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www.elsevier.com/locate/powtec

from the kinetic point of view

Huachung Tsui a, Chung-Hsing Wu b,c,*

a

Research and Development Department, Cotech Engineering Corporation, Fl.1, No. 13, Wu Chuan 1st Road, Wuku Industrial Park,

Hsin Chung, Taipei Hsien, Taiwan, ROC

b

Department and Graduate Institute of Bio-Industrial Mechatronics Engineering, National Taiwan University, Taipei, Taiwan, ROC

c

College of Science and Engineering, National United University, Miaoli, Taiwan, ROC

Received in revised form 10 October 2001; accepted 19 February 2003

Abstract

Circulating fluidized bed gasifiers used in integrated gasification and combined cycle (IGCC) possess unique design and operational

features: high gas velocity, high solid loading, and a large amount of circulating chars. As a consequence, their performance is noticeably

different from the conventional fluidized bed gasifier operating at lower gas velocity. At the same time, limited information has been

published to show how to operate the circulating fluidized bed from the kinetic point of view.

In order to study these aspects, kinetic models are developed using kinetic data from previous literature and two concepts of operating the

circulating fluidized bed gasifier from the kinetic point of view are presented in this paper. The results of the kinetic analysis using Johnson’s

kinetic data of a constant specific gasification rate of char (0.001 1/s) show that all species approach their equilibrium values after travelling a

distance of 2.5 m, which is set as the height of the gasifier. The resident time of the char in the bed is 0.86 s and the required circulation rate of

char and lime are 11.8 and 4.5 kg/s, respectively. In addition to Johnson’s kinetic data, Wen’s kinetic model is also applied in the kinetic

analysis. It shows a way to operate the gasifier in the fast fluidization regime with a superficial velocity between 3.6 and 4.9 m/s and a solid

loading between 50 and 100 kg/m3, these operating conditions are recommended by industrial experience. It points out the necessity to

predict the performance of the gasifier from the kinetic point of view in order to design the optimal geometry and operating methods that will

allow the gasifier to play a successful role in the clean coal technology system such as IGCC, high-performance power system (HIPPS), etc.

D 2003 Elsevier Science B.V. All rights reserved.

Keywords: Circulating fluidized bed; Gasifier; Kinetic model; Solid loading; Circulating chars

1. Introduction solving the transport and storage problem of coal and for

aiming at displacing fuel oil completely, heavily loaded

The world has large coal reserves; in the US, in partic- coal –water slurries (f 70% coal by weight) treated with

ular, they constitute 90% of all known fossil energy resour- additives (f 1% by weight) have been developed. Several

ces in that country. Although natural gas-fired combined demonstration projects have already proven the feasibility of

cycles currently predominate the power generation market, such coal utilization schemes [2]. To cope with the pollution

and interest is increasing in renewable energy sources, coal problems caused by coal combustion, development pro-

will likely maintain its share of the power generation market grams for ‘‘clean coal technologies’’ have been adopted

simply because it has the largest reserves and no alternative worldwide [3]—such as the integrated gasification and

is foreseen to replace it in the foreseeable future [1]. combined cycle (IGCC), the pressurized fluidized bed com-

However, coal usage has been hampered by pollution bustor (PFBC) combined cycle, ‘‘British Coal topping

caused by its transport, storage, and combustion. Partly for cycle’’ in the U.K. [4], the low emission boiler system

(LEBS) and the high-performance power system (HIPPS)

by the U.S. Department of Energy [5], etc. One of the most

* Corresponding author. Department and Graduate Institute of Bio-

Industrial Mechatronics Engineering, National Taiwan University, Taipei,

important chemical processes in the clean coal technologies

Taiwan, ROC. Tel./fax: +886-2-23693159. is coal gasification converting solid coal into gaseous fuel

E-mail address: chwu@ccms.ntu.edu.tw (C.-H. Wu). used to power turbine and subsequently to power generator.

0032-5910/03/$ - see front matter D 2003 Elsevier Science B.V. All rights reserved.

doi:10.1016/S0032-5910(03)00060-3

168 H. Tsui, C.-H. Wu / Powder Technology 132 (2003) 167–183

An advanced gasifier is required in IGCC to accomplish such forced to move towards the wall by centrifugal force and are

work. Conventional gasifiers that operate in either a bubbling collected for recycling, whereas small solid particles are

or entrained mode are not suitable choices because they do carried over by the flue gas. Another advantage of tangential

not provide efficient solid – gas mixing. A novel gasifier injection is that the injected air stays close to the cylinder wall

consisting of a circulating fluidized bed and a cyclone and most of the oxygen in the air can be expected to react with

combustor, shown schematically in Fig. 1, as developed by the char instead of the flue gas that is relative far from the

Foster Wheeler [6], is one of the most promising choices cylinder wall. The energy released in the cyclone combustor

because it provides good contact efficiency between gas and will be carried by the circulating solids to the circulating

solids and reduces the size of gasifier. fluidized bed to provide the required heat for the endothermic

The air enters the circulating bed at velocities high enough chemical reactions of coal gasification.

for the fluidized bed to operate in the ‘‘fast’’ or ‘‘circulating’’ A three-level approach, which involves thermodynamic,

regime. At these velocities, solid entrainment increases sig- kinetic, and hydrodynamic models, was used to analyze the

nificantly, and circulation of solids becomes necessary to operation of the gasifier shown in Fig. 1 [7]. This paper only

preserve a constant solid inventory in the bed. Thus, a cyclone presents the kinetic analysis. The feed rates of materials, the

is introduced to collect solids from the flue gas and recycle generation rate of product gas, and the circulation rate of char

them into the circulating fluidized bed. The cyclone is also used in the kinetic analysis come from the thermodynamic

used as a combustor to supply energy for the endothermic analysis by balancing the mass and energy of the gasifier at

gasification reactions. Therefore, the cyclone is referred to as equilibrium. The kinetic analysis will predict how the

a cyclone combustor. When the flue gas enters the cyclone chemical reactions approach equilibrium in the gas and

combustor tangentially, large solid particles in the flue gas are provides an estimate for the required circulating rate of char.

Fig. 1. Sketch of a novel gasifier consisting of a circulating fluidized bed and a cyclone combustor.

H. Tsui, C.-H. Wu / Powder Technology 132 (2003) 167–183 169

Coal water slurry fuel is used to show its feasibility in this Table 1

Reaction mechanisms and rate expressions of char – steam reaction (source:

coal utilization scheme. Gasification of coal water slurry fuel

Lowry [15])

consists of three steps: evaporation, devolatilization, and the

Source Reaction Rate expression

following char gasification. As the rate of evaporation and

mechanism

devolatiliaztion are fast compared to gasification, the gas-

ification rate of char is considered as the factor that domi- Walker Cf þ H2 OðgÞ K!

1

K1 ðH2 OÞ

et al. K2 Rate ¼

nates the gasification time of coal water slurry fuel in this H2 ðgÞ þ CðOÞ 1 þ K 1 ðH2 OÞ þ K 2 ðH2 Þ

K3 K3

kinetic analysis [8]. CðOÞ K!

3

COðgÞ

K1 ðH2 OÞ þ Kd ðCO2 Þ

Ergun and Cf þ H2 OðgÞ K!

1

Rate¼

K2 K1 K2 K5

Menster 1þ ðH2 OÞþ ðH2 Þþ ðCOÞ

2. Problem formulation K3 K3 K4

H2 ðgÞ þ CðOÞ

K3

2.1. Kinetics of coal gasification CðOÞ ! COðgÞ

CðOÞ þ CO K!

4

Numerous experiments have been performed to study the K5

been obtained from either the amount of coal converted or CH2 CCORT

Wen C + H2O(g) ! dx

dt ¼kv CH2 O ð1 xÞ where:

weight of gaseous products formed during gasification. CO + H2 K

Wide variations exist in the kinetic data reported in the coal Kv = volumetric rate constant;

gasification literature. The variation appears to be caused by K = equilibrium constant

differences in chemical and physical properties of the coal

and the experimental systems used. The chemical properties

1 contains some of the rate expressions and mechanisms

of coal, such as carbon, hydrogen, and oxygen contents,

developed for the char –steam reaction [15]. Carbon mon-

have significant effects on carbon conversion during gas-

oxide and hydrogen are the principal products of a char –

ification. As carbon content increases or as hydrogen and

steam reaction and their concentration may have a retarding

oxygen present in coal decrease, the rank of the coal

effect on the rate.

increases. In general, the reactivity of coal decreases as

The rate of char – steam reaction depends mainly on the

the carbon content increases or the oxygen and hydrogen

temperature and steam pressure. Fig. 2 shows the variation

contents decrease. In other words, lower rank coals are more

of char gasification rates with temperature at 1 atm steam

reactive than higher rank coals [12].

pressure [10]. Although there are wide variations in gas-

The physical properties of coal, such as particle size and

ification rates of different chars, they all increase exponen-

porosity, have significant effects on the kinetics of coal

tially with temperature. The variations in rates are due to

gasification. As the particle size becomes smaller the spe-

difference in chemical and physical properties of the chars.

cific contact area between the coal and the reacting gases

Fig. 3 shows the variation of char gasification rate with

increases, resulting in faster reaction. In general, coal gas-

steam pressure at different temperatures [12]. The rates

ification processes with entrained and fluidized bed reactors

increase with steam pressure but become independent of

use coal with an average size of 75 Am. Processes with fixed

pressure at pressures higher than about 10 atm.

bed reactors use larger size coal with diameter exceeding

300 Am. Porosity of coal is related to the pore volume and

2.2. Desulfurization during coal gasification

surface area present in the coal. It has been found [12] that

reactivity in gasification increases with an increase in pore

In developing coal gasification processes, the removal of

volume and surface area of low and medium rank coals.

the sulfur compounds has been of great concern because of

However, reactivity is not affected by changes in pore

their detrimental effects on air quality and their role in

volume and surface area in high rank coals with carbon

corrosion of equipment. The principal sulfur compound that

content larger than 85%. This is due to the smaller pores

evolves during gasification of coal is H2S with lesser

present in higher rank coals. As pores become smaller, the

portions of COS, CS2. Hot gas desulfurization proceeds in

access of reacting gases to the internal surface of the coal is

two steps when calcium-based sorbent is used. First, the

reduced, i.e. the process is controlled by the rate of diffusion

limestone (mostly CaCO3) is calcined to produce lime

into the coal.

(CaO) and CO2 as shown in Eq. (1). In the second step,

In experimental systems, coal is pyrolyzed to become

lime reacts with H2S to produce a stable sulfide CaS as

char, which undergoes conversion to gas by reaction with

shown in Eq. (2).

steam, carbon dioxide, and hydrogen. The kinetics and

mechanisms of reactions of coal char with steam, carbon

CaCO3ðsÞ ! CaOðsÞ þ CO2 ð1Þ

dioxide, and hydrogen were discussed in the previous liter-

ature [13,14]. In general, Langmuir-type adsorption equa-

tions have been used to represent gasification rates [9]. Table CaOðsÞ þ H2 S ! CaSðsÞ þ H2 O: ð2Þ

170 H. Tsui, C.-H. Wu / Powder Technology 132 (2003) 167–183

(C) and the concentration of available CaO (A) as follows:

dN

¼ K3 AC; ð3Þ

dt

where K3 is the rate constant of Eq. (2). The concentration of

available lime in the calcined limestone decreases as the

reaction of desulfurization proceeds in two ways: the avail-

able lime reacts with H2S (K3AC) or the surface of the

available lime is covered by CaS layer. The decrease rate of

available lime through the adsorption and desorption of CaS

layer equals the subtraction of the adsorption rate CaS layer

on the exterior of available lime (K1AC) to the desorption

rate of CaS layer on the exterior of inactivated lime (K2B).

Thus, the decrease rate of available lime ( dA/dt) could be

written as follows:

dA

¼ K1 AC K2 B þ K3 AC; ð4Þ

dt

where K1 is the rate constant of adsorption of CaS on the

surface of available lime and K2 is the rate constant of

desorption of CaS on the surface of inactivated lime. Sub-

stituting the expression A from Eq. (3) into Eq. (4) and

rearranging, Eq. (5) is obtained. From Eq. (5), the rate of

decrease of CaO(s) (dN/dt) is obtained as shown in Eq. (6),

Fig. 2. Variation of char gasification rates with temperature (source: where Ke = K1/K2. The decrease rate of CaO(s) (dN/dt) equals

Johnson [10]).

the desulfurization rate because 1 mol of CaO(s) reacts with 1

According to Abel et al. [16], the rate of Eq. (2) is fast, but mol of H2S, as indicated in Eq. (2). The kinetic constants K1,

the rate of Eq. (1) is relatively slow. In addition, CaCO3 is K2, and K3 are determined from experimental results via

chemically inert to H2S. One potential reason for limestone Arrhenius plots [19]. The pre-exponential constants and

not being able to remove H2S effectively is the relatively slow activation energy for the Arrhenius law are described in

calcinations, Eq. (1), that occurs under gasification condi- Table 2. The general Arrhenius expression is given in Eq.

tions. This problem can be solved in the proposed reactor (7). Form Table 2 and Eq. (7), the rate constants K1, K2, and

configuration. A large amount of CaO is recycled in the K3 can be determined. Substituting these rate constants into

gasifier, making the removal of H2S from the gas stream

relatively rapid. According to Schrodt and Hahnn [17], CaS

formed on the exterior of the sorbent prohibits further

reactions of the sorbent with H2S. Thus, CaS appears to form

a diffusion barrier for H2S penetration and this limits the

calcium utilization efficiency. This effect is taken into

account in modeling the process of desulfurization as follows.

A theoretical model for the reaction of CaO with H2S was

developed and experimentally verified by Pell et al. [18].

This model assumes that there is nothing adsorbed on the

surface of CaO at the beginning of reaction of desulfuriza-

tion. As reaction (2) proceeds, the rate slows down, and this

suggests that CaS is adsorbed upon the surface thereby

inactivating the surface. The total amount of lime (CaO) in

the calcined limestone could be categorized into two groups,

according to Pell et al. [18]. One group is the available lime

that can react with H2S to form CaS through reaction (2). The

other group is inactivated lime that cannot react with H2S

due to the adsorption of CaS layer on the surface of lime. The

concentrations of the total amount of lime, available lime,

and inactivated lime in the calcined limestone are specified Fig. 3. Variation of char gasification rates with pressure (source: Quader

as N, A, and B, respectively. The rate of reaction (dN/dt) [12]).

H. Tsui, C.-H. Wu / Powder Technology 132 (2003) 167–183 171

Coefficients of Arrhenius expressions for rate constants (source: Pell et al.

collisions via Eqs. (8) and (9). The kinetic analysis utilizes

[18])

Lindemann’s theory in the way that the gasification process

Constants Preexponential Activation energy

proceeds step by step and the number of C(o) complexes

(Ki) constants ( Pi) (Ei, kcal/gmol K)

reaches a stationary value after each time step. To reach a

K1 8.3 13.1

stationary value of C(o), the number of energized sites C(o)

K2 9.5 28.2

K3 13.1 22.9 desorbed through Eq. (10) should equal the number of the

Ke 1.2 15.1 energized sites C(o) generated through Eqs. (8) and (9) in a

small time interval Dt. Thus, the statement of Lindemenn’s

theory

_ can be written as Eq. (11), where negative values of

Eq. (6), the desulfurization rate (dN/dt) can be obtained if the

N c (atoms/s) represent the number of C(o) complexes

concentration of H2S (C) and the amount of unconverted

desorbed through Eq. (10), and positive values of X and

CaO(s) (N) are known.

Z represent the number of atoms of CO2 and H2 generated

d2 N dN through Eqs. (8) and (9) in the time interval Dt, respec-

þ ðK1 C þ K3 C þ K2 Þ þ K2 K3 CN ¼ 0 ð5Þ tively.

dt 2 dt

Nc Dt decomposition of CðoÞ through Eq: ð10Þ

dN K3 N C

¼ ð6Þ þ Z generation of CðoÞ through Eq: ð9Þ

dt 1 þ Ke C

þ ðX Þ Generation of CðoÞ through Eq: ð8Þ ¼ 0: ð11Þ

Ei

Ki ¼ Pi exp : ð7Þ A negative sign is added to X in the third term of Eq. (11)

RT

to represent the generation of energized sites C(o) because

2.3. Kinetic model of char gasification the decomposition of CO2 ( X) will implicate the gen-

eration of C(o) through Eq. (8).

The kinetic model of char gasification is derived from the In this reaction system, the total number of oxygen atoms

mechanism of the chemical reactions among the char, water is constant, being either present as energized sites C(o) or

vapor, and CO2. According to Johnson [10] and Ergun [11], contained in the gas species CO, CO2, and H2O. According

the mechanism of the reaction between the char and water to Lindermann’s [20] theory, the number of energized sites

vapor in the presence of CO2 can be written as Eqs. (8) – C(o) reaches a stationary value rapidly, implying that the

(10). They assume that there are many free sites Cf on the oxygen concentration in C(o) complexes will reach a sta-

char, which can adsorb oxygen from the dissociative chem- tionary number. Thus, the number of oxygen atoms con-

isorption of CO2(g) and steam as shown in Eqs. (8) and (9), tained in the gas species (H2O, CO2, CO) will also reach a

respectively. As this happens, the free site is energized and constant value because the total number of oxygen atoms in

becomes an occupied site (C(o)), which in turn is gasified to the chemical system is a constant. The statement indicating

produce CO(g), as shown in Eq. (10). The energized site C(o) a constant number of oxygen atoms in the gas species is

is a chemical complex on the surface of the char which can represented by Eq. (12), where Y is the total number of

be transferred into reaction product CO(g) without receiving atoms of CO generated through either Eq. (8) or Eq. (10)

additional energy. However, the process of desorption of the during the time interval Dt.

chemical complex C(o) (reaction (10)) is slower than Eqs.

(8) and (9), therefore the rate of desorption controls the Z disappearance of oxygen through the generation of H2

reaction rate. ¼ 2X appearance of oxygen through the generation of CO2

kV

COðgÞ þ CðoÞ ð8Þ

1

ð12Þ

k2

H2 OðgÞ þ Cf ! H2ðgÞ þ CðoÞ ð9Þ _

kV 2 There are four unknowns, N c, X, Y, and Z, in_Eqs. (11)

k3 and (12). Even if the rate of char gasification (N c) can be

CðoÞ ! COðgÞ : ð10Þ obtained from experiments, there are still three unknowns—

X, Y, and Z—in Eqs. (11) and (12). In order to solve the

As Eq. (10) is the rate-controlling step, the gasification problem, another governing equation was applied as fol-

process can be represented as a first-order reaction, i.e. the lows. The equilibrium constants, K1 and K2, of Eqs. (8) and

reaction rate is proportional to the concentration of C(o). (9), respectively, can be written as Eqs. (13) and (14).

According to Lindemann’s theory [20], for a first-order Dividing Eq. (14) by Eq. (13) and simplifying it will result

reaction, the number of energized molecules C(o) will reach to Eq. (15). It is interesting to note that Eq. (15) represents

a stationary value if the conversion of C(o) into CO via Eq. the equilibrium condition for the water – gas shift Eq. (16).

172 H. Tsui, C.-H. Wu / Powder Technology 132 (2003) 167–183

In the next section, the concentration of H2O, H2, CO and velocity are mainly due to the chemical reaction between

CO2 in Eq. (15) are related to X, Y, and Z in the small- char and steam.

compartment scheme. Thus, (Eqs. (11), (12) and (15) are the

governing equations, which can be solved for X, Y, and Z

Wc ¼ Wc0 þ Nc Dt ð17Þ

when Nc is known and a small-compartment scheme is used

in the next section.

0

WCO ¼ WCO þY ð18Þ

k1 ½CO ½CðoÞ

K1 ¼ ¼ ð13Þ

k1V ½CO2 ½Cf

WH2 ¼ WH0 2 þ Z ð19Þ

k2 ½H2 ½CðoÞ

K2 ¼ ¼ ð14Þ

k2V ½H2 O ½Cf WH2 O ¼ WH0 2 O Z ð20Þ

K2 ½CO2 ½H2 0

WCO2 ¼ WCO þX ð21Þ

K¼ ¼ ð15Þ 2

K1 ½CO ½H2 O

0

CO þ H2 O ¼ CO2 þ H2 : ð16Þ WCaO ¼ WCaO þ NH2 S Dt ð22Þ

WH2 S ¼ WH0 2 S þ NH2 S Dt: ð23Þ

A one-dimensional control volume analysis was devel-

oped to determine the extent to which the chemical reactions

of char gasification approach equilibrium in the region from To conduct the one-dimensional control

_ volume analy-

X1 = 0 to X1 = 2.5 m (the gasifier height) as shown in Fig. 1. sis, the five unknowns X, Y, Z, and N H2S appearing in the

The gasification of CWSF is assumed to occur in three above equations should be determined. The first three

consecutive steps: evaporation, combustion, and slow reac- unknowns—X, Y, Z—are obtained using the kinetic model

tion between char and steam. The processes of water developed

_ _ in the previous section. The last two unknowns,

evaporation, coal pyrolysis, and combustion complete at N c and N H2S, are determined by using experimental data in

X1 = 0. This assumption may not fit reality because the the literature [8 – 10]. Eqs. (11)– (13) derived in the pre-

evolution rate of the volatiles, which depends on various vious section can be rearranged to Eqs. (14) and (15),

factors such as particle size, pressure, and heating rate, may respectively. Eq. (24) is obtained by substituting Eqs.

be too slow to assume that coal pyrolysis has been completed (18) –(21) into Eq. (13).

at X1 = 0. A complete pyrolysis model would describe the 0

K2 ðWCO þ X ÞðWH0 2 þ ZÞ

composition and physical state of the char particle and the K¼ ¼ 2

ð24Þ

0

composition and evolution rate of the volatiles at all stages of K1 ðWCO þ Y ÞðWH0 2 O þ ZÞ

pyrolysis. However, the detailed mechanism of the evolution

and combustion of volatiles is not very well understood and

Z ¼ X Nc Dt ð25Þ

detailed experimental work is still required. Nevertheless,

this assumption is still a good approximation because in

general the reaction rates of water evaporation, coal pyrol-

Y ¼ X Nc Dt: ð26Þ

ysis, and combustion are much faster than that of the

gasification of the char. Based on this assumption, the initial Substituting Eqs. (25) and (26) into Eq. (24), results to Eq.

composition and superficial velocity of the gas mixture can (27), which contains only X.

be obtained from the thermodynamic analysis.

The variation of the composition and the superficial gas

velocity as X1 increases can be determined using Eqs. (17) – aX 2 þ bX þ c ¼ 0 ð27Þ

(23). The variation of the number of mole of species (based

where

on 1 mol of carbon in feed CWSF) as X1 increases can be

calculated from these equations. This information is then

utilized to obtain the composition of the gas mixture (mole a=1K _

fraction) and the superficial gas velocity. The variation in 0

b = KW H 2O

0

KW CO + W 0CO2_+ W0H2 N cDt _ _ _

0 0 0 0

the gas composition and the increase in the superficial gas c = KW H2OWH2O +KW H2O N cDt KWCO N cDt + K(N cDt)2+ W CO

0

2

0

W CO 2

N CDt.

H. Tsui, C.-H. Wu / Powder Technology 132 (2003) 167–183 173

The solution of Eq. (27) is written as Eq. (28) 2.5. Circulation rate and shrinkage of chars

pﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃ

b þ b2 4ac The circulation rate of char is calculated in the following

X ¼ : ð28Þ two steps. First, the cut-off diameter of the cyclone com-

2a

bustor is calculated according to the cyclone geometry and

the Rankine vortex flow condition [21]. Second, the tran-

Substituting the value of X into Eqs. (15) and (16), the

sient mass equations of char particles are developed. A trial

values of Z and Y are obtained._ _ and error method is applied to solve these equations by

The rates of gasification N c and desulfurization N H2S are

varying the initial diameter of char particle and the number

determined from experiments conducted by Wen [9], John-

of circulation of char particle in the gasifier until the

son [10], and Pell et al. [18]. Thus, two sets of kinetic data

diameter of char particle shrinks to the cut-off diameter

were used to indicate the influence of the rate of gasification

and the circulation rate of char is accumulated to the

on the performance of the circulating fluidized bed gasifier:

required amount. In the analysis using Johnson’s kinetic

one set from Johnson [10] as described in Fig. 2 and the

data, the circulation rate of char reaches such amount that

other from Wen [9] as described in Eq. (29). Johnson’s [10]

the chemical reaction of char gasification reach equilibrium

experiments indicate that the rate of the char –steam reaction

at X1 = 2.5 m. In the analysis using Wen’s kinetic model, the

depends mainly upon temperature and steam pressure for a

circulation rate of char reaches such amount that the fluid-

specific kind of char. Fig. 2 contains specific gasification

ized bed has a superficial velocity between 3.6 and 4.9 m/s

rates for different chars in steam at 1 atm. It shows that the

(12 –16 ft/s) and a solid loading density between 50 and 100

gasification rate increases as the temperature increases.

kg/m3, which are recommended for the bed to operate in the

Wen’s [9] experiments indicate that the rate of char gas-

circulating region by industrial experience [22]. The follow-

ification also depends on the concentration of H2O, H2, and

ing assumptions were made in conducting the analysis.

CO. This is shown in his kinetic model, Eq. (29), which

includes the concentrations of these species. In the equation,

1. The char is a spherical solid particle with a constant

KC – H2O is the equilibrium constant of char stream reaction

density.

and Kv is the rate constant for the gasification of coal char in

2. The shrinkage of the char is mainly due to the chemical

the temperature range from 1273 to 1473 K.

reactions between the char and the gas species (steam and

oxygen), i.e. the effects of attrition and agglomeration on

CH2 CCO RT the size of the particles have been neglected.

Nc ¼ Kv CH2 O Wc : ð29Þ

KCH2 O 3. A Rankine vortex [23] is formed in the cyclone

combustor, which is a combination of a central forced

_ vortex and a peripheral vortex.

The rate of desulfurization N H2S is obtained from the

kinetic model of Pell et al. [18], as indicated by Eq. (30). 4. The cut-off diameter of the cyclone combustor can be

The rate constants K3 and equilibrium constant Ke are determined by considering the motion of the particle on a

obtained from experiments [19] of the reaction between imaginary cylindrical surface as described by Ogawa [23]

CaO and H2S from 700 to 1200 K and Barth and Trunz [24].

5. All particles larger than the cut-off diameter are separated

from the product gas and all particles smaller than the

¼ K3 WCaO CH2 S :

N ð30Þ cut-off diameter are carried out of the cyclone combustor

H2 S

1 þ Ke CH2 S by the product gas.

The kinetic model of desulfurization described by Eq. (30) 2.5.1. Calculation of cut-off diameter of the cyclone

does not consider the effect of the water concentration on combustor

the rate of desulfurization. The effect of water concentration The separation of the particles and the gas in the cyclone

on the rate of desulfurization is still not well understood. combustor is caused mainly by the centrifugal force

However, water concentration should restrict the extent of imposed on the solid particles. The equation of motion of

desulfurization from the thermochemical_point _ of view. a solid particle in the cyclone combustor in the radial

Substituting the values of X, Y, Z, N c, N H2S into Eqs. direction can be written as Eq. (31)

(17) – (23), the composition of the product gas can be

determined after a time interval Dt or a distance DX1 = UgDt. dUr 1

Mp ¼ Mp Uh2 FD : ð31Þ

The final composition of the product gas at X1 = 2.5 m is dt r

influenced_ by the circulation rate of the char because the

value of N C is related to the circulation rate of the char. The term on the left-hand side is the inertial force. The

Using a computer simulation, the required circulation rate of first term on the right-hand side is the centrifugal force,

the char for the gasification reactions to reach equilibrium at and the second term on the right-hand side is the drag

X1 = 2.5 m was determined. force that is caused by the gas flow in the negative radial

174 H. Tsui, C.-H. Wu / Powder Technology 132 (2003) 167–183

direction. If the centrifugal force is larger then the drag Thus, Eq. (34) can be written as Eq. (35)

force, the solid particle will be accelerated in the radial

direction and be forced to move towards the wall of the

qp

cyclone combustor. The drag force FD in Eq. (31) can be Vr2 ¼ d2 V 2 : ð35Þ

9l De p h2

written as Eq. (32).

q The velocity Vr2 in Eq. (35) can be obtained by assuming

FD ¼ Cd Ap ðUr Vr Þ2 : ð32Þ

2 that the inward radial velocity of gas is uniformly distributed

over the imaginary cylindrical surface. Thus,

_ Vr2 is obtained

The expression for the drag coefficient Cd depends on the by dividing the volume flow rate of gas Q by the area of the

type of flow. According to Ogawa [23], the drag coef- imaginary cylinder surface

ficient Cd in Stokes flow can be written as Eq. (33). The

flow is considered as Stokes flow when the Reynolds

Q

number based on the diameter of the particle Rep is less Vr2 ¼ : ð36Þ

pDe H

than 4

24 Substituting Eq. (36) into Eq. (35) results to Eq. (37), which

Cd ¼ : ð33Þ is the expression for the cut-off diameter

Rep

!1=2

Substituting Eqs. (32) and (33) into Eq. (31) results to Eq.

1 9Ql

(34), which is the equation of motion in the radial dpc ¼ : ð37Þ

Vh2 pqp H

direction in Stokes flow.

Mp ¼ Mp Uh2 3pldp ðUr Vr Þ: ð34Þ

dt r the geometry indicated in Figs. 1 and 4 is calculated as

follows. The calculation is based on the following specified

The cut-off diameter of the cyclone combustor can be conditions:

determined by considering the motion of the particle on an

imaginary cylindrical surface as described by Ogawa [23] (1) The gasifier operates at 1150 K with a thermal capacity

and Barth and Trunz [24]. The imaginary cylindrical surface of 586 KW and a CWSF containing 30% water by

has a diameter of De and a height of H, as shown in Fig. 4. weight.

The cut-off diameter is the diameter of those particles that (2) The gasifier is fed with rates of CWSF, air, and

can stay on the imaginary surface in a state of mechanical limestone which were determined in the thermody-

balance, i.e. the radial velocity is zero (Ur = 0) and the namic analysis.

centrifugal force equals the drag force. When the particles (3) The product gas reaches chemical equilibrium on the

has diameters larger than the cut-off diameter, the centrifu- surface of the imaginary cylindrical surface.

gal force is larger than the drag force because the centrifugal (4) The feed air to the cyclone combustor is uniformly

force is proportional to the mass of the particle or dp3 but the distributed through 12 pipes of 2.54 cm (1 in.) diameter

drag force is proportional to dp, as indicated by the last term at 298 K.

of Eq. (34). As a result, particles larger than the cut-off (5) The tangential velocity on the imaginary cylindrical

diameter cannot pass through the imaginary cylindrical surface falls in the region of the free vortex of the

surface. For the same reason, when the particles have Rankine vortex.

diameters smaller than the cut-off diameter, the centrifugal (6) The mean density qp and the mean diameter of the char

force is smaller than the drag force. As a result, the particles are assumed to be 1200 kg/m3 and 50 Am, respectively.

smaller than the cut-off diameter pass through the imaginary

cylindrical surface and are carried out of the cyclone Condition (5) has generally been found to be true from

combustor by the flue gas. experimental results [21]. The density and the diameter of

The expression for the cut-off diameter is obtained by the char vary over a wide range depending on the physical

considering the equation of motion of particles that stay on and chemical properties of parent coal and the coal pyrolysis

the imaginary cylindrical surface and in a state of mechan- conditions. Thus, condition (6) is an approximation used to

ical balance under the following conditions: facilitate the calculation.

Based on (1), (2) and (3), the mass flow rate and the

1. Ur2 = 0. volume flow

_ rate of product gas through the imaginary

2. the centrifugal force equals the drag force. surface Q are calculated to be 0.103 kg/s and 0.43 m3/s,

3. the angular velocity of the particle equals that of the gas respectively. The height of the imaginary cylinder H_ is 1.54

(Uh = Vh). m, as indicated in Fig. 4. Substituting the values of Q , l, qp,

H. Tsui, C.-H. Wu / Powder Technology 132 (2003) 167–183 175

and H into Eq. (37), the relation between dpc and Vh2 is is calculated to be Vh = 6.13 m/s based on condition (4). Fig.

written as Eq. (38). 5 shows a sketch of Rankine vortex [25] of a combination of

a central force vortex and a peripheral free vortex. The

4 1

dpc ¼ 1:816 10 : ð38Þ relation between the tangential velocity Vu and the radius r

Vh2 is given in Eq. (39).

The value of Vh2 can be calculated under conditions (4) and Vh rh ¼ constant: ð39Þ

(5). From the thermodynamic analysis, 0.0435 kg/s of air

was required to be fed into the cyclone combustor. Thus, For the forced vortex, h equals 1 and for the free vortex h

tangential velocity of the air entering the cyclone combustor is found between 0.45 and 0.8 [25]. Based on condition (5),

176 H. Tsui, C.-H. Wu / Powder Technology 132 (2003) 167–183

Fig. 6. Mole ratio of gas species as a function of axial distance along the

gasifier.

Fig. 5. Sketch of the Rankine vortex [25].

As a result, the total mass consumption of a single

particle char in the ith circulation DWi (kg/s) can be written

the tangential velocity Vu2 can be calculated from Eq. (39) as Eq. (41).

with h = 0.5 as follows:

0:331 0:1

0:5 0:5 DWi ¼ 1þ þ DWgi ¼ 3:194 104 dp2i1 : ð41Þ

r 9 0:9 0:9

Vh2 ¼ Vh ¼ 6:13 ¼ 9:19 ðm=sÞ:

r2 4

A shrinking particle model is used to estimate the

shrinkage of the char particle after n circulations. The char

From Fig. 1, the values of r and r2 are obtained to be is assumed to have a constant density and to shrink

0.2285 m (9 in.) and 0.1015 m (4 in.), respectively. uniformly when it reacts with either steam or oxygen. The

Finally, the cut-off diameter of the cyclone combustor is diameter of the char dpn after n circulations can be written as

calculated to be 19.7 Am by substituting Vh2 = 9.19 m/s Eq. (42).

into Eq. (38).

! 13

2.5.2. Calculation of the char diameter dpn and circulation 6 X

n

dpn ¼ W0 DWi

rate of char Wn after n circulations pqp i¼1

The shrinkage of a single char in each circulation is due

! 13

to both gasification and combustion. From previous studies 6 p Xn

[26], it has been found that the rate of consumption of char ¼ qp dp30 3:194 104 dp2i1 ð42Þ

pqp 6 i¼1

is the product of its surface area and the rate coefficient Ks

(kg/s m2). The rate coefficient Ks (kg/s m2) for gasification

is estimated from Eq. (40) as follows: Under the assumption that the char particle has a constant

density qp and a uniform diameter dp0 when it enters the

cMp ¼ Ks As ð40Þ

char can be obtained as 0.001 (1/s) from Fig. 2 [10]. The

mean density qp and the mean diameter of char dp were

measured as 1200 kg/m3 and 50 Am, respectively. Substitut-

ing these values of c, dp, and qp into Eq. (40). Ks is

calculated to be 2.0 10 5 (kg/s m2). The required resi-

dence time of the char in the gasifier is found to be 0.86 s.

Thus, the mass consumption of a single char particle due to

the gasification in the ith circulation is DWgi = 0.00086Ks

(4pd 2pi 1). The energy balance of this system requires that it

has to burn 0.331 mol of char in the cyclone combustor and

0.1 mol of char in the circulating fluidized bed in order to

sustain 0.9 mol of endothermic steam – coal gasification Fig. 7. Mole ratio of gas species as a function of axial distance along the

process. gasifier.

H. Tsui, C.-H. Wu / Powder Technology 132 (2003) 167–183 177

gasifier, the_ number of char particles fed into the gasifier per

unit time N is obtained by dividing the feeding rate of char

by the mass of a single char particle

Wf Fc

N¼p : ð43Þ

dp30 qp

6

The circulation rate of char after n circulations can be

written as Eq. (44)

Wn ¼ N ðW0 þ ðW0 DW1 Þ þ ðW0 DW1 DW2 Þ

þ ðW0 DW1 DW2 DW3 Þ þ K þ ðW0 DW1

DW2 DW3 K DWn ÞÞ

!

Xn Fig. 9. Composition of product gas species as a function of axial distance

¼ N ðn þ 1ÞW0 ðn i þ 1ÞDWi along the gasifier.

i¼1

wf Fc

¼p ðn þ 1ÞW0 3:194 (44) by varying the initial diameter of char dp0 and the

dp30 qp number of circulation of char in the gasifier n until the

6 !

Xn system reaches steady or both Eqs. (45) and (46) are

4 2 satisfied.

10 ðn i þ 1Þdpi1 : ð44Þ

i¼1

Eqs. (42) and (44) are the transient mass equations of char

3. Results and discussion

particles circulating in the fluidized bed and cyclone com-

bustor. The system will reach steady state when the initial

3.1. Johnson’s kinetic data

diameter of char shrinks to become the cut-off diameter of

the cyclone combustor after n circulations

The results of the kinetic analysis using Johnson’s

dpn ¼ dpc ð45Þ kinetic data of a constant specific gasification rate (0.01

1/s) are presented in Figs. 6 – 11. The constant specific

and the circulating rate of chars becomes the amount gasification rate of 0.001 1/s was obtained from Fig. 2 at

required of operating the gasifier simultaneously 1150 K. In the kinetic analysis, the reactor temperature, the

thermal capacity of the gasifier, and the water concentra-

Ẇn ¼ Ẇre : ð46Þ tion of the CWSF, were fixed at 1150 K, 586 KW (2 106

Btu/h) and 30%, respectively. The kinetic models derived

As the system reaches steady state the particle size distri- in previous section were used to predict the required

bution and the circulating rate of char will not vary with circulation rates of char and lime for the chemical reac-

time. A trial-and-error method is used to solve Eqs. (42) and tions to reach equilibrium within the given height of the

Fig. 8. Mole ratio of gas species as a function of axial distance along the

gasifier. Fig. 10. Gas velocity as a function of axial distance along the gasifier.

178 H. Tsui, C.-H. Wu / Powder Technology 132 (2003) 167–183

reactions to equilibrium

_ _ from the curve of the mole ratio of

gas species

_ (X /X eq ) vs. the axial distance along the gasifier,

where X eq is the number of moles of the species in the

gasifier as the char gasification reaches equilibrium. These

figures show

_ _ that all species approach their equilibrium

values (X /X eq = 1) after the gas has traveled a distance of

2.5 m, which was set as the height of the gasifier as

indicated in Fig. 1. Fig. 9 shows the mole fraction of the

species as a function of the axial distance. It shows the

mole fractions of H2 and CO increase and the mole

fractions of H2O and N2 decrease with distance. This

increase in the mole fractions of H2 and CO and decrease

Fig. 11. Solid loading density as a function of axial distance along the of that of H2O are caused by the chemical reaction between

gasifier. the steam and the char. The decrease in the mole fraction of

N2 is mainly due to the generation of gas species of CO and

gasifier. It was found that the required circulation rates of H2 during char gasification. Fig. 9 also shows that the slope

carbon and lime were 11.8 and 4.5 kg/s, respectively, and or the mole fraction of CO2 increases slightly and then

the required residence time of the char in the gasifier was decreases with distance beyond X1 = 0.55 m. This phenom-

Fig. 12. Operating concept of the gasifier with equilibrium feed rates at 1150 K using Johnson’s [10] kinetic data.

H. Tsui, C.-H. Wu / Powder Technology 132 (2003) 167–183 179

enon is caused by the different shift direction of water – gas (47) to shift to the left, which makes the generation rate of

shift reaction H2 to be smaller than that of CO. Figs. 10 and 11 show the

gas velocity and the solid loading density as a function of

CO þ H2 OVCO2 þ H2 : ð47Þ the axial distance, respectively. The gas velocity is

obtained by dividing the volume flow rate of gas by the

Initially, the chemical kinetic makes reaction (47) to shift

cross-sectional area of the gasifier and the solid loading

to the right, this will generate CO2 and make the slope of

density is the ratio of the circulation rate of the solids to

CO2 curve positive. However, beyond X1 = 0.55 m the

the volume flow rate of gas. These figures show that the

chemical kinetic makes reaction (47) to shift to the left,

gas velocity increases and the solid loading density

this will consume CO2 and make the slope of CO2 curve

decreases as the axial distance increases. This phenomenon

negative. The comparison of the slope of CO curve with

is caused by the increase in the volume flow rate of gas as

that of H2 curve in Fig. 9 also shows the same shift

the char gasification reaction

tendency. Initially, the slope of H2 curve is larger than that

gasif ication

of CO curve, but becomes smaller than that of CO curve CðsÞ þ H2 O

! CO þ H2 ð48Þ

when X1 is beyond 0.55 m. The larger curve slope

represents the larger generation rate of gaseous species proceeds along the axial distance. The char gasification

and vice versa. Thus, the chemical kinetic initially makes reaction consume 1 mol of H2O(g) but generates total two

reaction (47) to shift to the right, which makes the mol of CO and H2.

generation rate of H2 to be larger than that of CO, but All three operating parameters (reactor temperature,

beyond X1 = 0.55 m the chemical kinetic makes reaction thermal capacity, and water concentration in the CWSF)

Fig. 13. Operating concept of the gasifier with equilibrium feeding rates using Wen’s [9] kinetic model.

180 H. Tsui, C.-H. Wu / Powder Technology 132 (2003) 167–183

The recycle ratio, the ratio of the circulation rate of lime to

the feed rates of CWSF, is calculated to be 203. When the

reactor temperature, the composition of the CWSF, and the

thermal capacity of the gasifier are specified, the maximum

volume flow rate in the gasifier is determined, i.e. the

maximum gas velocity in the gasifier is fixed. Industrial

experience indicates that a circulating fluidized bed should

operate at higher gas velocities than those indicated by Fig.

10 for improved performance [20]. In order to obtain higher

gas velocities, the unit should be operated at a higher

temperature and thermal capacity than those indicated in

Fig. 12. Thus, the following section demonstrates a way to

operate the facility at higher gas velocities by increasing the

reactor temperature and the gasifier’s thermal capacity.

Also, Wen’s [9] kinetic model is used in order to show

the effect of a more sophisticated and realistic gasification Fig. 15. The composition of gas as a function of axial distance along the

scheme. gasifier using Wen’s [9] kinetic model.

3.2. Wen’s kinetic model that the gasifier is required to operate at 1450 K with a

thermal capacity of 879 KW (3 106 Btu/h) and circulation

This section demonstrates how to obtain a superficial rates of char and lime of 15 and 4.5 kg/s, respectively, in

velocity between 3.6 and 4.9 m/s (12 – 16 ft/s) and a solid order to reach the specified range of gas velocity and solid

loading density between 50 and 100 kg/m3, which are loading density. The chemical reactions, however, do not

recommended by industrial experience [20]. In this analysis, reach equilibrium at a height of X1 = 2.5 m and only 88% of

Wen’s [9] kinetic model (Eq. (29)) was used to predict the the water is consumed. The emissions of H2S (0.15 lb of

gasification rate of the char in the gasifier. Wen’s kinetic SO2 per million Btu) based on the total conversion of H2S to

model (Eq. (29)) describes the gasification rate of char as a SO2 after combustion were found still to be below the

function of the reactor temperature and the concentration of allowed SO2 emission levels (1.2 lb per million Btu).

the species, steam, CO, and H2. A trial-and-error technique Fig. 13 shows the sketch of the gasifier with the feed

was used to determine the operating parameters and the rates of materials and the operating conditions that are

circulation rates of char and lime so that the superficial gas needed to reach the expected ranges of gas velocity and

velocity and solid loading density fell within the specified solid loading. The recycle ratio, the ratio of the circulation

range. In this method, the water concentration of the CWSF rate of lime to the feed rate of CWSF, is calculated to be

was fixed at 30%, but the other two operating parameters, 163. The equilibrium feed rates were calculated at 1450 K

the reactor temperature and the gasifier’s thermal capacity, for the gasifier’s thermal capacity of 879 KW (3 106 Btu/

were varied. The results of this trial and error method show h) and a CWSF containing 30% of water by weight. Fig. 14

Fig. 14. The consumption of steam as a function of axial distance along the Fig. 16. Gas velocity as a function of axial distance along the gasifier using

gasifier using Wen’s [9] kinetic model. Wen’s [9] kinetic model.

H. Tsui, C.-H. Wu / Powder Technology 132 (2003) 167–183 181

Fig. 19. Circulating rate of char as a function of axial distance along the

gasifier.

Fig. 17. Solid loading density as a function of axial distance along the

gasifier using Wen’s [9] kinetic model. decrease in the gasification rate of the char as the concen-

trations of CO and H2 increase in Wen’s kinetic model.

shows the consumption of steam as a function of axial

distance. It shows that after the gas has traveled a distance of 3.3. Circulation rate and shrinkage of chars

2.5 m, 88% of the steam has been consumed in the gasifier.

From the thermodynamic analysis, it was found that the The transient Eqs. 42 and 44 developed in Section 2.5

consumption of steam should be larger than 99% as the are solved by varying the initial diameter and the number

gasification reaches equilibrium. Thus, this figure indicates of circulation of the chars until the char particle shrinks to

that the gasification reactions have not reached equilibrium be the cut-off diameter and the circulation rate of chars

by the time the product gas reaches the exit at X1 = 2.5 m. equals the required circulation rate of chars. Figs. 18 and

The mole fractions of the gas species as a function of axial 19 show the results obtained by using Johnson’s kinetic

distance are shown in Fig. 15. The superficial gas velocity data at 1150 K. The circulation rate of char is accumulated

and the solid loading density are shown in Figs. 16 and 17, to such amount that the chemical reaction of char gas-

respectively. They show that the superficial gas velocity and ification reach equilibrium at X1 = 2.5 m. The diameter of

solid loading density are within the specified ranges of 3.6 – the char is plotted as a function of the number of circu-

4.9 m/s and 100 –50 kg/m3, respectively. lations in Fig. 18, and the circulation rate of the char is

It is interesting to compare Fig. 16 with Fig. 10. Fig. 16, plotted as a function of the number of circulations in Fig.

which was obtained using Wen’s [9] kinetic model, shows 19. Figs. 18 and 19 show that the circulation rate of char

that the gradient of the superficial gas velocity in the flow will reach a steady value of 11.8 kg/s after 2860 circu-

direction decreases as the axial distance increases. However, lations from the startup if the initial diameter of the char is

Fig. 10, obtained from Johnson’s [10] kinetic model, indi- 80.5 Am. The char particle is expected to shrink from 80.5

cates that the superficial gas velocity increases linearly as Am to the cut-off diameter of the cyclone combustor, 19.7

the axial distance increase. This difference is due to the Am, and be carried out of the cyclone combustor after 2860

circulations.

(1) The char – steam reaction in the gasifier does not reach

equilibrium at low char circulation of 11.8 kg/s and low

temperature of 1150 K. It needs to operate at higher char

circulation rate (15 kg/s) and higher temperature (1450

K) for the char –steam reaction to reach equilibrium. It is

suggested to predict the performance of the gasifier from

the kinetic point of view in order to design the optimal

geometry and operating methods that will allow the

gasifier to play a successful role in the clean coal

Fig. 18. Shrinkage of char as a function of axial distance along the gasifier. technology system such as IGCC, HIPPS, etc.

182 H. Tsui, C.-H. Wu / Powder Technology 132 (2003) 167–183

(2) It shows a concept to operate the gasifier from transient K2 Rate constant of desorption of CaS on the surface

to steady condition after the diameter of char particle of inactivated lime (l/s)

shrinks to equal the cut-off diameter of the cyclone K3 Rate constant of Eq. 2 (E/gmol s)

combustor and the circulation rate of char equals the Ke Equilibrium constant [0.3012 105 exp(7603.2/

required amount simultaneously. Whenever the system T)] (E/mol)

reaches steady condition the particle size distribution K1 Equilibrium constants of Eq. (8)

and the circulation rate of char will not change. K2 Equilibrium constants of Eq. (9)

(3) The use of coal water slurry as fuel has restricting effects K Equilibrium constants of Eq. (16)

on the performance of the gasifier to be used in IGCC kC – H2O Equilibrium constant [exp(17.64– 16810/T)]

because in this way the water feeding rate becomes Ks Surface rate coefficient (kg/s m2)

proportional to the char feeding rate and cannot be varied Kv Rate constant of char gasification[exp(24.3 –

independently. Accordingly, if the gasifier is operated 25,120/T)] (cm3/mol s)

under steady condition in IGCC its thermal capacity n Number of circulations of char

cannot be modified by only varying the water feeding N_ Total unconverted lime

rate without the change of operating temperature. N_ Feed rate of the char (particle/s)

(4) A large amount of circulating lime CaO in the gasifier N_c Rate of char gasification (atom/s)

makes the removal of H2S from the flue gas relatively N H 2S Rate of the reduction of H2S (atom/s)

easy. The emissions of H2S (0.15 lb of SO2 per million Mp Mass of a single particle [6qpdp3/p] (kg)

Btu) based on the total conversion of H2S to SO2 after P

_i Pre-exponential constant

combustion were found still to be below the allowed Q Gas volume flow rate through the imaginary

SO2 emission levels (1.2 lb per million Btu). surface (m3/s)

r Coordinate in the radial direction

List of symbols R Universal gas constant (cal/mol K)

A Concentration of available lime CaO in the Rep Reynolds number [(Ur Vr)dp/m]

calcined limestone, any units T Temperature (K)

As Surface area of single particle (m2) t Time (s)

Ap Cross-section of char particle (m2) Dt Time interval (s)

B Concentration of inactivated lime CaO covered by Ur Solid particle velocity in the radial direction (m/s)

CaS layers in the calcined limestone, any units Uh Solid particle velocity in the angular direction (m/s)

C Concentration of H2S (gmol/E) Ug Superficial gas velocity (m/s)

Cd Drag coefficient Vr Gas velocity in the radial direction (m/s)

Cf Free site on the surface of char available for Vr2 Gas velocity on the imaginary surface (m/s)

reaction Vh Air tangential entering velocity (m/s)

C(o) Occupied site or activated complex on the surface Vh2 Gas velocity in the angular direction on the

of the char imaginary surface (m/s)

De Diameter of the imaginary cylinder W Number of moles of gas species, char, or lime

dp Diameter of the solid particle (m) (mol) based on 1 mol of carbon in feed CWSF

dpc Cut-off diameter of the cyclone combustor (m) _ (mol)

dpi Diameter of the solid particle after ith circulation W

_c Circulation rate of char (kg/s)

(m) Wf Feeding rate of coal water slurry fuel (kg/s)

d pn Diameter of char particle after n circulations (m) W0 Initial mass of feeding char particle (kg)

dp0 The initial diameter of char (Am) W0 Moles of gas species or lime at the beginning of

Ei Activation energy (Kcal/gmol K) each time interval (mol)

FC Mass fraction of carbon in the CWSF DWgi Gasification of a single char particle in the ith

FD Drag force upon the solid particle in the radial circulation (kg)

direction (N) DWi Total mass reducation of a single char particle in

H Height of the imaginary cylinder (m) the ith circulation (kg)

h Exponential constants of Rankine vortex in Eq. X Converted atoms of in each time interval (mol)

(39) X1 Axial coordinate along the gasifier (m)

k1 Rate constant of Eq. (8) DX1 Traveling distance along the gasifier after a time

k1V Rate constant of Eq. (8) _ interval Dt

k2 Rate constant of Eq. (9) X_ Mole of gas species (mol)

k2V Rate constant of Eq. (9) Xeq Mole of gas species at equilibrium (mole)

k3 Rate constant of Eq. (10) Y Converted atoms of CO in each time interval (mol)

K1 Rate constant of adsorption of CaS on the surface Z Converted atoms of in each time interval (mol)

of available lime (E/gmol s) q Density of flue gas (kg/m3)

H. Tsui, C.-H. Wu / Powder Technology 132 (2003) 167–183 183

qp Density of solid particle (kg/m3) [13] R.J. Dry, I.N. Christensen, C.C. White, Gas – solids contact effi-

ciency in a high-velocity fluidized bed, Powder Technol. 52

m kinetic viscosity of gas

(1987) 243 – 250.

l Viscosity of gas (N s/m2) [14] J.R. Howard, Fluidized Beds Combustion and Applications, Science

c Specific rate of char gasification (l/s) Publish, 1983.

[15] H.H. Lowry, Chemistry of Coal-Utilization—Supplementary Volume,

Wiley, New York, 1963.

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