ELSEVIER
PII: SO016-2361(96)00204-9
Fuel Vol. 76, No. 3, pp. 257-265, 1997
© 1997 Elsevier Science Ltd
Printed in Great Britain. All rights reserved
0016-2361/97 $17.00+0.00
Study of modified calcium
hydroxides for enhancing SO2
removal dur=ng sorbent injection
in pulverized coal boilers
Juan Ad6nez, Vanessa Fierro, Francisco Garcia-Labiano and
Jos6 Maria Palacios*
Instituto de Carboquirnica (C.S.I.C.), P.O. Box 589, 50080 Zaragoza, Spain
*lnstituto de Cat~lisis y Petroleoquirnica (C.S.I.C.), Cantoblanco, 28049 Madrid, Spain
(Received 28 May 1996; revised 8 October 1996)
Several modified calcium hydroxides were prepared by lime hydration using NaC1, KC1, calcium
lignosulfonate, ethanol-water solutions and combinations of them, to obtain sorbents with enhanced
capacity to remove SO2. The sorbents were characterized in a drop tube reactor in similar conditions to
those existing during sorbent injection in pulverized coal boilers. The greatest increases in SO2 retention
were obtained with calcium lignosulfonate as additive or using ethanol-water solutions in the CaO
hydration process. The alkali promoters (NaCI and KC1) acted mainly on the product layer diffusivity.
Calcium lignosulfonate modified the pore size distribution of the calcined hydrate and decreased the mean
particle size of the modified calcium hydroxide by up to five times. The use of ethanol-water solutions
during the hydration process decreased the mean particle size of the modified hydrate and improved the
porous structure of the calcined hydrate, mainly by increasing the porosity. To combine the favourable
effects of these additives, several sorbents were prepared by combinations of them. The best sulfur retentions
were obtained with sorbents modified by a combination of calcium lignosulfonate and hydration with
ethanol-water solutions. The effect of the combination of additives on the sorbent properties was not the
same as that of their action separately, and their effect on sulfur retention was not cumulative. © 1997
Elsevier Science Ltd. All rights reserved.
(Keywords: sulfur dioxide removal; sorbent injection; calcium hydroxides)
The injection of calcium-based sorbents in pulverized
coal boilers is a subject of great interest for the control of
SO2 emissions, especially when it is combined with NOx
reduction by reburning with natural gas or coal, or by
means of LIMB technology. The main disadvantage of
this desulfurization process is the low sorbent utilization.
Since the molar volume of calcium sulfate is significantly
higher than that of calcium oxide, there is a loss of
porosity and pore blockage as the sulfation reaction
proceeds. The high temperatures and low residence times
(< 1 s) of the sorbents in the reactive zone of the boiler
are the factors determining this low sorbent utilization.
Retention is low when using limestones as sorbents
(~ 18%), and only a little higher with calcium hydro-
xides (~ 24%). However, sulfur retention (SR) can be
greatly improved by using modified calcium hydroxides.
Previous studies have shown that a smaller particle
size of the sorbent 1-3 and a higher specific surface area 4
improve SR. Porosity and pore volume distribution also
play an important role in reaching a greater SR 5'6. The
largest pores are regarded as more favourable in
avoiding both pore blockage and pore plugging. Sorbent
reactivity also increases when sintering is delayed 7 or
when the sulfation rate is promoted by increasing ionic
diffusion through the CaSO4 product layer 8. As a process
controlled by diffusion into the pores and in the product
layer 9-11, sorbent utilization can be improved decreasing
the aerodynamic particle size and agglomeration of the
particles after they are formed 12.
The presence of certain inert compounds in sorbents
can improve their utilization, thus increasing SR in the
boiler. Impurities present in the CaO and the additives
added to the hydration water could be responsible for the
differences in reactivity of modified calcium hydroxides.
The temperature and pressure during CaO hydration can
also affect the characteristics of the modified calcium
hydroxide 13.
Hydration with alcoholic solutions yields sorbents
with higher specific surface area and smaller particle
size 4. The relation between the specific surface area of
calcinates and sorbent reactivity is well known 3'8'14-16.
Borgwardt and Bruce 9 found that the sorbent reactivity
varies with the square of the specific surface area over the
2 1
range 2-63m g-. However, not only the specific
Fuel 1997 Volume 76 Number 3 257