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journal homepage: www.elsevier.com/locate/ijhmt

titanium dioxide in a rotary kiln

Ashish Agrawal, P.S. Ghoshdastidar ⇑

Department of Mechanical Engineering, Indian Institute of Technology Kanpur, Kanpur, U.P. 208016, India

a r t i c l e i n f o a b s t r a c t

Article history: This paper presents a computational heat transfer model of a rotary kiln used for the production of rutile

Received 24 February 2016 titanium dioxide by the calcination of paste-like hydrous titanium dioxide. The work details the mod-

Received in revised form 4 October 2016 elling of several chemical reactions occurring in the solid bed region along with turbulent convection

Accepted 7 October 2016

of gas, radiation heat exchange among hot gas, refractory wall and the solid surface, and conduction in

the refractory wall. Finite-difference techniques are used and the steady state thermal conditions are

assumed. The kiln is divided into axial segments of equal length. The solution is of marching type and

Keywords:

proceeds from the solid inlet to the solid outlet. The direction of gas flow is opposite to that of the solids.

Heat transfer

Rotary kiln

Mass balance of each species in the solid charge, and mass and energy balances of the solid and gas in an

Rutile titanium dioxide axial segment are used to obtain solids and gas temperatures, and species concentration at the exit of that

Simulation segment. The kiln length predicted by the present model is 45.75 m as compared to 45 m of an actual kiln

reported by Ginsberg and Modigell (2011). The steady-state axial gas and solid temperature profiles have

been also satisfactorily validated with the numerical results of the aforementioned paper. The output

data consist of refractory wall temperature distribution, the axial solids and gas temperature profiles,

axial solids composition profile, the length required for drying of the solid charge and the total kiln length

required to achieve 98% conversion of anatase TiO2 to rutile TiO2. A detailed parametric study with

respect to the controlling parameters such as percent water content (with respect to dry solids), solids

flow rate, gas flow rate, kiln inclination angle and kiln rotational speed lent a good physical insight into

the rutile-TiO2 production process in a rotary kiln.

Ó 2016 Elsevier Ltd. All rights reserved.

1. Introduction chloride process using chlorine gas. The last process step of the sul-

phate method, named calcination is performed in rotary kiln and

This paper presents a computer model of heat transfer during has been considered in the present work.

production of titanium dioxide white pigment in rutile form in a

rotary kiln. 1.2. Description of rotary kiln

1.1. Production of rutile titanium dioxide (TiO2) in a rotary kiln A rotary kiln consists of a refractory lined cylindrical shell

mounted at a slight inclination from the horizontal plane (Fig. 1).

Titanium dioxide is a white solid inorganic substance which is The kiln is rotated at a very low speed about its longitudinal axis

used as a pigment or whitener in paints, paper, plastics, textiles, and the raw charge comprising hydrous titanium dioxide in a

and other products. It occurs in several polymorphs, among them, moist cake form is fed into the upper end of the cylinder and a

anatase and rutile are manufactured in the chemical industry as hot combustion gas mixture at 1 bar flows from the other end.

white pigments. The pigment properties of rutile titanium dioxide The gas is a mixture of products on burning of natural gas in a sep-

are better than that of anatase titanium dioxide and are of more arate combustion chamber.

economical importance. Titanium dioxide white pigments are pro- In the present study, the kiln is considered to comprise three

duced from a variety of ores by two different processes, namely, sections. In the first section, the wet solids are heated to the satu-

the sulphate process using concentrated sulphuric acid and the ration temperature of water. In the second section, the liquid evap-

orates at constant temperature until the charge is completely

⇑ Corresponding author. devoid of moisture. In the third section, the solids are heated till

E-mail address: psg@iitk.ac.in (P.S. Ghoshdastidar). the required degree of conversion of anatase to rutile titanium

http://dx.doi.org/10.1016/j.ijheatmasstransfer.2016.10.024

0017-9310/Ó 2016 Elsevier Ltd. All rights reserved.

264 A. Agrawal, P.S. Ghoshdastidar / International Journal of Heat and Mass Transfer 106 (2017) 263–279

Nomenclature

Ae;k frequency factor for kth reaction (s1) qj net heat transfer for jth surface element in an axial seg-

Acg cross-section area of gas flow in an axial segment (m2) ment (wall or solids), (W)

Ag total surface area exposed to gas in an axial segment qr;z net heat transfer from gas to solids and wall (W)

(m2) R radius of the kiln, Fig. 2

ag gravitational acceleration (9.81 m/s2) Rex Reynolds number based on relative velocity between

Ai elemental area for ith element at inner wall in an axial wall and air outside the kiln

segment (m2) ReDh Reynolds number based on hydraulic diameter Dh

Aj,inner contact area between wall and solids per unit element Ru universal gas constant (8.314 J/mol K)

(m2) T g;z gas temperature at axial position z (K)

Cp specific heat at constant pressure (J/kg K) T j;inner inner wall temperature at jth surface element (K)

D diameter of the kiln (m) T s;z solids temperature at axial position z (K)

Dh hydraulic diameter of gas flow (m) Dt residence time (s)

dm_ k;z depletion rate of the reactant of kth reaction in an axial To,av average temperature at outer wall (K)

segment (kg/s) U circumferential speed of the kiln (m/s)

_ v;z

dm evaporation rate of moisture content in wet solid in vg mean velocity of gas (m/s)

concerned axial segment (kg/s) Vz axial velocity of solids (m/s)

Ea;k activation energy for kth reaction (J/mol) x radial coordinate (m), Fig. 2

Eb blackbody emission per unit area (W/m2) Xk mass fraction of the solid component k

f percentage of moisture content on dry basis in wet so- y circumferential coordinate (m), Fig. 2

lids z axial coordinate (m)

Fgj shape factor between gas and surface element j

Fij shape factor between surface elements i and j (including Greek letters

j = i) a fill angle (deg), Fig. 2

Gr Grashof number arf thermal diffusivity, Eq. (4)

hcgw average convective heat transfer coefficient from gas to b volumetric thermal expansion coefficient (K1)

refractory wall in an axial segment (W/m2 K) C fill angle (radian)

hcj local convective heat transfer coefficient from gas to jth e emissivity

element of solids (W/m2 K) fk;z degree of conversion of kth reaction at axial position z

hfg latent heat of vaporization of water (J/kg) r Stefan–Boltzmann constant (5.67 108 W/m2 K4)

ho convective heat transfer coefficient from outer wall to h as defined in Fig. 2 (deg)

surroundings (W/m2 K) l dynamic viscosity (kg/m-s)

hws contact heat transfer coefficient between wall and solids m kinematic viscosity (m2/s)

(W/m2 K) n Darcy friction factor, used in Gnielinski [35] correlation

Dhi heat of reaction for ith reaction (J/kg) q density (kg/m3)

k thermal Conductivity (W/m K) sg transmissivity of the gas

L length of the kiln (m) Ds time step (s)

L1 length of the first section of the kiln (m) / kiln inclination angle (deg)

L2 length of the second section of the kiln (m)

L3 length of the third section of the kiln (m) Subscripts

m_ g;z gas mass flow rate at axial position z (kg/s) a air

m_ k;z mass flow rate of the kth component of solid charge at

cr chemical reaction

axial position z (kg/s) g gas

m_ s;z solids mass flow rate at axial position z (kg/s) gs gas to solids

Mwk molecular weight of kth component of solids (g/mol)

i element number of the wall or the solid

nk Order of kth reaction j element number of the wall or the solid

N total number of surface elements in an axial segment k number of reaction, also number of component in solid

Nk rotational speed of the kiln (rev/min) charge

Nr number of surface elements exposed to gas in an axial

l liquid

segment O2 oxygen

Ns number of surface elements covered by solid in an axial s solids

segment sh shell or outer wall

NuDh nusselt number based on hydraulic diameter Dh

SO2 sulphur dioxide

Pg wetted perimeter of gas flow in an axial segment (m) rf refractory wall

Pr Prandtl number v vapour

q1;z net heat transfer from gas and exposed wall to solids

w water

(W) ws wall to solids

q2;z net heat transfer from covered wall to solids (W) z at an axial distance z from the solids inlet

qcr;z net heat energy absorbed or released by chemical reac- z + Dz at a distance z + Dz from the solids inlet

tions at axial position z (W)

qgp;z thermal energy associated with the released gaseous

products of chemical reactions (W) Abbreviations

CFD Computational Fluid Dynamics

A. Agrawal, P.S. Ghoshdastidar / International Journal of Heat and Mass Transfer 106 (2017) 263–279 265

form of Arrhenius rate law.

namely, (i) studies related to modelling without chemical reac-

tions; and (ii) studies related to modelling with chemical reactions.

The literature review that follows covers these aspects.

Fig. 1. Simplified schematic diagram of a rutile-TiO2 rotary kiln.

dioxide is achieved and then are released from the kiln. The calci- Sass [1] developed a computer model for heat transfer in a

nation process produces TiO2 pigment with a rutile content of rotary kiln dryer using empirical relationships for radiation heat

around 98%. The lengths of the first, second and third sections of transfer calculations. Kamke and Wilson [2] developed a computer

the kiln are denoted by L1, L2 and L3, respectively. The total length model of a single-pass, rotary drum dryer for drying of wood par-

of the kiln is L which is the sum of three individual lengths. Heat ticles with or without a center-fill flighting section. Cook and

transfer processes in the kiln, the nomenclature of the kiln and Cundy [3] presented an analytical model for the heat transfer pro-

the coordinate system are shown in Fig. 2. cess taking place between the heated wall of a rotating cylinder

and the solid contained in it with an initial moisture content equal

to 2–7% of the mass of the dry solids. Ghoshdastidar and Unni [4]

developed a steady-state heat transfer model of drying and pre-

1.3. Basic solution methodology heating of wet solids in the non-reacting zone of a cement rotary

kiln. Ghoshdastidar et al. [5] have reported simulation results

A model of heat transfer among the gas, refractory wall and based on an improved heat transfer model for a rotary kiln used

solid has been developed. The radiation heat transfer is modelled for drying and preheating of wet iron ore. Ghoshdastidar and Agar-

by dividing the solid surface and the wall into surface elements. wal [6] performed a numerical simulation and optimization study

The turbulent convection heat transfer from the gas to the wall of heat transfer in a rotary kiln used for drying and preheating of

and solid is estimated by a stand-alone CFD model assuming a wood chips with superheated steam. Liu et al. [7] obtained an ana-

non-rotating kiln with stationary solid bed. It is in this part that lytical solution to predict axial solid transport in rotary kilns. Sch-

FLUENT, a commercial software which applies the finite-volume midt and Nikrityuk [8] carried out a 2D numerical simulation of

method is made use of. The local convective heat transfer coeffi- transient temperature distribution by granular mixing in a hori-

cients obtained from the FLUENT simulation are then supplied to zontal rotary kiln. Sonavane and Specht [9] presented a finite-

the main computer program developed in-house. Since the refrac- element method based numerical analysis of heat transfer in the

tory wall is alternately heated and cooled during each revolution, wall of a rotary kiln.

the quasi-steady heat conduction in the wall is present. The energy

equation for the wall is discretized using the finite-difference tech- 1.4.2. Studies related to modelling with chemical reactions

nique. The mass and energy balance equations are solved for the This can further be sub-categorized into two parts, namely, (i)

solid and the gas assuming only axial temperature variation, since production of titanium dioxide; and (ii) production of other

the solid and the gas are well-mixed in the cross-sectional plane of chemicals.

the kiln, giving rise to uniform temperature in the transversal sec-

tion. The ‘‘well-mixed” assumption is valid since the solid bed 1.4.2.1. Production of titanium dioxide. Ginsberg and Modigell [10]

motion is in rolling mode (as the kiln speed is small) and the gas developed a comprehensive one-dimensional dynamic model of a

flow is turbulent. A number of higher order as well as fractional rotary kiln for the production of titanium dioxide white pigment.

Fig. 2. Schematic cross-section of a rotary kiln showing heat transfer processes, the fill-angle and the coordinate system.

266 A. Agrawal, P.S. Ghoshdastidar / International Journal of Heat and Mass Transfer 106 (2017) 263–279

Their numerical predictions matched very well with the measure- 4. To conduct a detailed parametric study with respect to mois-

ment data. Based on heat and mass transfer equations, Dumont ture percent (dry basis), mass flow rate of the solid, mass flow

and Bélanger [11] described a simplified process model for making rate of the gas, kiln inclination angle and kiln rotational speed

of titanium dioxide in a rotary kiln. Roubal et al. [12] developed the in order to get a good physical insight into the manufacturing

Kalman Filter design based on the reduced model of the process in process of rutile titanium dioxide in a rotary kiln.

an attempt to control the titanium dioxide production in a rotary

kiln. In both studies, dehydration and desulphurisation steps were 2. Problem formulation

not considered. Also, Koukkari et al. [13] introduced the RATEMIX

model by combining multicomponent thermodynamics with In this section the reaction processes, modelling of radiation

chemical kinetics and applied in calcination of metatitanic acid and conduction, gas convection, reaction kinetics, and, mass and

to produce rutile titanium dioxide in a rotary drum calciner. energy balances in the solids and gas are presented in detail.

1.4.2.2. Production of other chemicals. Spang [14] developed a 2.1. Reaction Processes Occurring in a Rutile-TiO2 Rotary Kiln

dynamic partial-differential equation model of cement kiln incor-

porating a flame model. Manitius et al. [15] described a mathemat- In the sulphate process, ilmenite or titanium slag as raw mate-

ical model for production of aluminium oxide by calcination of rial is digested with sulphuric acid and results in a solution con-

basic ammonium aluminium sulphate. A steady state mathemati- taining TiOSO4 and FeSO4 . After removing iron and other

cal model of cement kiln was presented by Guruz and Bac [16] impurities by vacuum crystallization from the solution, titanium

using zone method. Watkinson and Brimacombe [17] performed sulphate is hydrolysed to hydrous titanium dioxide. It largely con-

experimental work on pilot-scale rotary kiln for calcination of sists of slurry of TiOðOHÞ2 (metatitanic acid) and a relatively small

limestone with parametric study. Watkinson and Brimacombe amount of TiOSO4 H2 O. This solid charge is then fed into a rotary

[18] observed the effects of enriching the combustion air with oxy- kiln to undergo calcination process and finally, rutile titanium

gen in a rotary lime kiln. Hard and Mu [19] calculated sensitivities dioxide is produced. In addition to moisture evaporation at satura-

of certain process variables on fuel rate and solids throughput in tion temperature, following chemical reactions take place inside

modelling a phosphate nodulizing kiln. A detailed steady-state the rotary kiln as wet solids move from the inlet to the outlet of

heat transfer model of burning of Plexiglas in a rotary kiln was the kiln.

developed by Ghoshdastidar et al. [20]. A 3D steady state model Dehydration of metatitanic acid and TiOSO4 H2 Ooccurs in the

of a rotary calcining kiln was presented by Bui et al. [21] for the range of 100–250 °C [31] (Reactions 1 and 2). Reaction 3 results

petroleum coke. Davis [22] reported a model for magnetite oxida- in loss of sulphur trioxide (which immediately decomposes into

tion during iron ore pellet induration in a rotary kiln. A model was SO2 and O2) from titanyl sulphate at about 650 °C [32] and finally,

developed for iron oxide pelletizing to simulate effects of under phase transformation of anatase to rutile takes place exothermally

bed injection on kiln fuel requirements and magnetite oxidation in the range of 700–950 °C [32] (Reaction 4).

by Davis [23]. Georgallis et al. [24] presented a 3D model for rotary The above mentioned reactions are listed in Table 1a along with

lime kiln which included evolution and combustion of species and their respective heat of reactions, pre-exponential factors, activa-

granular bed motion with calcination reaction. Marias et al. [25] tion energies and orders of reaction. The composition of wet solids

modelled pyrolysis of aluminium waste in a rotary kiln. Mintus at the solid inlet is given in Table 1b.

et al. [26] predicted solid composition and temperature profiles

and fuel requirement based on their one-dimensional cell model 2.2. Radiation exchange among hot gas, refractory wall and the solid

for wet process rotary cement kilns. Mujumdar and Ranade [27] surface

presented a 1D model to analyse key processes occurring in solid

bed of cement kilns. Mujumdar et al. [28] developed Rotary Since the gas temperature is high, thermal radiation plays an

Cement Kiln Simulator by integrating the separate models for important role. The radiation is modelled by dividing the wall into

pre-heater, calciner, rotary kiln and cooler. Flow and transport pro- surface elements as shown in Fig. 3. Each axial segment of the

cesses were modelled in a calciner for cement production by refractory surface is divided into Nr surface elements of equal size.

Fidaros et al. [29]. Shahriari and Tarasiewicz [30] modelled a clin- The solid surface is divided into Ns surface elements. This can be

ker rotary kiln using operating functions concept. considered as a 2-D enclosure since the surface elements are quite

long. The temperature of the solid surface element and the gas are

1.5. Objectives of the present work assumed to be uniform in each axial segment. The wall surface ele-

ments are assumed diffuse and gray. It is to be kept in mind that

The above literature review reveals that only a few models [10– the surface elements exchange radiation only with the surfaces

13] of titanium dioxide rotary kiln are available. The main differ- of the same axial segment which is sufficiently long. Since the

ence between the present and aforementioned ones is that the lat- hot gas contains CO2 and H2O and it is treated as radiatively

ter do not have the capability of predicting the kiln length required participating.

to produce rutileTiO2 for a given set of input parameters. The pre- The radiation heat transfer is computed by using the theory of

sent work is an attempt to fill this gap in the existing literature. Hottel [33] for a gray enclosure containing a gas which emits,

The objectives of the present study are as follows. absorbs and transmits radiation. If the gas volume is enclosed by

N gray surface elements at different temperatures, the net energy

1. To develop a detailed computer model of heat transfer with gain, qj at a particular surface can be expressed as

chemical reactions during the production of rutile titanium " #

dioxide in a rotary kiln; eþ1 X

N

qj ¼ Ag F gj eg Eb;g þ Ai F ij sg Eb;i Eb;j Aj ð1Þ

2 i¼1

the desired solids composition as predicted by the present

model with that of the actual kiln reported in Ginsberg and where e is the emissivity of the wall. Eq. (1) is valid when e is

Modigell [10]; greater than 0.8, which is true in the present case. For the calcula-

3. To predict axial distributions of solid temperature, gas temper- tion of shape factors, F ij expressions derived by Ghoshdastidar

ature, composition of the solid charge within the kiln; et al. [20] have been used. eg and sg are the emissivity and transmis-

A. Agrawal, P.S. Ghoshdastidar / International Journal of Heat and Mass Transfer 106 (2017) 263–279 267

Table 1a

Reactions, kinetics and heat of reaction data (Ginsberg and Modigell [10]).

S. No. Reaction Equation Frequency Factor Activation Energy Heat of Reaction Order of Reaction

Ae;k (s1) Ea;k (kJ/mol) Dhk (kJ/mol) nk

2 TiOSO4 H2 O ! TiOSO4 þ H2 OðgÞ 5.0 105 75 90 0.50

3 TiOSO4 ! TiO2 ðaÞ þ SO2 ðgÞ þ 0:5O2 5.0 109 230 396 0.30

4 TiO2 ðaÞ ! TiO2 ðrÞ 1.7 1023 491 -5.6 0.67

Table 1b

Mass fractions of reactants (Ginsberg and Modigell [10]).

1 TiOðOHÞ2 0.8894

2 TiOSO4 H2 O 0.1106

Fig. 3. Section of the kiln showing surface elements of the wall and the solid.

sivity of the gas. The value of gas emissivity has been taken directly

from Ginsberg and Modigell [10]. The gas transmissivity has been

calculated using the expression,sg ¼ 1 eg , assuming gas reflectiv- Fig. 4. A two-dimensional grid showing triangular elements in a cross-sectional

plane of the TiO2 kiln.

ity to be zero and Kirchhoff’s law of radiation to be valid.

2

In direct fired kilns of small diameter operating at solids tem- n ¼ ð0:79lnðReDh Þ 1:64Þ ð2aÞ

perature up to 1100 K gas convection may be significant (Brima-

Gnielinski correlation is valid for,

combe and Watkinson [34]). In order to bring more precision in

the calculation of connective heat transfer from main heat source 0:5 6 Pr 6 2000 and 3000 6 ReDh 6 5 106

in the rotary kiln, that is hot gas mixture, local convective heat

transfer coefficients on the exposed surfaces of refractory and solid NuDh and ReDh are the Nusselt number and Reynolds number,

bed are estimated a priori, via a secondary model of heat transfer. respectively, based on hydraulic diameter for the gas region, Dh .

In this secondary model, a non-rotating kiln containing a station- Dh is expressed as

ary solid bed is simulated using a finite volume-based commercial 4Acg

CFD package ANSYS-FLUENT 15.0. An unstructured mesh with tri- Dh ¼ ð2bÞ

Pg

angular cross-section prisms as elements is generated using com-

mercial software Gambit 2.4.6. Fig. 4 shows a two-dimensional where Acg and Pg are cross-sectional area and wetted perimeter of

grid constructed via triangular elements in a cross-sectional plane gas flow in an axial segment, respectively.

of the TiO2-kiln.

pD2 C sin C

The length of the kiln used for this simulation is predicted from Acg ¼ 1 þ ð2cÞ

4 2p 2p

the main model. Since local convective heat transfer coefficients

are not known in advance, average values for gas–solids and gas- a

360 a

refractory contact surfaces at each axial location are estimated P g ¼ pD þ D sin ð2dÞ

360 2

using a correlation (Eq. (2)) for Nusselt number developed by

Gnielinski [35] for turbulent flow in a smooth pipe. where C and a are the fill angle of solids in radians and degrees,

respectively.

ðn=8ÞðReDh 1000ÞPr

NuDh ¼ ð2Þ ReDh is expressed as

1 þ 12:7ðn=8Þ1=2 ðPr2=3 1Þ

qg v g Dh 4m_ g

where, n is the Darcy friction factor and for smooth tubes, which is ReDh ¼ ¼ ð2eÞ

lg P g lg

given by

268 A. Agrawal, P.S. Ghoshdastidar / International Journal of Heat and Mass Transfer 106 (2017) 263–279

where qg , v g , lg and m

_ g are the average density, mean velocity, covered by solids exchange heat with solid through surface contact

dynamic viscosity and mass flow rate of gas mixture, respectively. (Helmrich and Schugërl [39]). It may be noted that the sticking of

The average convective heat transfer coefficient from gas to some rutile TiO2 to the inner refractory wall at various axial loca-

refractory wall in an axial segment is given by tions will alter the contact heat transfer coefficient which can only

be obtained from an experiment on a similar kiln. The authors

NuDh kg don’t have any data regarding this aspect available in the published

hcgw ¼ ð2fÞ

Dh literature and hence, an average value of contact heat transfer coef-

where kg is the mean thermal conductivity of the gas mixture. The ficient (377 W/m2 K) for the TiO2 kiln as estimated by Ginsberg and

average convective heat transfer coefficient from gas to solids in an Modigell [10] has been used.

axial segment is assumed to be an order of magnitude higher than The heat transfer coefficient for convection from outer wall to

that from gas to refractory wall [36,37]. surroundings is calculated as (Suryanarayana et al. [38]):

The Reynolds Number based on the hydraulic diameter of gas " ! #0:35

0:11ka Re2x

flow cross-section is found to be 101,672. The standard k-omega ho ¼ þ Gr Pra ð4Þ

turbulence model is implemented. The conjugate heat transfer is

Dsh 2

considered at the interfaces of gas–solids and gas-refractory.

where, Dsh is the outer diameter of the kiln, ka and Pra are the ther-

Thermo-physical properties of gas mixture, refractory wall and

mal conductivity and Prandtl number of the surrounding air respec-

bulk solid are listed in Table 2. At the solid inlet of the kiln the mass

tively, Rex is the Reynolds number based on relative velocity

flow rate and temperature of gas mixture are as given in Table 2. At

between the cylindrical wall and the external air surrounding the

the outer peripheral wall and end walls of the kiln, a mixed bound-

kiln. Gr is the conventional Grashof number characterizing natural

ary condition is specified with a heat transfer coefficient as esti-

convection.

mated using a correlation given by Suryanarayana et al. [38]. The

momentum, turbulent kinetic energy, turbulent dissipation rate pD2sh x

Rex ¼ ð4aÞ

and energy equation are solved with the second order upwind dif- 2ma

ferencing scheme. The convergence criteria selected for the gov-

where, x is the angular velocity of the rotary kiln and ma is the kine-

erning equations are 103 for the continuity, momentum, k and

matic viscosity of surrounding air.and

omega equations, and 106 for the energy equation.

A grid independence test is performed based on average wall ag bðT o;av T a ÞD3sh

Gr ¼ ð4bÞ

function heat transfer coefficients at the interfaces of gas–solids m2a

and gas-refractory. The optimal value of total number of cells used

in the 3D computational domain is 3154424. The computations are where, ag is the gravitational acceleration, b is the volumetric ther-

performed on SONY workstation with core i5 processor and 4 GB mal expansion coefficient, T o;av is the average temperature on outer

memory by using ANSYS-FLUENT 15.0. wall of the kiln and T a is the surrounding temperature outside the

The local convective heat transfer coefficients for each circum- kiln.

ferential element (Fig. 3) in each axial segment are obtained from

the aforesaid simulation. The range of the same is found to be 2.5. Reaction rates

12.16 W/m2K to 21.08 W/m2K. These local values are imported

into the main model (at the same locations in computational For any reaction, the rate of change in degree of conversion of

domain of the main model) as input data and convection heat the reaction is assumed to be governed by kinetic expression (Eq.

transfer from gas to solids and gas to refractory is estimated. (5)), which is a modified form of Arrhenius rate law:

dfk;z Ea;k

2.4. Conduction in the refractory wall ¼ Ae;k exp ð1 fk;z Þnk ð5Þ

dt Ru T s;z

The conduction in the refractory wall is modelled assuming where fk;z denotes the degree of conversion of kth reaction at axial

quasi-steady heat conduction since wall elements of the kiln are position z, Ru is the universal gas constant, T s;z is the mean solids

alternately heated and cooled during each revolution by gas and temperature at axial position z, Ae;k , Ea;k , nk are the frequency factor,

solid, respectively. Only radial heat conduction in the wall is taken activation energy and order of kth reaction, respectively. The values

into account, assuming negligible conduction in the circumferen- of Ae;k , Ea;k and nk are provided in Table 1a.

tial and axial direction as the kiln dimensions are much larger in The degree of conversion, fk;z is defined as

those directions. A non-rotating coordinate system is used to _ k;0 m

m _ k;z

model the wall conduction equation (Eq. (4)). Because the refrac- fk;z ¼ ð6Þ

_ k;0 m

m _ k;f

tory thickness (0.25 m) is appreciably smaller than kiln diameter

(2.3 m), the ratio being about 10.9%, the effect of curvature is

neglected and hence, Cartesian coordinates are used instead of

cylindrical coordinates for the sake of simplicity.

@T @2T

U ¼ arf 2 ð3Þ Table 1c

@y @x Molecular masses of various components in solid charge.

where U is the circumferential speed of the wall and arf is the ther- S. No. Component Molecular weight

k Mw (g/mol)

mal diffusivity of the wall.

The boundary condition for the inner wall depends on whether 1 TiOðOHÞ2 97.88

2 TiOSO4 H2 O 177.94

the surface element is exposed to the gas or it is covered by solids.

3 TiOSO4 159.93

The radiation heat transfer, qj from the gas to the inner surface ele- 4 TiO2 ðaÞ 79.87

ments is obtained from Eq. (1). In addition, convection heat trans- 5 TiO2 ðrÞ 79.87

fer is calculated from the local convective heat transfer coefficients 6 H2 OðlÞ 18.02

7 H2 OðgÞ 18.02

as discussed in Section 2.3. Surface elements of the kiln that are

A. Agrawal, P.S. Ghoshdastidar / International Journal of Heat and Mass Transfer 106 (2017) 263–279 269

where m _ k;0 and m _ k;f are the initial and final mass flow rates of the ichiometry of reactions 1, 3 and 4, its new mass flow rate at exit

reactant of kth reaction respectively, m _ k;z is its mass flow rate at of this axial segment is given as,

any axial position z.

Mw4 Mw4

With the help of degrees of conversion of the reaction at any _ 4;z exit ¼ ½m

½m _ 4;z entry dm

_ 4;z þ _ 1;z þ

dm _ 3;z

dm ð10Þ

Mw1 Mw3

axial segment, using Eq. (6), the amount of depletion per second

for different species of solid charge ðdm _ k;z ) are estimated. Using where ½m_ 4;z entry is the mass flow rate of TiO2 ðaÞ at entry of axial seg-

this information, based on stoichiometry of the chemical reactions, ment and dm _ 4;z is the decomposed amount during this reaction in

updated mass flow rates of solid species (that is, the mass flow that axial segment. Mw4 is the molecular weight of TiO2 ðaÞ.

rates at the exit of that axial segment, m _ k;z ) are estimated. Mass flow rate of TiO2 ðrÞ, as it is generated from reaction 4, is

Table 1c lists the components in solid charge with corresponding updated as well in a similar way,

index k and their respective molecular weights.

_ 5;z exit ¼ ½m

½m _ 5;z entry þ dm

_ 4;z ð11Þ

_ k;z entry and ½m

If ½m _ k;z exit are the mass flow rates of kth species at

the entry and exit of axial segment ‘z’ and dm _ k;z is the amount of _ 5;z entry and ½m

where, ½m _ 5;z exit are the mass flow rates of TiO2 ðrÞ at

depletion per second of reactant in kth reaction in that segment, entry and exit of that axial segment.

then using molecular masses Mwk , following expressions are Mass flow rate of water vapour that is released as gaseous pro-

obtained for updated mass flow rates at the exit of the segment. duct from reaction 1 and 2, is tracked at each axial segment before

Eqs. (7)–(12) show the expressions for updated mass flow rates it is mixed into hot gas mixture. Again based on stoichiometry of

of solid components in each axial segment and are written based reactions 1 and 2, amount decomposed per second in segment is

on the stoichiometry of the chemical reactions. estimated as,

Reaction 1:

Mw7 Mw7

_ 7;z ¼

dm _ 1;z þ

dm _ 2;z

dm ð12Þ

TiOðOHÞ2 ! TiO2 ðaÞ þ H2 OðgÞ Mw1 Mw2

In reaction 1, reactant TiOðOHÞ2 or metatitanic acid is thermally Here, Mw7 is the molecular weight of water.

decomposed into TiO2 (a) and water vapour. TiOðOHÞ2 is denoted From the knowledge of enthalpies of reactions, heat generation

by index 1, as shown in table. Updated mass flow rate of this com- due to chemical reactions in an axial segment can be estimated and

pound at exit of axial segment is given by following expression. expressed as:

_ 1;z exit ¼ ½m

½m _ 1;z entry dm

_ 1;z ð7Þ _ 1;z Dh1 þ dm

qcr;z ¼ dm _ 2;z Dh2 þ dm

_ 3;z Dh3 þ dm

_ 4;z Dh4 ð13Þ

where ½m_ 1;z entry is the mass flow rate of TiOðOHÞ2 at entry to the where, Dh1 , Dh2 , Dh3 and Dh4 are the heat of reactions for Reactions

segment and dm _ 1;z is the amount of depletion of TiOðOHÞ2 per sec- 1 to 4 and are given in Table 1a.

ond in that segment.

Reaction 2: 2.6. Mass and energy balances in solids and gas

Similarly, in reaction 2, reactant TiOSO4 H2 O is decomposed into three sections. In the first section, wet solid charge is heated to

TiOSO4 and water vapour. TiOSO4 H2 O is denoted by index 2, as the saturation temperature of the entrained liquid. In the second

shown in table. Its new mass flow rate at exit of axial segment is section, liquid evaporates at constant temperature and in the third

given by following expression. section dry solid charge is heated till the required conversion of

anatase TiO2 to rutile TiO2 is achieved.

_ 2;z exit ¼ ½m

½m _ 2;z entry dm

_ 2;z ð8Þ The mass and energy balance of the solid in each segment either

in first and third segment gives the expression for exit solid tem-

where ½m_ 2;z entry is the mass flow rate of TiOSO4 H2 O at entry to seg-

perature of that segment, T s;zþDz for that section while the same

ment and dm _ 2;z is its decomposed amount per second during that performed on an axial segment in second section of the kiln gives

axial segment. _ v;z . The end of the sec-

the expression for the rate of evaporation, dm

Reaction 3: ond section is indicated where the cumulative m _ v is equal to the

TiOSO4 ! TiO2 ðaÞ þ SO2 ðgÞ þ 0:5O2 predetermined amount of water to be evaporated per second. Sim-

ilarly, mass and energy balance of hot gas contained in an axial

TiOSO4 is a product of reaction 3 and is used as a reactant in reac- segment in any of the three sections of the kiln gives the expres-

tion 3. TiOSO4 is denoted by index 3, as shown in table. Based on sion for T g;zþDz for that section.

stoichiometry of both reactions, following expression can be writ-

ten for updated mass flow rate of TiOSO4 at exit to that axial 2.6.1. Mass balance in Sections I and III

segment. In solids region (Fig. 5),

Mw3 m _ s;z dm

_ s;zþDz ¼ m _ g;z ð14Þ

_ 3;z exit ¼ ½m

½m _ 3;z entry dm

_ 3;z þ _ 2;z

dm ð9Þ

Mw2

_ 3;z entry is the mass flow rate of TiOSO4 at entry to axial seg-

where ½m

ment and dm _ 3;z denotes the amount depleted per second in that

segment. Mw2 and Mw3 are the molecular weights of TiOSO4 H2 O

and TiOSO4 respectively.

Reaction 4:

TiO2 ðaÞ ! TiO2 ðrÞ

TiO2 ðaÞ is produced from reactions 1 and 3. It is consumed in reac-

tion 4, where it is converted into final product that is TiO2 ðrÞ.

TiO2 ðaÞ is denoted by index 4, as shown in table. According to sto- Fig. 5. Mass balance of any axial segment in first and third sections of the kiln.

270 A. Agrawal, P.S. Ghoshdastidar / International Journal of Heat and Mass Transfer 106 (2017) 263–279

_ s;zþDz are the mass flow rates of the solids at any Dz

Dt ¼ ð23Þ

axial position z and z + Dz respectively. dm _ g;z is the total amount Vz

of released gaseous products from chemical reactions in an axial

where V z is the axial velocity of the solids. Note that V z ¼ U tan /.

segment.

For derivation of this expression see Ghoshdastidar and Agarwal [6].

_ g:z ¼ dm

dm _ H2 OðgÞ;z þ dm

_ SO2 ðgÞ;z þ dm

_ O2 ðgÞ;z ð15Þ So,

Here, dm _ H2 OðgÞ;z , dm

_ SO2 ðgÞ;z and dm

_ O2 ðgÞ;z are the amounts of H2 OðgÞ, X

Ns X

Ns

q1;z ¼ qj þ hcj Aj ðT g;z T s;z Þ ð24Þ

SO2 ðgÞ and O2 ðgÞ releasing from chemical reactions in solids in that

j¼1 j¼1

axial segment.

In gas region (Fig. 5), where qj is the total radiation heat transfer to the jth element of

m _ g;z dm

_ g;zþDz ¼ m _ g;z ð16Þ solid.

_ g;z and m

_ g;zþDz are the mass flow rates of the gas at any axial X

Ns

where m q2;z ¼ hws Aj;inner ðT j;inner T s;z Þ ð25Þ

position z and z + Dz respectively. and, j¼1

_ w;s ¼ m

m _ w;g ð17Þ _ H2 OðgÞ;z cp;v þ dm

qgp ¼ T s;z ðdm _ SO2 ðgÞ;z cp;SO2 þ dm

_ O2 ðgÞ;z cp;O2 Þ ð26Þ

where m _ w;g is the mass flow rate of evaporated moisture content in In gas region (Fig. 7),

first section, that is accumulated in gas from the second section of

_ g;z cp;g þ m

T g;z ðm _ w;g cp;v Þ þ qr;z qgp;z

the kiln. T g;zþDz ¼ ð27Þ

m_ g;zþDz cp;g þ m _ w;g cp;v

2.6.2. Mass balance in Section II where qr;z is the total heat transfer from gas to solids and wall. cp;g is

In solids region (Fig. 6), the specific heat of gas at constant pressure.

m _ s;z dm

_ s;zþDz ¼ m _ g;z ð18Þ

2.6.4. Energy balance in Section II

and,

In solids region (Fig. 8),

m _ w;s;z dm

_ w;s;zþDz ¼ m _ v;z ð19Þ q1;z þ q2;z qgp;z qcr;z

_ v;z ¼

dm ð28Þ

where, m_ w;s;z is the mass flow rate of moisture content in wet solids hfg

in second section of the kiln at any axial position z.

where, dm _ v;z is the evaporation rate of moisture content in dry solid

In gas region (Fig. 6),

in concerned axial segment and hfg is the latent heat of vaporization

m _ g;z dm

_ g;zþDz ¼ m _ g;z ð20Þ of water in J/kg.

For this section,

and,

_ w;g;zþDz ¼ m

m _ v;z

_ w;g;z dm ð21Þ T s;zþDz ¼ T s;z ¼ 373 K

¼ Saturation temperature of water at 1 bar

where m_ w;g;z is the mass flow rate of evaporated moisture content

present in gas in second section of the kiln at any axial position z. In gas region (Fig. 9),

_ g;z cp;g þ m

T g;z ðm _ w;g;z cp;v Þ T s;z dm

_ v;z cp;v þ qr;z qgp;z

2.6.3. Energy balance in Section I T g;zþDz ¼ ð29Þ

In solids region (Fig. 7), _ g;zþDz cp;g þ m

m _ w;g;zþDz cp;v

_ s;z cp;s þ m

T s;z ðm _ w;s cp;l Þ þ q1;z þ q2;z qgp;z qcr;z

T s;zþDz ¼ ð22Þ 2.6.5. Energy balance in Section III

_ s;zþDz cp;s þ m

m _ w;s cp;l

In solids region (Fig. 10),

where, m _ w;s is the mass flow rate of moisture content present in wet

_ s;z C p;s þ q1;z þ q2;z qgp;z qcr;z

T s;z m

solids in first section of the kiln. It remains same throughout the T s;zþDz ¼ ð30Þ

section. cps and cpl refer to specific heats (at constant pressure) for _ s;zþDz cp;s

m

dry solids and moisture content respectively. Also, q1;z is the heat In gas region (Fig. 10),

transfer to the solids from gas and exposed surface elements of

the kiln through convection and radiation, q2;z is the heat trans- _ g;z cp;g þ qr;z qgp;z

T g;z m

T g;zþDz ¼ ð31Þ

ferred to the solid through surface elements of kiln in direct contact m _ g;zþDz cpg

with solids, qgp;z is the thermal energy associated with the released

gaseous products of chemical reactions and qcr;z is the heat gener-

3. Overall method of solution

ated by the chemical reactions in Dz distance or Dt time, where

Dt is computed from

A computer program in FORTRAN 95 was developed to obtain

the numerical results for the present problem. The input data

required for the program are shown in Table 2. The specific heat

of the dry solids is calculated by using Eq. (34) from the specific

heat of individual components listed in Table 1c.

X

5

C p;s ¼ X k C p;k ð32Þ

k¼1

where X k and C p;k are the mass fraction and specific heat of compo-

nent k respectively. k = 1 to 5 correspond to TiOðOHÞ2 , TiOSO4 H2 O,

Fig. 6. Mass balance of any axial segment in second section of the kiln. TiOSO4 , TiO2 ðaÞ and TiO2 ðrÞ respectively.

A. Agrawal, P.S. Ghoshdastidar / International Journal of Heat and Mass Transfer 106 (2017) 263–279 271

Fig. 7. Energy balance of any axial segment in first section of the kiln.

the new composition of the solids at the inlet of the second seg-

ment is determined, the new cross-sectional area of the solids

and the new fill-angle are estimated and hence, new shape factors

are computed. The solids and gas temperature, and species compo-

sition at the exit of the second segment can be calculated in the

same way as described earlier. The solution then proceeds by the

analysis of each succeeding segment. The process is continued till

the end of the kiln. The end of the kiln is indicated by the position

where the degree of conversion for the last reaction, that is, ana-

Fig. 8. Energy balance for solids in any axial segment in second section of the kiln. tase to rutile titanium dioxide conversion has reached 98%. Thus

the kiln length can be computed.

A time step of Ds = 0.1 s is used for calculations. Since the initial

A mixture density relation is used to calculate the effective den- temperature distribution of the refractory wall is not known, an

sity of wet solids from the densities of the components as given in arbitrary temperature is assumed at all grid points in the refractory

Table 1d. wall. The solution converges where there is no further change in

the temperature at each grid point as s ? 1. This temperature dis-

qs;dry solids þ 100

f

ql

qs ¼ ð33Þ tribution represents the steady state temperature distribution of

1 þ 100

f

the wall.

where f is the percent of moisture content with respect to dry Grid independence tests have been performed to obtain the

solids, ql is the density of liquid water and qs;dry solids is the density optimum grid spacing values in the circumferential and radial

directions. The number of grid points used in the circumferential

of dry solids.

direction is 150 and that in the radial direction is 61. In addition,

1 sensitivity analysis for axial segment length, Dz with respect to

qs;dry solids ¼ ð34Þ

X

5 predicted kiln length is also performed. It is found that the pre-

X k =qs;k dicted kiln length and hence axial solid and gas temperature distri-

k¼1

butions remain more or less unchanged while Dz is changed from

where qs;k is the density of the component k in solid charge. 0.10 to 0.25 m. The largest value of Dz in this range is taken in

The solution is initiated at the solids entrance of the kiln and order to save CPU time. Therefore, Dz used in this study is 0.25 m.

proceeds to the outlet. In an axial segment, the gas and solids tem- The simulations are performed on a high performance comput-

perature being known, the steady state refractory wall tempera- ing system (having Terra-flops rating). The CPU time required for a

ture distribution is calculated by solving Eq. (3) through the False simulation with the input data (Table 2) is approximately 46.43 h.

Transient Approach. The solid temperature and mass flow rate The output data consist of refractory wall temperature, solids tem-

are known at the inlet. Similarly, gas temperature and gas mass perature, gas temperature, solids composition, individual lengths

flow rate are known at the solid inlet (which is actually the exit of first, second and third sections of the kiln (L1, L2, L3), and the

for the gas since the gas is flowing countercurrent to the solid total kiln length (L). The capability of this model to predict the kiln

flow). Thus, the energy balance equations (see Section 2.6) are length is unique and has not been found in earlier TiO2-kiln mod-

solved for the first segment, and solid composition, solids, and els. The overall solution algorithm is described next in a step-by-

gas temperature are obtained at the exit of the first section. Once step fashion.

Fig. 9. Energy balance for gas in any axial segment in second section of the kiln.

272 A. Agrawal, P.S. Ghoshdastidar / International Journal of Heat and Mass Transfer 106 (2017) 263–279

Fig. 10. Energy balance of any axial segment in second section of the kiln.

Material properties of the solid components (Ginsberg and Modigell [10]).

1. Input the data for various kiln geometrical, flow, thermo-

S.No. Component Density (kg/m3) Specific heat (J/mol K)

physical and chemical kinetics parameters.

2. Input the solids composition, solids temperature and gas 1 TiOðOHÞ2 2540 142

2 TiOSO4 H2 O 2430 208

temperature at solids inlet.

3 TiOSO4 2890 133

3. Set m =1 for the first axial segment. 4 TiO2 ðaÞ 3900 70

4. Calculation of solid fill angle in the segment. 5 TiO2 ðrÞ 4240 70

5. Shape factor calculations for radiative heat echange among 6 H2 OðlÞ 1000 76

gas, wall and solid bed.

6. Calculation of heat transfer by convection from Eq. (2) and

radiation from Eq. (1). Table 2

7. Estimation of refractory wall temperature distribution by Input data to the program (Ginsberg and Modigell [10]).

solving energy equation by false transient method using 1. Rotary Kiln

explicit finite-difference scheme. (a) Diameter (inner) 2.3 m

8. Calculation of total heat transfer (convection + radiation) (b) Refractory

from gas and to solids in that segment. (i) Thickness 0.25 m

(ii) Thermal Conductivity 1.6 W/m K

9. Calculation of mass flow rates of solid species at the exit of (iii) Specific heat 950 J/kg K

that segment using modified Arrhenius equation for each (iv) Density 2310 kg/m3

reaction. (v) Emissivity 0.8

10. Calculation of thermal energy absorbed or released in that (c) Rotational speed 0.33 rpm

(d) Angle of inclination 2.29°

segment due to chemical reactions in the solid bed.

2. Solid

11. Calculation of the temperatures of solids and gas at the (a) Inlet temperature 308 K

exit of that segment using global mass and energy balances (b) Mass flow rate (dry) 1.309 kg/s

for solids and gas, respectively. (c) Percent water (on dry basis) 75.14

12. Update the gas and solids flow rates at the exit of the (d) Emissivity 0.8

3. Gas

segment. (a) Outlet temperature 648 K

13. Check whether degree of conversion of final reaction (i.e., (b) Specific heat 1356 J/kg K

that is conversion of anatase titanium dioxide to rutile (c) Mass flow rate 6.218 kg/s

titanium dioxide) has reached 98%. If it has reached this (d) Emissivity 0.422

(e) Dynamic viscosity 3.58 105 kg/m-s

value, print the total kiln length, wall temperatures and

4. Water Vapor

axial distributions of solids composition, solids (a) Latent heat of vaporization$ 2.258 106 J/kg

temperature and gas temperature. (b) Specific heat $ 2042.71 J/kg K

14. If it has not reached, then proceed to next axial segment, 5. Specific heat of sulfur dioxide$ 627.99 J/kgK

m=m+1, and repeat the procedure from steps 4 to 13. 6. Specific heat of oxygen$ 919.83 J/kgK

7. Contact heat transfer coefficient 377 W/m2K

15. Grid independence test in two-dimensional refractory 8. Ambient temperature outside the kiln 287.15 K

zone and sensitivity analysis for axial segment length with

$

respect to predicted kiln length are performed. Chase [40].

secondary model in ANSYS-FLUENT (as discussed in

Section 2.3).

17. From the secondary model, local convective heat transfer 4. Results and discussion

coefficients from gas to wall and solids are obtained and are

imported back to the main model at the same physical This section firstly presents comparison of the results with that

locations. of an earlier work. Following that, results of the parametric study

18. Same procedure consisting of steps 1 to 14 are repeated in are shown to see the effect of variation in moisture content (dry

this modified model and final output is received in terms of basis), dry solids mass flow rate, gas mass flow rate, rotational

total kiln length, wall temperatures and axial distributions speed of the kiln, and angle of inclination of the kiln on the axial

of solids composition, solids temperature and gas solid and gas temperature distributions, axial profiles of percent

temperature. conversion of anatase TiO2 to rutile TiO2 as well as on the predicted

length of the kiln and the rate of production of rutile TiO2.

A. Agrawal, P.S. Ghoshdastidar / International Journal of Heat and Mass Transfer 106 (2017) 263–279 273

4.1. Validation of Results with the Numerical Results of Ginsberg and after towards solid outlet similar to that predicted by the present

Modigell [10] computer model.

The kiln length predicted by present model turns out to be 4.2. Axial composition profile of the solid charge

45.75 m as compared to the actual kiln length of 45 m reported

in Ginsberg and Modigell [10]. The predicted kiln length is only Fig. 12 shows axial composition distribution moisture content,

1.67% larger than the actual kiln, indicating an excellent match. reactants and the final product. The graph clearly shows the pre-

Fig. 11 illustrates the comparison of the present axial solid and sent model has been able to simulate the chemical reactions prop-

gas temperature profiles with those computationally obtained by erly. The thermal decomposition of TiOðOHÞ2 and TiOSO4 H2 O

Ginsberg and Modigell [10]. It may be noted that no steady-state (that is, Reactions 1 and 2 as shown in Table 1a) starts close to

experimental data are found in Ginsberg and Modigell [10]. It the kiln entrance. In the first section of the kiln, Reaction 1 pro-

can be seen from Fig. 11 that general trends of both the profiles ceeds at much faster rate than Reaction 2. It starts slowing down

show a good agreement with Ginsberg and Modigell [10]. In the at the beginning of the second section of the kiln and remains slow

first section of the kiln, solid temperature increases slowly to the till any moisture is left in solid charge. This is because of the fact

saturation temperature of the wet solids and it takes about 37% that solid temperature remains constant within second section.

of the kiln length. At this point, the second section begins and In the third section, due to increase in solid temperature, Reaction

evaporation of water takes place. The temperature remains con- 1 speeds up for a while and then remains slow and steady. Reaction

stant at the saturation point. The second section covers about 2 also progresses rapidly in the third section. The production of

47% of the kiln length and is the largest among all the three sec- titanyl sulfate from this reaction and increasing solid temperature

tions. The length of this section largely depends on the amount lead to commencement of Reaction 3 where the desulphurization

of moisture present in the wet solids. Right from the beginning produces TiO2(a) and SO3. The SO3 that is released is immediately

of the third section, temperature increases at a higher rate due to decomposed into SO2 and 0.5O2. This reaction is over at 954 K.

large heat transfer from hotter gas and wall in that region. From Before completion of Reactions 3 and 1 (Table 1a), final reaction

about 92% to 98% of the kiln length, there is decay in @T @z

s

. It is caused of phase transformation of anatase TiO2 to rutile TiO2 (Reaction

by higher energy requirement of third reaction, where decomposi- 4) initiates very slowly and exothermally at around 910 K. Due to

tion of titanyl sulfate occurs. The temperature increases thereafter the facts that, more TiO2(a) is being produced by both reactions

till the final reaction, that is, the phase transition of TiO2 (a) to TiO2 1 and 3 and it is an exothermal reaction in nature, the production

(r) is completed. The final reaction is exothermic in nature and of rutile TiO2 occurs at a very fast rate in the last section of the kiln.

hence, unlike other reactions, it releases thermal energy to gas

region. Completion of this reaction also marks the end of the third 4.3. Parametric study

section of the kiln length. The predicted temperature profiles also

qualitatively agree with Dumont and Bélanger [11] which shows In this section, the effect of various parameters on the predicted

that pre-heating and moisture evaporation take place in nearly length of the kiln, rutile TiO2 production rate, axial solid and

70% of the kiln length and solid temperature rapidly rises there- gas temperature distributions, and axial variation in solids

Fig. 11. Axial solid and gas temperature distributions: Comparison with the numerical solution of Ginsberg and Modigell [10].

274 A. Agrawal, P.S. Ghoshdastidar / International Journal of Heat and Mass Transfer 106 (2017) 263–279

Table 3a

Predicted Kiln Length and Rutile TiO2 Production Rate vs. Moisture Percent (Dry Basis).

Moisture Percent (Dry Basis) L1 (m) L2 (m) L3 (m) L = L1 + L2 + L3 (m) Rutile TiO2 Production Rate (kg/hr)

60.0 17.0 18.5 9.75 45.25 3649.68

75.14 17.25 21.0 7.5 45.75 3648.24

90.0 17.75 23.0 6.0 46.75 3646.80

Table 3b

Predicted Kiln Length and Rutile TiO2 Production Rate vs. Dry Solids Mass Flow Rate.

Dry Solids Mass Flow Rate (kg/s) L1 (m) L2 (m) L3 (m) L = L1 + L2 + L3 (m) Rutile TiO2 Production Rate (kg/hr)

1.0 14.25 19.75 9.75 43.75 2789.28

1.31 17.25 21.0 7.5 45.75 3648.24

1.6 20.0 21.75 6.25 48.0 4458.96

Table 3c

Predicted Kiln Length and Rutile TiO2 Production Rate vs. Gas Mass Flow Rate.

Gas Mass Flow Rate (kg/s) L1 (m) L2 (m) L3 (m) L = L1 + L2 + L3 (m) Rutile TiO2 Production Rate (kg/hr)

4.0 17.0 15.75 3.25 36.0 3641.76

6.218 17.25 21.0 7.5 45.75 3648.24

8.0 17.0 23.75 12.25 53.0 3651.12

Table 3d

Predicted Kiln Length and Rutile TiO2 Productiion Rate vs. Kiln Inclination Angle.

Inclination Angle (deg) L1 (m) L2 (m) L3 (m) L = L1 + L2 + L3 (m) Rutile TiO2 Production Rate (kg/hr)

1.4 16.25 20.0 7.75 44.0 3651.12

2.29 17.25 21.0 7.5 45.75 3648.24

5.0 18.75 23.25 7.5 49.5 3642.48

A. Agrawal, P.S. Ghoshdastidar / International Journal of Heat and Mass Transfer 106 (2017) 263–279 275

Table 3e

Predicted Kiln Length and Rutile TiO2 Production Rate vs. Kiln Rotational Speed.

Rotational Speed (r.p.m) L1 (m) L2 (m) L3 (m) L = L1 + L2 + L3 (m) Rutile TiO2 Production Rate (kg/hr)

0.21 16.5 20.5 8.25 45.25 3651.12

0.33 17.25 21.0 7.5 45.75 3648.24

1.0 18.25 22.25 7.25 47.75 3639.24

composition is discussed. In Tables 3a–3e, predicted kiln length the kiln. Table 3a shows that with the increase in moisture percent

values and rutile TiO2 production rates for various parameters from 60 to 90 the rate of production of rutile Titanium dioxide

are shown and the base values (Table 2) are highlighted in bold decreases slightly from 3649.68 to 3646.8 kg/hr. This is because

letters. of higher kiln length required for drying in the case of larger water

content in the solids. On the other hand, as dry solids mass flow

4.3.1. Predicted kiln length as a function of various parameters rate increases from 1 kg/s to 1.6 kg/s the production rate substan-

Table 3a reveals that, as the moisture percentage is increased tially rises from 2789.28 kg/hr to 4458.96 kg/hr (Table 3b). This is

from 60 to 90, the lengths of the first and second sections of the because of higher amount of solid charge being processed and fas-

kiln increase. This is because of the fact that more amount of mois- ter rate of final reaction per unit time. Table 3c indicates higher gas

ture will require large amount of heat to reach the saturated state flow rate results in larger production of rutile TiO2 per unit time.

and then to get vapourized. Therefore, lengths of the both sections This is because solid temperature is slightly higher in the third seg-

will be higher for this case. This rise in length of the second section ment of the kiln which accelerates the rate of reaction. Increasing

also causes delay in completion of Reaction 1 and 2 as they speed kiln inclination angle and kiln rotational speed reduces the rutile

up only after evaporation is finished. On the contrary, the length of titanium dioxide production rate (Tables 3d and 3e) since the kiln

the third section decreases on increasing water content. This can has to be longer and hence the solids residence time in the kiln is

be explained as follows. Though it takes longer for water to get more.

vaporized, the fill-angle of the kiln and amount of dry solid mass

available in third section remains same and it has to meet the same 4.3.3. Axial solid and gas temperature distribution as a function of

requirement of phase transformation in chemical reactions. Now, various parameters

total heat transfer to the solids in last section for the solid with Fig. 13 shows that, with the increase in moisture content in wet

higher water content will be greater than that for solid with lower solids, axial gas temperature and @T s

increase in third section of the

@z

water content. This is because of exposure of the dry solid to the kiln while axial solid temperature with respect to percentage kiln

hotter gas in the former case as heating starts at a longer distance length decreases. The explanation of this trend is as follows. For

from the solid inlet. The combined effect on total length is that it is a larger amount of water in the solid charge, the wet solid will have

greater for higher moisture content case. Table 3b reveals that as to travel a longer distance to be totally moisture-free. This implies

dry solids mass flow rate increases from 1.0 kg/s to 1.6 kg/s, pre- that the same amount of dry mass of solid will have to be heated to

dicted kiln length increases from 43.75 m to 48.0 m. This is the same exit temperature. It may be noted that the fill angle

because higher solids residence time is needed to achieve the remains the same in the third section no matter what the original

desire objective and hence more kiln length is needed. Here, mois- moisture content is. So, the dry solid will be exposed to hotter gas

ture percentage remains same but amount of moisture present in in the case of high moisture content as the heating starts close to

wet solids increases which raises the length of the second section. the kiln exit which is the inlet for the hot gas. Therefore, to reach

However, the length of the third section decreases due to higher the requisite exit temperature, the dry solid will have to travel a

heat transfer from gas and wall to solids. The overall effect is that smaller percentage length of the kiln and hence the axial temper-

the predicted kiln length increases. As gas flow rate at inlet ature gradient of the solid is larger. The axial solid temperature at

increases from 4 kg/s to 8 kg/s, total kiln length increases from the same percentage kiln length will be obviously lower. Fig. 14

36.0 m to 53.0 m (Table 3c). Near solids inlet, in spite of lower depicts that, for higher solid mass flow rate, gas temperature is

gas residence time at higher gas flow rate, there is enough heat considerably higher in the third section of the kiln. This is because

transfer to the material to reach the boiling point of water in for larger solid mass flow rate, the fill angle increases resulting in

almost same distance as in lower gas flow rate cases. However, reduction in the mean beam length as the gas volume decreases.

at latter stages of second section, effects of higher gas flow rate Hence, the loss of heat by the gas by radiation is smaller and hence

are evident on processing of solid charge, as lower gas temperature the gas temperature is high. Fig. 15 indicates that increasing gas

at the same axial location results in less heat transfer to solids, and flow rate causes significant drop in gas inlet temperature. The rea-

lengths of second and third section increase significantly. Table 3d son is that higher gas flow rate means less gas residence time and

reveals that as the kiln inclination angle changes from 1.4° to 5°, hence the kiln has to be longer (see Table 3c). Thus, solid temper-

predicted kiln length increases from 44 m to 49.5 m. This is ature is higher at the same percent kiln length in the third segment

expected because, as inclination angle increases, axial velocity of of the kiln. Gas on the other hand loses more heat to the solid and

solid also increases as V z ¼ U tan / a nd hence the residence time hence the gas temperature drops in the last section of the kiln for

of the solid is less. Hence, to reach the same composition of solids higher gas flow rates. Finally, lower kiln inclination angle and

at the exit, greater kiln length is needed. At higher rotational speed lower rotational speed result in lower gas temperature and higher

of the kiln, the axial velocity of the solid increases and therefore, solid temperature at the same percent kiln length in the third sec-

the solid particles are exposed to gas for less amount of time. This tion of the kiln (graphs not shown). This is because of more resi-

results in slower progression of reactions and therefore, to obtain dence time of the solids in the kiln which leads to shorter kiln

same solids chemical state of the product, length of the kiln has length.

to be increased (Table 3e). Finally, lower kiln inclination angle and lower rotational speed

result in lower gas temperature and higher solid temperature at

4.3.2. Rutile TiO2 production rate as a function of various parameters the same percent kiln length in the third section of the kiln (graphs

The rate of production of rutile TiO2 is calculated by dividing the not shown). This is because of more residence time of the solids in

mass of rutile TiO2 produced, by the residence time of the solids in the kiln which leads to shorter kiln length.

276 A. Agrawal, P.S. Ghoshdastidar / International Journal of Heat and Mass Transfer 106 (2017) 263–279

Fig. 13. Axial solid and gas temperature distributions for different moisture percentages (dry basis).

Fig. 14. Axial solid and gas temperature distributions for different mass flow rates of the dry solids.

4.3.4. Axial composition of solid charge as a function of various section of the kiln. As the third section comes latter for higher

parameters moisture content case, these reactions along with the

Fig. 16 shows the effect of moisture content on the percent con- decomposition of TiO.SO4 to TiO2 (a) and final reaction of

version of Anatase TiO2. It is revealed that both Reactions 1 and 2 conversion occur later and relatively faster due to higher gas

(Table 1a) progress faster as solids enter the third and the last temperature.

A. Agrawal, P.S. Ghoshdastidar / International Journal of Heat and Mass Transfer 106 (2017) 263–279 277

Fig. 15. Axial solid and gas temperature distributions for different mass flow rates of the gas.

Fig. 16. Axial profiles of percent conversion of anatase TiO2 to rutile TiO2 for different moisture percentages (dry basis).

Fig. 17 depicts how solids mass flow affects the percent conver- and second sections because of larger solid mass flow rate and also

sion of anatase TiO2. At higher dry solids mass flow rates Reaction 3 larger amount of moisture to be evaporated per unit time. How-

and the final reaction are delayed due to requirement of longer first ever, at the same percent kiln length near the exit reactions occur

278 A. Agrawal, P.S. Ghoshdastidar / International Journal of Heat and Mass Transfer 106 (2017) 263–279

Fig. 17. Axial profiles of percent conversion of anatase TiO2 to rutile TiO2 for different mass flow rates of the solids in the last 20% of the kiln length.

Fig. 18. Axial profiles of percent conversion of anatase TiO2 to rutile TiO2 for different mass flow rates of the gas in the last 20% kiln length.

A. Agrawal, P.S. Ghoshdastidar / International Journal of Heat and Mass Transfer 106 (2017) 263–279 279

at a faster rate as compared to the cases of lower dry solids flow [5] P.S. Ghoshdastidar, G. Bhargava, R.P. Chhabra, Computer simulation of heat

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