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INTERNATIONAL SYMPOSIUM ON SPOUTED BEDS

Developments in Spouted Bed Technology


K I S H A N B. MATHUR and NORMAN EPSTEIN
Department of Chemical Engineering, University of British Columbia, Vancouver, B.C.

The spouted bed, though originally developed for drying of Le lit s&cial fluidis6 avec giclage (spouted bed), bien qu'a
COQTX granular s~lids,has, over the last decade, proved to be ait 6th originellement mis au point pour secher des matibes
of interest for carrying out a remarkably wide variety of opera- solides 21 gros grains, s'est aver6 intkressant depuis la dern%re
tions. These include not only other diffusional and/or thermal dkceunie pour effectuer des opCrations t r b variCes. Parmi l e ~ -
operations such as heating or cooling of solids, drying of soh- dites opbrations, on peut citer non seulement celles qui sont
tions and suspensions onto inert bed particles, particle basks sur la diffusion et/ou la chaleur (chauffage ou refroidis-
coating, and granulation, but also certain mechanical functions sement de matitres solides, dchage de solutions et de suspm-
like solids blending, comminution and aerosol collection from a sions sur les particnles inertes dn lit, enrobage des particles el
gas stream. The use of spouted bed reactors for several chemical granulation), mais aussi certaines fonctions mbcaniques (mC
pracesses - coal carbonization, shale pyrolysis, ore roasting, langes de matikres solides, reduction en petits fragments et
cement clinker production, and thermal cracking of petroleum captage des aerosols d'un courant gazeux). L'emploi du lit
- has also received attention. fluidis6 avec giclage dans plusieurs procMb chimiques (carbo-
'l'his paper presents a review of the above developments, nisation du charbon, pyrolyse des schistes argileux, grillage des
supplemented in a few cases by recent results of research being minerais, production de cinient non broy6 et craquage ther-
carried out at the University of British Columbia. The parti- mique du petrole) a aussi retenu l'attention.
cular features of a spouted bed which play the key role in each On fait, dans le prksent travail, une revue des dkveloppe-
type of application are identified, some new applications are meuts pr6citks et y ajoute dans certains cas les rksultats rkents
suggested and consideration given to the future industrial de travaux de recherches exCcut6s Q 1'UniversitC de Colombie
potential of individual processes. britannique. On identifie les caracthristiques particulitres d'un
lit fluidis6 avec giclage qui jouent le principal rble dans chaqne
type d'application; on sugghe Cgalement des nouvelles applica-

T he spouted bed technique"', originally developed


a s a method for contacting coarse solid particles
with gas, consists in forcing a jet of gas vertically up-
tions et considere le potentiel industriel, dans l'avenir, pour
des procCdCs individuels.

wards through the mass of solid particles. The high-


velocity jet causes a stream of solids to rise rapidly stands by itself, relying on the use of coarse heat-
upwards in a hollowed central core or spout within the carrier particles which permit high gas flow rates to
bed. The particles, having reached somewhat above the be used.
bed level, fall back onto the annular space between the A summary of the work carried out on each of the
spout and the container wall and travel downwards as above applications, under the broad categories of
a packed bed. The gas flares out into the annulus as physical operations and chemical processes, follows.
it travels upwards. Thus, a systematic cyclic pattern A few suggestions for new applications are also in-
of solids movement is established with effective con- cluded.
tact between the gas and the solids.
The operations for which the use of a spouted bed
has already attracted attention are remarkably varied. A - PHYSICAL OPERATIONS
The main features of the various applications a r e
summarized in Table 1, which also shows the stage of A.1 Diffusional
development in each case. For drying, heating, and The processes grouped together under this heading
cooling of granular solids, and for gas cleaning, the all involve mass transfer accompanied by heat trans-
chief attraction of a spouted bed is the same a s that fer.
of a fluidized bed, namely good solids agitation com-
bined with effective gas-solids contact. For these (a) Drying of grmular sdids
operations, as also f o r solids blending, spouting serves By f a r the most popular application of spouted beds
the same purpose for coarse particles as fluidization has been drying of coarse, heat-sensitive granular
does for fine materials. In coating and granulation, t h e materials which include a range of agricultural prod-
main advantage arises from the regular cyclic motion ucts, wood chips, various polymeric materials, ammo-
otf solids which permits deposition of successive lay- nium nitrate and manganese chloride. The available
ers on the particles, allowing enough residence time data f o r both experimental and industrial driers are
in the annulus between depositions for each layer to summarized in Table 2. Although the range of mois-
dry before the next one is deposited in the spout; tures and drying conditions vary widely, it is seen
while the attrition caused by inter-particle collisions in that there is always a wide temperature gap between
the spout plays a key role in drying of suspensions the hot a i r and the bed. This feature of spouted bed
and solutions onto inert particles, as well a s in com- drying represents its main advantage over convention-
minution, coal carbonization, shale pyrolysis and iron al non-agitated driers, in which the smaller tempera-
ore reduction. The application of spouting to thermal ture gap necessitates that the air temperature be kept
cracking of petroleum, where the short residence time much lower in order to avoid thermal damage to the
of the vapors in the bed is a critical requirement, particles.

The Canadian Iournul of Chemical Engineering, Vol. 52, April, I974 129
TABLE
1
SUMMARY OF REPORTEDSPOUTED BED APPLICATIONS

Application Main Features Stage of development


1. Drying of granular Particularly suitable for heat-sensitive materials such as agricul- In industrial use.
materials [references in tural products, polymers, etc. Agitation of solids permits the use
Table 21 of high temperature air and therefore rapid drying, minimiiing the
risk of thermal damage. Also suitable for sticky solids since ag-
glomerates disintegrate in the high velocity spout.
2. Granulation (6-8) Melt or solution is atomized into the bed, which is spouted by hot In industrial use.
gas. Initial bed consists of product granule nuclei, which build UD
by a mechanism of layer-by-layer growth as they cycle in the bed.
A well-rounded granule of uniform structure is thereby produced.
3. Drying of suspensions Same principle as in (2) except that bed consists of inert particles, In industrial use.
and solutions@, e.g. glass beads. Solution is atomized into the lower region, coats
the particles. the coating becoming urogressively more fragile as
it dries until it is knocked off by inter-particle collisions. Fine
product is collected overhead.
Applications where drying and chemical reaction occur concur-
rently in a bed of inert solids have also been reported:
(a) production of magnesium oxide from hydrated magnesium Laboratory-scale work in a 7.6
chloride [SS]. cm dia column.
(b) oxidation of sodium sulphide present in lime mud from the Process conditions for continuous
cheniical recovery system of a kraft pulp mill [67]. operation have been established,
using a 15 cm dia reactor.
4. Reaction-granulation Process combines fertilizer granulation with neutralization in the Preliminary work on bench scale.
(10-12)
same spouted bed unit. Acid spray and amrronia vapours are
introduced with the hot air jet. Bed consists of product granules.
5. Tablet coating(13-16) Batch operation. Coating solution introduced with hot air as in (2) In industrial use.
and (3). Compared to conventional coating pans, spouted bed gave
more uniform coatmg, better batch to batch uniformity, shorter
batch time, and lower overall cost.

6. Coating of nuclear fuel


particles(18-a2)
The bed of fuel particles is spouted with hydrocarbon vapours plus
helium, and is maintained a t a high temrerature ( w 1500°C) by
heat input from a surrounding furnace. Pyrolytic deposition of
Laboratorr scale investiga-
tions. E fect-of process condi-
tions on microstructure of coat-
carbon occurs, giving a uniform and tough coating. ing has been studied in detail.
7. Gas cleaning (a) Spouted bed used for regenerating spent adsorbent (activated Not known.
charcoal granules) in conjunction with a fluidized bed for
vapour adsorption in a gas cleaning system 1251.
(b) Bed of coarse inert particles is used for removal of micron-size Preliminary experiments in a 15
particulates from the spouting gas. Capture occurs by inertial cm dia column.
impaction and diffusional mechanisms [35].
8. Pre-heating of coal(*e) Coal of about 6 mm size heated to 250°C in continuous operation, Preliminary study in a 15 cm dua
as pre-treatment before coking in coke ovens. Promising outcome, column.
multi-stage operation visualized for large scale.
9. Cooling of fertilizers(27) Double-deck installation with multiple sDouts for cooling up to In industrial use.
30,000 kg/hr of fertilizer from 120°Cto 40°C.
10. Solids blendingP. 33) Rapid and effective blending of granular solids ( olymer chips) I n industrial use.
achieved a t lower power cost than in mechanical bhnders. Econo-
mics of spouted bed blending is particularly favourable for large
batch sizes.
11. ComminutionW Particulate solids are finely ground by adding to the bed a pro- Preliminary experiments in a 15
portion of hard and heavy particles of another material (e. g. glass cm dia column.
beads) to serve as the grinding medium. Ground product is elu-
triated by the spouting air and is collected overhead. Advantage
over conventional mills visualized for duties requiring grinding
simultaneously with intimate gas-solids contact e.g. for drying,
cooling, heating or reaction.
12. Low-temperature coal Use of coarse particles (2.5 mm) together with the violent agitation Detailed investigation in a 15 cm
~arbonization(a7~40-42) in the spout region allowed continuous operation without the dia carbonizer.
problem of agglomeration. Process worked well with a variety of
Australian coals a t carbonization temperatures 450 - 650°C.
13. Shale pyrolysis (‘3, 44) Continuous operation with coarse shale of up to 6 mm size, temre- Bench scale operation showed
ratures of 510 to 730°C. Attrition of particles in the spout was spouted bed process to be feasi-
beneficial, since the outer surface of a particle became fragile on ble.
loss of organic matter and was broken off exposing fresh surface
for retorting. Fine spent shale collected in an overhead cyclone.

130 The Canadian Journal of Chemical Engineering, Vol. 52, April, 1971
TABLE1 (CONCLUDED)

14. Iron ore reduction Good solids agitation, absence of fines in the reaction zone and Effect of process variables has
( 4 6 , 4 7 , 48. 68) breakdown of agglomerates in the spout, all together, enabled re- been thoroughly studied, though
duction to be carried out at temperatures up to 1OOO"Cwithout on a very small scale.
the solids becoming sticky. More rapid and complete reduction of
coarse ore, as well as of ore-fuel pellets, to sponge iron was conse-
quently achieved than occurs in fixed or fluidized beds.
15. Cement clinker productior Decarbonated cement granules of 1-3 mm dia were spouted at 1350 Preliminary bench-scale work, to
(49) - 1550°C. The gas inlet tube was used as clinker Froduct outlet, t e followed by experiments at
the terminal velocity of the granules increasing sufficiently during 1550 - 1750°C.
the process for cleancut separation of the product, but too rapidly
for complete conversion of the feed.
16. Charcoal activationP) Spouted bed process developed for producing coarse granular ac- In industrial use.
tivated carbon using steam and flue gas a t 1000 - 1500°C as
spouting medium. Batch industrial unit in operation since 1970,
capable of activating a charge of 150 - 200 kg in 80 - 90 min.
17. Thermal cracking of Bed of 1-4 mm size heat carrier particles was spouted with steam Optimum process conditions
petroleum (crude oil. plus petroleum vapours to produce ethylene and Fropylene at have been determined on a
heavy oil and naphtha) 550 - 860°C. W e of coarse solids allowed operation at higher gas bench scale.
( 6 0 , 5)) velocities, hence with shorter contact times, than in fluidized or
packed beds. Ethylene yield, being favoured by a short contact
time, was consequently higher. Heat economy was improved by
the use of a spouted bed combustion chamber in conjunction with
the cracker.

TABLE
2
DATAON
AVAILABLE SPOUTED BED DRYING
OF GRANULAR SOLIDS

Eed geometry Moisture content


%, dry basis Feed Air Air Ed
4 P. D, H rate rate temp. temp. Soice
Material dried mm Mglm3 cm cm Feed Product kglhr kglhr "C "C ref. no.
Bench or pilot
:;cale
Wheat 4.0 1.4 30 30-122 20-36 17-29 110-270 242-278 100-177 38-54
Wheat 3.6 1.5 23 91 25 15-19 28-43 143-156 97-166 45-75
Wheat 4.1 1.4 15 9-2 1 20-44 4-12 Batch 35-53 60-180 -
Wheat 4.1 1.4 15 14 21-30 14-18 1.8-3.6 35 70-145 -
Coffee beans 11 x 20 0.9 15 61 45 12 6.5 38 160 68
Peanuts (whole) 10 X 23 0.3 30-61 - 30 15 Batch - - -
Wood chips < 16 - 30 38-46 150-190 49-58 36-59 360 400-600 75-88
Styrene 0.6-1.2 1.o conical 8-25 1-30 0.2-0.3 0.5-5 108-192 80-160 -
polymers ? = 24"-50'
Polyvinyl
chloride 0.4 1.o - -
Polyvinyl formal 1.8 1.2 - -
Calcothar 0.7 3.5 22 17-28 3-290 - 0.2-3.5 3-85 70-120 -
SG-1 copolymer 2.2 1.3 - -
MnC12.4H20
(dehyd.) 2-5 - 10 <43 - - 0.5-5 12-24 350-500 20-320
Activated
carbon 0.6-0.8 0.4 7 15 12 0.2 0.19 1.7 110 -
Superphosphate 3-6 0.8 17.6 45 12 4-5 48 - 155-160 -
Geiatine (2-step >5 - 17.6 8 59 30 0.53 157 28 -
process) 25 30 15 0.91 - 50 -
Industrial scale
Peas 6.7-7.5 1.4 61 214 23-68 21-47 1000-1700 !600-3 100 124-284 15-78
Lentils 4.4 - 61 214 25 17 1160 1470 297 69
Flax 2.2 1.1 61 214 35 14 890 1600 448 67
Ammonium
nitrate 1-4 0.9 61 117 7-8 <1 100-125 410 155-165 65-75
Polymer
granules - - 122 -244 Other inf nation no .eleased

The Canadian lournal of Chemical Engineering, VoZ. 5 2 , April, 1974


-
Figure 1 - Pilot wheat drier of Mathur
and Gishler'2).

Figure 2 - Layout of an industrial drier


for agricultural product^'^'.
n
BLOWER

4 AIR

'COOLED WHEAT RECEIVER S a l l a n ~ ' ~ 'amounted


, to more than twice that f o r a
conventional moving bed type of drier commonly used
in North America. The overall picture which emerges
from the above comparisons is that spouted bed drying
The pilot wheat drier used by Mathur and Gishler"', offers large savings in capital cost and space over
which may be regarded as typical of a continuous conventional drying methods, a t no additional operat-
granular-solids drying system, is shown in Figure 1. ing cost. It should be noted that for materials which
Wet solids enter the upper part of the annulus and tend to stick or form lumps during drying and there-
become rapidly intermixed with the bed material, fore cannot be easily handled in conventional driers,
which discharges continuously through an overflow the advantage of using a spouted bed would become
pipe so that the desired bed level is maintained. The much greater. Examples of such materials in Table 2
overflow is located diametrically opposite t h e feed are manganese chloride, ammonium nitrate, and gela-
point in order to minimize shortcircuiting. Hot solids tin granules, all of which tended to cake so badly t h a t
leaving the drier are brought in contact with cold air attempts to dry them even in fluidized beds were un-
in a second column to cool them down to a safe storage successful. For such materials, the breakdown of em-
temperature. Some additional drying also occurs in the bryonic agglomerates in the high velocity spout con-
cooler by virtue of the sensible heat available in the stitutes a crucial advantage.
particles. Since uniformity of bed temperature is not
required during cooling, the cooler may be operated as ( 6 ) Drying of suspensions and solutions
a moving packed bed, a s shown in Figure 1. Adequate
cooling of the hot wheat was obtained in the moving (i) I n a bed of seed particles: gramdation
bed a t approximately half the a i r flow rate used in
the drier, though a somewhat wider column had to be The use of a spouted bed for producing millimeter
used - 38 cm dia as against 30 cm dia for the drier - size granules starting from pastes, suspensions o r so-
to allow sufficient residence time. Moisture removal lutions, was first proposed by Berquin"', and forms
in the cooler amounted to about $" of that in t h e drier. the subject of a patent issued to P.E.C. of France'",
Up to 270 kg/hr of wheat, through a dry basis mois- and of a later patent to I.C.I. of Britain"). The bed
ture range of 4%, could be dried in a system of this in this process consists of particles of the material
size, using 177°C inlet air. which is to be granulated (seed granules), and the
liquid phase is injected into the base of the bed to-
The layout of a similar industrial installation con- gether with the hot spouting gas as shown in Figure
sisting of a 61 cm dia spouted bed drier (with a 1.78 3. A thin layer of the liquid i s deposited on the circu-
m deep bed) and a 76 cm dia moving bed cooler is lating particles as they pass through the liquid spray,
shown in Figure 2. Two such units have been in satis- which is dried by the action of hot gas as the particles
factory operation in Canada for over ten years, for travel further up the spout and down the annulus.
drying peas, lentils and flax. The a i r for the spouter Thus a particle builds up by a mechanism of layer-
is heated by direct combustion of natural gas and a by-layer growth as i t cycles in the bed, with opportun-
steady bed temperature is ensured by t h e provision of ity for each layer to dry before the deposition of the
a modulating valve on the burner, actuated by a tem- next layer. The granule produced by this mechanism
perature controller in the bed. This installation is is well-rounded and of uniform structure, since any
capable of drying almost 2000 kg of peas per hour irregularities are evened out as the particle builds up.
through an 8.8% moisture range (dry basis), though The process lends itself to continuous operation and
the capacity varies considerably for different types yields a product of uniform size with only small pro-
of peas (see Table 2 ) . portions of undersized or oversized materials.
On t h e economics of spouted bed drying, P e t e r s ~ n ' ~ ) Such a process can also be carried out in a fluidized
has estimated that, while the capital cost of the plant bed, but the use of a spouted bed enables granules of a
in Figure 2 was only about 1/3 of an equivalent cascade much larger size to be produced. Apart from this, the
drier, the operating cost of the two types was compar- existence of a high voidage high-gas velocity zone a t
able (0.4 cents/kg of peas). The similarity in operat- the bottom of the spout, which is also the hottest zone
ing costs, despite the fact that the air consumption in in the bed, provides an ideal location for injecting the
a spouted bed drier is substantially lower, arises from liquid spray. Rapid evaporation of water in this region
the higher blower delivery pressure required in the causes the temperature of the hot gas to fall sharply
spouted drier. Thus, in wheat drying, t h e power cost before i t comes in contact with the bulk of t h e bed
f o r a spouted bed drier, as worked out by Becker and solids. Higher inlet gas temperatures can therefore

132 The Canadian Journal of Chemical Engineering, Vol. 5 2 , April, I974


RECYCLE SOLIDS 1 EXIT GAS To CYCLONE

Figure 3 - Spouted bed


tem, after Berquin"').

-
granulation sys-

Figure 4 - Reactor-granulator of Vyzgo


et al. for producing nitric-phosphate fer-
ti1izer"O'.

be used without causing thermal damage to the bed to remove the last few percent of moisture from the
particles than would be permissible in a fluidized bed, product. Spouted bed granulation, on the other hand,
with consequent improvement in evaporation rates. places no restriction on the maisture content of the
The most important advantage, however, arises from liquid phase, uses compact equipment, and is capable
the systematic cyclic movement of particles in a spout- of producing a dry product in one step.
ed bed, as against the more random motion in a fluid- With highly concentrated solutions, such as are nor-
ized bed, since with the former, agglomeration is mally processed in a prilling tower, e.g. in the manu-
avoided so that the granules produced are uniform in facture of ammonium nitrate and urea, cold rather
size, and possess a homogeneous layered structure. than hot air can be used in the spouted bed system,
In comparing spouted bed granulation with other with consequent thermal economy. The melt is pre-
conventional granulation techniques, Berquin'" has heated to a temperature above its crystallization point
pointed out that granulation in a rotary drum or in a and crystallization commences during atomization of
system where the liquid phase is sprayed into a stream t h e melt as a result of rapid cooling of the liquid drop-
of hot gas, both yield a fine product containing a wide lets by the action of the high velocity cold air stream.
range of particle size. For obtaining large granules of The subsequent process of particle build-up and drying
unliform size, the prilling process is usually employed i s the same as described above. Another variation of
but this can be used only with solutions of very low the process covered by the Berquin patent concerns
moisture contents. If the moisture content is more than the granulation of materials which a r e normally in
a few percent, the height of the prilling tower required solid form a t ambient temperature but which can be
becomes prohibitive. In any case, a prilling tower be- melted without deterioration of properties. Examples
ing commonly 30 meters or more tall, represents a of materials quoted a r e metals such a s lead and bie-
large capital expenditure and is therefore economic- muth, their alloys, sulphur, and organic substances
ally viable only for large capacities. Even with such such as naphthalene. The temperature of the spouting
heights, the prills produced sometimes require further gas (which may be an inert gas such as nitrogen, if
drying using other equipment such as rotary driers necessary) is kept below the melting point of the ma-

TABLE3
SP~UTED
BEDGRANULATION
- PERFORMANCE
DATAREPORTED
BY BERQUINW

Product
Feed solution Air temperature Weight of
Particle Moisture "C Air flow Capacity bed of
Moisture Temperature size content rate Mg/hr ot seed gra-
Material % "C mm % Inlet Outlet m3/sec product nules, Mg
______
Complex fertil-
izer (nitro- 27 cold 3 - 3.5 2.4 170 70 13.9 4 -
phosphorus) W%)
Potassium 68 cold 4-5 - 200 60-65 13.9 1 1
chloride (oversize <5%)
Ammonium
nitrate 4 175 2.5 4 - 0.2 col rl 55 13.9 9.5 1.5
Sulphur 0 135 2-5 0 cold - 0.0111 0.04 0.008

*Injecting 1 litre/hour water as spray into the spouting air reduced the air requirement to 0.007 m3/sec for the same product output.

The Canadian Journal of Chemical Engineering, Vol. 5 2 , April, 1974 133


terial to {begranulated, which is pre-melted and intro- (ii) In a bed of i n e r t solids
duced into a bed of seed granules together with the
spouting gas, as before. The atomized droplets cool An ingenious method f o r drying of solutions (evapo-
down t o a temperature close to the solidification point rative crystallization) and suspensions in a bed of
in the lower part of the spout but actual solidification inert particles of spoutable size, e.g. glass beads of
does not occur until the droplets are deposited on the 3-6 mm diameter, has been developed a t the Leningrad
bed particles in the upper, low-voidage, part of the Institute of Technology's*9'for applications where the
spout. dried solids are ultimately required in the form of a
Some performance data reported by Berquin, for fine powder rather than as large granules. The solu-
each of the above three types of applications a r e given tion, containing u p to 85% water, is atomized into the
lower region of a bed spouted with hot air, deposits
in Table 3, while a sketch of the granulating system
used is shown in Figure 3. Included in the sketch is a s a thin film on the glass beads passing through t h a t
region, and subsequently dries as in the granulation
the arrangement f o r recycling of undersized and
crushed oversized material. Berquin has, however, not- process described in the previous section. The film,
however, does not continue to grow on the glass beads
ed that practically no oversized granules were pro-
during successive cycles ; it becomes progressively
duced, while the proportion of undersized particles in
the overflow from the granulator could be kept to a fragile as i t gets drier and is knocked off the particle
surface by inter-particle collisions in the spout. With
minimum by "judicious location of the overflow pipe".
the relatively large and heavy inert particles used,
This effect was made possible by a certain degree of
the film is reduced to a fine powder during the colIi-
classification which reportedly occurred, with the large
granules segregating out in the upper part of the sions, is elutriated out of the bed by the spouting air
and collected as the product in an overhead cyclone.
annulus near its periphery.
The technique of spouted bed granulation has proved The cyclic process of deposition, drying and demoli-
to be useful for even a wider range of solid materials tion of the surface proceeds continusuly provided t h a t
than those cited by Berquin. Extensive data on granu- the bed temperature for a given feed rate of solution
lation of materials such a s inorganic pigments, orga- is maintained a t a sufficiently high level so that the
nic dyes and a number of other heat-sensitive sub- proportion of wet and sticky particles in the bed under
stances have been reported by Romankov and Rash- steady-state conditions remain small, and the spout-
kovskaya"', for both bench-scale and industrial-sized ing movement in the bed as a whole is not jeopardized
units. The system used by the Soviet workers is es- by agglomeration of the wet particles. Stability of the
sentially the same as that of Berquin, but they expe- process depends not only on the rate of drying of the
rimented with different feeding arrangements and wet film but also on the mechanical properties of the
found t h a t for viscous pasty materials, introducing dried film since, if this film were to adhere tenacious-
the feed into the top of the bed through a vibrating ly t o the particle surface, it would simply continue to
feeder worked well. For high-moisture content solu- grow as in granulation. The minimum moisture con-
tions, on the other hand, injecting the feed into the tent attainable also depends on the attrition character-
high-temperature lower region of the bed, either co- istics of the dried surface film since the attrition rate,
axially with the spouting air as in Figure 3 or side- in addition t o being dependent on hydrodynamic fac-
ways through the column wall, proved more suitable. tors such as air velocity, size and density of the inert
It should be noted that although the spouting columns particles, etc, is also a function of moisture content.
used by Romanov et a1 in their granulation experi- For instance, if the surface film of a particular mate-
ments were of cylindrical-conical shape, the operating rial becomes very fragile when its moisture content
bed depths were so small that in most cases the bed reaches x%, then the process would obviously not per-
would have remained within the lower conical part mit drying that material to less than x% moisture.
of the apparatus, unlike Berquin's granulator in Fig- Since the mechanical properties of a surface film and
ure 3, the overflow pipe location of which shows that its dependence on moisture content are specific proper-
the bed extended to a considerable height into the ties of a material, t h e suitability of spouted bed dry-
cylindrical part. ing f o r a given application and the optimum size and
density of the inert particles must be determined by
On the mechanism of the process, Romankov and co- experiment.
workers have noted that side by side with the growth
of the original bed granules, a certain number of new The method described has been successfully used by
particles are constanly formed within the bed, partly the Leningrad group for drying a wide variety of
by breakdown of the growing particles due to attrition materials, including organic dyes and dye-interme-
and partly by evaporation of those liquid droplets diates, lacquers, salt and sugar solutions, and various
which fail to deposit on existing particles. These new- chemical reagents. Detailed data for both laboratory-
ly formed particles, together with the fine recycled scale and industrial driers can be found in the Roman-
particles, serve as nuclei for t h e formation of new kov-Rashkovskaya book"'. Included in the book is a
granules, although a certain proportion of these fine comparison of the actual costs incurred in t h e Soviet
particles is elutriated out of the bed before they have Union in drying a black dye using different types of
an opportunity to grow. Steady-state operation is driers, at an industrial plant of 6000 kg/24 h r capac-
therefore possible only when the rate of formation of ity. The total drying cost per 1000 kg of dried dye
granules of the desired size range is so balanced by the containing 5% moisture, starting from a 65% mois-
net rate of appearance of fresh nuclei in the bed that ture paste, is quoted a s 24.3 roubles for the spouted
the size distribution of the bulk bed material re- bed drier as against 46 - 46 roubles for a double-drum
mains substantially unchanged with time and within drier of the same capacity. Reger et a1"' have empha-
the limits of spouting stability. Thus, the key operat- sized that close control of the exit a i r temperature (or
ing variables are not only the temperature of the inlet bed temperature) is essential to the success of the dry-
air and feed rate of the liquid phase which would con- ing process; if i t falls below a certain minimum value,
trol the growth rate, but also the size distribution and the glass beads tend to stick together, disrupting the
rate of recycle of fine solids. spouting action, while an upper limit on i t is placed

134 The Canadian Iournal of Chemical Engineering, Vol. 52> April, 1974
by consideration of thermal damage to the dried prod- tween 60 and 65°C. While the importance of proper
uct. acid distribution has been emphasized by these work-
Spouted beds of inert particles have also been used e r s too, they did not adopt any special measures t o
for carrying out chemical reaction concurrently with keep the neutralization zone free of solid particles, as
drying. Thermal decomposition of hydrated magnesium did Vyzgo et al. Instead, the acid was atomized ver-
chloride has been achieved f o r producing magnesium tically upwards through a central nozzle located con-
oxide'eE', using a bed of -3 +8 mesh aluminum silicate centrically with the gas inlet pipe and projecting
pellets maintained a t 500°C to 700°C by hot spouting slightly into the bed. Such an arrangement appears t o
gas. Another application involves spouted bed drying have proved quite satisfactory, at least f o r the limited
of lime mud from the chemical recovery system of a range of experimental conditions explored.
kraft pulp mill, in order to achieve complete oxidation
of the sulphide present in the mud'B''. The drying step
is intended to avoid the evolution of odorous HzS gas ( d ) Pmticle coating
from the subsequent calcining operation, and to in-
crease the calcining capacity of the kiln at the same (i) Deposition from a liquid solution
time. The principle of spouted bed granulation can also be
used for coating of particles and has been successfully
applied at Abbott Laboratories by Singiser and co-
(c) Spouted bed as a reactor-granulator w o r k e r ~ " ~ ~in' ~t 'h e pharmaceutical industry to tablet
The possibility of using a spouted bed as a combined coating, where the requirements for uniformity of
reactor-granulator, a s well as drier, has been explored coating thickness are particularly stringent. The ar-
by two independent groups of investigators, a t Tash- rangement for feeding the coating liquid into the
kent in the USSR"o~")and a t Trail in Canada"". Both spouted bed was similar to that used by Berquin (see
groups initially tried using a fluidized bed for carry- Figure 3 ) ) but the operation was carried out batch-
ing out the combined process, but found t h a t the use wise presumably because this ensured equal residence
of a spouted bed yielded a rounder, smoother and hard- time in the bed for the individual particles, production
er granule without the problems of agglomeration and rates involved in tablet manufacture being relatively
scaling of the distributor plate, as well as of reactor small in any case. The operation consists in loading a
walls, encountered in fluidized bed operation. batch of tablets to be coated into the colunm, turning
Vyzgo and co-workers"o' experimented with produc- on the hot a i r supply to spout t h e bed and then starting
ing nitric-phosphate fertilizer mainly in a 32.5 cm dia the flow of the preheated coating liquid through the
reactor. The bed consisted of product granules (1.5 pneumatic atomizing nozzle. The rate of liquid flow
mm size) and was spouted with a gaseous mixture of is so regulated that the spouting action is not impaired
air and ammonia a t 100 - 120°C. Preheated acid solu- due to stickiness caused by excessive surface moisture
tion, obtained by the nitric acid decomposition of rock on the tablets. After the desired quantity of coating
phosphate and containing 25 - 50% moisture, was solution has been supplied to the bed, a period of
atomized into the spouting gas a few centimeters below drying to remove any residual solvent from t h e coat-
the point of its entry into the bed (see Figure 4). A ing is allowed a t a reduced air flow rate with the bed
grate with about 50% open area was placed in the gas in a quiescent condition. Since drying of the solution
inlet pipe a t the level of the liquid injection so t h a t during the coating operation occurs almost instanta-
the linear velocity immediately above the grate, at t h e neously, there is little danger of solvent penetration
gas flow rates used, became sufficiently high to en- into the tablet core, and therefore the final drying of
sure that the section of the pipe between the grate the coated batch takes only a few minutes. Coating
and the narrow end of the cone remained substan- times required for 70-100 kg batches in a 38 cm dia
tially free of particles. This arrangement, according column were between 1and 1.5 hours, the inlet and exit
to the authors, is a key feature of the process since it a i r temperatures being typically 63°C and 27°C re-
enabled neutralization, which is accompanied by rapid ~pectively"~'.
evaporation of moisture, to be completed before the The results of film thickness measurements made by
products of reaction made contact with the bed solids. Singiser and L~wenthal"~',which are reproduced in
The subsequent granulation process within the bed Table 4, demonstrate t h e uniformity of coverage ob-
occurs in the same way a s described in the previous tained in spouted bed coating.
section. The bed temperatures observed in these expe- Good batch to batch uniformity was also achieved,
riments were 60 - 75°C) and the product moisture since once proper operating conditions (namely charge
contents less than l%"O'. The authors have claimed weight, flow rate and temperature of air, and feed
that the fertilizer produced contained a higher pro- rate and temperature of the coating liquid) had been
portion of assimilable phosphates (90% of the total established for each product, close control of these
phosphates 1 than is commonly achieved. Formation could be easily exercised. The workers a t Abbott Lab-
of undesirable phosphates during ammoniation was oratories have reported t h a t tablets coated by this
avoided by the intensive mixing in t h e neutralization process consistently met the pharmaceutical standard
zone, while deterioration caused by local overheating W.S.P. XV enteric test), thus eliminating the need
during the granulation step was minimized by virtue fnr rpcoating and subsequent retesting. A similar in-
of the well-mixed nature of the solids. dustrial unit is known to be in satisfactory operation
The Canadian work cited above was primarily con- in Canada"".
cerned with ammoniation of phosphoric acid to produce Examples of other commercial operations, for which
ammonium phosphate fertilizers, and was carried out the coatinn technique described above should be well
in a 14 cm dia column using bed depths of 2 to 3 col- suited. are encapsulation of pelletized artificial fish
umn diameters. Acid concentrations tested were 23% food to make i t water-resistant, and of seed grain to
and 40% PsOS, with ammonia to air ratio in the spout- delay germination. Some preliminary experimental
ing gas in the 5-1096 (by volume) range. Bed tempe- work on the former application has been carried out
ratures recorded under these conditions varied be- a t the University of British Columbia"". Coating of

The Canadian lournu1 of Chemical Engineering, Vol. 5 2 , April, 1974 135


Tablet Face Tablet Wall
Average Average
Taibet Surface Tablet thickness*, Range, thiC!ir.eSS*, Range,
sue, mm Shape area, mm2 wt., mg Pm wn pm wm
___---___-- __I__

10 Standard concave 285 500 107 89 - 133 97 76 - 114


10 Deep cup 259 500 136 114 - 159 109 82 - 133

granular fertilizers and other chemical substances to gas cleaning developed by NBmeth et al(") makes use
protect them against caking in storage or to reduce of a spouted bed for carrying out the desorption step
their rate of solution are further possibilities, men- in the process, presumably with steam as the spouting
tioned by Nichols"'. fluid, while a fluidized bed is used for adsorption. The
spent adsorbent (for example, activated charcoal gra-
(ii) Thermo-chemical deposition nules) is fed into the base of the desorber by entrain-
ment into the spouting gas, and the regenerated part-
Several investigations on coating of uranium oxide icles from the top of the spouted bed overflow into the
and uranium carbide particles with pyrolytic carbon, surrounding moving bed drier (see Figure 6 ) . Apart
in an apparatus of the type shown in Figure 5, have from the intensive gas-solid contact provided by the
been reported in recent years('8-2z),mainly from the spouting action in the desorber, the choice of a spout-
U.S.A. Only small coating units (less than 50 mm dial ed bed in this case is dictated by the particular con-
have been used with shallow beds (HID,< 2.6) of figuration of the equipment which requires elevation
uniform-sized particles in the size range 0.2 to 0.6 of the solids from the bottom of the adsorber to the
mm. While the experimenters themselves have de- top of the drying compartment. Since the vertical
scribed the process as "fluidized {bedcoating", Abdel- transport of solids was achieved a t one-tenth the gas
razek'z'l, who made a detailed study of the hydrodyna- velocity for pneumatic conveying, a considerable sav-
mics of beds similar to those used in the coating expe- ing in power cost was realized by combining the de-
riments, has identified the coating unit as a spouted sorption process with vertical transport through the
bed system. use of a spouted bed, instead of transporting the sol-
The use of carbon-coated nuclear fuel particles hold ids pneumatically as for a hypersorber. The novelty
potential for high-temperature, gas-cooled convertor of the system as a whole lies in its compactness,
reactors, but the technical feasibility of this concept achieved by arranging the adsorption, desorption, dry-
depends on the ability of the coating to retain its ing and heating zones in the form of concentric cylin-
structural integrity during reactor service"8). Since drical compartments.
failure can arise from a large number of causes such
as fuel swelling, fission-gas pressure, thermal expan-
sion or contraction of coating, radiation damage, chem-
ical reaction of fission products with inner coating
surface, etccZ3),
the properties of the coating required, ._
which depend on the micro-structure of the deposited
carbon, are highly specific. The investigations using
spouted beds have therefore been mainly concerned
with determining the structural characteristics of car-
bon coatings formed under varying deposition condi-
**
HELIUM METHANE

tions, e.g. of bed temperature, the particular hydro-


carbon used (methane, propane, acetylene, etc.) , its
concentration in the spouting gas, gas flow rate, and
METERS
the surface area of the bed solids.
The same coating process has also been considered
at Harwell in Britain, but the only unclassified report SPOUTED BED
on it'"' is concerned with the hydrodynamic behavior
of shallow spouted beds consisting of 0.5 to 6.4 mm dia
spherical particles with densities up to 11 Mg/m3.
The choice of a cone-bottomed vessel for pyrolytic
coating is dictated not by any particular desire to
obtain spouting in preference to fluidization, but
rather by the necessity of avoiding the use of a dis-
tributor plate, since deposition on the plate itself can
cause its blockage'"'"). Nevertheless, the resulting
spouted bed appears to serve the process well.

(e) Sorption
Figure 5 - Schematic diagram of a pyrolytic carbon spouted
A continuous adsorption setup ("Ecosorber") for bed coateP).

136 The Canadian Journal of Chemical Engineering, Vol. 5 2 , April, 1974


A ,SPOUTED BED DESORBER
spouted bed process a strong candidate f o r cooling of
coarse solids.

(a) Solids heating


The possibility of preheating coking coal (6 nun
particle size) in a bed spouted with hot air or steam,
as a means for increasing the output of coke-ovens,
has been experimentally investigated by Malek and
Walsh‘281with promising results. In continuous runs
carried out on a 15 cm dia unit, coal temperatures Up
to 250°C were achieved without agglomeration, using
TO BOTTOM inlet fluid temperatures up to 350°C. These workers
OF SPOUTER also experimented with a multi-stage unit of the type
shown in Figure 7 not only with coal but also with
Figure 6 - Continuous adsorption equipment (“Ecosorber‘’)
sand, obtaining higher throughput rates and heat util-
developed by NCmeth et a1‘2J’.
ization efficiencies with multistage operation (see
Figure 8). On the basis of these results, Malek and
(f) Potential diffusional Merations Walsh consider t h a t a 2- or 3-stage operation would be
the most efficient, the effect of increasing the number
There are other diffusional operations, or variants of stages from 3 to 4 being small.
of the above, which suggest themselves as possible
candidates for spouted beds, but which have yet to be
tested. Vapor impregnation of porous solids, e.g. ( b ) Solids cooling
steaming of wood chips, is the converse of solids dry- The design of a large capacity cooler based on the
ing and could presumably be carried out by using the spouting principle has been developed by Fisons Ltd.
vapor as the spouting fluid. This operation, as well for cooling granular fertilizer“”. A multi-spout sys-
as the simpler adsorption used in gas cleaning, is sug- tem is used in a large rectangular vessel with a per-
gestive in its execution, of gas dehumidification by forated plate as its base. The flow rate of cooling air,
hydration of coarse anhydrous solids such a s calcium which enters the bed through the perforated base, is
chloride or calcium sulphate granules, and also of de- sufficient to induce localized spouting action i n the
sublimation by buildup to coarse solids such as naph- solids above each perforation, giving rise to a multi-
thalene or p-dichlorobenzene “moth balls”. On t h e other tude of spouting cells each with its own upward-mov-
hand, removal of a low volatility liquid (e.g. an oil)
ing dilute-phase spout surrounded by a downward-
from the pores of granules could possibly be accom- moving aerated dense-phase annulus. The bed in this
plished by partial pressure distillation (e.g. steam condition would appear t o be rather similar to a nor-
distillation) using hot entraining vapors (e.g. super- mal fluidized #bed.However, a t the operating a i r flow
heated steam) as the spouting fluid, supplemented if
rate, the multiple-spouted bed is considerably more
necessary by internal o r jacketed heating. dense and in more orderly movement than is usual
In each of these operations, as well as any others in a fully fluidized bedcz7’where, with t h e coarse par-
that might be devised, the inherent features of spout- ticles involved, the air-jet issuing from each perfora-
ed beds such as high jet velocities, good solids recir- tion would transform into large bubbles within a short
culation, continuous operation, etc. would only justify distance from the inlet point. The Fisons multi-spout
the commercial use of a spouted bed if these advan- cooler is arranged in a double-deck, on the same lines
tages were not eclipsed by some of the disadvantages, as the two stage system of Malek and Walsh for pre-
such as attrition of solids, moderately high power con- heating of coal just described. Hot solids are fed into
sumption, non-uniformity of particle residence times, the upper stage and discharged from the lower, flowing
etc. It is an engineering commonplace that technical from one to the other through a n internal downcomer,
feasibility of a given process does not necessarily im- counter-current to the flow of the cooling air. Three
ply its practicability on a large scale without compar- such units have been in industrial operation at the
ative assessment against alternate means of perform- Fisons Fertilizer Plant a t Immingham, England, for
ing the same function. cooling 12-28 Mg/hr of fertilizer through a range of
40-80 centigrade degrees. Estimated thermal efficien-
A.2 Thermal cies are well in excess of 80%.

Heating or cooling of coarse granular solids without (c) Food processing


concomitant mass transfer may be carried out in a
spouted bed, in much the same way as drying or ad- Cooking of foodstuffs, although it may involve both
sorption, by transferring heat from or to spouting gas. volatilization and chemical reaction, is probably often
The full benefit of the technique is however realized thermally controlled. The roasting of coffee beans has
only in the case of heating of thermally-sensitive par- been accomplished in a spouted bed using superheated
ticles, since the well-stirred nature of the bed permits steam as the spouting fluid‘as’. Since only a small
the use of higher hot gas temperatures than would amount of volatile material was driven over with the
otherwise be possible without thermal damage to the steam, i t seems likely t h a t hot a i r would be almost a s
particles. For continuous heating of solids, higher heat effective as steam.
transfer rates can therefore be achieved than in a Other thermally controlled treatments of food should
non-agitated system. In a cooling operation, on the also lend themselves to successful execution in a spout-
other hand, the mixing of solids in the bed is not of ed bed. One possible application is the freezing of peas,
critical value, but the ease with which solids can be beans, corn and other food particulates, either whole
fed into and discharged from the bed, together with or diced, using refrigerated s u b z e r o a i r as the spout-
the intimacy of gas-particle contact, still make the ing fluid. Unlike fluidization in deep beds, where food

T h e Canadian Journal of Chemical Engineering, Vol. 52, A#ril, 1974 137


VIBRATING FEEDER
r - 7

om '
I
.- \\
/
I
s,
,
, I

'--I--!-'.
: I
I :
II ,,
3 4
NO. OF STAGES

Figure 8 - Performance data for stage-


wise operation obtained using apparatus
of Figure 7'2R'.

-
Figure 7 Multi-stage spouted bed unit
of Malek and Walsh for preheating
cDQ1'26'.
Column dia = 15.2 cm complex due to high power inputs. I n addition, the
Orifice dia = 1.27 cm need for providing a storage container separate from
the more expensive mechanical blender is eliminated
with spouted bed operation, since here the blender
processing usually involves immersion of the edible itself consists of nothing more than a simple storage
matter in a fluidized bed of inert the corre- vessel, connected for a i r supply.
sponding spouted bed operation would be more adapt- The power consumption for spouted bed blending
able to spouting of the relatively large grains of food depends on the scale of operation, but in genera1 it is
themselves, providing they are sufficiently rugged to less than for mechanical blending. According to Bow-
withstand the jet action of the gas. Although tray'3o) ers et a1'52', power consumption per ton of solids to
or belt'31' freezers with shallow fluidized beds of large maintain a bed in the spouted state remains substan-
food particles are in commercial use, the difficulty tially constant as the diameter of the blender increases,
with sticking of particles onto the gas distributor whereas the time required for blending increases with
plate, which is sometimes encountered, would be elim- increasing blender size. The total energy input per ton
inated by the use of a spouted bed. A further advan- of material blended therefore increases with increas-
tage should arise in the compactness of the equipment, ing scale of operation. Typical power consumption for
since the residence time requirement in spouted bed spouting a bed of polymer chips has been quoted by
operation could be met by employing a deeper bed but these workers as 3.7 W / k g (5 h.p./ton) with blending
one which occupied much less floor area, compared to time varying between 10 minutes and 120 minutes,
fluidized bed freezers. depending on blender size. The corresponding total
work input would therefore range between 2.2 t o 27
A.3 Mechanical kJ (kW - sec) per kg of solids blended. The compar-
In all the applications discussed so far, effective able figures given for a mechanical blender are of the
contact between the bed particles and the spouting order of 10 W/kg and u p to 100 kJ per kg of solids
fluid is of primary importance. The operations de- blended.
scribed in this section, on the other hand, rely entirely
on inter-particle contacts, brought about by mechanical ( b ) Comminution
agitation of the bed solids. For these operations, the The concept of using a spouted bed as a grinding
fact that agitation is caused by the action of a gas jet mill for comminution of particulate solids is a logical
rather than by some other stirring device is really in- extension of the method for drying of suspensions and
cidental, the gas-particle interaction, which does of solutions in a bed of inert solids, described earlier.
course occur, being only of secondary importance. Experiments a t the University of British Columbia'w)
have shown that with suitable choice of inert solids to
(a) Solids blending serve as the grinding medium, and of operating condi-
The spouting technique has proved successful on the tions, the grinding rates obtained are high enough to
) of practical interest. For example, a 28 cm deep bed
industrial scale for blending of polyester p ~ l y m e r ( ~ ~ * ' ~be
which is initially produced in the form of small lumps consisting of -4 1-10 mesh urea mixed with an equal
or chips and requires subsequent blending to obtain weight of 5 mm dia glass beads, after 10 minutes of
improved uniformity in the spun fibre. The blending spouting in a 15 cm dia coloumn with a 12.7 mm dia
operation is carried out batchwise, the use of a spouted a i r inlet, yielded over one kilogram of finely ground
bed in preference to a mechanical blender being pa& urea (54% passing 100 mesh), which was elutriated
icularly advantageous for large batch sizes (above out of the bed by the spouting air and was collected in
67 mSor 2000 ft3), when the mechanical design of the an overhead bag filter (see Figure 9). I n general, the
blender and of the drive transmission system become size range of particles that were carried out of the

138 The Canadian Journal of Chemical Engineering, VoZ. 52, A H l , 1974


bed showed only a small overlap with the size range ticles, and continuous regeneration of these particles
of active particles remaining in the bed. The rate of would be easy to arrange. The technique could have
elutriation can therefore be taken as the effective rate application to air pollution control, as well as to high
of grinding. The bed spouted smoothly without any temperature gas cleaning in conjunction with heat
noticeable segregation of the two solids except when recovery.
the inert to active solids density ratio exceeded 3. The Preliminary experiments to pursue the above idea
grinding rate tended t o drop off with spouting time, have been carriedout recently at U.B.C.'S5'.With liquid
as would be expected in any batch grinding operation. aerosols predominantly in the 1 to 3 micron size range,
A few continuous runs, in which a stream of urea collection efficiencies of over 90 % have been achieved,
particles was fed into the top of the bed to replenish using 15 ern dia x -45 cm deep beds of cement
the carry-over, using mean residence times similar to clinker particles ( 4 = 1.7 mm). Efficiencies obtained
the durations of the batch runs (10 - 30 minutes) , in- with solid aerosols, however, were substantially lower
dicated continuous operation to be equally effective. because aerosol particles failed to adhere permanently
Particle breakdown in a spouted bed apparently oc- to the target particles and were consequently re-en-
curs as a result of relatively low energy impacts in trained. Work to overcome the re-entrainment prob-
the spout region. The grinding performance is there- lem by taking advantage of electrostatic forces is cur-
fore comparable with that of a conventional tumbling rently in progress.
type of mill, rather than of high speed mills like ham-
mer mills or fluid-energy mills. Comparative tests with
urea and cement clinker carried out in a laboratory B - CHEMICAL PROCESSES
ball mill and a rod mill showed that for a similar size
reduction, spouted bed grinding rates were similar B.1 Solids as reactants
to those obtained in the tumbling mills. The energy
consumption for comminution alone is estimated to be ( a ) Low temperature coal carbonization
higher for spouted bed grinding, but in view of the
fact that size-classification is also achieved a t no addi- Low temperature carbonization of coal is a thermo-
tional expenditure of energy, unlike the situation for chemical process involving the evolution of volatile
tumbling mills, the energy consumption for spouted matter from coal in the approximate temperature
bed operation could become competitive. The more im- range 450 - 700°C to form cake. Interest in low tem-
portant advantage of spouted bed grinding over con- perature carbonization centres on the fact that the
ventional methods, however, is considered to be the amount of tar produced, which is an important source
compactness and simplicity of the equipment, arising of liquid fuel, is 3 - 5 times greater than in high
out of the absence of any directly driven mechanical temperature (900 - 1175°C) carboni~ation'~~'. Low
parts. This should reflect itself in lower capital costs. temperature char is softer and more friable than the
The maintenance cost should also be substantially low- coke-oven product produced at high temperatures, and
er particularly when grinding abrasive materials since, is more suitable for use as a smokeless fuel and as a
with the grinding action occurring in the hollowed blend component f o r certain metallurgical purposes.
central core of the bed and not against the vessel walls, In recent years, the main incentive for the development
wear and tear of the main vessel will be avoided. The of the low temperature process has come from its
maximum benefit of a spouted bed mill would be real- adaptability to continuous operation through the use
ized f o r operations requiring comminution simulta- of a fluidized bed where the heat necessary for endo-
neously with effective gas-solid contact. Examples of thermic carbonization is more rapidly, efficiently and
such operations are grinding of hygroscopic or moist uniformly transferred to coal than in a coke oven,
and sticky materials, of solids which tend to become especially if the heat is supplied by partial combustion
plastic with rise in temperature e.g. insecticides, re- of the char within the bed itself's'*s8'. The use of a
sins, gums etc., of easily oxidizable or potentially ex- fluid-solid system a t high temperatures is ruled out
plosive materials which must be ground in a complete- by a severe caking problem, caused by an increase in
ly inert atmosphere, and processes requiring chemical the plasticity of coal particles when subjected to a high
reaction between the solids and the gas simultaneously rate of temperature rise. The problem arises even
with grinding. during low temperature carbonization, if the particles
are fine. Thus in a fluidized bed cafbonizer, with coal
( c ) Potential mechm.ca1 Operations
particles in the 30 - 200 mesh range, it becomes neces-
sary to operate with a large char recycle to avoid ag-
The particle attrition feature of a spouted bed, glomeration - recycle ratios (char/coal) as high as
though undesirable for some operations, has turned out 10/1 have been recommended for certain types of
to be of critical value for others, namely, drying of ~0a1(~~).
suspensions and solutions on inert particles, coal car- It was to avoid the agglomeration problem that Rat-
bonization, shale pyrolysis, iron ore reduction and cliffe and other workers a t the University of New
comminution (see Table 1 ) . I t therefore seems reason- South Waleg'37,40,41,4e)
applied the spouted bed tech-
able to assume that the dehusking of grain, and more nique to coal carbonization since, with the use of
generally the skinning of particles possessing a re- coarse particles, the heating rate and therefore the
moveable outer layer, could also be achieved by promot- caking tendency was decreased. Also, the high velocity
ing controlled attrition during spouting. spout served to break up any agglomerates as soon as
Dust and mist collection from gases is another me- they were formed. Although provision was made for
chanical operation in which some of the special fea- recycling the char if agglomeration occurred, recy-
tures of spouted beds could be exploited. The high cling did not in fact prove to be necessary in any of
velocity spout region should be effective in aerosol the experimental runs carried out. Several different
removal by inertial impaction and the annular region types of Australia coals were investigated using par-
for removal by diffusional deposition. High gas ticles of -6 +10 mesh size and bed temperatures in the
throughput rates should ,be possible since spouted bed range of 450 - 650°C. The heat of carbonization was
operation would permit the use of coarse target par- provided by combustion within the bed using a mix-

T h e Canadian Journal of Chemical Engineering, Vol. 5 2 , April, 1974 139


THERMOCOUPLE

!
-
Figure 10 Berti's shale pyrolysis appa- -
Fignre 11 Quartz reactor used by SO-
ratus with a tapered spouted bed reac- viet workers for iron ore reduction expe-
tor(44). riments. The reactor was surrounded by
a heating furnace'48'.

Figure 12 - Apparatus used by Heertjes


et a1 for producing Portland cement
linker"^'.
ture of air and nitrogen as the spouting medium. The A - feed pipe
proportion of the two gases provided the means for B - reaction zone
controlling the bed temperature. Yields and analyses C - gas inlet tube
of the gas and char produced were determined in each D - product outlet tube
run, but not of tar and light oil. The rate of carry-over E - gas inlet slot
of fines, which contained a proportion of dust from the F. G - ejector burners
coal feed in addition to the char elutriated out of the H - cooling device
bed, was found to be generally high - of the order of
15% of the coal feed. Feed rates varied between 6.4
and 10 kg per hour, the corresponding values of mean
residence time being 44 to 29 minutes. The main out- down to 5.1 cm dia over a height of 45.7 cm (with a
come of the work was t h a t the use of coarse particles 12.7 mm dia gas inlet), so that the large increase in
permitted by a spouted bed, together with the attrition volumetric gas flow along the height was offset by
occurring in the high velocity spout, were effective the increase in cross-sectional area of the bed. The
in avoiding the problem of agglomeration for a wide removal of the reacted solids was so arranged, by lo-
variety of coals, although the oxidizing atmosphere cating a conical exit tube in the upper part of the
used during carbonization must have also inhibited reactor j u s t above the top of the spout, that the rela-
agglomeration to some extent. tively light and small shale particles were preferen-
tially carried out by the gas stream, the rest of the
(6) Shale Pyrolysis solids falling back onto the annulus of the bed.
The process, once started, is self-sufficient in heat,
During mining and crushing of oil shale, 10-20% the heat required for pyrolysis of the organic matter
of the shale produced is too coarse (up to 6 mm par- becoming available from combustion of coke which de-
ticle size) to be effectively processed in a fluid-bed posits on the rock, as well as by combustion of the
retort. An investigation to determine the feasibility light hydrocarbons produced. For starting up, a direct-
of carrying out pyrolysis of this coarse material in a fired propane furnace was used for preheating the bed
spouted bed retort has been reported by Bertic4n,44), in order t o form the initial coke and to initiate its
using the experimental system shown in Figure 10. combustion, which occurs only above 480°C. The shale
The outer surface of the particle undergoing pyrolysis feed was then started and the reactor temperature
becomes soft and friable due t o loss of organic matter controlled by adjusting t h e ratio of recycle gas (which
and is broken off by attrition in the spout region. is essentially free of oxygen) to a i r in the spouting
Fresh surface for retoring is thus continually ex- fluid, the rate of combustion of the coke being propor-
posed as the particle cycles in the bed until the fine tional to the partial pressure of oxygen. The opera-
spent shale, which is also less dense than the unspent tional limits of the reactor were found to be 510 -
coarser material, is elutriated out of the bed. At the 650°C with shale feed rates of 4.5 - 9.0 kg per hour.
same time, some breakdown of cold feed particles also The upper limit on the feed rate was imposed not by
occurs by explosive cleavage a s they enter the hot bed. the residence time requirement in the reactor, but by
The spent shale is collected in an overhead cyclone, insufficient carry-over of spent shale from the reac-
while the gas stream proceeds through the oil recov- tor. Average residence times of 5 - 10 minutes are
ery system consisting of a direct-contact water cooler, considered sufficient for complete pyrolysis as against
a demister unit for coagulating the oil mist formed i n 15 - 44 minutes in the experimental runs. Berti there-
the cooler, and an oil cyclone f o r recovering t h e oil fore suggests t h a t the capacity of the reactor could
in the form of an oil-water emulsion. To maintain be considerably increased by discharging the spent
spouting stabiIity the main body of the reactor was shale (which would presumably segregate out at the
n a b conieal, tapering from 16.5 cm dia a t the top top of the bed) into a sealed hopper through an over-

140 The Canadian Jozcrnal of Chemical Engineen'ng, Vol. 52, April, 1974
flow pipe in the wall of the reactor. The oil yields, ex- give u p to 15% carbon in the granules. The tern-
pressed as percentage of theoretical yield (hypothetical perature range investigated was 800 -1000°C.
value based on total organic matter, assuming t h a t The temperature required for rapid reduction was
100%)of it is recoverable as oil), were less than 50%. found to be 900°C with low carbon content and
The low yields have been attributed by Berti to the 950°C with high arbo on'^''.
large heat loss from the reactor wall compared to the Work on spouted bed reduction of iron ore has been
process heat requirement (-20% 1. Higher yields carried to a somewhat larger scale (batch size: 100 -
would therefore be expected in a larger sized unit 400 g m ) by Ozawa'BB',who has recently reported expe-
where the proportion of heat lost would be substan- rimental results on reduction of Indian and Hamers-
tially lower. ley ores by hydrogen gas.

(c) Iron ore redwtion ( d ) Cement clinker production

A major difficulty encountered in fluidized bed The insulated alumina concrete reactor portrayed in
processes for iron-ore reduction is the tendency of the Figpre 12 was used recently for the experimental pro-
particles to become tacky a t temperatures above 500"C, duction of Portland cement clinker by means of a .
leading to build-up of sponge iron on the reactor walls, spouted .bed'"'. The diameter of the gas inlet tube was
and poor fluidization. The temperature restriction 5 cm and its length 55 cm, while the reactor diameter
thus imposed limits t h e reduction rate and a t least was 15 cm. The solids fed to the reactor were dried,
one process (H-iron process of Hydrocarbon Research decarbonated cement granules of 1 - 3 mm dia, while
Inc.) uses a high pressure, with accompanying com- the spouting fluid was a hot mixture of ai r and burned
plication in the loading and unloading operation, to natural gas. The shrinking and sticking together of the
raise the rate of reduction to a practical cement particles during sintering caused an increase
Laboratory-scale experiments using a spouted bed in their terminal velocity, so that highly selective
reactor with both specially-prepared ore-f lux pellets product separation could be effected in the gas inlet
and coarse particles of the ore itself have been carried tube by setting the gas velocity in this tube at the
out by Soviet worker^'^^^^^^^^', who have reported t h a t terminal velocity of the clinker product. However, a t
the special features of spouting, namely, rapid well- the reactor temperature range of 1350 - 1560"C, the
ordered mixing of solids, absence of dead zones and of conversion of the feed during the particle residence
fines from the reaction zone, and attrition of agglo- time was incomplete. Further experiments are planned
merates in the spout region, enabled reduction of t h e at 1550 - 1750°C as an attempt to rectify this defect.
ore to be carried out a t temperatures as high as 700 -
1000°C without the problem of stickiness. Three dif- (e) Chmcoal activatiori
ferent processes have been studied, using unusually
shallow beds housed in a quartz reactor (see Figure A recent report from R~rnania'~''briefly describes
11) : the development of a spouted ,bed surface for produc-
ing activated carbon, which has passed through the
Reduction of fluxed ore-fuel pellets of 2-3 mm laboratory and pilot plant stages and is now in indus-
dia (prepared from iron ore concentrate, lime and trial use. The spouted bed was chosen in preference
coke in a composition similar to that used in a to a fluidized bed, firstly because a coarse granular
blast furnace process) with water gas, to obtain product was required, an3 secondly to avoid operation-
sponge iron. Comparative tests carried out in a al difficulties associated with using a distributor
spouted bed and a packed bed showed that t h e plate a t the high inlet gas temperatures involved
process of reduction in a spouted bed began to (1000 - 1500°C). The spouting gas consisted of steam
occur intensively a t 900 C, while temperatures of
O
and com,bustion products obtained by burning the
more than 1000°C were required in a packed bed. vapor leaving t h e bed with pre-heated air i n the space
In spouted bed experiments, 97 - 98% reduction above the bed. Both decolorizing and gas-absorbing
of iron in the pellets was achieved in 3 minutes varieties of active carbon in different granule sizes
a t about 1000°C without sintering the pellets or could be conveniently produced by varying the starting
burning them onto the reactor walls'46'. materials and controlling the operating conditions of
Reduction of the ore itself 'by hydrogen and by the furnace t o suit the specifications of the desired
mixed gas (58% CH,, 33.6% H2, 6.0% CO, plus product. The criteria used for scaling-up the furnace
CO1 and 0,) to obtain sponge iron and concentrate to industrial size have been described by the Rumanian
powder. Four different types of ore of size frac- w~rkers'"~~~~'.
tions 0.215 - 0.50 mm and 0.5 - 1.0 mm were tested
in 20-gram batches over the temperature range
700 - 1000°C. With hydrogen as the spouting B.2 Solids as heat carrier or catalyst
fluid, the degree of reduction reached 93 - 95%
within one minute of heating a t temperatures The use of a spouted bed for carrying out vapor
above 7OO0C, while temperatures over 800°C were phase reactions in the presence of non-reacting solid
required with mixed gas. No difficulty due to particles has attracted relatively little attention, de-
stickiness was encountered up t o a temperature of spite the fact that i t possesses several of the same
1000°C. Detailed data on yields and chemical properties which have been responsible for the wide-
compositions of both sponge iron and metallic spread application of fluidized beds in this area, viz.
powder obtained from the different ores under intimate gas-solids contact, ease of addition and with-
various conditions have been rep~rted'~''. drawal of solids, good agitation and therefore uni-
formity in bed temperature. Two possible explanations
Reduction of ore-carbon granules of 0.5 - 1.0 mm come to mind:
and 1 - 2 mm size by natural gas - .(92.4% CH4,
6.2% Hz, plus CO and O,,) The granules used in (1) since heterogeneous gas phase reactions are fa-
these experiments were made from hematite ore vored by a large surface to volume ratio of the
containing 64% Fe, with coke breeze added to solids, the use of coarse particles and therefore

The Canudian Journal of Chemical Engineering, Vol. 52, April, 1974 141
was obtained from the CO and COB contents of the
gas, by assuming that these two gases were produced
entirely by reaction between steam and the deposited
carbon. A large amount of data from continuous runs,
showing the effect of the operating parameters of the
system (see Table 5 for range of conditions and mate-
rials used) on yields of total gas, ethylene, propylene,
methane, hydrogen and carbon f o r each of the three
JACKETED SPOUTED
BED REACTOR feedstocks used have been reported by Uemaki et al.
Their main findings, a s illustrated by the data for
cracking of naphtha, are as follows:
(1) Yields of ethylene and propylene, a s well as of
total gas, increased linearly with reaction tempe-
rature up to about 800°C and began to decrease
at higher temperatures. The maximum yield values
SUPERHEATER obtained were 45% for ethylene, 20% for propy-
GEAR PUMP
lene, and 80% for total gas.
(2) In experiments using different bed depths a t a
Figure 13 -Thermal cracking unit of Uemaki et alcS0).The fixed gas flow rate rate (and bed temp. -820"C),
reactor was 13 cm in diameter with a 1.6 cm dia gas inlet the maximum yield of ethylene (-50%) was ob-
orifice. tained a t a gas-solids contact time of 0.3 sec and
of propylene (-14%) a t 0.15 - 0.2 sec. The con-
tact times quoted are nominal values, obtained by
of a spouted bed would not be advantageous for dividing the packed height of the solids in the
such reactions, and reactor by the superficial velocity of t h e spouting
(2) since a gas phase chemical reactor involves pro- gas. The gas was assumed t o be steam, neglecting
longed operation with the same bed of solids, un- the effect of the small proportion of oil vapors
like applications involving continuous solids pro- on volumetric flow rate.
cessing, the cumulative attrition of particles due ( 3 ) However, when the change in contact time was
to impact in the high-velocity spout would become brought about by varying the gas flow rate with
excessive with most solids. a fixed bed depth of solids, the dependence of
Although the above two considerations would seem to ethylene and propylene yields on contact time was
dictate heavily against the use of a spouted bed as a found to be less distinct, although yield values
chemical reactor, recent work by Uemaki et alc50~s1) at the maximum contact time of 0.4 sec. were
demonstrates t h a t neither one is completely over-rid- noticeably lower than a t shorter times.
ing, and indeed conditions in a spouted bed may be Thus a difference in behavior with respect t o
more favorable than in other fluid-solid systems for contact time was observed, depending upon
carrying out reactions requiring short contact times. whether the variation in contact time was achieved

(a) Thermal cracking of petroleum


TABLE5
The reaction investigated by the Japanese workers
was the thermal cracking of petroleum - crude oil, MATERIALS
& CONDITIONS
USEDIN THERMAL
heavy oil, and naphtha - to produce ethylene and CRACKING
EXPERIMENTSW
propylene in spouted beds of coarse inert particles -.

(alumina, chromia-alumina and coke, in the size range Feedstock Density, Mg/m3 B. P. Range, "C
-
1 4 mm). High temperature cracking of hydrocar-
bons (at temps. > 600°C) is not a catalytic reaction, Naphtha 0.690 (ZOOC) 1 - 124
the role of the solid particles being to provide surface Heavy oil 0.873 (25°C) i - 360
Crude oil (Arabia) 0.850 (20°C) i - 303
for carbon deposition, and to serve as heat carriers for
the endothermic cracking reaction so that isothermal
conditions are maintained in the reaction zone, name-
ly the bed. Since yields of ethylene and propylene are
Solids
Aluminum oxide
I Density,
Mt?lm3
2.24
Particle
size, m m
0.99 - 2.79
Shape
factor*
0.42
favored by a short contact time, the rationale for using Chromia-alumina 2.90 1.65 - 3.96 0.45
a spouted bed of coarse particles in preference to a Cole 1.42 1.17 - 2.36 0.70
fluidized bed of fine particles was essentially t h e high-
er permissible gas flow rate in the former system. E e j weight -
1.0 2.5 kg
The experimental system used (see Figure 13) con- Reiction temp. 550 - 860°C
sisted of a 13 cm dia x 75 cm high reactor (cone angle
60", gas-inlet dia 16 m m ) , surrounded by a heating Flow rates
jacket for supplying supplementary heat to the bed Feedstock 0.7 - 3.0
kt?lhr
by burning water gas. The primary source of heat Steam 7 - 16
supply was superheated steam, which, in combination kglh7
with the oil-feed pumped into the approach pipe to the
reactor, served as the spouting medium. The gaseous Steam/fee Mock 4.5 - 12
kglkt?
products from the reactor, after passing through a
cyclone and a condenser, were collected in a gas hold- Nominal contact 0.18 - 0.36
er. The volume of the gas produced in each run was time Eec.
measured with a wet test meter and detailed analysis
of the gas samples was carried out chromatographical- *From equation of Shirai(5Z)for pressure drop in fixed beds.
ly. An estimate of the carbon deposited on the solids

142 The Canadian Journal of Chemical Engineering, Vol. 5 2 , April, I971


Figure 14 - Comparison of ethylene and m

-
propylene yields from thermal cracking 1
3 1.0 -
of naphtha for spouted bed'50', moving w 0.8 -
bed's3' and fluidized bed'54',as reported 1
I- 0.6 -
by Uemaki et al'Jo'. L 0.4 -
2
8

-
Figure 15 Estimated nominal contact
0.2 -
€02 €63 703 7% Boo 8% 900 950 times in fluidized and spouted beds'sa',
REACTION TEMPERATURE, 'C I I , ,
0.3 0 5 0.8 1.0 2 4 6 8 10
H/Dc

by varying the bed depth a t a constant flow rate, this case remains short even in relatively deep beds. A
or varying the flow rate at a constant bed depth. comparison between the estimated contact times for
The explanation lies in the arbitrary definition a spouted bed and a fluidized bed, presented in Figure
of nominal contact time in a spouted bed, which 15, illustrates the above point. Thus, under typical
would bear a different relationship to the real conditions, the contact time in a fluidized bed is seen
contact time in the two situations, depending to become progressively higher than in a spouted bed,
mainly on the distribution of gas between the a s the bed height to diameter ratio is increased above
spout and the annulus. Since t h e gas-flow rate unity. A further advantage of the spouted bed over
through the annulus of a given bed would remain the fluidized bed, mentioned by Uemaki e t al, is the
almost unchanged with increasing total gas flow somewhat greater flexibility which the former allows
rate, the real contact time in the annular part of in controlling the contact time, not only by changing
the bed would decrease only slightly a s the gas the bed depth but also by varying the diameter of gas
flow rate is increased. The contact time for the inlet.
spout gas would no doubt decrease considerably,
but since the gas passing through the spout con- ( b ) Solid catalvsis
stitutes only a fraction of the total gas, the effec- The subject of solid catalysis i n spouted beds is still
tive contact time in the bed as a whole, and there- an open field. I t is easy t o imagine the technical prac-
fore the yields of ethylene and propylene, would ticability of a dual spouted bed catalytic cracker and
show only a weak dependence on the nominal con- regenerator using a TCC-type pelletized catalyst'"',
tact time, as experimentally observed. analogous to fluid catalytic cracking and regeneration,
(4') A comparison of the ethylene and propylene yields a s well a s to the dual spouted bed thermal cracker and
for the spouted bed reactor with yields reported combustion chamber mentioned above. Whether such
by other workers for fluidized and moving bed a combination would be economically feasible is an-
reactors, obtained under their respective optimum other question, yet to be answered. The continuing
operating conditions, has been presented by Uema- wide use of fixed packed beds of granular or pelletized
ki et a1 (see Figure 14). The maximum ethylene catalysts and catalyst carriers as chemical process
yield is seen t o be clearly higher for the spouted reactors, in which catalyst regeneration o r re-activa-
bed, while the propylene yield is not significantly tion requires periodic shut-down of each unit, remains
different. Comparative data for cracking of crude an incentive for developing alternatives such as spout-
oil also showed t h e same trend. ed beds, in which the catalyst pellets or granules can be
Uemaki et a1 have estimated that the operating gas treated continuously.
velocities for the moving and fluidized bed systems of
Figure 14, which would be limited by hydrodynamic Nomenclature
considerations, could not have exceeded 0.3 m/sec and
1.3 m/sec respectively (0.8 U,f for moving and 5.0 d, = particle diameter
D, = column diameter
Unlffor fluidized beds), a s against 2.0 m/sec used by H = bed depth
them in the spouted bed reactor. With the bed depth U = upwards gas velocity - superficial
used in each case, which was presumably the optimum, Urn!= minimum fluidization velocity - superficial
the ratio of contact times, spouted : fluidized : moving U,, = minimum spouting velocity - superficial
bed works out to 0.65:1.0:4.3. The advantage of using 8 = included angle of cone
P, = particle density
a spouted bed is thus attributed to t h e short contact
time achieved under optimum hydrodynamic condi-
tions, the critical effect of contact time on the yield Acknowledgnaents
of ethylene in particular having already been demon- Continuing financial support from the National Research Council
of Canada is gratefully acknowledged.
strated under item (2).
I n further comparing the spouted bed with t h e fluid-
ized bed in this context, Uemaki e t al have pointed out References
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* * *

244 Tke Camdian Journal of Chemical Enginewing, VoE. 52, April, 1974

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