine particles are
charged and transported through a separation zone. Finseth
e t a l . 11 and Ciccu e t a l . 5 - 9 have used pneumatic trans-
port and charging methods, whereas the commerci al
unit 16'17 uses mechanical agitation for transport and
Fuel 1997 Vol ume 76 Number 8 801
Dry triboelectrostatic beneficiation of f/y ash: H. Ban et al.
Table 1 Carbon content of fly ash versus carbon burnout and coal
mineral matter content
Mineral matter in coal Carbon burnout Carbon in ash (wt%)
(wt%) (wt%)
10 99 8.3
10 97 21.2
20 99 3.8
20 97 10.7
Feeder
,?#/
Carrier Gas
Charger
IIcII
Copper
Plates
- -15 kV
Figure 1 The principle of dry triboelectrostatic separation of
carbon and fly ash
charging. The research reported in this paper used
pneumatic transport processing.
Very little information has been published in which
physical and chemical properties of fly ash are related to the
separation purities that can be attained using dry triboelec-
trostatic separation. Those properties expected to play an
important role include particle size and size distribution, ash
mineralogy, extent of liberation between the carbon and ash
forms, the form of the carbon, and surface segregation of
elemental species. Hower et ~1. have presented an
overview of potential forms of carbon and minerals,
including the glassy phases which dominate as-received
fly ashes, thi spine1 minerals, magnetite, and the carbons.
The carbon phases were shown to include inertinite, a coal
maceral which has been observed to pass through a boiler
unburnt, and the forms which were recognized as isotropic
and anisotropic coke.
There is a need to optimize dry fly ash separation
technologies because of the vast amount of coal ash
produced in the USA and the growing interest in applying
superior technologies because of their economic and
environmental performance. In this paper, the results from
triboelectrostatic separation of coal fly ashes using a
laboratory-scale system are presented. The design of the
triboelectrostatic separation system and the data obtained on
the ashes in this study will be used in future work to
optimize ash separation using feed rates typical of industrial
and utility systems.
EXPERIMENTAL
A laboratory-scale triboelectrostatic separation system,
shown in Figure 2, was used in the fly ash beneficiation
study. The fly ashes were fed to the tribocharging unit by a
vibratory feeder which was contained in a sealed environ-
ment tank. Each ash was metered into a pneumatic transport
tube where it was entrained in N2 carrier gas. The gas-
particle mixture was then passed through the Cu tribochar-
ger loop where the fly ash was charged by particle-wall
(and particle-particle) contacts. The exit of the charger was
connected to a separation chamber which contained a
parallel Cu plate configuration, across which was estab-
lished a high-intensity electric field. A filter was placed at
the bottom of the separation chamber to retain any particles
not deflected to the Cu plates. The exit of the separation
chamber was connected to an induced-draught fan.
A sample of -10 g of each ash was weighed and loaded
into the vibratory feeder. The average carrier gas flow
velocity in the Cu tribocharger was - 15 m s-, The electric
field strength was maintained at 200 kV m-l.
Ash samples were acquired from either electrostatic
precipitator (ESP) hoppers or storage silos at commercial
pulverized coal boilers. Prior to separation tests, the samples
were evaluated for particle size and carbon content. After
the triboelectrostatic separation, samples were collected
from the separation chamber (see below) and their weight
and carbon content determined. Representative sample
fractions were also examined using scanning electron
microscopy (SEM) and energy-dispersive spectrometry
(EDS).
Fly ash fractions were prepared for petrographic analysis
by mixing 1 g, or less in some cases, of fly ash with an epoxy
Custom
Gas Blend
Izced Draft
Filter
Figure 2 Schematic of the experimental setup
802 Fuel 1997 Volume 76 Number 8
Dry triboelectrostatic beneficiation of fly ash: H. Ban et al.
laced with Sudan Black dye. The 2.54 cm di amet er e poxy-
fly ash pellets were polished to a final polish of 0.05 #m.
Petrographic examination was conducted using oil i mmer-
sion objectives at 400 magnification.
RESULTS AND DI SCUSSI ON
During operation of the triboelectrostatic separator system,
the carbon-enriched component was deposited on the
negative electrode and the ash-enriched component was
deposited on the positive electrode. The deposits were in the
form of long, narrow ribbons of material, starting from near
the exit of the transporting tube and extending to the end of
the copper plates. Analysis of up to four sequential axial
sections of the deposited samples showed the carbon content
to be highest at the top of the negative electrode and lowest
at the top of the positive electrode. The carbon content on
the positive electrode increased with distance from the inlet
of the electrostatic separator, while the carbon content on
the negative electrode decreased with distance from the
inlet. Since the carbon and ash contents on the electrodes
could be represented by a continuous distribution, it was
possible to make an arbitrary split of the separated products
that satisfied desired purity requirements. However, as in
any physical separation process, higher-purity products are
achieved at the expense of lower yield.
A procedure was established for sample collection and
analysis. For each test, a total of 12 sample fractions were
collected: ten were from five axial regions on each of the
two electrodes, one was from the centre filter at the bot t om
of the separator, and one was removed from the Plexiglass
windows at the edges of the Cu electrodes. These fractions
as well as the feed were weighed and analysed for carbon
content, and the data were plotted in a manner similar to a
washability or release analysis c u r v e 1 9 , 2 0 , using the analogy
of each fraction as either a float or sink product.
Consequently these data include an assessment of mass
balances, because ash not collected by the gas filter syst em
was also taken into account.
Carbon and ash recovery data, and particle size and
carbon distributions, for fly ash sample A are shown in
Figures 3-5. Sample A was obtained from a utility boiler
burning bituminous coal having a sulfur content of ~2 wt%.
Over 65 wt% of the ash was recovered with a carbon content
8
o o _ _ - I
t t
4 o . , I
i ,
3 0 :
20 t---
1 0 - -
>150 150- 75 75- 45 45- 38 38- 25 <25
Si ze (microns)
Figure 3 Fly ash mass, carbon concentration and carbon mass
distributions in each size fraction of fly ash sample A
>
8
n~
-
( / 1
<
100
80
60
40
20
0
. . . . . . ~ . . - - . - ~ ; L . - - - - i - . . . . . i ' . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .
~ i ~ : : :
. . . . . . . ~ - - - - - - ~ . . . . . . . i . . . . . . . i - - - . - - ~ . . . . . . . . . i . . . . . . . ~ . . . . . . . ~ . . . . . .
. . . . . . 4 - - - - - . ~ ' - - - ~ - - . - - 4 1 ~ . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .
. . . . . . 4 - - - - - - ~ . - - - - - i ~ - - - - - - 4 - - - - - . ~ . , - - - - 4 ~ . . . . . . . . . . . . . . . . . . . . . . . . .
. . . . . . . ~ - - - - - - ~ - - - ~ - - - - - , 4 - - - - - - ~ , , - . - - - ~ - - - - - - 4 . . . . . . . . . . . . . . . . . . . .
I I I I
0 2 4 6 8 1 0
Carbon %
F i g u r e 4 Ash recovery curve of fly ash sample A (from low-S
bituminous coal), showing C concentration in ash-enriched product
1 0 0 ...... ~ . . . . . . . . i..-...~..----i...---i...-..~..---~......~----..~ ......
. . . . . . i - . - - - - i - - - - . . ' . - . i - . . - . . i . - - - - - i . . . . . - i - - - - . . i - . - - - i - . - - . . ; . . . . . .
~80 . . . . . . i - - - - - - i . - - - - - i - - - ' - - - . - - i - - - - - - ~ - - - - - - i - - - - - - i - - - - - - b . - . - - ~ . . . . . .
>
8 6 o
o 2 0
o
0 10 20 30 40 50
Carbon%
F i g u r e 5 Carbon recovery curve of fly ash sample A, showing C
concentration in carbon-enriched product
8
t - -
( / )
<
100
80
60
40
20
0
. . . . . b - - - . - i - - - - - i . . - - - - " . . . . . i . - - - . ~ - . - . . - i - - - - - - : ' - . - - - - i . . . . .
. . . . . . ~ - - - - - - ~ . - , - - i - - - ~ - - - - - - ~ , - - . . - i - - - - , : : - - - - - - ~ - - , - - , . ' - - - - - - ' . , . . . . .
. . . . . ; . - - - - - . L - . - - ; . . . . . i - - - . . ( , - - - . - i - - - - - ~ - - - - - ; - . - - - ~ - - - - - - ~ . . . . .
" ' " e J . . . . .
i 12 i
i ; " i " ; " i " i
0 2 4 6 8 10 12
Carbon %
F i g u r e 6 Ash recovery curve of fly ash sample B (from high-S
bituminous coal), showing C concentration in ash-enriched product
of < 3 wt%, while - 5 0 % of the carbon in the ash was
recovered with a carbon content > 35 wt%. The particle
size distribution data showed that a significant amount of the
ash was of size > 150/~m and < 25/~m. This wide
distribution of particle size presents a significant challenge
to dry separation systems, due to an order-of-magnitude
range of aerodynami c drag and gravitational forces.
Separation results for fly ash sample B are presented in
Figures 6 and 7. This sample was obtained from a utility
Fuel 1997 Vol ume 76 Nu mb e r 8 8 0 3
Dry triboelectrostatic beneficiation of fly ash: H. Ban et al.
0 10 20 30 40 50
Carbon %
Figure 7 Carbon recovery curve of fly ash sample B, showing C
concentration in carbon-enriched product
burning bituminous coal having a sulfur content of
-3.5 wt%. The ash recovery data are plotted for one-stage
and two-stage processing schemes. A one-stage processing
scheme would not include recycle of material passing
through the electrostatic chamber, whereas a two-stage
scheme would recycle such material, i.e. particles not
reporting to either positive or negative plates. The data show
that the second-stage separation increased the ash recovery
by - 15 wt%, and hence it may be important to recycle ash
that is not influenced by the electric field. Overall for sample
B, nearly 55 wt% of the ash was recovered with a carbon
content of < 3 wt%, while > 60% of the carbon was
recovered with a carbon purity > 40 wt%.
The partitioning of glass, mullite, spinel, quartz and the
carbon forms for three additional Class F fly ashes2 is shown
in TabEe 2. All these samples originated at industrial sites
and represent a broad range of carbon concentrations. In all
cases, samples collected on the positive electrode had a
greater concentration of glass than those collected on the
negative plate; samples collected on the negative plate had a
greater concentration of the various carbon forms.
Table 2 Partitioning (vol.%) of mineral and carbon forms for three type F fly ashes
Plant Producta Ash Carbon Glass Mullite Spine1 Quartz Isotropic C Anisotropic C Inertinite
C feed 92.2 7.6 86.6 0.8 3.2 0.6 3.8 4.6 0.4
negative 74.6 26.8 45.0 4.0 3.0 1.0 22.0 21.0 4.0
positive 99.6 0.6 97.6 0.6 1.0 0.2 0.4 0.0 0.2
centre 90.4 7.2 72.4 2.4 3.8 2.0 8.0 8.4 3.0
D feed 77.0 23.4 69.8 0.8 1.0 0.4 10.4 15.2 2.8
negative 49.8 50.2 28.0 1.0 0.0 0.0 24.0 43.0 4.0
positive 97.2 3.0 96.6 0.0 0.0 0.0 1.2 1.5 0.6
centre 66.2 39.2 40.5 0.5 0.5 1.0 24.0 31.0 2.5
E feed 55.4 44.4 38.4 2.0 0.4 18.4 11.2 20.0 9.6
negative 36.3 60.6 17.0 1.0 1.0 2.0 37.0 35.0 7.0
positive 78.8 17.4 86.8 0.0 0.0 0.8 6.0 4.4 2.0
centre 60.8 41.2 57.0 0.5 1.0 4.0 15.0 20.5 2.0
Negative, positive and centre denote material collected from the negative and positive electrodes and bypass filter respectively
100 _I
I
90
t-l
0 Isotropic Coke
B Anisotropic Coke
20
10
0
Cf C- C+ CO Df D- D+ DO Ef E- E+ EO
Feed &Separated Fractions
Figure 8 Distribution of carbon forms based on petrographic
analysis. Symbols following C, D, E have the following
connotation: f, original feed ash; +, product collected from posi-
tive plate; -, product collected from negative plate; 0, product not
reporting to plates but collected in bypass filter
The distribution of the carbon forms obtained by
petrographic analyses is shown in Figure 8 and Table 2.
These data suggest that the efficiency with which carbon
could be removed may be related to the amount of carbon in
the feed; however, no mass balances were performed for
these petrographic samples. Sample C, with 8.8 vol.%
carbon in the feed, had 0.6 vol.% carbon in the glass-rich
positive-plate fraction, while sample E, with > 40 vol.%
carbon in the feed, had > 10 vol.% carbon in the glass-rich
fraction. The results for sample C are similar to the carbon
removal efficiencies obtained from idealized samples
containing physical mixtures of spherical glassy carbon
and silica particles12, from which > 95% removal of carbon
could be attained. If samples C and E were strictly physical
mixtures of carbon and ash, and if the forms of the mineral
and carbon phases did not influence separability, it could be
expected that the carbon content of the ash-enriched product
on the positive plate for sample C would be as low as 0.4%,
whereas the carbon content of the ash-enriched product for
sample E would be -2%. That these values were not
attained attests to the possible importance of ash properties
influencing maximum separation efficiency.
No clear trends are evident in Figure 8 for mullite, spine1
and quartz beneficiation. This is possibly a consequence of
the low quantities of these components and/or the broad size
804 Fuel 1997 Volume 76 Number 8
Dr y t ri boel ect rost at i c benef i ci at i on o f f l y ash: H. Ban et al.
di s t r i but i on o f t he c o mp o n e n t s i n t he f e e d. St udi es o f t he
s i ze di s t r i but i on o f o t h e r fl y a s he s h a v e s h o wn t hat a
u n i f o r m di s t r i but i on o f p e t r o g r a p h i c c o mp o n e n t s i s not
c o mmo n f or a fly a s h or f o r s i mi l a r s i ze r a n g e s i n di f f e r e nt
fl y a s he s 18. I s o t r o p i c a nd a n i s o t r o p i c c a r b o n s t e nd t o b e
c o n c e n t r a t e d i n t he l a r ge s t s i ze f r a c t i ons ( > 75 # m) as
c o mp a r e d wi t h t he mi n e r a l ash, whi l e s o me fl y a s he s h a v e
s i gni f i cant a mo u n t s o f c a r b o n e v e n i n t he f i nes t s i ze
f r act i ons . I n ma n y as hes , t he < 25 # m f r a c t i on c a n f o r m
7 0 - 8 0 wt % o f t he t ot al 18.
I n all cas es , t he fl y a s h wh i c h r e p o r t e d t o ne i t he r a
pos i t i ve n o r a n e g a t i v e e l e c t r ode , but r a t he r t o t he f i l t er at
t he b o t t o m o f t he s e pa r a t or , c o n t a i n e d l a r ge r pa r t i c l e s t han
t hat wh i c h r e p o r t e d t o t he p o s i t i v e or n e g a t i v e pl at es . Th e s e
l a r ge r pa r t i c l e s c o mp r i s e d gl as s , c a r b o n a nd s pi nel s , t he
l a r ge s t b e i n g p r e d o mi n a n t l y s pi nel s . La r ge , ma s s i v e par t i -
cl es t e nd t o h a v e s ma l l e r c h a r g e / ma s s r at i os t ha n s mal l , l i ght
pa r t i c l e s b e c a u s e t r i b o c h a r g i n g p r o d u c e s pa r t i c l e s h a v i n g
ne a r l y c ons t a nt va l ue s o f c h a r g e p e r uni t s ur f a c e a r e a 14.
Th e r e f o r e , e i t he r t he e l e c t r i c a l f o r c e ( F = qE, wh e r e q i s t he
c h a r g e on a pa r t i c l e a nd E i s t he e l e c t r i c f i el d i nt ens i t y) wa s
not s t r ong e n o u g h t o pul l t he h e a v y pa r t i c l e s t o an e l e c t r ode ,
or t he s e pa r t i c l e s we r e def l ect ed, r e a c h e d an e l e c t r o d e a nd
t hen b o u n c e d o f f as a c o n s e q u e n c e o f c h a r g e a nd/ or
mo me n t u m e x c h a n g e .
Th e S EM r es ul t s f or s a mp l e s c o l l e c t e d on t he b y p a s s f i l t er
s h o we d n e a r l y s phe r i c a l pa r t i c l e s wh i c h a p p e a r e d t o be
pa r t l y o x i d i z e d c oke . Al s o, pa r t i c l e s c ons i s t i ng o f a mi x t u r e
o f a s h wi t h c a r b o n we r e o b s e r v e d . Th e c h a r g i n g o f t he s e
mi x e d c a r b o n - a s h pa r t i c l e s wo u l d be mi n i ma l b e c a u s e no
d o mi n a n t p o l a r i t y s pe c i e s wa s pr es ent . Al t h o u g h t he
p e t r o g r a p h i c a n a l y s e s s h o we d a s s e mb l a g e s wh i c h c ons i s t e d
o f c a r b o n mi x e d wi t h ash, i t i s i mp o r t a n t t o me n t i o n t hat t he
a c t ua l c o u n t o f s uch pa r t i c l e s wa s l ow a nd c o u l d b e b i a s e d
as a c o n s e q u e n c e o f wh i c h c o m p o n e n t - - a s h or c a r b o n - -
wa s o b s e r v e d wi t hi n t he e y e p i e c e c r os s - ha i r s .
C O N C L U S I O N S
Thi s s t udy has s h o wn t hat dr y t r i boe l e c t r os t a t i c s e p a r a t i o n
o f fl y a s h has t he pot e nt i a l t o s e p a r a t e unbur nt c a r b o n f r o m
fly ash. L a b o r a t o r y t es t s on a s i mp l e pa r a l l e l - f l ow s e p a r a t o r
s h o we d t hat 6 0 - 8 0 wt % o f t he a s h c o u l d b e r e c o v e r e d
h a v i n g a c a r b o n c ont e nt < 5 wt %, and up t o 50% o f t he
c a r b o n c o u l d be r e c o v e r e d as ma t e r i a l wi t h a c a r b o n c o n t e n t
> 50 wt %. Th e o v e r a l l c ol l e c t i on e f f i c i e n c y a p p e a r s t o be
r e l a t e d t o t he a mo u n t o f c a r b o n i n t he f e e d a nd i s p r o b a b l y
i nf l ue nc e d by t he s i ze di s t r i but i on o f t he c o mp o n e n t s a nd
t he a mo u n t o f mi x e d pa r t i c l e s . Ad d i t i o n a l s t udi es s houl d b e
i ni t i at ed t o e v a l u a t e t he e f f e c t s o f a s h p r o p e r t i e s on
s e pa r a t i on, wi t h t he goa l o f o p t i mi z i n g t he be ne f i c i a t i on
pr oc e s s .
R E F E R E NC E S
l Manz, O. E., in Tenth International Ash Use Symposium,
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7 Alfano, G., Carbini, P., Carta, M., Ciccu, R., Del Fal, C.,
Peretti, R. and Zucca, A., Journal of Electrostatics, 1985,
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8 Ciccu, R., Ghiani, M. and Ferrara, G., Powder and Particles,
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9 Ciccu, R., Peretti, R., Serci, A., Tamanini, M. and Zucca, A.,
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