Environ. Sci. Technol.
1997, 31, 2319-2325
Effect of Sulfur Impregnation Method
on Activated Carbon Uptake of
Gas-Phase Mercury
JOHN A. KORPIEL AND
RADISAV D. VIDIC*
Department of Civil and Environmental Engineering,
943 Benedum Hall, University of Pittsburgh,
Pittsburgh, Pennsylvania 15261-2294
The dynamics of granular activated carbon (GAC) adsorbers
for the uptake of gas-phase mercury was evaluated as a
function of temperature, influent mercury concentration,
and empty bed contact time. Sulfur-impregnated carbons
exhibited enhanced mercury removal efficiency over virgin
carbon due to the formation of mercuric sulfide on the carbon
surface. The effect of the sulfur impregnation method
on mercury removal efficiency was examined through experi-
ments conducted on commercially available sulfur-
impregnated carbon (HGR) and carbon impregnated with
sulfur in our laboratory (BPL-S). Although HGR and BPL-S
possess similar sulfur contents, BPL-S is impregnated at a
higher temperature, which promotes a more uniform
distribution of sulfur in the GAC pore structure. At low
influent mercury concentrations and low temperatures,
HGR and BPL-S performed similarly in the removal of mercury
gas. However, as the temperature was increased above
the melting point of sulfur, the performance of HGR
deteriorated significantly, while the performance of BPL-S
slightly improved. At high influent mercury concentrations,
HGR performed better than BPL-S, regardless of temperature.
For both HGR and BPL-S, the observed dynamic mercury
adsorptive capacities were far below the capacities
predicted by the stoichiometry of mercuric sulfide formation.
In HGR carbon the sulfur is very accessible, but ag-
glomeration that occurs at high temperatures causes the
sulfur to be relatively unreactive. In BPL-S carbon, on
the other hand, the sulfur remains in a highly reactive form,
but its location deep in the internal pores makes it relatively
inaccessible and prone to blockage by HgS formation.
Introduction
In the past couple of decades, environmental control agencies
have expressed increasing concern about the release of
mercury to the environment. Two types of combustion
processes that are major sources of mercury emissions are
coal-fired power plants (CFPPs) and municipal waste com-
bustors (MWCs). It is estimated that world-wide fossil fuel
combustion produces 1500 t of mercury annually from
electricity generation and 1210 t from other industrial uses,
with CFPPs accounting for 10-15% of the U.S. total mercury
emissions (1). Mercury emissions from CFPPs exist in various
valence states: elemental Hg0 and oxidized Hg2+ forms, such
as HgCl2 and HgO. Elemental mercury gas, however, is the
dominant form of mercury in the plume of a CFPP, ranging
from 92% to 99% of the total mercury concentration in the
* Corresponding author phone: 412-6124-1307; fax: 412-624-0135;
e-mail: vidic@engrng.pitt.edu.
S0013-936X(96)00926-1 CCC: $14.00  1997 American Chemical Society
air (2, 3). Several studies (4-6) have indicated that electro-
static precipitators are ineffective in removing volatile ele-
ments such as mercury, allowing at least 90% of the mercury
to be discharged into the atmosphere.
Control of Mercury Emissions. Currently there are no
regulations on the control of mercury emissions from the
electric utilities. However, the Clean Air Act Amendments of
1990 (Title III, Section 112[b][1]) required the major sources
to use maximum available control technology and mandated
the U.S. EPA to perform a study on the significance of mercury
emissions from various sources.
Air pollution control processes capable of controlling
mercury emissions include activated carbon adsorption (7-
12) and wet scrubbing (13, 14). Activated carbon adsorption
can be accomplished in two different processes: powdered
activated carbon (PAC) injection and fixed-bed granular
activated carbon (GAC) adsorption. PAC injection involves
the injection of PAC directly into the plant’s flue gas stream
where it adsorbs gas-phase mercury and is collected in
downstream particulate control devices, such as fabric filters
or ESPs. In situations in which fixed-bed GAC adsorption
may be used, the adsorber should be placed downstream of
the flue gas desulfurization (FGD) units and particulate
collectors, serving as the final treatment process before the
flue gas is discharged into the atmosphere. Although wet
scrubbing is primarily intended for the removal of SO2 from
the flue gas, it can provide significant removal of mercury
under certain conditions (15, 16).
Sinha and Walker (9) investigated the effect of sulfurization
of activated carbon on the mercury adsorptive capacity at 25
and 150 °C. At 25 °C, they found that the adsorptive capacity
was greatest for the virgin carbon and decreased with
increasing sulfur loading. However, at 150 °C, the adsorption
of mercury by the virgin carbon was negligible compared to
that of the sulfur-impregnated carbons, due to the mercury
reacting with sulfur on the carbon surface to form HgS.
Otani et al. (12) discovered that increasing the sulfur
content of activated carbon from 0% to 13.1% by weight causes
an increase in mercury adsorptive capacity at 36 °C. They
also observed that the amount of mercury adsorbed by sulfur-
impregnated activated carbon is much less than that predicted
by the stoichiometry of the reaction Hg + S f HgS, which
led to a conclusion that some fraction of the impregnated
sulfur does not participate in the reaction with mercury gas.
The unreacted sulfur is considered to be chemically adsorbed
and stable.
Krishnan et al. (15) observed that temperature had an
insignificant effect on Hg0 sorption by HGR, a commercially
available sulfur-impregnated carbon, within the first 4 h of
the experiment. Beyond 5 h, HGR at 140 °C captured more
Hg0 than HGR at 23 °C. Heat treatment of virgin activated
carbon samples at 140 °C for 4 h resulted in a significant
reduction in mercury capture. The authors explained that
this was due to the deactivation or depletion of surface active
sites. Exposing HGR to heat treatment, however, did not
affect its dynamic adsorptive capacity, because the primary
sorption site (S) was not deactivated.
Livengood et al. (16) found that chemically pretreating
virgin activated carbon with sulfur can greatly increase the
removal capacity. The relative superiority of sulfur-impreg-
nated carbon with respect to virgin carbons was enhanced
at lower temperatures. The authors found that the dynamic
mercury adsorptive capacity of activated carbon decreased
with increasing temperature, decreasing inlet mercury con-
centration, and increasing particle size.
Vidic and McLaughlin (17) investigated the effects of
temperature, mercury concentration, and method of sulfur
VOL. 31, NO. 8, 1997 / ENVIRONMENTAL SCIENCE & TECHNOLOGY 9 2319
FIGURE 1. Schematic representation of the experimental setup.
impregnation on mercury removal performance using three
different carbons: F-400 (virgin carbon), HGR (commercial
sulfur-impregnated carbon), and F-400S (F-400 impregnated
with sulfur at 600 °C under inert atmosphere). The authors
observed that the sulfur-impregnated GACs showed much
greater adsorptive capacity than virgin activated carbon,
especially in the temperature range of 25-90 °C. The
enhanced performance of sulfur-impregnated carbon was
due to the chemisorption of mercury facilitated by the
formation of HgS on the carbon surface. The mercury removal
efficiency by HGR was found to be highly temperature specific,
exhibiting poor performance at 140 °C. At the low mercury
concentration of 55 µg/m3, F-400S performed better than
HGR while containing 21% less sulfur. This was explained
by the improved method of sulfur impregnation at 600 °C,
which promotes more uniform distribution of the sulfur in
the GAC pore structure. Sulfur analysis revealed that the
chemically bonded sulfur found on F-400S is less likely to be
volatilized at higher temperatures, while the condensed sulfur
found on HGR is easily removed at temperatures greater than
140 °C.
The main objective of this study was to further understand
the role of different impregnation methods on the availability
of sulfur to bond gas-phase mercury and the corresponding
impact on the dynamics of a fixed-bed adsorption systems
under various process and operational conditions.
Materials and Methods
Two types of activated carbon were used in this study: HGR
and BPL-S. HGR, a commercially available sulfur-impreg-
nated carbon, was supplied by the manufacturer (Calgon
Carbon Corporation, Pittsburgh, PA) in 12 × 30 and 4 × 10
U.S. Mesh sizes. BPL-S was produced by impregnating a
bituminous coal-based virgin activated carbon, BPL (Calgon
Carbon Corporation, Pittsburgh, PA), with sulfur in a pure
nitrogen atmosphere at 600 °C. The particle sizes used in
this study were 60 × 80 and 4 × 10 U.S. Mesh size, having
geometric mean particle diameters of 0.021 and 0.49 cm,
respectively. Prior to their use in the experiments, the carbon
was dried in an oven at 105 °C for 24 h and stored in a
desiccator. The sulfur contents of HGR and BPL-S are 9.7%
and 10.0%, respectively.
A mercury permeation device manufactured by VICI
Metronics (Santa Clara, CA) was used as the source of
elemental mercury (Hg0) throughout the study. The per-
2320 9 ENVIRONMENTAL SCIENCE & TECHNOLOGY / VOL. 31, NO. 8, 1997
meation device was designed to provide a uniform and stable
release of mercury gas into the carrier gas stream at a given
temperature. The permeation device was sealed in a glass
permeation tube holder with inlet and outlet ports and was
immersed in a temperature-controlled oil bath. Industrial
grade nitrogen was used in the experiments as a carrier gas
to transport the mercury gas out of the permeation tube
holder. The flow rate of the carrier gas stream was controlled
by Model FC-280S mass flow controllers (MFCs) connected
to a Model RO-28 readout/control box (Tylan General,
Torrance, CA). Two three-way valves, placed immediately
upstream and downstream of the glass permeation tube
holder, were used to bypass the permeation device when
flushing the system with clean carrier gas. By varying the oil
bath temperature and the carrier gas flow rate, a wide range
of mercury concentrations could be generated. A schematic
representation of the experimental setup is shown in Figure
1.
A mercury trapping impinger solution was used to collect
batch mode mercury samples in order to calibrate the atomic
absorption spectrophotometer and to determine the total
mercury concentration in the effluent stream from a fixed-
bed carbon adsorber. The impinger solution used for
absorbing the gas-phase mercury was prepared with 1.5%
potassium permanganate in 10% (3.6 N) sulfuric acid as
described by Shendrikar et al. (18). All glassware was covered
with aluminum foil due to the instability of the impinger
solution in the presence of light, and the solution was always
used within 12 h from the time it was prepared.
Analytical Methods. The concentration of elemental
mercury in the gas stream was measured continuously by a
Perkin-Elmer Model 403 atomic absorption spectrophotom-
eter (AAS) (Perkin-Elmer, Norwalk, CT) fitted with an 18-cm
hollow quartz gas cell (Varian Australia Pty. Ltd., Mulgrave,
Victoria, Australia). The wavelength of the mercury hollow
cathode lamp (Fisher Scientific, Pittsburgh, PA) was adjusted
to 253.7 nm. Calibration of the AAS was performed by passing
a mercury laden gas at a flow rate of 1.0 L/min through the
quartz cell while capturing the effluent gas in an impinger
train consisting of two 250-mL gas impingers with coarse
fritted cylinders (Corning, Inc., Horseheads, NY) connected
in series. The mercury-laden stream was collected for 1 h,
with AAS absorbance and flow rate measurements recorded
at 5-min intervals. After the impinger train was taken off-
line, the solutions were transferred into PTFE bottles, and 10
mL of concentrated nitrohydrochloric acid (aqua regia) was
used to rinse off any mercury that might have condensed on
the glass walls.
Liquid-phase mercury standards were prepared by spiking
clean impinger solution with a known volume of 1000 µg/L
mercury atomic absorption solution (Aldrich Chemical
Company, Milwaukee, WI). A 15-mL solution containing 12%
sodium chloride and 12% hydroxylamine sulfate in DI water
was added to each PTFE bottle to reduce the excess per-
manganate. The bottles were vigorously shaken, vented to
release the pressure generated by the reaction, and stored for
liquid-phase analysis. All liquid-phase mercury analyses were
performed using a Varian Model VGA-76 gas generation
accessory (Varian Australia Pty. Ltd., Mulgrave, Victoria,
Australia) according to EPA Method 7470 (19). The gas-phase
mercury detection limit for the analytical system used in this
study was 2.4 µg/m3.
The sulfur content of activated carbons was measured
using a Leco Model SC 132 sulfur determinator (Leco
Corporation, St. Joseph, MI). Activated carbon surface areas
were determined using an Orr surface-area pore-volume
analyzer Model 2100 (Micromeritics Instrument Corporation,
Atlanta, GA) and calculated using the nitrogen BET isotherm
method.
Adsorber Experiments. For short empty-bed contact time
(EBCT) experiments, the experimental adsorber consisted of
a 0.64 cm inner diameter stainless steel column containing
100 or 200 mg of 60 × 80 U.S. Mesh size carbon. Two 200
U.S. Mesh size stainless steel screens were used to secure the
GAC bed, and the walls of the column were threaded in order
to accommodate various bed depths. For long EBCT experi-
ments conducted at elevated temperatures, the experimental
adsorber consisted of a 2.2 cm inner diameter stainless steel
column containing 10 g of 4 × 10 U.S. Mesh size carbon. For
long EBCT experiments conducted at room temperature, an
experimental adsorber consisted of a 2.4 cm inner diameter
acrylic column that was charged with 10 g of 4 × 10 U.S. Mesh
size carbon to yield a GAC bed depth of 3.7 cm. One 80 U.S.
Mesh size stainless steel screen was used to secure the GAC
bed in both cases.
Throughout the study, the adsorbers were operated in
downflow mode to minimize the potential for fluidization of
the packed bed. The adsorbers were placed in a temperature-
controlled oven in order to regulate the temperature of the
influent gas and the GAC bed. To ensure that the temperature
of the influent gas is the same as the temperature of the bed
by the time the gas reached the bed, 3.5 m of coiled Teflon
tubing was placed in the oven upstream of the adsorber inlet.
Two three-way valves, one immediately upstream and the
other immediately downstream of the oven, allowed the
adsorber to be bypassed until the onset of the adsorption
experiment.
Prior to the start of each experiment, both the mercury
permeation device and the adsorber were bypassed, while
the clean carrier gas was passed through the AAS cell at the
desired flow rate for a 1 h warm-up period. After the energy
level of the lamp was stabilized, the absorbance reading of
the AAS was zeroed. At this time the mercury permeation
device was placed on-line, and the system was allowed to
stabilize for a period of 2 h, after which time the absorbance
reading was recorded. The adsorber was placed on-line, and
the time was recorded as time zero. The effluent mercury
concentration was continuously monitored, and the dynamic
adsorptive capacity of the GAC was computed by integrating
the area above the breakthrough curve.
Quality Assurance/Quality Control Experiments. The
following conclusions summarize the findings of QA/QC
experiments performed on the experimental system:
(a) Gas-phase mercury calibration curve for the AAS is
independent of the flow rate of mercury-laden gas through
the hollow quartz cell.
TABLE 1. Comparison of GAC Types
GAC type sulfur content (% by wt) BET Asp (m2/g)
BPL 0.7 1026
HGR 9.7 482
BPL-S 10.0 824
(b) Adsorption of mercury onto the tubing and experi-
mental adsorbers was found to be negligible.
(c) Temperature of the influent mercury stream was in
equilibrium with the oven temperature at the inlet to the
adsorber.
(d) Combustion of the spent carbon in an oxygen
atmosphere at 900 °C, with subsequent collection of the
emitted gases into an impinger train, revealed that the mass
of mercury adsorbed by the carbon was within 1% of the
mercury mass computed by integration of the area above the
breakthrough curve.
(d) Interference in the AAS measurement of elemental
mercury due to possible HgS formation in the gas phase
downstream of the adsorber containing sulfur-impregnated
carbon is negligible.
Results and Discussion
Effect of Impregnation Method on Sulfur Distribution. HGR
is manufactured by condensing sulfur gas onto BPL carbon
at relatively low temperatures, while BPL-S carbon was
produced by impregnating sulfur onto BPL carbon at a
temperature of 600 °C. Although the different impregnation
methods yielded similar sulfur contents (Table 1), sulfur
impregnation of HGR and BPL-S carbons caused a 53% and
20% decrease in the initial BET specific surface area of 4 ×
10 U.S. Mesh size BPL carbon, respectively (Table 1). Due
to the higher impregnation temperature, the sulfur in BPL-S
carbon is suspected to be more evenly distributed in the pore
structure, occupying the deeper, narrower pores. The sulfur
in HGR carbon, on the other hand, is most likely condensed
at the external surface of the carbon, blocking the access to
the narrower high energy pores.
Thermogravimetric analysis (TGA) was conducted by
heating samples of BPL, HGR, and BPL-S carbons up to 400
°C in an argon atmosphere. Figure 2 shows that BPL and
BPL-S carbons underwent negligible decreases in weight,
while the weight of the HGR carbon sample decreased by
8.5%. Since both HGR and BPL-S carbons are manufactured
by impregnating BPL carbon with sulfur, this outcome implies
that BPL-S carbon lost a negligible amount of its impregnated
sulfur, while HGR carbon lost 88% of its sulfur content. This
shows that the bonding of sulfur molecules to the carbon
matrix is much stronger in BPL-S than in HGR carbon.
Sulfur exists in several allotropes, including Sλ (S8 rings),
Sπ (S8 chains), and Sµ (chains of variable length), with S8 rings
as the only form at room temperature (20-22). Since the
sulfur gas at 200 °C is in the form of S8 (76.5%) and S6 (23.5%)
rings (20, 22), it is reasonable to assume that HGR carbon
contains sulfur predominantly in the form of voluminous S8
rings. At 600 °C, sulfur gas possesses a significant fraction
of S6 (58.8%) and S2 (16.4%) molecules (22), which are less
voluminous and more reactive because they possess a greater
fraction of sulfur terminal atoms (23). Therefore, the smaller
S2 and S6 chains can more easily migrate into the narrower
pores of the carbon matrix and, as the carbon cools down to
room temperature at the completion of the impregnation
process, steric hindrance impedes reformation of the more
voluminous allotropic Sλ from the other two allotropes (23-
25). Thus, BPL-S carbon possesses greater proportions of
sulfur in the more reactive S2 form than the normal proportion
indicated by the corresponding equilibrium constant.
VOL. 31, NO. 8, 1997 / ENVIRONMENTAL SCIENCE & TECHNOLOGY 9 2321
FIGURE 2. Thermogravimetric analyses of activated carbons in argon atmosphere.
FIGURE 3. Effect of flow rate on mercury uptake by HGR carbon.
Based on the discussion presented above, it is believed
that the sulfur in HGR carbon is predominantly in the form
of S8 rings and is weakly bonded to the carbon surface in the
macroporous region of the carbon particle. On the other
hand, the sulfur in BPL-S carbon is strongly bonded to the
carbon surface in the microporous region of the carbon
particle, requiring mercury to diffuse a longer distance for
chemisorption to occur. A much larger proportion of the
sulfur in BPL-S carbon is believed to be in the form of S2 and
S6 chains, which are more reactive than the S8 rings present
in HGR carbon.
GAC Performance at Short EBCT. All adsorber experi-
ments conducted at short EBCT (e0.11 s) utilized 60 × 80
U.S. Mesh size GAC. Experiments were conducted at 140 °C
using 100 mg of HGR carbon and an influent mercury
concentration of 55 µg/m3. As shown in Figure 3, the
performance of HGR carbon improved as the flow rate
increased from 0.1 to 5.0 L/min. Although the dynamic
mercury adsorptive capacity was observed to increase with
increasing flow rate, it was in all cases negligible as compared
to the capacity predicted by the stoichiometry of HgS
formation (0.607 g of Hg/g of HGR).
2322 9 ENVIRONMENTAL SCIENCE & TECHNOLOGY / VOL. 31, NO. 8, 1997
If the external mass transfer is the rate-limiting step in the
overall process of mercury uptake from the gas phase, then
an increase in the flow rate, which results in a decrease of the
concentration boundary layer thickness, should have caused
an improved rate of mercury uptake from the beginning of
the experiment. Since this was not observed experimentally,
it can be concluded that the external mass transfer resistance
is negligible under these experimental conditions. Similarly,
internal mass transfer resistance is typically not considered
a rate-limiting step for gas-phase applications of activated
carbon. In addition, it has already been suggested that sulfur
in HGR carbon is located in a macroporous region of a GAC
particle, making it easily accessible for mercury molecules.
The only other possibility is that the rate of mercuric sulfide
formation and subsequent diffusion into the sulfur bulk phase
is the rate-limiting step in the adsorption dynamics of HGR
carbon. As the flow rate is increased at a given mercury
concentration, the mercury loading rate (µg/min) increases,
causing an increase in the amount of mercury molecules that
contact the sulfur surface in a given time period. Higher
mercury loadings establish a surface excess of mercury, which
increases the rate of HgS formation and drives the HgS
FIGURE 4. Effect of temperature on mercury breakthrough from HGR and BPL-S adsorbers.
FIGURE 5. Mercury breakthrough from HGR adsorber in on-line/off-line operation.
molecules to diffuse more rapidly into the sulfur bulk phase.
The increasing mercury loading rates accelerate the exo-
thermic reaction of HgS formation, resulting in thermal
agitation, which breaks up the sulfur chains more rapidly.
The resulting increase in the number of sulfur terminal atoms
causes the reactivity of the impregnated sulfur to increase.
This hypothesis is further discussed later in the text.
In order to compare the effect of temperature on the
performance of HGR and BPL-S carbons, adsorber experi-
ments using 200 mg of 60 × 80 U.S. Mesh carbon were
conducted for a duration of 10 h at the low influent mercury
concentration of 55 µg/m3, a flow rate of 1.0 L/min, and at
temperatures of 25, 90, and 140 °C. The breakthrough curves
illustrated in Figure 4 show that HGR and BPL-S carbons
performed similarly in the uptake of mercury at 25 and 90 °C.
However, when the temperature was increased to 140 °C, the
performance of BPL-S carbon improved slightly while
HGR carbon exhibited significant deterioration in the ability
to remove mercury from the feed stream. This may be due
to the fact that 140 °C is above the melting point of sulfur
(115.2 °C), which induces the sulfur that is weakly bonded to
the surface of HGR carbon to melt and agglomerate as a liquid
in the form of long polymer chains (20) and decreases the
sulfur surface area available for contact with the incoming
mercury molecules. Thus, the performance of HGR carbon
at 140 °C may be limited by the slow diffusion of mercury
through the liquid-state sulfur. The stronger bonding and
more uniform distribution of sulfur in BPL-S carbon prevented
the sulfur from agglomerating, which ensured that the
performance of BPL-S carbon did not deteriorate at higher
temperature.
An adsorber experiment in which the mercury-laden gas
was periodically diverted around the adsorber (while the
temperature of the adsorber was maintained constant) was
VOL. 31, NO. 8, 1997 / ENVIRONMENTAL SCIENCE & TECHNOLOGY 9 2323
FIGURE 6. Effect of mercury concentration on mercury uptake by HGR and BPL-S carbons.

FIGURE 7. Effect of temperature on mercury uptake by HGR and BPL-S carbons at 1.0 s EBCT.

conducted at 140 °C using the influent mercury concentration TABLE 2. Summary of HGR Performance in Each Mercury
of 55 µg/m3, a flow rate of 1.0 L/min, and 100 mg of 60 × 80 Loading
U.S. Mesh HGR carbon. As shown by the breakthrough curve
(Figure 5), four mercury loading steps were performed over mercury duration Hg uptake cumulative Hg uptake
a period of 8 days. Note that in the first two loading steps, loading Step (h) (µg of Hg/g) (µg of Hg/g)
after 100% breakthrough was reached and the adsorber was 1 4.1 34.9 34.9
bypassed for over 1 day, the adsorber exhibited additional 2 5.6 45.4 80.3
capacity after it was placed back on-line. The performance 3 13.5 155.0 235.3
of HGR in each mercury loading step is summarized in Table 4 21.1 263.0 498.3
2.
The following is a possible explanation for the behavior state bulk sulfur is slow, the HgS monolayer blocks the
illustrated in Figure 5. By the time 100% breakthrough is incoming Hg molecules from reacting with the bulk sulfur
reached in the first loading step, the available surface area that is still available in the carbon pores. During the period
of the sulfur agglomerates is completely covered by a that the adsorber was bypassed, the HgS molecules had
monolayer of HgS. Since the diffusion of HgS through liquid- sufficient time to diffuse into the sulfur liquid phase, breaking

2324 9 ENVIRONMENTAL SCIENCE & TECHNOLOGY / VOL. 31, NO. 8, 1997

up sulfur chains to provide additional sulfur terminal atoms
to react with mercury molecules in a subsequent loading
step. The observation that the mercury removal performance
actually improved in the third and fourth loading step may
be due to the fact that the sulfur polymer chains began to
break apart into smaller chains as more and more mercury
reacted with sulfur, thereby increasing the fraction of sulfur
terminal atoms, which led to an increase in the rate of HgS
in the later part of the column experiment.
Figure 6 illustrates the effect of the influent mercury
concentration on the performance of HGR and BPL-S carbons
at 140 °C. As discussed earlier, BPL-S carbon performed
significantly better than HGR carbon at 140 °C and low influent
mercury concentration of 55 µg/m3. Figure 6 shows that as
the influent mercury concentration was increased from 55 to
684 µg/m3, the performance of HGR carbon improved while
the performance of BPL-S carbon deteriorated to the extent
that it performed worse than HGR carbon. The deterioration
in the performance of BPL-S carbon at high concentrations
may be due to the rapid formation of large HgS molecules
that can block the access to the narrower pores and prevent
the mercury molecules from accessing the highly reactive S2
molecules that are present in the microporous region of the
BPL-S carbon. The inaccessibility of sulfur in BPL-S carbon
may also explain observations in other experiments that the
dynamic mercury adsorptive capacity was less than 1% of the
capacity predicted by the stoichiometry of HgS formation
(i.e., less than 1% of the impregnated sulfur was consumed
by the time 100% breakthrough was reached).
GAC Performance at Long EBCT. Column experiments
at long EBCT (1.0 s) were performed at high mercury
concentration (684 µg/m3) in order to accelerate mercury
breakthrough for such high carbon masses in the adsorber.
Figure 7 shows the mercury uptake by HGR and BPL-S carbons
as a function of time at temperatures of 25 and 140 °C. Similar
to the results observed at the short EBCT, HGR carbon
performed better than BPL-S carbon under the condition of
high influent mercury concentration and high temperature.
HGR carbon also performed better than BPL-S carbon at room
temperature, although the performance of both carbons
improved with temperature decrease.
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Received for review November 1, 1996. Revised manuscript
received February 21, 1997. Accepted April 3, 1997.X
ES9609260
X Abstract published in Advance ACS Abstracts, June 1, 1997.
VOL. 31, NO. 8, 1997 / ENVIRONMENTAL SCIENCE & TECHNOLOGY 9 2325