CHEMICAL REACTION ENGINEERING AND RESEARCH AND

DEVELOPMENT OF GAS SOLID SYSTEMS

Department of Chemical Englneerlng

Unlverslty of Tokyo
Bunkyo-ku, Tokyo 113 Japan

ABSTRACT

A general procedure 1s proposed for znnovatlve research and development of gas-solld

reactor systems, with a brief explanation of the slgnlflcsnce of each step m the pro-
cedure.

Based upon the contactlng mode between gas and solid phases, as well as the ways of
supplymg the-l energy to the reacting regions, various types of gas-solld reactor
systems are classlfled by using tables of so called "matrix" form, for thermal cracklng
and gaslflcatzon of heavy 0x1s. gaslflcatzon of coal, gaslflcatlon of solld waste, cal-
clnatlon of limestone, cllnkerlng of cement and reduction of iron ore.

The importance of fundamental concepts 1s emphasized for successful research and develop-
ment by presentlng several examples, namely, calclnatlon of llmestone, thermal crackzng
of heavy 011s and gaslflcatlon of solld waste materials.

In connectlon with the dlrectlon In which fundamental research should be orlented, four
primary ways of thlnklng are proposed, which can be applied to obtain lnnovatlve Ideas
for further research and development In this field.

One example of the author's practical experience was selected to show the role of the
fundamental research In the course of large scale development. F-ally the author out-
lines the role of chemcal reactlon englneerlng to Innovate the novel gas-solid reactor
systems which may be Inevitable for simultaneous solutzon of the three big E's. namely,
Energy. Environment and Economy

KExwoHDs

Bench scale reactor, biomass, calclnatlon, cement, coal, contactlng mode, cllnkerlng,
development, gaslflcatlon, Iron ore, limestone, pllot plant, reduction, solld waste,
scale up factor, thermal cracking.

INTRODUCTION

Parallel to the development of lndustrles all over the world, people have become more
aware of Its serious drawbacks, namely envrronmental problems. So far, almost all types
of pollution abatement lnstallatlons have Just been added to the conventional processes,
sacrlflclng energy and economical benefit. The energy crlsls seems to have attenuated
the serious concern about environmental problems for the moment. It 1s well understood
that we should endeavor to acquire multzple resources for energy, for example, coal, 011
sand bitumen, blo-mass, and also solid waste materials. In addltlon, the petroleum that
we now have should be utlllzed as efflclently as possible. Nevertheless, It 1s lnevl-
table that we will encounter big environmental problems If we again Ignore the consequen-
ces of continuous pollution, which may be generated from these alternate sources of
energy.

As long as we stick to conventional technologies that have been employed, It may be

quite dlfflcult to achieve a simultaneous solution to the above problems, namely, a
1887
 D KUNII

clean environment and new energy sources m accordance wzth sufflczent economy. It 1s
urgent, therefore, to develop new technologies which can supply us with clean energy,
economically, wlthout ermttlng any pollutants In the course of energy conversion.

For the optimum utllizatlon of a given amount of energy, the most reallstlc approach
may be to raise the thermal efflclency appreciably zn any lndustrles which are consum-
mg huge amounts of hydrocarbon resources. Consequently, furnaces and kilns In various
lndustrles may be the first targets for improvement To meet the strict requirements
for the simultaneous solution to the three big E'S, Energy, Environment, and Economy,
drastic improvements are needed In these furnaces and kilns, sometimes through changes
In their basic prlnclples

In addrtlon to the overall shortage of petroleum In the world, demand for the lighter
fractions like gasoline, naphtha and kerosene 1s lncreaslng compared to the heavy frac-
tlon.5. This 1s partly because of environmental regulations and partly because of the
exporting status In the producrng countries. This trend ~111 spur the utlllzatlon of
heavy fractions as a raw material for so-called C,chemlcal Industries. New technologies
are needed for the processing of heavy 011s as well as for lnnovatlve chemical synthesis
In order to produce profltable products and clean energy. Technologies to be developed
In the above area can be simultaneously applied to the utzllzatlon of tar sand bitumen
or natural asphalt.

In order to compensate for the shortage of petroleum, utlllzatlon of coal 1s Increasing,

not only for combustion, but also for gaslflcatlon and llqulfacatlon. This 1s lnevltable,
but one must take into account the ash content which takes Its toll on the environment

Even now, huge amounts of combustible materials which are thrown away, or lnclnerated
are generatzng severe problems for the environment. Such a waste of energy resources
1s mainly attributed to the lnefflclent method of collection, even though a high per-
centage of such combustzbles as paper, wood, fiber, and plastics are In the waste
materials.

From the standpoint of chemical reaction englneermg, the energy conversion of biomass
seems very attractive because the amount of energy In agricultural and forestry wastes
1s known to be enormous_ Furthermore, energy plantations on a large scale will generate
favorable economical developments In troplcal areas In the future, compensating for the
decreasing productlon of fossll fuels. Energy plantations can give us a possible solu-
tlon to pollution free productlon of energy, provided that In advance we are careful In
maklng a long term assessment of Its Impact on environmental circumstances.

ProductIon of the above two energy sources, namely, solid waste and baomass, IS spread
over a vast area of the world. Contrary to the production of petroleum and coal, these
two energy sources should not follow the conventional productlon techniques In terms of
the larger the more efflclent. In contrast, one should make new technologies to convert
these materials efflclently to clean energy, which can be utlllzed locally at the site
of the material productlon For local operation, It should be easy, sample and safe to
operate,

These are only some examples of new areas to be lnvestlgated and developed In the near
future. st111, one may lmaglne that there are a number of problems whzch should be
challenged for simultaneous solution of the three big E's, Energy, Environment and
Economy.

PROPOSED PROCEDURE FOR RESEARCH AND DEVELOPMENT OF GAS SOLID

REACTOR SYSTEMS

Almost all of the problems previously mentioned involve gas-solld reactlon systems, In
which solids change their physlcal and chemical propertles drastlcally with the elapsing
of time. For the research and development of any creative processing system dealing
with the materials mentloned, extensive znvestlgatlons should be made In the fzeld of
chemical reactzon englneerlng. According to the author, the research and development
of any gas soled reactor system may be done In the following way

1) Fundamental research to study the physlcal and chemical

changes In the main reaction system.

2) Selectzon of a contacting mode between solids and gas as well

 Chenucal reactlon engmeermg and research and development 1889

as the method to supply thermal energy to the reactor.

Invention of a new contacting mode If necessary.

3) Conceptual design.

4) Experimental work with a bench scale reactor and feaszblllty

tests.

5) Investlgatlons of the flow patterns of both sollds and gases

In cold reactors for scale up and mock up tests.

6) Development of mathematical slmulatlon models as guide lines

for the scale up procedure.

7) Design of a pilot plant to conflrm If the above selectlon

was correct.

8) Process design and cost estlmatlon.

9) Construction and operation of the pilot plant and search for

any new problems which could become obstacles to further
development.

10) Analysis of data and modlflcatlon of the slmulatlon models If

necessary, More precise cost estlmatlon.

11) Design of commercial reactor on the basis of the slmulatlon

models.

Since considerable funding, as well as a great deal of man-power are needed for the
development of any lnnovatlve chemical processes, one should proceed to item 7) with
upmost care for the success of further development. In order to achieve this, the
Importance of Items 2) and 3) 1s emphasized here In addltlon to the fundamental research
work.

Items 1) and 2) are very closely llnked to each other. It sometimes happens that a con-
cept for development starts from items 2), 3), or even 4), In order to conflrm that It
can be realized In practice. After recelvlng favorable results from such a concept, one
may determlne the exact condltlons for the fundamental experlmental work.

In cases where no contacting mode satlsfles the requirements for the lnnovatlve proces-
sing, one can modify the conventional contacting modes to meet the requirements or even
invent a new contacting mode If possible.

The fundamental feature of any chemical process with a gas solrd system 1s almost always
deternuned by selecting both a contacting mode and the method of suppllng the thermal
energy to the reactor. Different cnmblnatzons of these two factors give completely dlf-
ferent chemical processes to each other provldlng several alternatlves

The Importance of Item 3). namely, the conceptual deszgn, should be emphasized here since
the success or failure of any research and development should almost always be determined
m this stage, not only economically but also technrcally.

By applzcatlon of all of the available %nformatlon, experience, and englneerlng know-how,

an approxzmate conceptual design should be made for the alternatlves using the same
thoroughness of calculation for each. Not only the estimated costs, but also the opera-
blllty of the processes should be compared In detail In this stage one could estimate
the degree of dlfflculty In the scale up of the chemical processes concerned. Taking
into conslderatlon all of these matters, one could select the optimum process as far as
the present knowledge 1s concerned. Since th1.s procedure seems somewhat cumbersome,
lrttle attention has been pald to It, resulting m the mIserable faxlure of development
after spending huge sums of money If It 1s xmpsslble to select only one of the alter-
natlves, two or three processes should be developed to the next stages, namely, to
items 4), 51, and 6).

There 1s no need to stress the Importance of the experimental work with a bench scale
reactor, the lnvestlgatlon of flow patterns, and the mathematical slmulatlon models,
 D KUNII

because they are the primary subJects of chemical reaction englneerlng. A number of
works have been reported In these categories so far, but mainly on the "known" reactor
systems. In order to contribute to the simultaneous solutron of the three big E's, how-
ever, many complex and unknown reactlon systems must be challenged from now on After
acqulrlng enough lnformatlon on alternative processes with respect to ltmes 4), 5), and
61, one can choose the technlcally best alternatlve from the other competitors.

When lncorporatlng experlmental data with englneerlng knowledge of flow patterns In the
reactor system, mathematical slmulatlon models, (so-called simulator), become the power-
ful tools or guide lines for successful scale up of the lnnovatlve chemical processes.
The pllot plant can be designed on the basis of the mathematical szmulatlon models,
predlctlng Its performance characterlstlcs.

Scale up factors from the bench scale to the pllot plant and from the pllot to the
commercial plant have always been under dlscusslon by R & D managers and engineers.
The author thinks that the scale up factors depend on the degree of understanding of the
complex phenomena taking place In the reactor system as a whole, not only qualltatlvely
but also quantltatlvely by the managers and engineers no matter how big the reactor
becomes. When everything can be predicted by the slmulatlon models, one can design the
commercial plant directly from the bench scale reactor.

The valldlty of the mathematzcal slmulatlon model can be tested by comparison of the
predlctlon of the design stage with the practical experzmental data taken from the pllot
plant. If the colncldence 1s good, one can utlllze the models for the design of the
commercial reactor with sufflclent confidence. In the case where one notices an appre-
clable difference between these two, one must seek out the Incorrect lnformatlon and
improve the slmulatlon models.

Another purpose of the pzlot reactor 1s to find out any other important phenomena In
the reactor system which were not detected In the bench scale but could become serious
problems In the commercial scale reactor. Therefore, as long as 1000 hours of opera-
tlon at steady state 1s usually needed. In order to ellmlnate the posslbllty of failure
at the commerczal stage, the experlmental work should be conducted most carefully at
this stage. After acqulr=ng all data avazlable m the pllot reactor, one 1s In the posl-
tlon for deslgnlng further, namely to the commercial scale reactor. According to the
author's opmlon, chemical reactlon englneerlng should deal with all of the items from
1) to 111, because the ultimate purpose of engkneerlng 1s to create and establish any
useful technologies for llvlng.

On the basis of the guldellnes elaborated above, chemical engineers can take an Important
role =n the design procedure of pilot and commercial reactors, with lntzmate cooperation
from sclentlsts and engineers In other fields, namely analytzcal chemists and material,
mechanical, electrlcal, lnstrumentatlon, computation, and construction engineers The
above actlvlty utzlzzes as much as possible the so-called process englneerlng, which has
been developed as the design procedure of commercial plants with conventional technolo-
goes

MAIN FACTORS TO DETERMINE THE SPECIFIC FEATUF33S OF A GAS SOLID

REACTOR SYSTEM

It goes without saying that the fzrst factor to determrne the speclflc features of a gas
solid reactor system 1s the reaction condltlons sultable for acqulrlng the desirable
products, namely, temperature, pressure, and contact tzmes for both gas and solld streams.
With the aid of the ncessary background from chemical reactzon englneerlng, this Infor-
matlon should be taken as precisely as possible.

The second factor 1s the contacting mode between the gas and solid phases. For the pro-
cesslng of the materlals previously mentloned, one can line up the available contacting
modes as schematzcally shown In Fig. 1. Lets choose here some examples of gas-solld
reactor systems, whzch seem Important In connection wzth the energy and envlronmental
problems. Table 1 gives an overall Idea, suggesting what types of contacting modes have
been utlllzed so far for hzghly endotherrmc gas solld reactor systems.
 Chemlcaf reactlon engmeermg and research and development 1891

a) FIxed bed b) Vertical c) Horizontal or d) Fluldlzed bed

moving bed lncllned movxng bed

e) Pneumatic f) Rotary g) Flat hearth h) Bubbles m

conveying cylinder molten bath

Fig 1 Contacting modes for gas solid reactor systems

Table 1 Contactlng modes utlllzed for endo-thermlc gas solld

reactor systems
A Commerczal~zed B Pllot plant scale

Contacting Gaslflca- Gaslflca- Gaslflca- Calclna- Cllnkerlng Reduction

mode tlon of tlon of tlon of tlon of of cement of iron
pitch coal solid llmestone ore
waste

a) Fixed bed A

b) Vertical
A A A A A
moving bed

c) Horizontal,
lncllned A
movlnq bed
d) Fluldlzed
bed A A A A B A

e) Pneumatic
B B A
conveying

f) Rotary B A A
cylinder

g) Flat
hearth A

h) Bubbles II-J
A B
molton bath
 D KUNII

Table 2 Classxflcatlon for thermal cracking and gaslflcatxon of heavy 011s

Hoechest
 Chemxal reactlon engmeermg and research and development 1893

Table 3 Classlfxcatxon for gaslflcatxon of coal

water qas

Gas

ash
1894 D KUNII

Table 3 Contznued

'neumatlc
:onveylng

Kellog

In order to specify the features of any of the reactors for endo-thermlc reactions
given In Table 1, one needs an addltlonal factor, namely the method used to supply the
necessary heat Into the reactlon zone, which may be classlfled as follows

(1) Indlrect heating 111 furnaces flrlng conventzonal fuels

(2) Utlllzatlon of exothermlc reactlons
2-l) Partial oxldatlon for gaslflcatlon of coal
2-2) Hydrogaslflcatlon for gaslflcatlon of coal
2-3) Applzcatlon of CO for direct reduction of iron ore
etc.
(3) Heat carriers
3-l) Gaseous heat carrier
3-2) Llquzd heat carrier
3-3) SolId heat carrier
(4) Electrrc heating

As long as we generate electric energy mainly by burning petroleum and coal, the large
scale appllcatlon of electric heating for the above chemical processing seems to be
uneconomical for the near future.

The comblnatlon of contacting mode with a method for heat supply gives a speclflc feature
of gas-solid reactor systems. The example shown In Table 2 1s for thermal cracking and
gaslflcatlon of heavy 011s or pitch. For processing of lighter oils, another contacting
mode 1s also used for the gas-llquld phase, namely the free flow. This 1s Included m
Table 2, where one can compare the advanced chemical processes for heavy 0x1s with the
conventional ones of lighter 011s
 Chemuzalreactlon engmeermg and research and development 1895

Table 4 Classlflcatlon for gaslflcatlon of solld waste and bxomass

'neumatxc
:onveylng

Garrett

Landguard

c t s 35/9-F
 D KIJNII

A number of coal gaslflcatlon processes have been commerclallzed and are under develop-
ment, some of which can be classlfled on the baszs of the above matrix shown In Table 3
It should be notlced that enormous efforts have been made for development of gaslflcatlon
processes using the fluldlzed bed prznclple.

Slmzlar classlflcatlons can be made for gaslflcatlon of solid wastes as given In Table 4,
where one can find apparent analogy with Tables 2 and 3. In spite of the big differences
among raw materials, one can unify almost all of the chemical reactor processes dealing
w~_th heavy 011s. coal and solld waste Biomass IS a far easier material to qasrfy,
compared to the preceding materials. Since biomass contains few pollutants and little
ash, qaslflcatlon plants for biomass are much safer to operate than those for solid waste.

Calclnatlon of limestone requires a great deal of energy. The necessary heat for this
process LS always supplled by direct heat transfer from flue gas at a high temperature,
and then this process corresponds to the gaseous heat carrier system. Because of this,
the main feature of any such process can be speclallzed by the contacting mode between
the lAmestone and the stream of flue gas Table 5 gives the schematic diagram of several
reactors for calclnatlon of limestone.

For reduction of fuel consumption 1n the calcznatlon of limestone, heat should be recov-
ered from both the flue gas and the calclned lime. Depending on the size of the lime-
stone, some of the contacting mode have been used for the heat recovery units In the
reactor system, namely vertical moving bed, horizontal or lncllned movzng bed, fluldlzed
bed and pneumatic conveying modes.

The cost of energy has risen by more than 50% for the manufacturing of cement. Because
of this, heat recovery from both the flue gas and the clinker IS very important to
create an efflclent cement cllnkerlng system. Table 6 qlves a schematlcal diagram of
some examples for such a system WIthIn the cllnkerlng process, the calclnatlon of
lzmestone In the raw materials needs the greatest amount of heat. IHI and Mltsublshl
H.I. companies have independently developed systems III which zntermedzate calclners are
Integrated into the cllnkerzng systems as shown In Table 6. By appllcatlon of such
calclnatlon reactors, they claim that the capacity of the rotary kiln for cllnkerlng has
almost doubled. The necessary heat for cement cllnkerlng 1s supplled by a direct heat
transfer from flue gas at a high temperature. This 1s slmzlar to the systems for cal-
clnatlon of llmestone where the method to supply heat corresponds to the gaseous heat
carrier system.

Blast furnaces for Iron and steel making are the biggest reactors In the gas solld
reactlon systems and consume vast amounts of energy using coking coal and heavy 011.
In order to use powdery iron ore, however, slnter furnaces are usually needed to obtain
hard lumps of Iron ore to be fed into the blast furnaces To meet the strlgent regula-
tlons for pollution control1 of SOx and NOx, for Instance, some steel mills have Instal-
led pollution abatement processes at nearly the same expense as the expected proflts of
the company. In addltlon, a shortage of coking coal 1s antlclpated In the future

In some areas of the developing world, rnlnl-mills are becomlng more economical and
attractive for local prosperity. To meet this world trend, a number of the research
and development efforts have been carried out to establzsh sound technologies for a
direct reduction process of powdery zron ore. Some of these have been conunerclallzed
because of their low construction cost and shorter construction time than the blast
furnace system. There are three methods to supply heat energy into the reacting zone,
namely, partial oxldatlon, gaseous heat carrier, with or without utzllzlng the exother-
mlc reactlon between CO and Fe203.
 Chemwxl reactlon ewneermng and research and development 1897

Table 5 Classzflcatlon for calclnatxon of lunestone

co-current cross flow

co-current
Vertical llmestone

heat recove limestone

fluldlzed
Pluldxzed
Dorr-Olive

llmestone
?neumatxc
zonveyxng

mestone
CalclmatlC

Rotary kiln preheater

1898 D KUNII

Table 6 Classzf~cat~on for clmkerlng of cement

Losche shaft kiln

ertlcal

composite pellets
(anthracxte and
raw materxals)

heat recovery
pneumatic and
lndlrect heat-

raw mate

I H I. NSP
Onoda FtSP

Smith NSP

Mltsublshl NSP
 Chemical reactlon engmeermg and research and development

Table 7 Classxfxcatlon for reduction of Iron ore

reductxo

last furnace

H Iron

ecycle gas

partial oxydatlon
 D KUNII

IMPORTANCE OF FUNDAMENTAL CONCEPTS IN RESEARCH AND DEVELOPMENT

It 1s most Important for leading engineers to decide what s&Jects should be lnvestlgated
on the basis of their prominent forslght Into future trends. For the successful develop-
ment of any lnnovatlve process system, however, conceptual design should be completed as
early as possible to meet the requzrements, selecting suitable contacting modes as
described previously. In other words, fundamental concepts for the research and develop-
ment are almost always determlned In stages 2) and 3) in the previous section. A couple
of examples of process development shall be given In th1.s sectlon, for which the funda-
mental concepts were extremely important In the course of their development.

Research and Development of Moving Bed Reactors for Calclnatlon of LImestone

Let us focus our attention on the reactors for calclnatlon of llmestone first As shown
ln Table 5, the moving bed 1s the sunplest contacting mode for lumps of limestone, but
At 1s dlfflcult to control the calclnatlon temperature to prevent overcalclnatlon because
combustion takes place In the void spaces wIthIn the moving bed. To solve this dlffl-
culty, Beckenbach designed his kiln In which the high temperature combustion gas partly
flows downwards, parallel to the descending dIrectIon of the limestone.

Supported by the Mlnlstry of International Trade and Industry (MITI), an offlcal con-
sortlum asked the author for his leadershlp to develop a handy reactor for calclnatlon
of Ilmestone, which would be sultable for domestlc use. He was involved at that time
In lnvestlgatlons on the flow pattern of a gas stream In the flxed bed. He explalned
the combustion of fuel gas wIthIn the void spaces by use of the consecutzve mlxlng
model as shown In Fig 2. It was found, theoretzcally, that the combustion zone could
hardly have reached the central portlon of the bed when the fuel gas was sent Into the
bed horizontally from the side wall, resulting in the Incomplete calclnatlon of the
portzon.

Since there was enough lnformatlon on the calclnatlon of a single lump of limestone,
development of the reactor started from item 2) In the procedure previously proposed
Dealing with the large lumps of limestone, the moving bed was chosen as the appropriate
contacting mode, whereas better contact was required between the burning gas and the
solids. The author and his collaborator found an idea to send a fraction of the air
necessary for combustion znto the bed of sollds at a higher level than the inlet of
fuel gas By doing so, It was predlcted theoretically that another combustion would
take place above the level of the air Inlet, and that the burning zone could reach
the central portlonof the bed as shown In Fig. 3. The detalled contacting mode between
solids and the burnrng gas stream was selected this way.

combust&le gas
air fue fuel
combustion gas gas gas
- =
region where
combustion
takes place

Frg. 2 A model of gas mlxlng m a Fig. 3 Prlnclple to control the combustion

bed of solld lumps of fuel gas wIthIn the void spaces
 Chcmlcal reactlon engmeermg and research and development 1901

Item 3) namely the conceptual design, was carried out by using the simple model shown
in Fig 3 For domestic use In rural dlstrlcts, It requires the use of heavy 011 Instead
of fuel gas. The conceptual design of the outside combustion chamber was made, In which
the fuel 0x1 was partially burnt with the starving air, producing lean fuel gas at a
high temperature.

In connection with Item 41, a two dlmenslonal model reactor, with a front wall made of
23 cm x 40 cm srllca glass as shown m Fig. 4, was used for visual observation of the
combustion phenomena. The contour of the burnzng zone was measured and compared with
those calculated on the basis of the above mlxlng model. The approximate colncldence
suggested the adequacy of this Idea.

In order to simulate the discharge portlon of the moving bed reactor, a mock up vessel
of medium size was construced, whereln lumps of sollds were discharged slowly, corres-
pondlng to the practical condltlon. Putting marked sollds in the moving bed, the flow
pattern of the solids was measured, glvlng reliable data for the design Sufflclent
lnformatlon had already been acquired on the flow pattern of gas In a flxed or moving
bed, so It was not necessary to perform any mock up test for It In thus stage of Item 5)

Cm the basis of the simple model mentloned above, a mathematical model was made as a
guIdelIne for the developmental work. NumerIcal computations were carried out under
drfferent operating condltlons, revealing the operablllty as well as a comparatively
high value of thermal efflclency. Th~_s step corresponds to Item 6)

In connection with item 7), a pilot combustion chamber, shown In Fzg. 5, was desIgned.
constructed and operated, conflrmlng that the partial combustion of heavy 0x1 was
carried out by the starving air In a steady state.
llca glass
h

I\
T
, fzxed bed of.
limestone

air

fue
gas
+
tlon fire
J

Fig. 4
with
7=+r1ck
Two dlmenslonal
fron wall
air
model
made
reactor
of slllca
air

Fig. 5
50-60%

PIlot
heavy
of
equivalence
stolchlometrlcal

combustion
011 20 - 40
chamber
lltre/hr
glass

c
Based on the guldellnes for design procedure, a pilot plant was deslgned and constructed.
Operablllty and thermal efflclency were almost the same as estimated, suggesting succes-
sful appllcatlon In industry At present, nearly ten commercial reactors of this type
have been constructed, contrlbutlng to the small companies In the Japanese lime Industry
(Kunll, 1970).

In ordinary calclnataon reactors with the vertical moving bed prlnclple, llmestone as
large as 3 - 8 cm should be fed to assure steady combustion of combustible gas wrthln
the void space and to prevent a large pressure droplnthe gas stream flowing through the
moving bed. One of the author's collaborators, Chlsakl, Intended to calclne the under-
sized llmestone whzch cannot be fed into an ordinary calcznatlon reactor Since the
amount of undersIzed 1s usually one order less than the lumps of llmestone sultable for
ordinary reactors, he planned to develop an effzclent calclnatlon reactor for small capa-
cltles A conceptual design for this type of reactor 1s shown In Fig. 7. Here. the
calclnatron reactor 1s composed of four portlons, namely the preheating zone for lime-
stone with a moving bed contacting mode, the combustion zone In the free board, the
calcznatlon zone where high temperature combustion gas 1s circulated by means of an air
Jet blown znto the central part of the reacor, and the cooling zone for calclned lime,
With sufflclent lnformatzon on calclnatlon of limestone, he began this work from
Item 31, namely the conceptual design, In the procedure previously outllned.
1902 D KUNII

It should be noted that the maln part of the calclner rotates slowly to attain efflclent
contact between the combustion aas and the small sized lImestone. By adequately combIn-
Ing the above four zones, he was able to keep the pressure drop throughout the reactor
wlthln the allowable range for a conventzonal blower despite the small size of the
llmestone
n llmestone limestone

combustion

valve

Fig 6 Pilot plant of a moving bed Fig. 7 Top-shaped calclnatlon reactor,

reactor for calclnatlon of lime- designed by Chlsakl
stone. Kunll Kiln 5-7 tons/day
(Kun~, 1970)

Since Chzsakl had enough englneerlng znfonnatlon and experience through h1.s work on the
development of the calclnatlon reactor, Kunll kiln, he was able to start from the stage
corresponding to Item 3). Following the strategy for development given by the author,
Chlsakz and his collaborators In the Kunneppu Lime Company carried out cold tests to
study the flow pattern of sollds In the preheating zone and to confirm the capacity of
the air get In the moving bed (This step corresponds to Item 5). A commercial calcl-
nation reactor was lmmedlately deslgned by appllcatlon of a simple computation model,
and then constructed at the plant site of the company. The operation of the first
commercial plant was begun successfully without using a hot pllot reactor. For the
moment, three commercial reactors are under operation, calclnlng small size llmestone
for small scale companies.

Production of Oleflns from Heavy 011 In a Fluldlzed Bed Reactor of Coke Particles

Antlclpatlng the lnevltable appllcatlon of heavy 011s for production of oleflns, Kunz.1
and Kunugl started fundamental lnvestlgatlons =n thermal cracking of heavy 011s In
fluldlzed bed reactors as early as In 1964. They made conceptual designs for a number
of alternative Ideas, and selected a clrculatlon system of coke particles between a
fluldlzed bed reactor and a fluldlzed bed regenerator, the basic Idea of which 1s given
In Fig. 8. In other words, the research and development was lnltlated from the stages
corresponding to Items 2) and 3). The reasons why coke particles were chosen are as
follows
a) applicable for very heavy 011s like vacuum residue
b) less erroslon
c) no need to supply heat carrier under stable operation

Kunugl and his collaborators cracked a variety of heavy 0~1s In a mlnlature reactor of
3 cm I D. under a wzde range of experrments, obtaznlng sufflclent data for further
development_ Their actlvlty corresponds to Item 1).

Formation of carbon around the nozzle to feed the heavy 0~1 znto the hot fluldlzed bed
was antlclpated to become a serious drawback to development. In order to overcome this
problem, Kunll and his collaborators used a single fluldlzed bed reactor of 7 cm I.D ,
which was deslgned to study the carbon formatlon around the feed nozzle as well as the
rate of carbon deposit on the fluldlzed carbon particles. This stage In their work also
corresponds to ltem 1). Based upon the lnformatzon galned from the above experiments.
Kunll deslgned an appropriate nozzle suitable to spray heavy 0x1 Into a fluldlzed bed
horzzontally. Details of the nozzle tip are shown m Fig, 9.
 Chemical reactlon engmeermg and research and development 1903

cracked qas

feed 0x1

Prac-
tlon of cracked

Fig. 8 Clrculatxon system for crack- Fig. 9 Details of nozzle txp used in the
lng heavy or1 in fluzdxzed hot reactor system in bench scale
bed reactor (I0.u-1~~. 1975) (Kun~, 1974)
A Steam B The-couple
c Nozzle tip

When aroplets of heavy 0x1 were InIected Into the fluxdlzed bed of hot coke partzcles,
it was predlcted that some amount of coarse agglomerates or even lumps would be formed.
In th1.s case, ordinary clrculatlon systems so far developed could no longer be applzed,
because such agglomerates or lumps would clog the pneumatxc conveyxng lift lmes. The
above clrculatxon system was deslgned to overcome this dlfflculty antlclpated at the
first stage of research actlvlty. A transparent cold model was made to conform the
steady clrculatlon of coke partxcles between two fluldzzed beds, (8 cm and 10 cm I.D.
respectively).

I I

Fig. 10 SchematIc dlagram of the bench scale reactor system (Kunzx, 1974)
A crackzng reactor H heater P PumP
B regenerator I 011 nozzle Q to vent
C combustxon chamber J scrubb3_ng cooler R- measurmg cylinder
D dust seperator K cooler for 0x1
E cooler condenser L flow meter S strainer
F mist seperator M compressor T axr blower
G gas holder N vessel for water U nitrogen cylxnder
feedlng
 D KUNII

A bench scale reactor system was constructed XL which hot coke particles were circulated
between a fluldlzed bed cracking reactor and a regenerator, the dlmenslons of which were
almost the same as the cold model Flqure 10 qlves a schematic dlaqram of the bench
scale reactor system, correspondlnq to item 4) In the procedure Khafgl and Quwalt
crude o~_ls were cracked smoothly in this system, suqqestlnq the feaslblllty of this
process Details of this experlmental work can be found elsewhere, (Kunll, 1974)

The Agency of Industrial Science and Technology In the MInIstry of InternatIonal Trade
and Industry of the Japanese Government, deslqnated the above process as a natlonal pro-
Ject and contracted five leadlng companies In Japan for large scale development early In
1967 (Chlyoda Chemical Enqlneerlng and Construction Co., Toyo Soda Manufacturlnq Co.,
Maruzen Petrochermcal Co., Mltsul Petrochemical Co , and Mltsublshl Petrochemical Co )
A mock up plant was lnltlally constructed to obtain sufflclent data for a smooth and
stable clrculatlon system as in Item 5). Several mathematical models were developed
to simulate the operation characterlstlcs of the process system, and to design the first
pilot plant with a capacity of five tons of heavy 011 per day Th1.s stage corresponds
to Item 6)

The shapes and dlmenslons of both the cracklnq reactor and the regenerator, as well as
the feed 011 nozzle were detennlned on the basis of the results of the precedlnq funda-
mental Investlqatlons. The maxlmum inner diameters of both the crackrnq reactor and the
regenerator were about 60 cm and 104 cm respectively, whereas the total helqht of the
slender fluldlzed beds were about 700 cm. This stage corresponds to Item 7). Parallel
to the construction of the first pilot plant, process deslqn was made to estimate the
cost of ethylene, as In Item 8)

The first run of operation of the pllot plant was started In October, 1969 to test the
operablllty of this clrculatlon system Three different oils, namely Arabian light
crude, KhafJl crude, and vacuum residue from Khaf-Jl crude, (asphalt) were cracked
smoothly to produce a conslderable amount of oleflns as predlcted from the fundamental
data The test operations proved that this cracklnq process functloned satlsfactorlly,
assuring smooth and stable operation for different kinds of 011s with residual carbon
Indexes ranqlnq from four to twenty-five percent, without appreciably chanqlnq the
operating condltlons The first cooperative works for development of this process ended
In 1972, (Kunll., 1975).

Enqlneers of two companies, namely Mltsublshl Petrochermcal and Chlyoda have made further
improvements In the pllot plant, and operated It satlsfactorlly to produce oleflns from
vacuum residue of crude 011 since the end of 1973 Total operation time attalned was
nearly one year, lncludlng the precedlnq cooperative works About 800 hours of operation
were run continuously wlthout InterruptIon, and shut down proceeded as scheduled,

In 1975, the Agency of Industrial Science and Technology, MITI, decided to further
develop the above process and contracted a consortium, which was orqanlzed of SLX lead-
Ing Japanese companies, Chlyoda Chemical Enqlneerlng and Construction Co., Mltusblshl
Petrochemical Co , Sumltomo Chemical Co., Showa Electra-chemical Co., Idemltsu Petro-
chemical Co. and Toyo Soda Co. Prior to the second cooperative development, a mock up
plant was construced to confirm the operablllty and flexlblllty of the above clrculatlon
system, the size of which was about the same as the second pllot plant to be deslgned.
Followlnq basIcally the same procedure as was used for the first one, the second pllot
plant of the reactor system was dealqned to crack 120 tons of such heavy 011s as atmos-
pherlc and vacuum residues per day The construction of the plant was completed at the
end of 1979. Test operation 1s scheduled to start In 1980.

Gaslflcatlon of Solid Waste Materials In a Fluldlzed Bed Reactor of Sand

Several types of qaslflcatlon processes of solId waste materials have been developed so
far for a simultaneous solution to envlronmental and energy problems Some of them,
however, leave a great deal of char which should be burnt further, other use oxygen
which 1s expensive, and at111 others need a considerable amount of such valuable mater-
lals as coke and llmestone, throwlnq out much slug from which metals are dlfflcult to
seperate. Ideal gaslflcatlon processes of solid waste, on the other hand should fulfill
the following requirements

a) production of clean gas with moderate or hlqh calorlflc value

b) complete combustion of char wlthln It
c) easy separation of metals from the burnt ash
 Chemical reactlon engmeermg and research and development 190.5

d) exclusion of oxygen, coke or limestone

e) exclusion of any addltlonal lnstallatlons for abatement of air or water
pollution

The author and his collaborators foresawthat the above severe requirements could be
technically satzsfled by appllcatlon of a clrculatzon system slmllar to the Kunll-
Kunugl Process, using sand particles as the solId heat carrier Instead of coke Based
on the development strategy given by the author, Hasegawa, Fukuda and their collabora-
tors In the Tsuklshlma Chemical Machinery Company made a conceptual design of a new
gaslflcatlon process, called the Pyrox Process early In 1973, The above declslon cor-
responds to items 2) and 3) In the procedure previously proposed

As for item 4), munlclpal solId waste taken from a practical lnclneratlon plant was
dried and dlslntegrated to a size of under 1.2 mm. The waste was then fed continuously
Into a single fluldlzed bed reactor of 50 mm I.D., In which lnnert solId particles of
sizes between 60 and 150 mesh were fluldlzed by the super-heated steam. The feed rate
of dry raw materials was about one kllogram per hour. Gaslflcatlon In this bench scale
reactor was carried out very smoothly, glvlng good data on the product gas

Parallel to these experimental works, a cold model was made of transparent plastlces to
improve the clrculatlon system for appllcatlon of a different heat carrier, sand partl-
cles. This step IS ltem 5). Based upon the znformatzon obtained above, a simple
design procedure was made as a guIdelIne for further development, corresponding to
item 6).

A small pilot plant with a capacity of ten kilograms of solld waste per hour was deslgned,
constructed, and operated smoothly glvlng sufflclent data for further development Dry
solid waste was taken from a practical lnclneratlon plant, and dlslntegrated to a size
ranging from 1 mm to 6 mm, which was sent Into the gaslflcatzon reactor of 10 cm I.D. as
shown In Fig. 11

Fig 11 Flow sheet of small pilot plant, 10 kg of dry solid was per hour (Kunzx, 1977)
1.2 evaporator 5 regenerator 11, after burner
3. feed hopper 6,7, cyclone collector 12. air compressor
4. gaslflcatlon 8. air heater 13 cooler
reactor 9.10 scrubber 14 LPG

In the plant, the necessary heat for gaslflcatlon was supplled by combustion of char In
the regenerator, resulting In the clean lnorganlc materzals being discharged from the
process. The operation was very smooth, glvlng a number of data, such as the favorable
data shown below

Temperature of reactor 7oooc

Dry gas. lncludlng Cop 0.50 m3 (N-T-P )/l kg of dry solId waste
Net calorlflc value of dry gas 3500-4300 kcal/m3 (N-T P.)
 D KUNII

By removxng CO:! from the product gas, clean fuel gas wxth a hxgh net calorxfxc value of
between 5700-6900 kcal/m'(N.T P ) could be obtaxned. [Note that the net calorlfxc value
of methane gas 1s 8567 kcal/m3(N T.P 11 It was found that the hydrogen chloride from
vinyl chloride resin was converted to NHsCl by reacting with NH3 formed from the other
part of the solid waste In the gasxflcatxon reactor. Because of thus, there 1s no need
In this process to add the de-chlorlnatlon xnstallatxons, which are xnevltable for
conventional lnclneratxon plants to meet the strlngentregulatxons for emlsslon of chlo-
rune The above actlvltxes correspond to stems 7) and 9) In the small scale pllot plant.

Process deslqn and cost estxmatlon, namely Item 8), followed on the basis of these
results,reveallng the feaslblllty of this process for future requirements of pollutxon
free conversion of soled wastxto clean energy with high avallablllty. A mock-up plant
was constructed and operated under normal temperature to acquire the most desxrable
conflguratzon of the down comer lines for sand particles. The plant was 10.5 m An height
and was composed of a model reactor and a regenerator, with maxlmum Inner dxuneters of
45 cm and 60 cm respectxvely

MIT1 granted flnanclal support for this process In 1975 as one of the Important tech-
nologles for speedy development In accordance with the design procedure previously
developed, a demonstratxon plant was deslgned and construced In 1976. The gaslflcatlon
reactor and the regeneratore are almost the same sxze, 2 m .x.nmaximum inner diameter and
13 m In height. The capacity of the plant 1s 40 tons per day for munlclpal solid waste,
and 24 tons per day for paper and pulp sludge with nearly 80 per cent water. Compared
to the small pllot plant, the scale up factor 1s 400 times. After startxng up In the
middle of 1976, the demonstration plant operated smoothly, gasxfylng paper and pulp
sludge, munlclpal solld waste, waste plastics collected from factories of plastic com-
modztles, and blocks of spent tire. Total operation time was about 6000 hours, between
April 1976 and May 1978, lncludxng two continuous long runs of 1200 hours wxthout
lnteruptlon (Kunll, 1977, Haseqawa, 1980).

Throughout the continuous operation, the plant demonstrated sufflclent operablllty and
flexxblllty for the qaslflcatlon of the variety of materials mentxoned above. The
favorable performance characterlstlcs of the process mzght be attributed to both the
violent solid mlxlnq In the fluldlzed bed as well as to the smooth clrculatxon of sollds
between the reactor and the regenerator The gross calorlflc value of the dry gas pro-
duced by the gaslflcatlon reactor was measured as follows-

Pulp sudqe with 78% water (wet basis) 4820 kcal/m3 (N.T.P.)
Munlclpal waste with 45% water (wet basis) 40cj0kcal/m3 (N-T P 1
Industrial waste plastics 10,100 kcal/m3 (N T P.)
50/50 mzxture of pulp sludge and zndustrxal plastic waste 8,800kcal/m3(N T.P.)

It was found that the above process was very sultable for gasxflcatlon of soled waste
contalnlng much plastxc to produce clean fuel gas with a high calorlflcvalue,as hlqh as
methane gas. The emlssxon of pollutants from the regenerator was very small for every
run, as low as S0,20-40ppm and NO,30-50ppm.

In Funabashl City near Tokyo, three commercial plants wxth thus process, each of which
has a capacity of 150 tons of munlclpal solid waste per day, are under construction at
the moment, for pollution free treatment of garbage as well as the recovery of clean
fuel gas with a high calorxflc value It 1s believed that the above process can contrx-
bute much to the simultaneous solution of envlronmental and energy problems m the future,

HOW TO FIND THE DIRECTION IN WHICH FUNDAMENTAL RESEARCH SHOULD BE ORIENTED

No one doubts the importance of fundamental research actlvltles for the successful devel-
opment of any chermcal process dealxnq with gas-solid reactxons It does not mean, how-
ever, that only the combxnatlon or accumulation of the sclentlflc and fundamental znvest-
xgatxons can result In the successful development In such an urgent fxeld as energy
conversion. Instead, the so-called engxneerlnq way of thxnkxng xs sometxmes lnevxtable
xn order to fxnd xnnovatxve Ideas whxch have never been reported. Let us discuss how to
find them using examples of gas-solxd reactxon systems m the fxeld of energy conversion.
As a primary way of thlnklnq, the author proposes the following

a) Appllcatxon of a contacting mode to other purposes

b) Optimum comblnatxon of knowncontactxnq modes and slmplxfxcatlon
 Chemical reactlon engmeermg and research and development 1907

cl Creation of new contacting modes

d) Multi-functional prlnclple

Research and development of the Pyrox Process for gaslflcatlon of garbage 1s an example
of Item a) because it was conceived after successful operation of the first KK Process
pilot plant. Extending this procedure, the author has proposed a novel reactor system,
which can simultaneously produce tar, rich gas, and raw synthesis gas for methane or
menthanol from char, a schematlc diagram 1s given In Flq 12.

It 1s well known that cement was first cllnkered In long rotary kilns up until two
decades ago The heat exchange sectlon of the rotary kiln was replaced by the suspen-
slon preheater, and then the flash or fluldlzed calclnators were Integrated, resulting
In the shorter kiln and increased production In other words, the present feature of
cement cllnkerlng 1s the result of an optimum comblnatlon of known contactlng modes,
which 1s consldered to be the second step of development. The third step may be the
slmpllflcatlon of the system, keeping the optimal way of synthesis. Figure 13 shows a
pIlot plant for a slmpllfled cllnkerlnq _ system,
_ which was operated successfully by
Sanarl-and his collaborators, (Heta, 1968)
tar
rich gas Hz, CO

fl. bed
ler

burne;
combustion
hamber for
tartlnq up

steam L-i- steam

-9 12 Conceptual diagram of the Fw 13 A small pllot plant for fluldlzed
optimum utlllzatlon process of cllnkerlng of cement
coal, independent of Its
characterlstlcs

To calclnate limestone gravel with a size of l-3.5 cm In a fluldlzed bed, a new type of
contactlnq mode was conceived by the author and was successfully deslqned by his colla-
borators, which was the comblnatlon of three zones, namely the preheatlnq, calclnatlnq
and cooling zones Compared to ordinary calclnatlon reactors with moving beds, the
capacity per unit volume of the reactor was almost lo-15 times greater. It must be
notlced that a small fluldlzed bed of 35 cm I D and 60 cm In height was able to calcln-
ate 20 tons of llmestone per day

Based upon the englneerlng experiences from the above lnvestlgatlons, the author deslgned
a novel process for direct reduction of iron ore In a fluldlzed bed at such hlqh tempera-
tures as 1000°C A small pllot plant was constructed and operated smoothly by the
author's collaborators, (Ohno, 1974) Green pellets made of powdery iron ore and pul-
verlzed coal were fed into the reactors contlnously, and they were reduced to give as
high of a conversIon as 94% metallc iron in the product. The above research 1s another
example of item a), namely the appllcatlon of a contacting mode to other pruposes as
well as ltme c), to create new contacting mode.

As explalned In the preceding sectlon, the clrculatlon system of sand between two fluid-
lzed beds 1s very efflclent for pollution free qaslflcatlon of garbage as well as biomass.
For local and small scale gaslflcatlon of biomass, however, the above system can be
slmpllfled as shown In Fig 16, keeping the overall functions of the previous process.
Instead of the orlglnal two fluldlzed beds, a single vessel can be seperated Into four
sections by means of two partlons plates, through which thermal energy can be transfered
from the hlqh temperature reqlon to the cold region. This method of thlnklng corresponds
1908 D KUNII

to item b) as well as to Item c) Parallel to the fundamental lnvestlgatlon on the gas-

lflcatlon of biomass, physlcal experlmentatlon IS also going on for the development of
the above clrculatlon system In the author's laboratory.

pellet
gas
0.5-lcm
solld
4 h I&

.zed

rn0Vll-l .g
from-
bed
partial\
combustor

+ L sample
V 'air metal Fe
94%

Fxz 14 A pllot plant of fluldlzed bed Fig. 15 A small pilot plant for direct
reactor, 0.4 m I.D. 20 tons/day reduction of Iron ore In a
For clznkerlng of cement, fluldlzed bed.
pellet 8 mm
For calclnatlon of coarse lime-
stone, 1-3.5 cm

In order to explain item d), namely the multi-functzonal prlnclple proposed by the
author, let us take the direct reduction system of Iron ore as an example All systems
commerclallzed so far are mainly composed of three processes, I.e. pelletzzatlon, gasl-
flcatlon of raw hydrocarbons, and redcutzon processes. Because of such comblnatlons,
thermal efflclency for any conventional direct reduction system xs always lower than

I gas

composite

.H20
coke - CO2
mass or
Id waste
02
steam

gas H2.CO

V
selective discharge

Fig. 16 Single vessel gaslfLcatlon Fzg. 17 Szngle vessel reactor propased for
process of biomass simultaneous slnterlng, reduction
and gaslfzcatlon of composite pel-
lets made of powdery zron and heavy
011.
 Chemical reactlon engmeenng and research and development 1909

that of the blast furnace system. To overcome the high thermal efflclency In the blast
furnace system and to ellmlnate the pollutants emrtted from various parts of the system,
the author conceived of a novel process using the multi-functIona prlnclple, which
means a way of thlnklng of how to realize every Important phenomena simultaneously.

Suppose that a composite material made of 80% wt. powdery Iron ore and 20% wt. heavy 011
with a low sulphur content, 1s fed Into a fluldlzed bed of fine carbon particles with a
high temperature as shown In Fig 17. The physical feature of the composite material
looks somewhat like tooth paste, only black, not white, and can be fed Into the bed as
a form of soft pellets or granules, 3-10 mm In size As soon as the soft pellets enter
the fluldlzed bed, they are lmmedlately slntered and partially reduced wlthln a few
nunutes Heavy 0x1 1s simultaneously gaslfled by the oxygen from the Iron ore. The
hydrogen and carbon mon-oxide gases are generated and are recycled to the bottom of the
reactor for the final reduction of slntered pellets after removing the water vapor and
carbon dloxlde gas as shown In Fig. 17.

Wlthln a violent fluldlzed bed of fine carbon particles, the partially reduced and sin-
tered pellets come statlstlcally downwards even though all the pellets are moving up and
down locally. The slntered pellets can be reduced almost completely by the reducing gas
which 1s sent into the bottom portlon of the fluldlzed bed.

The fine carbon particles are useful to supply the necessary heat for such endothermic
reactions as reduction and gaslflcatlon. The single fluldlzed bed 1s seperated Into
two regions by lnsertlng an appropriate devices such as the partltlon plate shown In
Fig 17. This plate IS inserted between the regions where the fine carbon particles
are continuously circulated. The mixture of the residual 011 and very fine carbon par-
tlcles, seperated from the produced gas, 1s InJected Into the lower part of the heating
region In order to make up the necessary carbon to be gaslfled In the upper part of
the heating region, fine carbon particles are gaslfled by oxygen and steam in the state
of a violent fluldlzed bed. The fine carbon particles circulate from the heating region
to the reduction region, conveying the maxor part of the necessary heat energy In the
latter region In addltlon, the residence characterlstlcs of the slnterlng pellets
seem different from that In any ordinary fluldlzed bed reactor with continuous solid
feed, and seems to be capable of the higher conversion of pellets at the bottom of the
reactor.

To assess the feaslblllty of the above process, several lnvestlgatlons are needed, not
only on the fundamental features of the reactlon, but also on the movement of sollds

a) Fundamental lnvestlgatron of the simultaneous slnterlng, reduction, and

gaslflcatlon of single pellets, experlmental and theoretlcal
b) Simultaneous reactlons of coarse pellets In the back mix fluldlzed bed at
high temperatures.
c) Residence characterlstrcs and segregation of coarse solids In a fluldlzed
bed of fine particles.
d) Selective discharge of coarse sollds from the fluldlzed bed composed of
coarse solids and fine particles.
e) Conflrmatlon of the process concept using a bench scale slmulatlon reactor
In which the pellets are thoroughly reduced
f) Optimum conflguratlon of the reactor for the clrculatlon of fine particles
and for the desirable residence and segregation characterlstlcs of pellets

Some of these subJects have been lnvestlgated and others are under lnvestlgatlon at the
moment In the author's laboratory, with favorable prospects so far, (Hasegawa, 1979).
Through this kind of actlvlty, the author belleves that fundamental subJects can be
found by maklng such a rough conceptual design as shown In Fig 17, conceived by the
multi-functIona prlnclple

These primary ways of thInkIng are rather on a lower level of the hierarchy to conceive
of any rnnovatlon or creation. The highest level 1s deflnltaly the direct lntultlon
lssulng from the instantaneous reorganlzatlon of all the necessary knowledge and Infor-
matron stored In the Inventor's brain. It 1s well known that the so-called braln
storming, horizontal, or reversal ways of thlnklng can help to motivate the lgnltlon of
lntultlon Nevertheless, the utlllty of the above primary ways of thInkIng cannot be
neglected, because one can still apply these ways for lnnovatlon to conform to the
requirements for solutions to the three big E's_ Through accumulating experiences of
successful lnnovatlons by appllcatlon of these primary ways of thlnklnq, one can fermen-
tate his capabIlIty for Intultlon, which 1s most Important for any lnnovatlon at higher
levels
1910 D KUNII

THE IMPORTANCE OF FUNDAMENTAL RESEARCK ON THE COURSE OF LARGE SCALE

DEVELOPMENT

In some cases where a novel but complex reactor system 1s developed on a large scale,
It sometimes happens that research engineers encounter queer phenomena which they were
unable to predict at the stage of fundamental research_ They should recognize their
rncomplete knowledge on the exact phenomena concerning the reactor system. Engineers
should guess the most Important sublect which might control the total characterlstlcs
of the system, and then start the fundamental research as quickly as possible In order
to clarify the unknown phenomena. It goes wlthout saying that a chemical reaction
englneerlng background 1s essential here for this flndlng and planning. Only one
example may be enough to explain the importance of fundamental research during the
development work on a larger scale.

In the early stage of development of the KK Process previously mentioned, the author
used a bubbling bed model to design the first stage pllot plant on the basis of a
well known assumption, r-e., the uniform temperature throughout a fluldlzed bed When
the pilot plant was operated at a steady state for a long period, It was found that an
excessive amount of fine coke was elutrlated from the fluldlzed bed m the regenerator,
far more than predlcted by theories at the earlier stage. This problem could have
proved fatal to this proIect because It was generally thought that an addltlonal amount
of coke particles should be supplied to the reactor system even In commercial scale.

The author lmmedlately conceived that this conventional assumption might be wrong and
guessed that the high temperature stablllty would have occured on single coke particles
dispersed In the rlslng bubbles In the bed. A two dlmenslonal fluldlzed bed reactor
was made In great haste which had a 24 cm X 35 cm wide transparent front wlndow for
visual observation. Single bubbles of the air were InJected consecutively Into the
lnclplently fluldlzed bed of carbon particles kept at 600-800°C A movie picture
showed that a number of carbon particles were dispersed In the rlslng bubble and lgnlted
suddenly, showing a typlcal feature of high temperature stablllty. The excessive elu-
trlatlon of fine coke particles was attributed to the rapId combustion of coke particles
at a far higher temperature than the fluldlzed bed Itself, and to the breakage of the
porous coke to fines On the basis of these new fIndIngs, the combustion system of the
regenerator was improved somewhat to prevent the unfavorable high temperature stablllty.
After the above Improvement, the elutrlatlon of fines was reduced drastlcally, enabling
smooth operation wlthout suppllng more coke, even for such light 0x1s as ArabIan light
crude

The flndlngs of this phenomena lnltlated the fundamental research work In this field,
(Aoyagl, 1974, Yoshlda, 1974). Experimental and theoretlcal lnvestlgatlons have been
made In accordance with the orthodox ways of chemical reaction englneerlng, Furthermore,
It was suggested that the high temperature stablllty seems likely to take place -just
above the ordinary dlstrlbutor where solids cannot move so violently. This phenomenon
1s sometimes fatal for such highly exothermlc reactlons In fluldlzed beds as partial
oxldatlon of carbonaceous sollds, because of the slnterlng trouble.

CONCLUSIVE REMARKS

In this plenary lecture, the importance of chemical reactron englneerlng has been empha-
sized in the field of gas-solid reactor systems, which are important for th& simultaneous
solution of Environment, Energy and Economy problems For the ordinary catalytic
reactor systems, It 1s quite essential to find more efflclent catalysts or chemical
reactions, gustlfylng the necessity of the extensive lnvestlgat>ons with a purely chem-
lcal aspect It 1s clear that the fundamental Investlgatlons are slmllarly unportant
also In the gas-solId reactor systems. Nonetheless, one should not Ignore the close
llnkage between fundamental research and the englneerlng way of thlnklng, namely, the
contacting mode, the way to supply the-l energy, the conceptual design, and the mathe-
matlcal slmulatlon models. Chemical reactlon englneerlng can take an important
role, therefore, In fIndIng out the fundamental subxects which should be persued m the
field of gas-solid reactor systems from now on. In other words, chemical reactlon engl-
neerlng can contrlbute to useful lnnovatlons In the gas-solld reactor systems, where
sollds change their chemical propertles, more than those In catalytic reactor systems.

Through the overall research and development of any lnnovatlve process system, the
mayor portlon of man-power and budget 1s spent during the scale up period, namely from
the pllot plant to the commercial size plant. In the large scale development, no failure
 Chemical reactlon engmeenng and research and development 1911

1s permitted. If engineers are bold enough to skip the fundamental research necessary
to understand every Important phenomena which are taking place m their system, they
are always In a posltlon to suffer the mlserable consequence of failure at the last
stage of development. It 1s strongly urged here to plan the schedule for such Innova-
tlve development as early as possible, In order to have enough time for such fundamental
Investlqatlons, which may be found m the course of large scale development.

Research and development of any lnnovatlve processes, espeolally durlnq the last half
of the period, 1s a spell of restlessness, tears and struggle for development engineers
because they are always challenged by new problems which have never been experienced
before. Only when engineers are confident enough to be able to predict what ~~11
happen In their novel reactor on a large scale, are they In a posltlon to successfully
gump to the hundreds or even thousands scale up factor.

Successful development strongly depends upon the degree of understandlnq of the complex
phenomena which may take place In the large scale reactor, Justlfylng the substantial
role of chemical reaction englneerlng, ranging from the fundamental to the scale up
strategy.

ACKNOWLEDGEMENT

The author would like to express his appreclatlon to the Mznlstry of International Trade
and Industry, Japan, for qrantlng the fmanclal support to develop several processes In
which he has engaged. In addltlon, the co-authors of papers referred to In this paper
and other researchers, engineers and technlclans who have partlclpated m the research
and development work mentloned In this paper deserve thanks for contrlbutlng In many
ways to the author's englneerlng experience.

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