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Ind. Eng. Chem. Res.

1991,30,1289-1293 1289
Sahimi, M. On the Determination of Transport Properties of Dis- sorption, May 7-12,1989, Sonthofen, Bavaria, Federal Republic
ordered Systems. Chem. Eng. Commun. 1988,64,177-195. of Germany; Mersmann, A. B., Scholl, S. E., Ma.; Engineering
Sahimi, M.; Gavalas, G. R.; Tsotsis, T. T. Statistical and Continuum Foundation: New York, 1990.
Models of Fluid-Solid Reactions in Porous Media. Chem. Eng. Stauffer, D. Introduction to Percolation Theory; Taylor & Francis:
Sci. 1990,45, 1443-1502. London, 1985.
Sahimi, M.; Hughes, B. D.; Scriven, L. E.; Davis, H. T. Real-Space Stinchcombe,R. B.; Watson, B. P. Renormalization Group Approach
Renormalization and Effective-Medium Approximation to the for Percolation Conductivity. J.Phys. C: Solid State Phys. 1976,
Percolation Conduction Problem. Phys. Reo. E 1983,28,307-311. 9,3221-3247.
Schopper, J. R. A Theoretical Investigation of the Formation Fac- Wakao, N.; Smith, J. M. Diffusion in Catalyst Pellets. Chem. Eng.
tor/Permeability/PorodlityRelationship Using a Network Model. Sci. 1962, 17, 825-834.
Geophys. Prospect. 1966,14, 301-341.
Sing, K. S. W. The Use of Gas Adsorption for the Characterization Received for reuiew May 14, 1990
of Porous Solids. In Fundamentals of Adsorption; Proceedings Revised manuscript receioed November 19, 1990
of the Third International Conference on Fundamentals of Ad- Accepted December 2, 1990

Kinetics of the Conversion of Calcium Sulfate to Ammonium Sulfate

Using Ammonium Carbonate Aqueous Solution
Elamin M. Elkanzi* and Mohamed F.Chalabi
Department of Chemical and Petroleum Engineering, U.A.E. University, P.O.Box 17555, Al-Ain, U.A.E.

A two-step procedure is described for measuring the intrinsic rate of the slurry reaction between
calcium sulfate and ammonium carbonate. In the first step, experiments were conducted following
the shrinking core model concept to get estimates of the kinetic parameters. These estimates were
then used in a mathematical model to predict an experimental program under which the conditions
of chemical reaction control is likely. The second step is to measure the intrinsic kinetic parameters
under these favorable conditions. A simple power law model fitted to the experimental data of the
second step predicted an activation energy of 72 kJ/mol and a pseudo-first-order reaction with respect
to ammonium carbonate. The procedure may prove useful in measuring the intrinsic kinetics of
fluidaolid heterogeneous reactions and may reduce the effort put on experimental work to establish
favorable conditions for chemical reaction control.

Introduction appreciable amounts even at high conversions of calcium

Ammonium sulfate for use as a fertilizer is generally sulfate when the overall reaction was carried out in a
manufactured from anhydrous ammonia and strong sul- fluidized bed reactor. These findings suggest that the first
furic acid. An alternative process originally developed in two steps may not control the overall reaction.
Germany as long ago as 1909 (Higson, 1951)is now in use. The purpose of this paper is to report a kinetic study
It is based on combining ammonia and carbon dioxide to
produce ammonium carbonate, which then reacted with
gypsum or anhydrite in a three-phase slurry reactor to
CaS04.2H20(s)+ (NH4)&03(aq) -
for the reaction described by the equation

CaC03(s) + (NH4)2S04(aq)+ 2H20(1) (1)

yield ammonium sulfate and calcium carbonate. However,
little work is reported regarding the kinetics of the reac- A two-step procedure is to be investigated in order to
tions involved (Ganz et al., 1959; Chalabi et al., 1975). This measure the intrinsic rate of the above reaction. The first
may be attributed to the complexity resulting from the step is to establish reaction conditions under which
influence of physical processes that must take place in chemical reaction control is likely. These reaction con-
order for the overall reaction to proceed. In the three- ditions, namely, calcium sulfate particle size, calcium
phase gas-liquid-solid system involved here, the overall sulfate slurry concentration, ammonium carbonate initial
rate of reaction at any instant of time may be controlled concentration, rate of mixing, and reaction temperatures,
by one or more of the following steps: (1) gas-liquid mass are predicted by using a mathematical model based on the
transfer; (2) chemical reaction between ammonia solution relative importance of the resistances offered by steps 3-5
and carbon dioxide to form ammonium carbonate; (3) above. The kinetic parameters of the model are estimated
transfer of ammonium carbonate solution through the experimentally by using the shrinking core model concept
liquid-solid film; (4)diffusion of ammonium carbonate (Levenspiel, 1972). The second step is to measure the
solution through the calcium carbonate product layer; ( 5 ) intrinsic kinetics of the reaction by using an experimental
chemical reaction at the surface of unreacted calcium program predicted from the results of the first step.
sulphate core. Mathematical Model
As these steps take place in series, it is evident that the As far as is known, the effects of mass-transfer limita-
slowest step would be rate controlling. Andrew (1954),in
an investigation on carbon dioxide absorption by partially tions on the course of reaction 1 have not yet been in-
carbonated ammonia solutions, reported that the rate of vestigated. Previous experimental investigations (Ganz
carbon dioxide absorption is controlled by the reaction et al., 1959; Chalabi et al., 1975) have shown that the
between carbon dioxide and ammonia. Chalabi et al. calcium sulfate conversion increases with decreasing size
(1975)reported that ammonium carbonate was present in of calcium sulfate particles and with decreasing slurry
concentrations. Therefore it seems a reasonable assump-
tion that the chemical reaction occurs mainly at the surface
* Author to whom correspondence should be addressed. of the available calcium sulfate. As the reaction proceeds,
0888-588519112630- 1289$02.50/ 0 0 1991 American Chemical Society
1290 Ind. Eng. Chem. Res., Vol. 30, No. 6, 1991

the calcium sulfate will be used up, but the particles may The effective diffusivity of (NH,),CO, solution through
become coated with solid calcium carbonate product. ciolid CaC03 may be estimated from the molecular diffu-
Higson (1951) provides a photomicrograph of reaction riivity using a solid tortuosity factor (Satterfield, 1980;
magma in which crystals of calcium sulfate and aggregates Epstein, 1989). The value of the reaction velocity constant
of deposited calcium carbonate are clearly shown. This has not been reported in literature. Estimates of this
evidence and the above-mentioned findings would suggest parameter have to be determined experimentally. Here
that the overall reaction can be visualized to take place the application of the Shrinking core model to the reaction
via the following sequence: (a) mass transfer of aqueous would yield an estimate of the apparent reaction rate
ammonium carbonate from the bulk liquid phase to the constant provided that the assumptions and conditions
external surface of the calcium sulfate particle; (b) diffu- embodied in the model are approached. With these pa-
sion of aqueous ammonium carbonate through the de- rameters being established, eq 6 becomes a function of
posited calcium carbonate product layer; (c) chemical re- calcium sulfate particle size and of speeds of mixing and
action at the core surface. of temperature. A plot of ACA/C, versus calcium sulfate
The relative importance of each of these steps will particle size, with temperature and with speed of mixing
change as the reaction proceeds. The model equations as parameters, would yield a family of curves from which
describing the rates of the steps at one position in the the conditions under which chemical reaction control is
reactor are given as likely may be predicted.
step a: (-rb = k,ap(CAL - )
,C (2) Experimental Section
step b: this is modeling the shrinking core model for a The first set of experiments were conducted to establish
first-order reaction: an estimate for the apparent reaction rate constant under
conditions approaching those embodied in the shrinking
d/dr (P(dCA)/dr)= 0 rc C r C dp/2 (3a) core model. The reaction conditions selected were as
(1)Calcium sulfate slurry concentration was of 5% by
weight (Ganz et al., 1959; Chalabi et al., 1975).
step c: (-rA) = upkCAc r = rc (4) (2) Ammonium carbonate aqueous concentration was
Considering the progress of reaction from fresh solid kept constant at ita saturation value at each temperature.
spherical particle to acompletely converted particle in an In this manner the calcium sulfate conversion would be
isothermal, irreversible fmborder reaction, the average rate a function only of its slurry concentration. This would
of reaction of the fluid reactant (A = (NH,),CO,) based ensure that the time for complete conversion and the ap-
on unit surface area of particle may be obtained by com- parent reaction rate constant be constant for constant
bining eqs 2-4 as follows: temeprature, particle density, and diameter. The as-
sumption of pseudo-first-order kinetics embodied in the
(-r~)av = CAL/P/(~+
J (dp/4De) + (3/k)l (5) shrinking core model would also be approached.
(3) Calcium sulfate particle size was kept below 50 pm.
Since the shrinking core model envisages the overall pro- (4) The temperature was varied between 10 and 20 "C
cess as composed of three resistances in series, the con- in steps of 5 "C. These temperatures were lower than those
centration difference of the transferring component (N- used in previous work.
H1)2C03over each of these steps will be inversely pro- (5) Speed of mixing (impeller speed) was kept constant
portional to the resistance to transfer in that step. From at its maximum value of 2200 min-'.
eq 5 we have The second set of experiments were conducted to es-
ACA/CAL= [l/kn + (dp/4De)l/[l/k, + dp/4De + 3 / k ] tablish the intrinsic rate expression for the reaction under
(6) conditions predicted by the mathematical model of eq 6.
The independent parameters investigated include ammo-
where ACA is the difference in concentration of (NH4)&03 nium carbonate concentration, temperature, and conver-
between the liquid bulk (C,) and that at the gypsum core sion time.
of a particle (CAc). Reduction of the mass-transfer re- Apparatus. All experiments were conducted in a l-L
sistances to low values allows chemical reaction to be rate three-necked round-bottom flask supplied with a stirrer,
controlling. Equation 6 is used to make estimates of the thermocouple ports, a sampling port fitted with a micro-
relative importance of the resistances to mass transfer, filter, and suction pump. Agitation of the reactor contents
diffusion through product layer, and chemical reaction. was carried out with a pitched-blade turbine having three
Although none of these resistances could be predicted with blades. The turbine was driven by a variable-speed motor.
confidence, it was thought that the effort might lead to The reactor temperature was maintained constant by a
a worthwhile reduction in experimental work, before constant-temperature bath provided with a thermoelectric
conditions were established where the reaction was truly controller. The reactor was operated in a batch manner.
the rate-determining step. Materials. The calcium sulfate used in this study was
Analar quality microfine powder. The ammonium car-
Estimation of Model Parameters bonate used was of the commercial type (NH4HC03+
The liquid-film mass-transfer coefficient may be esti- NH2COONH4)genral reagent quality. Deionized water
mated in the case of a mechanically agitated reactor from was used. Other chemicals used as reagents in analysis
correlations reviewed by Pandit et a1 (1986): were all of the AnalaR type.
Procedure. For each experimental run, a weighed
(ha/ U ) N s $ 7 6 ( d p U p ~ / p ~ ) o 3.04
.6 (7) amount of ammonium carbonate was charged to the re-
actor containing 500 mL of deionized water. Stirring of
when 17 C N b C 270 and 13.7 C N h C 3200, or from the reactor content, at 36.6 revolutions/s, was then started.
k,/ U = 2.165/ (Nb)O.*(Ns,)
2/3 (8) When the desired temperature had been reached, calcium
sulfate already cooled to the reaction temperature was
when N b C 17. added as required for the reaction to start. It is important
Ind. Eng. Chem. Res., Vol. 30,No. 6,1991 1291
to charge first the ammonium carbonate because of its
highly negative heat of solution. .55 -
The course of the reaction was followed by means of
1-mL clear-liquid samples that were analyzed for ammo- 45-
nium sulfate content through the determination of the
sulfate radical. The analytical method devised was based
on measuring light absorption by a turbid suspension
caused by reacting barium chloride with the already
treated sample containing ammonium sulfate. For this
purpose a Pye Unicam Model SP8-400double-beam UV-
vis spectrophotometer was used. The analytical method D 1 :291K
is quite sensitive, and ammonium sulfate concentrations
as low as 1 X lo4 M can be detected. The accuracy of the
method depends upon the sample being dilute and
& T
281 n

therefore the original 1-mL sample goes through a series

of dilutions. Corrections to the analytical results were 0 2 4 6 8
12 14 16

made on account of the sulfate content of dissolved calcium

sulfate, of the withdrawal of liquid by sampling, and of Figure 1. Shrinking core model.
dilution due to the generation of water by reaction.
In the first set of experiments the data were taken in
the temperature range 10-20 O C , ammonium carbonate
concentrations corresponding to the saturation value at
each temperature, and calcium sulfate concentration of -2.5-

0.05 kg/L of water.

In the second set of experiments the data were taken
under the conditions predicted by the mathematical model,
namely, the temperature range and calcium sulfate particle
size. Ammonium carbonate initial concentrations ranged

from 0.1 to 0.2 M and calcium sulfate was present in exceas.
Different initial concentrations of ammonium carbonate -1.5 -
were used so as to measure the kinetic parameters over a
wider range of concentrations.
Rssults and Discussion
3.4 1.12 1.45 1.47 3 50 1.52 1.55
For the process design, it is important to obtain the 1 I 103 n"
kinetic expression for the reaction of eq 1. This reaction 1

is the most important and effective one occurring during Figure 2. Arrheniua plot of the shrinking core model.
the ammonium sulfate production process. A two-step
procedure is followed in this study: (a) determination of C, at any temperature was kept nearly constant by using
the conditions under which the reaction is chemically excess carbonate. Thus all the parameters in eq 10 are
controlled and (b) measurement of the intrinsic kinetic constant at each temperature, and hence k would change
parameters under the conditions determined in step (a). with temperature in approximately the same ratio as the
Results from the kinetic analysis of each step are discussed reciprocal of T. A plot of In 1/r against the reciprocal of
separately. absolute temperature is illustrated in Figure 2. The slope
Reaction Conditions. The conversions for calcium of the line indicates an apparent activation energy of 70
sulfate with time, at temperatures of 10,15, and 20 OC and kJ/mol for the reaction of eq 1. The apparent reaction
ammonium carbonate concentration of 1.38,1.60, and 1.85 rate constant can be represented by
kmol/m3 (saturation value at each temperature, respec- k = 1.54 X (11)
tively) were obtained. These experimental data were an-
alyzed on the basis of the shrinking core model. Levenspiel Since the stirring speed was kept constant at 36.6 revolu-
(1972) showed that when the rate is controlled by the tions/s, the value of k, can be estimated from eq 7. An
chemical reaction at the core surface, then for both order of magnitude value for the effective diffusivity De
shrinking and constant-size particles the solid reactant of 3 X lo-" m2/s is estimated from the molecular diffu-
conversion is given by sivity by using a solid tortuosity factor. Substitution of
these values in eq 6 allows the calculation of the fractional
t/T = 1 - (1 - x)1/3 (9) change in concentration with the particle diameter. Figure
3 illustrates some of the results as a plot of ACA/Cfi vs
where calcium sulfate particle diameter with temperature as a
T = pBdp/2bkCfi (10) parameter. As expected, the fractional change in con-
centration decreases with decreasing particle size at each
The experimental data were plotted on the basis of eq 9 temperature. Figure 3 indicates that with particles of less
for all three temperatures as illustrated in Figure 1. The than 50 pm and with temperature of 10 OC or lower, the
values of T were obtained from the slopes of the lines in mass-transfer limitations on the rate of reaction would be
Figure 1. The value of k can then be calculated from eq less than 2%. Therefore it seemed likely that with a
10. It was assumed that the size distribution of calcium stirring speed of 36.6 revolutions/s, with temperatures of
sulfate particles remains constant and an average value for 10 "C or lower, and with particle sizes below 50 pm, the
dp of 30 pm was used. The molar density of calcium sulfate reaction of eq 1 would be effectively controlled by the
is 24.6 kmol/m3. The value of b can be obtained from eq speed of the chemical reaction. Besides the effect of the
1. The saturation concentration of ammonium carbonate, particle size on mass-transfer limitations, the effect of
1292 h d . Eng. Chem. Res., Vol. 30, No. 6, 1991

(5) T i 293 K

_1 20
( 4 )
5 1 -


o 1 i 278 K

0 20 40 60 80 1W 12C

Figure 3. Fractional change in concentrationsv8 particle diameter Figure 4. Continuous reaction model.
(es 6).
8 ,

Tuble I. Experimental Results for the Reaction Starting

with 0.1 ka mol/m8 (NHACO, Aqueous Solution
reaction (NH,)$O, concn, kg mol/m3 X lo2
time, min T = 273 K T = 278 K T = 283 K
0 0 0 0
10 0.5 0.8 1.2
20 0.9 1.5 2.3
30 1.3 2.1 3.3
40 1.7 2.1 4.1
60 2.4 3.8 5.4
80 3.0 4.7 6.5
100 3.1 5.4 7.3
120 4.3 6.1 1.9
140 4.8 6.1 8.4
160 5.2 1.2
180 5.6 1.6 I5 352 355 357 3 5 362 365 357 37
f I 10 '. K1

temperature level should not be overlooked. In fact, the

reaction of eq 1 is both reversible and parallel with respect Figure 5. Arrhenius plot of the continuous reaction model.
to ammonium carbonate. Nowak et al. (1989) studied the irreversible reaction, is best satisfied. The integral form
kinetics of the decomposition of ammonium carbonate in of the kinetic equation is
aqueous solutions. They found that the reaction is second
order with respect to ammonium carbonate concentration In C,/CA = k,t (12)
and has an activation energy of 98.9 kJ/mol. Therefore, The fitting of the above equation to the experimental
low-temperature level and low concentration level would data is illustrated in Figure 4. The rate constants k, a t
not favor the decomposition of ammonium carbonate. To different temperatures were calculated from the regression
minimize the effect of this side reaction in comparison to analysis of these data.
the main reaction of eq 1, and to make mass-transfer lim- An Arrhenius plot shown in Figure 5 gives an activation
itations small, the following reaction conditions may be energy of 72 kJ/mol for the reaction of eq 1. From this
used for the study of the intrinsic rate of the reaction of plot the estimated frequency factor is 4.4 X lo9 s-l at an
eq 1: (i) calcium sulfate concentration of 5 wt 90' (Ganz ammonium carbonate concentration of 0.1 kmol/m3 and
et al., 1959; Chalabi et al., 1975); (ii) ammonium carbonate in the temperature range 0-10 O C . At these conditions the
aqueous concentration of 0.1-0.2 kg mol/m3; (iii) speed of following equation holds:
mixing of 36.6 revolutions/s; (iv) temperature range of 0-10
OC; (v) calcium sulfate particle sizes below 50 pm. k, = 4.4 X lo9 exp(-17234/Rl') (13)
Intrinsic Rate Measurement. Several runs were made The rate of reaction was found to be independent of the
using ammonium carbonate initial concentrations of 0.1, initial concentration of ammonium carbonate in the range
0.15, and 0.2 kmol/m3. Calcium sulfate concentration was 0.1-0.2 kmol/m3.
kept constant a t 5 wt 9'O (this is in excess of its stoichio- Substituting the value of k, from eq 13 into eq 6 and
metric proportion of eq 1). This would allow the surface using a particle diameter of 50 pm and the previously
area to remain essentially constant during the course of estimated values of k, and De,the percent fractional change
the reaction and the rate to be independent of the calcium in concentration was less than 0.019i for the temperature
sulfate concentration. Each run was repeated in duplicate range studied. This clearly demonstrates that mass-
and repeated for a third time to check reproducibility. transfer limitations were negligible and that the rate of
Concentration vs time results were as presented in Table conversion is controlled by the reaction step.
I for the initial concentration of ammonium carbonate of
0.1 kg mol/m3. Conclusions
Having correlated the results in the absence of mass- The work presented in this paper applies a general
transfer limitations, it was found that the kinetic equation method involving a two-step procedure for the measure-
representing the continuous reaction model, of a firsborder ment of intrinsic kinetics of fluid-solid heterogeneous
Ind. Eng. Chem. Res. 1991,30, 1293-1300 1293

reactions. The method has been applied to the measure- t = reaction time, s
ment of the intrinsic kinetics of the conversion of calcium U = slip velocity, m/s
sulfate to ammonium sulfate using aqueous "onium U, = relative velocity between a particle and liquid generated
carbonate solution. In the first step the conditions for because of impeller action, m/s
chemical reaction control were established. In the second X = fractional conversion
step the intrinsic kinetics were measured under the con- Greek Letters
ditions established in the first step. pL = liquid viscosity, kg/ms
The experimental findings showed that the main ad- pB = molar density of calcium sulfate, kmol/m3
vantage of this method is that it helps to predict the re- pL = liquid density, kg/m3
action kinetics by establishing the conditions where the 7 = time required for complete conversion, s
chemical reaction is truly the rate-controlling step.
Registry No. CaS04, 7778-18-9; (NH4)2C03, 506-87-6; (N-
Under the experimental conditions studied here, the H4)2S04,7783-20-2.
kinetics of the conversion of calcium sulfate to ammonium
sulfate using ammonium carbonate aqueous solution were Literature Cited
tentatively represented by a pseudo-fmt-order model, and
an activation energy of 72 kJ/mol was obtained. Andrew, S. P. Carbon dioxide Absorption by Partially Carbonated
Ammonia Solutions. Chem. Eng. Sci. 1954, 3, 279.
Chalabi, M. F.; Younis, S. M. Conversion of CaS04 into (NH4)804
Nomenclature at Ammoniated Gypsum Slurries by Co, Gas. Presented at Chisa
a, = area per unit volume, m-l International Congress on Chemical Engineering, Prague, Che-
b = stoichiometric coefficient (eq 10) cozlovakia, 1975.
CA = concentration of aqueous ammonium carbonate, Conversion of Gypsum or Anhydrite to Ammonium Sulfate. Nitro-
gen 1967, No. 46.
kmol/m3 Epstein, N. On tortuosity and the tortuosity factor in flow and dif-
CAc= concentration of aqueous ammonium carbonate at the fusion through porous media. Chem. Eng. Sci. 1989,44,777-779.
core surface, kmol/m3 Fertilizer Manual; No. IFDC-R-1; International Fertilizer Develop-
C, = concentration in bulk liquid, kmol/m3 ment Center: AL, December 1979.
C, = initial concentration, kmol/m3 Ganz, S. N.; Leibovish, S. B.; Gorbman, S.I. Conversion of CaS04
Ck = concentration at the surface of the solid, kmol/m3 into (NH4)2S04by Agitating a Mixture of Gypsum Slurry, NHS
ACA = molar concentration drop of component A, kmol/m3 and Coz in a Variable Speed Disc Mixer. Zh. A'klad. Khim. 1959,
De = effective diffusivity of aqueous ammonium carbonate 32,975-978.
solution through calcium carbonate ash layer, m2/s Higson, G. I. The Manufacture of Ammonium Sulfate from Anhy-
drite. Chem. Ind. 1951, Sept 8,750-754.
d, = particle diameter, m Levenspiel, 0. Chemical Reaction Engineering, 2nd ed.; Wiley New
k = apparent reaction rate constant, m/s York, 1972.
k, = intrinsic rate constant, s-l Nowark, P., Skrzypek, J. The Kinetics of Chemical Decomposition
k, = liquid-film mass-transfer coefficient, m/s of Ammonium Bicarbonate and Carbonate in Aqueous Solutions.
NRe = Reynolds number, defined by N R =~ dpUeL/pL, di- Chem. Eng. Sci. 1989,44, 2375-2377.
mensionless Pandit, A. B.; Joshi, J. B. Maes and Heat Transfer Characteristics
N k = Schmidt number, dimensionless of Three Phase Sparged Reactors.
R = gas constant, cal/mol K Satterfiold, C. N. Heterogeneow Catalysis in Practice; McGraw-Hilk
New York, 1980.
r = particle radius, m
(-rA) = rate of reaction, kmol/m3 s
r, = core radius, m Received for review May 25, 1990
T = temperature, K Accepted December 8, 1990

Heterogeneous Photocatalytic Oxidation of Phenol with Titanium

Dioxide Powders
Tsong-Yang Wei and Chi-Chao Wan*
Department of Chemical Engineering, National Tsing Hua University, Hsinchu, Taiwan, Republic of China

The photocatalytic oxidation of phenol in oxygenated solution with suspensions of titanium dioxide
powders has been investigated. The experimental results indicate that there is an optimum value
for the Ti02content. Sufficient O2supply is needed, but a too high gas flow rate induces large bubbles
that eliminate the gas residence time and the gas/liquid contact interface. The initial concentration
of phenol demonstrates a negative effect on the pseudo-first-order reaction rate constant. A
mechanism of the phenoxide ions being adsorbed on the Ti02 surface has been proposed to account
for this inverse effect. Moreover, the different pH regions affect the competitive adsorption between
the phenoxide ions and OH- ions on the Ti02 surface, which in turn influences the generation of
the hydroxyl radicals on the T i 0 2 surface.

Introduction the degradation of this compound to reach the safety level

Phenol is a major pollutant and under strict effluent in the range of 0.1-1 mPL-' is not easy. Many conven-
restriction. owingto its and solubility in water, tional methods have been proposed to treat phenol solu-
tions (Devlin and Harris, 1984; Eisenhauer, 1964, 1968;
Getoff, 1986; Hackman, 1976; Kharlamova and Tedoradze,
* To whom correspondence should be addressed. 1981; Sadana and Katzer, 1984; Sharifian and Kirk, 1986;
0888-5885/91/2630-1293$02.50/00 1991 American Chemical Society

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