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1974 Developments in Spouted Bed Technology
1974 Developments in Spouted Bed Technology
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-
The Canadian Iournul of Chemical Engineering, Vol. 52, April, I974 129
TABLE
1
SUMMARY OF REPORTEDSPOUTED BED APPLICATIONS
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
4 AIR
-
granulation sys-
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.
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
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
(e) Sorption
Figure 5 - Schematic diagram of a pyrolytic carbon spouted
A continuous adsorption setup ("Ecosorber") for bed coateP).
om '
I
.- \\
/
I
s,
,
, I
'--I--!-'.
: I
I :
II ,,
3 4
NO. OF STAGES
-
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
!
-
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'.
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.
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
(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
-
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
that for a given solid material, the only means f o r ( 1 ) Matbur. K. B., Sroutcd Beds, Chapter 17 of "Fluidizatim" (eds.
J. F. Davidson and D. Harrison), p. 711-743, Academic Press,
controlling the contact time in a fluidized bed is by London (1971).
reducing the depth of bed, but this cannot be done ( 2 ) Mathur, K. B. and Gishlei, P. E.. J. App. Chcm. 5. 624 (1955).
(31 Peterson. W. S.. Can. f . Chem. En=. 40. 226 f19621.
beyond a certain limit since a sizeable depth is re- ( 4 ) Beckef, H. A. and Sa1lans.- H. R., Chem. .Eng. Sci. 13. 97 (1961).
quired for maintaining isothermal conditions. The gas ( 5 ) Berquin, Y. F.. Genie Chimique 86, 45 (19E1).
( 6 ) Berquin, Y. F., U.S. patent no. 3,231,413 tn Potasse e t Engrais
flow rate for spouting, on the other hand, increases Chimiqueq. Paris. 1966 ( B i i t . pate?t no. "62 6 5. 1-64).
( 7 ) Nichols, F. P., British patent no. 1,039,117 to ICI Ltd.. London,
with increasing bed depth so that t h e contact time in 1966.
244 Tke Camdian Journal of Chemical Enginewing, VoE. 52, April, 1974