Polychlorinated dibenzo-p-dioxin/polychlorinated dibenzofuran releases into the atmosphere from the use of secondary fuels in cement kilns during clinker formation

Article abstract of DOI:10.1021/es049641a

The aim of this study was to evaluate the influence of using waste materials, such as tires or meat meal, as a secondary fuel during clinker production on the polychlorinated dibenzo-p-dioxin (PCDD)/polychlorinated dibenzofuran (PCDF) emission levels to the atmosphere. For this purpose, three different cement plants in Spain were chosen to conduct the project in different sampling episodes. Different materials were separately evaluated in each plant: the first plant included the addition of meat meal in the kiln, the second plant used rejected tires, and the third plant used a mixture of both. In all cases, PCDD/F emission values remained below the limit established by the European Union Directive of 0.1 ng I-TEQ/Nm³, with values ranging from 0.001 to 0.042 ng I-TEQ/Nm³. The major contribution to total TEQ in the majority of cases came from 2,3,7,8-tetrachlorodibenzofuran owing to its relatively higher levels and 2,3,4,7,8-pentachlorodibenzofuran because of its TEF of 0.5. The remaining 15 toxic congeners collectively provided only a minor contribution to TEQ. Furthermore, no marked differences were found compared with reported data obtained from Spanish cement kiln plants using conventional fuel. This fact indicates that the addition of used tires or meat meals had no effect on PCDD/ PCDF emission levels.

Full text of DOI:10.1021/es049641a

Environ. Sci. Technol. 2004, 38, 4734-4738
being secondary fuels in cement kiln plants. Cement
Polychlorinated Dibenzo-p-dioxin/
Polychlorinated Dibenzofuran
Releases into the Atmosphere from
the Use of Secondary Fuels in
Cement Kilns during Clinker
Formation
production involves heating the raw materials at very high
temperatures in a rotary kiln to induce chemical reactions
that produce a fused material called clinker. Combustion of
primary fuels, mainly fossils such as coal and petroleum coke,
is commonly used to attain high temperatures required to
form cement. Nevertheless, the operating conditions achieved
in cement kilns offer an attractive technology for combusting
wastes including those classified as hazardous and the so-
called alternative, additional, supplementary, or secondary
fuels since in many cases an energy output similar to that
of fossil fuels can easily be obtained. Furthermore, inherent
conditions of the cement kiln mimic those of hazardous waste
incineration. For instance, the gas residence time in the kiln
is more than 3 s while the temperature exceeds 1500 °C, and
destruction of organic compounds can be assumed. Some
typical wastes commonly involved in cement formation are
waste oils, spent organic solvents, sludges, meat meals, and
automobile tires.
E S T E B A N A B A D , K A R E L L M A R T IÄ N E Z ,
J O S E P C A I X A C H , A N D J O S E P R I V E R A *
Mass Spectrometry Laboratory, Department of
Ecotechnologies, IIQAB-CSIC, Jordi Girona 18-26,
08034 Barcelona, Spain
It is well-known that combustion processes also imply
the formation and release into the atmosphere of minor
amounts of unwanted byproducts resulting from incomplete
combustion. In many cases, these products such as poly-
chlorinated dibenzo-p-dioxins (PCDDs) and dibenzofurans
(PCDFs) may be highly toxic (1, 2). As a result, stringent
regulations, mainly governing stack gas emissions, have been
enforced in recent years in an attempt to reduce the emissions
of pollutants into the air (3).
To our knowledge, only a few papers on the use of waste
in cement kilns have been published, and no particular
attention has been paid to the evaluation of the releases into
the atmosphere following the use of secondary fuels during
clinker manufacture. Furthermore, the reports focused
mainly on the elaboration of atmospheric emission inven-
tories (4-10).
Interesting data were reported by Fiedler et al. regarding
the first results from stationary source emission in Thailand.
In that paper, results from the evaluation of PCDD/ F emission
from cement kilns, with and without the use of tires and
liquid waste, revealed concentrations far below the 0.1 ng
I-TEQ/ Nm3 limit.
Results of the PCDD/ PCDF emission measurements of
16 cement clinker kilns operating (suspension preheater kilns
and Lepol kilns) in Germany were reported by Schneider et
al. in 1996. The study included both plants using raw material
alone and those using secondary fuels. In all cases, air
pollution control systems (APCSs) were based on the use of
an electrostatic precipitator (ESP). The operating plants
revealed an average concentration of 0.02 ng I-TEQ/ Nm3
(12). More data on the analysis of PCDDs/ PCDFs and dioxin-
like PCBs revealed emission values from cement kilns around
0.0016 ng WHO-TEQ/ Nm3, with a minor PCB contribution
of 0.0002 ng WHO-TEQ/ Nm3 (13).
The aim of this study was to evaluate the influence of
using waste materials, such as tires or meat meal, as a
secondary fuel during clinker production on the polychlori-
nated dibenzo-p-dioxin (PCDD)/polychlorinated dibenzofuran
(PCDF) emission levels to the atmosphere. For this
purpose, three different cement plants in Spain were
chosen to conduct the project in different sampling episodes.
Different materials were separately evaluated in each
plant: the first plant included the addition of meat meal
in the kiln, the second plant used rejected tires, and the third
plant used a mixture of both. In all cases, PCDD/F
emission values remained below the limit established by
the European Union Directive of 0.1 ng I-TEQ/Nm3, with values
ranging from 0.001 to 0.042 ng I-TEQ/Nm3. The major
contribution to total TEQ in the majority of cases came
from 2,3,7,8-tetrachlorodibenzofuran owing to its relatively
higher levels and 2,3,4,7,8-pentachlorodibenzofuran
because of its TEF of 0.5. The remaining 15 toxic congeners
collectively provided only a minor contribution to TEQ.
Furthermore, no marked differences were found compared
with reported data obtained from Spanish cement kiln
plants using conventional fuel. This fact indicates that the
addition of used tires or meat meals had no effect on PCDD/
PCDF emission levels.
1. Introduction
Waste management is a current topic of discussion world-
wide; however, no fully satisfactory definitive solution has
been proposed. Minimization, reutilization, recycling, landfill
disposal, composting, and a variety of combustion processes
are common practices being attempted for implementation
and consolidation in this difficult task. Moreover, the best
solution must be healthy and environmentally friendly and,
in many cases, is highly dependent on the time and place.
Experience shows that no proposal should be accepted or
rejected before the procedure has been extensively assessed.
Data reported from 5 different sites in the U.K. as part of
the compliance monitoring survey undertaken by the U.K.
Environmental Agency yielded 14 individual measurements.
No comments were provided on the type of process or APCS.
Nevertheless, the results revealed average values of 0.058 ng
I-TEQ/ Nm3 (n ) 14) (7). Similarly, French experience on the
use of secondary fuels in cement plants was also reported.
PCDD/ F emission values from 40 measurements collected
in cement plants using meat meal as a secondary fuel were
compared to those obtained from 22 measurements taken
in plants using fossil fuels with no notable differences (14).
Preliminary data on PCDD/ PCDF emission from cement
kiln plants operating in Spain had already been reported in
In recent years, the use of certain waste materials to
provide some of the energy requirements for industrial
processes has grown significantly, one of the most notable
* Corresponding author phone: 34-93-400.61.67; fax: 34-93-
204.59.04; e-mail: jraeco@iiqab.csic.es.
9
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10.1021/es049641a CCC: $27.50
2004 Am erican Chem ical Society
Published on Web 08/10/2004

coke at 8.5 Mg/ h, and used automobile tires at a dosage of
1 Mg/ h representing 9.4% thermal substitution. Used tires
were previously crushed and injected in the precalciner. The
APCS in plant 2 also consisted of fabric filters. Finally, plant
3 presented a dry process with a tower containing four
cyclone-type vessels. Raw materials were fed into the kiln at
a dosage of 110-125 Mg/ h. Conventional fuel was combined
with both residues, used tires and meat meal, at a dosage of
0.7-1.2 Mg/ h for tires and between 0.6 and 0.7 Mg/ h for
meat meal, with a total thermal substitution of 13-14%. The
final configuration of the plant included an ESP as an APCS
device. The operating conditions, sampling schedules, and
proportions of conventional fuel and waste materials are
summarized in Table 1.
For gaseous matrixes, sampling was made with a stack
gas sampler of the filter/ condenser method, fulfilling the
minimum requirements described in EN-1948:1996 part 1,
as extensively documented in previous studies (18, 19).
2.2. Extraction and Cleanup. Prior to the extraction
process, samples were spiked with labeled PCDD/ PCDF
standards described in the EN-1948 methods. Analytes were
removed from XAD-2 and the filter by Soxhlet extraction
using toluene for 24 h. The toluene extracts were then
transferred to n-hexane and rotary-concentrated prior to the
cleanup process.
The cleanup procedure was based on the use of the Power
Prep system (FMS Inc., Boston, MA). The automated system
cleanup employs multilayer silica, basic alumina, and PX-21
carbon adsorbents (FMS Inc.). The n-hexane extracts were
loaded and pumped through individual sets of multilayer
silica followed by a basic alumina column with n-hexane.
Interferences were eliminated with n-hexane/ dichloro-
methane (98:2). PCDDs/ PCDFs were then eluted from the
alumina column and transferred to the PX-21 carbon column
with a mixture of n-hexane/ dichloromethane (1:1). Finally,
interferences were eluted with 12 mL of ethyl acetate/ toluene
(1:1) in the forward direction, and PCDDs/ PCDFs were
collected from the carbon column in the reverse direction.
All solvents, acetone, dichloromethane, toluene, n-hexane,
and ethyl acetate, for organic trace analysis were purchased
from Merck (Germany) (20).
2.3. Instrum ental Analysis. Purified extracts were ana-
lyzed by HRGC-HRMS on a GC 8000 series gas chromato-
graph (Carlo Erba Instruments, Milan, Italy) coupled to an
Autospec Ultima mass spectrometer (Micromass, Manches-
ter, U.K.), using a positive electron ionization (EI+) source
and operating in the SIM mode at resolving power of 10000.
Chromatographic separation was achieved with a DB-5 (J&W
Scientific, California) fused-silica capillary column (60 m ×
0.25 mm i.d., 0.25 µm film thickness) with helium as carrier
gas in the splitless injection mode (1-2 µL). The temperature
program was 140 °C (1 min) to 200 °C (1 min) at 20 °C/ min,
then at 3 °C/ min to 300 °C, and hold isothermally for 20 min
at 300 °C. Confirmatory analyses were performed by using
polar GC capillary columns such as a J&W DB-DIOXIN GC
column (21).
2.4. Quality-Control Criteria. Quality criteria were based
on the applications of quality control (QC) and quality
assurance (QA) measures such as analysis of a blank sample
covering the complete analytical procedure, analysis of
certified reference materials, or participation in intercali-
bration exercises as a current quality policy of the Laboratory
of Dioxins, which have been reported in previous works (19).
FIGURE 1. Diagram of a cement kiln plant examined in this study.
the framework of the Spanish Dioxin Inventory. Provided
data refer to 20 cement plants, 18 of which operate with a
dry process and 2 more use wet processes; in all cases fossil
fuels were used as primary fuels. Results ranged from 0.0006
to 0.0472 ng I-TEQ/ Nm3 with an average value of 0.007 ng
I-TEQ/ Nm3 (n ) 20) (5).
The potential impact of clinker plants was also evaluated
in the surroundings of two different cement kiln plants in
Spain. In particular, temporal variations of both PCDD/ F
and heavy metals in two environmental matrixes such as
soils and herbages were studied. From the findings obtained
in both studies, no relevant influence on the neighborhood
was observed (15, 16).
This work presents the results of the studies conducted
to evaluate PCDD/ PCDF emissions into the atmosphere at
three Spanish cement kiln plants using secondary fuels in
clinker production. In particular, two different types of waste
materials (meat meal and used tires) and a mixture of both
were separately evaluated in duplicate in several sampling
campaigns. In all cases, operating conditions included dry
processes, and the APCSs were based on the use of fabric
filters (FFs) in two plants and an ESP in the third plant. Current
practices complying with the minimum requirements in-
dicated in well-accepted procedures, such as EN-1948:1996,
were fulfilled for the analyses (17).
2. Materials and Methods
2.1. Sam pling Strategy. A measurement program was
undertaken in two sampling campaigns at three different
plants in Spain. In all cases, clinker was formed in a dry
process. All plants presented a state-of-the-art configuration
with a preheater consisting of a vertical tower containing a
series of cyclone-type vessels depending on the plant. A
diagram of a typical cement kiln plant and some operating
condition details are shown in Figure 1.
In particular, in plant 1, the tower contained five cyclone-
type vessels. Raw materials were fed into the kiln at the cold
end at 230 Mg/ h; meanwhile, conventional fuel, mainly
petroleum coke, at a dosage of 15.6 Mg/ h, was combined
with meat meal at a dosage ranging from 1.6 to 2 Mg/ h,
which signifies 4.8-6% thermal substitution. Injection of
waste materials was performed in the calciner and the main
burner (highest temperature zone). In this case, the APCS
devices consisted of fabric filters. In plant 2, raw materials
were injected at a dosage of 100 Mg/ h at the top of a tower
with four cyclone-type vessels. In this case, combustion
conditions included a mixture of conventional fuel, petroleum
3. Results and Discussion
In this study, the use of waste materials as a secondary fuel
during the formation of clinker in several Spanish cement
kilns was evaluated. Three different plants, coded plant 1,
plant 2, and plant 3, were selected for the project. Owing to
the complexity and cost of the study, two different sampling
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TABLE 1. Operating Conditions and Sampling Schedule for Assessment of the Use of Waste Materials as Secondary Fuels in a
Cement Kiln Plant
plant 1
plant 2
plant 3
type of process
dry process
dry process
dry process
preheater
five cyclone-type vessels
230
coke pretroleum
15.6
m eat m eal
1.6-2
calciner
four cyclone-type vessels
100
coke pretroleum
8.5
used tires
1
preheater
9.4
fabric filters
07/16/2002
12/11/2002
four cyclone-type vessels
110-125
raw m aterial dosage (Mg/h)
conventional fuel
prim ary fuel dosage (Mg/h)
secondary fuel
secondary fuel dosage (Mg/h)
feeding point
percentage therm al substitution
APCS
first cam paign
coke pretroleum
5.7-7.8
m ixed m eat m eal and used tires
15.6
calciner and preheater
13-14
electrostatic precipitator
09/13/2002
4.8-6
fabric filters
05/15/2002
03/26/2003
second cam paign
07/17/2003
3
TABLE 2. PCDD/PCDF Concentrations (pg/Nm ) of Emission Samples Collected in Cement Kilns Using Secondary Fuelsa
plant 3, used tires
plant 1, meat meal
plant 2, used tires
plus meat meal
first
second
first
second
first
second
compound
campaign
campaign
campaign
campaign
campaign
campaign
2,3,7,8-TCDF
33.97
4.42
6.36
8.35
3.89
6.15
NQ (3.33)
12.61
4.47
6.62
0.89
1.20
1.79
0.56
0.85
NQ (0.13)
1.80
0.84
32.50
5.11
8.47
49.11
3.07
29.24
4.13
1.66
3.16
NQ (0.91)
2.07
NQ (0.93)
2.11
NQ (1.78)
NQ (0.93)
NQ (0.94)
NQ (0.90)
NQ (0.99)
1.65
4.01
1780.69
17.83
203.11
9.50
22.95
4.79
3.98
8.06
1.45
4.85
1.26
0.93
3.17
1.35
5.96
1,2,3,7,8-PeCDF
2,3,4,7,8-PeCDF
1,2,3,4,7,8-HxCDF
1,2,3,6,7,8-HxCDF
2,3,4,6,7,8-HxCDF
1,2,3,7,8,9-HxCDF
1,2,3,4,6,7,8-HpCDF
1,2,3,4,7,8,9-HpCDF
OCDF
12.38
38.71
36.30
28.95
37.79
13.98
96.38
18.85
76.16
NQ (0.98)
10.36
6.22
15.80
43.48
19.08
23.46
NQ (4.58)
50.24
8.99
22.36
0.93
3.02
3.19
14.49
0.00
19.03
NQ (0.091)
0.73
0.32
0.90
2,3,7,8-TCDD
NQ (0.90)
NQ (1.16)
NQ (2.74)
NQ (2.33)
NQ (2.59)
8.19
20.15
193.02
30.87
43.52
3.25
36.16
5.70
NQ (0.03)
NQ (0.06)
NQ (0.11)
0.55
N. Q.(0,11)
3.44
7.74
34.78
0.17
7.35
0.61
5.00
0l67
1,2,3,7,8-PeCDD
1,2,3,4,7,8-HxCDD
1,2,3,6,7,8-HxCDD
1,2,3,7,8,9-HxCDD
1,2,3,4,6,7,8-HpCDD
OCDD
total TCDF
total TCDD
total PeCDF
total PeCDD
4.65
7.43
8.57
5.70
10.62
33.22
47.48
141.12
53.14
102.05
67.14
151.51
99.33
85.00
66.64
0.026
0.62
7.06
45.43
85.00
81.34
59.54
216.57
80.01
265.96
120.16
141.16
95.56
0.042
13.92
132.62
3.26
29.48
8.41
12.48
22.06
17.79
14.34
0.005
total HxCDF
total HxCDD
total HpCDF
24.59
36.06
0.009
2.64
5.86
0.002
total HpCDD
2.05
0.021
total I-TEQ (ng/Nm 3)
a
In parentheses are given the quantification lim its. NQ ) nonquantifiable.
campaigns were designed to obtain two values from each
experiment. Two different types of waste materials, used tires
and meat meal, were assessed since they are the most
abundant and accessible candidates for use in cement kilns
in Spain.
In plant 1, the addition of meat meal as a supplementary
fuel in combination with conventional fuel consisting of
petroleum coke in the previously indicated proportions was
assessed. Likewise, plant 2 employed used tires together with
conventional fuel. Finally, in plant 3, the experiments
consisted of the addition of a mixture of used tires and meat
meal, respectively, as described in previous sections. Thus,
two sampling campaigns in three different plants yielded a
total of six sampling collection episodes.
Summarized data including congeners and total PCDD/
PCDF concentrations are shown in Table 2. In general terms,
the results expressed in TEQ were far below the limit of 0.1
ng I-TEQ/ Nm3 established by the European Union Directive
(3), with values ranging from 0.002 to 0.042 I-TEQ/ Nm3 with
an average value and median of 0.017 and 0.014 ng I-TEQ/
Nm3 (n ) 6), respectively. Moreover, the results are consistent
with those reported in the literature. Cement clinker kilns
operating in Germany revealed an average concentration of
0.02 ng I-TEQ/ Nm3 (12). Data on the analysis of PCDDs/
PCDFs and dioxin-like PCBs revealed emission values from
cement kilns around 0.0016 ng WHO-TEQ/ Nm3, where PCBs
had only a minor contribution of 0.0002 ng WHO-TEQ/ Nm3
(13). Data from the U.K. revealed average values of 0.058 ng
I-TEQ/ Nm3 (n ) 14) and median values of 0.032 ng I-TEQ/
Nm3 (n ) 14) (7).
PCDD/ PCDF concentrations between 0.0003 and 0.0029
ng I-TEQ/ Nm3 were reported from Thailand in cement plants
burning hazardous liquid wastes and tires, respectively. It is
remarkable that no significant differences were observed
when the use of secondary fuels was compared with data
obtained under normal conditions without the use of
secondary fuels, with mean values between 0.0008 and 0.0105
ng I-TEQ/ Nm3 (6). Taking into account these findings, our
data were compared with previous results obtained from
emission samples collected in cement plants not using
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FIGURE 2. Congener distribution of 2,3,7,8-PCDDs/PCDFs (pg/Nm3) in cement kilns using secondary fuels.
secondary fuels during clinker formation. Thus, emission
data collected between 2000 and 2001 from 20 Spanish
cement plants covering more than 29 kilns yielded over 40
measurements submitted to the Spanish Dioxin Inventory.
In summary, overall results revealed values from 0.001 to
0.054 ng I-TEQ/ Nm3 (22). Statistics were calculated by the
Kruskal-Wallis tests which compares medians within each
group (23), with the P value being greater than 0.05 (0.13).
Therefore, no statistically significant differences were found
among the medians at the 95% confidence interval levels.
Conventional analysis of congeners and their distribution,
commonly called chemical fingerprint analysis, is widely used
as an important tool to link the presence of these contami-
nants to a specific source. A representative congener-specific
concentration profile of the 2,3,7,8-chloro-substituted PCDDs/
PCDFs is shown in Figure 2. The results presented a similar
combustion byproduct profile with a notable presence of
PCDFs (mainly tetrachorodibenzofuran (TCDF), pentachlo-
FIGURE 3. Congener distribution of 2,3,7,8-PCDDs/PCDFs (in TEQ
rodibenzofuran (PeCDF), and hexachlorodibenzofuran (Hx-
CDF) followed by heptachlorodibenzo-p-dioxin (HpCDD)
and octachlorodibenzo-p-dioxin (OCDD)) compared to
PCDDs (18, 19). In contrast, a remarkable particularity was
the presence of 2,3,7,8-TCDF in a significant number of
samples as occurs in emissions from kilns operating without
the addition of secondary fuels (5). Unfortunately, owing to
the low number of samples, this hypothesis could not be
statistically corroborated at the 95% confidence level.
values) in cement kilns using secondary fuels.
contribution of each congener expressed as TEQ values for
all species studied.
The emission of polychlorinated dibenzo-p-dioxins and
dibenzofurans was evaluated in cement kiln plants operating
under normal conditions and using secondary fuels. In all
cases, the emitted PCDD/ F concentrations were consistent
with those reported in the literature and complied with the
present EU Directives limit for PCDD/ PCDF emission.
Moreover, no statistical differences were found between data
obtained from the use of conventional fuel alone and those
obtained from the use of secondary fuels. Therefore, from
these findings it can be concluded that the addition of used
In terms of TEQ, an analogous situation was found when
TEQ profiles were compared. In all cases, the major con-
tribution stemmed from the 2,3,7,8-TCDF and the 2,3,4,7,8-
PeCDF with the other congeners remaining in a minor
proportion. As an example, Figure 3 shows the relative
9
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(10) UNEP. Standardized Toolkit for Identification and Quantification
of Dioxin and Furan Releases; UNEP Chemicals: Geneva,
Switzerland, January 2001, 2003; http:/ / www.chem.unep.ch/
pops/ newlayout/ repdocs.html.
tires or meat meal had no effect on emission results in keeping
conditions.
Acknowledgments
(11) Fiedler, H.; Chareonsong, P.; Mayer, J.; Hartenstein, H. U.
This project was carried out in the framework of a col-
laboration between OFICIEMEN and the Spanish Council
for Scientific Research (CSIC). We thank Marina Romay, Asier
Otxoa de Eribe, and Pedro Mora from OFICEMEN for
encouragement in the elaboration of this study, Dr. Albert
Manich for comments on statistics, and Eric Jover and Nuria
Garc´ıa for comments and critiques. We also thank Ms. M. G.
Martrat and Mr. M. A. Adrados for excellent work in sample
preparation (extraction and FMS purification) and J. Saulo´
for HRGC-HRMS analysis.
Organohalogen Compd. 2002, 59, 211.
(12) Kuhlmann, K.; Schneider, M.; Su¨ llenbo¨ hmer, F. Organohalogen
Compd. 1996, 27, 78.
(13) Luthardt, P.; Mayer, J.; Fuchs, J. Chemosphere 2002, 46, 1303.
(14) Capmas, A. ATILH, 2003. The French Cement Industry experi-
ence in the use of waste fuels. 5th Colloquia of managers and
technicians of cement plants, Sevilla, February 2003.
(15) Schuhmacher, M.; Agramunt, M. C.; Bocio, A.; Domingo, J. L.;
de Kok H. A. M. Environ. Int. 2003, 29, 415.
(16) Schuhmacher, M.; Agramunt, M. C.; Bocio, A.; Domingo, J. L.;
de Kok, H. A. M. Chemosphere 2002, 48, 209.
(17) European Standard, Stationary source emissions- Determination
of the mass concentration of PCDDs/PCDFs; EN-1948-1,2,3:1996;
European Committee for Standardization: Brussels, 1996.
Literature Cited
(1) Olie, K.; Vermeulen, P. L.; Hutzinger O. Chemosphere 1977, 6,
455.
(2) Rappe, C. Fresenius’ J. Anal. Chem. 1994, 348, 63.
(3) Council Directive 2000/ 76/ EC of 4 December 2000 on the waste
incineration. Official Journal; European Union, 12/ 28/ 2000; L
332/ 91-111.
(4) Chen, C. Chemosphere 2004, 54, 1413.
(5) Fabrellas, B.; Ruiz, M. L.; Abad, E.; Rivera, J.; Sanz, P. Organo-
halogen Compd. 2002, 56, 139.
(18) Abad, E.; Caixach, J.; Rivera, J. Chemosphere 2003, 50, 1175.
(19) Abad, E.; Adrados, M. A.; Caixach, J.; Rivera, J. Environ. Sci.
Technol. 2002, 36, 92.
(20) Abad, E.; Caixach, J.; Rivera, J. J. Chromatogr., A2000, 893, 383.
(21) Abad, E.; Caixach, J.; Rivera, J. J. Chromatogr., A 1997, 786, 125.
(22) OFICEMEN. www.oficimen.es, 2003.
(23) Siegel, S. Non-parametric statistics for the behavioural sciences;
(6) Fiedler, H. Organohalogen Compd. 2003, 63, 1.
(7) Alcock, R. E.; Gemmill, R.; Jones, K. C. Chemosphere 1999, 38,
759.
MacGraw Hill Book Co., Inc.: London, 1956.
(8) Quass, U.; Fermann, M.; Bro¨ ker, G. Chemosphere 2004, 54, 1319.
(9) UNEP. Dioxin and Furan Inventories, National and Regional
Emissions of PCDD/F; UNEP Chemicals: Geneva, Switzerland,
1999.
Received for review March 8, 2004. Revised manuscript re-
ceived June 14, 2004. Accepted June 15, 2004.
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