Science of the Total Environment 491492 (2014) 118122

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Science of the Total Environment

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POP emissions from a large sinter plant in Taranto (Italy) over a ve-year
period following enforcement of new legislation
Vittorio Esposito a,, Annamaria Maffei a, Donato Bruno a, Berenice Varvaglione a, Salvatore Ficocelli a,
Carmelo Capoccia b, Maria Spartera a, Roberto Giua c, Massimo Blonda c, Giorgio Assennato c
a
b
c

ARPA PUGLIA, Environmental Protection Agency of Apulia, Department of Taranto, Via Anteatro 8, 74100 Taranto, Italy
ARPA PUGLIA, Environmental Protection Agency of Apulia, Department of Lecce, Via Miglietta 2, 73100 Lecce, Italy
ARPA PUGLIA, Environmental Protection Agency of Apulia, Corso Trieste 27, 70126 Bari, Italy

H I G H L I G H T S

Sinter plant is a major emitter of PCDD/F to air due to high pollutants content and high exhaust gas ow
Drastic reduction of pollutants emission was enforced by legislation
Active carbon injection proved effective in PCCD/F removal from sinter exhaust gas
Yearly mass release of PCDD/F to air still in the multigram-per-year range for Taranto plant

a r t i c l e

i n f o

Article history:
Received 15 November 2013
Received in revised form 14 March 2014
Accepted 14 March 2014
Available online 3 April 2014
Editor D. Barcelo
Keywords:
Dioxin
Stack emissions
Integrated steelworks
Sinter plant
Abatement techniques
Legislation

a b s t r a c t
PCDD/F in exhaust gas emission samples was determined by the Environmental Agency of Apulia for a sinter
plant located in Taranto (Italy) starting from June 2007 following an Agreement Act between plant owners
and the Regional Government with the aim to assess and improve the environmental performances of the
plant. The rst two sampling campaigns yielded results ranging between 3.42 and 8.34 ng I-TE/Nm3 that were
soon considered revelatory of a high potential impact on the surrounding environment and the public, prompting
for immediate action. As a rst outcome, a Regional Regulation (LR 44/2008) was enforced in order to reduce
PCDD/F emissions by plants operating in the metal sector, including sinter plants. After installation of a urea addition plant to the sinter mix as a process-integrated abatement technique the emissions ranged from 0.86 to
3.59 ng I-TE/Nm3. In order to reach compliance to the newly introduced emission limit value of 0.4 ng I-TE/
Nm3 the urea plant was removed in favour of active-carbon injection as an end-of-pipe technique. Subsequently,
during year 2011 emission values ranged from 0.095 to 1.97 ng I-TE/Nm3, while in 2012 the observed range was
0.058 to 0.91 ng I-TE/Nm3. As a better evaluation of the potential impact of the sinter plant emissions, a yearly
mass-ow was estimated using exhaust gas PCDD/F concentrations and plant operational parameters (3.4
M Nm3/h). Mass-ow was estimated to be as high as 165 g I-TE/year for 2007 using yearly average concentrations
or 248 g I-TE/year using the peak-value of 8.34 ng I-TE/Nm3.
2014 Elsevier B.V. All rights reserved.

1. Introduction
Starting from mid-2007 (Esposito et al., 2012; Primerano et al.,
2007) the Environment Protection Agency of Apulia has performed
several measurements of Persistent Organic Pollutant (POP) stack emissions for a number of industrial plants located in a large industrial area
near Taranto. Although information and estimates of a signicant yearly
mass ow for dioxins and PCBs from integrated steelworks were already
available and published in relevant European inventories since year 1993
(Lahl, 1993, 1994; Kinzel et al., 1994; Broker et al., 1999; Anderson and
Corresponding author. Tel.: +39 99 9949764; fax: +39 99 9946311.
E-mail address: v.esposito@arpa.puglia.it (V. Esposito).

http://dx.doi.org/10.1016/j.scitotenv.2014.03.077
0048-9697/ 2014 Elsevier B.V. All rights reserved.

Fisher, 2002), the actual measurements were in exceedance of those estimates and prompted the need of a more in-depth investigation of the fate
and transport of POPs from emissions and release to the various environmental compartments in the Taranto area and ultimately transfer to the
food-chain through animal farming and shery, as well as the evaluation
of available abatement techniques to be applied to the existing plant in
order to reduce the overall impact (Anderson et al., 2001; Buekens
et al., 2001).
In early 2008 high levels of dioxin and dioxin-like PCBs were found
in food samples of animal origin that were collected from farms located
in the immediate surroundings of the industrial area (Diletti et al., 2009)
causing immediate alarm among citizens and authorities. As an immediate response to the events, as soon as December 2008 a Regional

V. Esposito et al. / Science of the Total Environment 491492 (2014) 118122

Regulation (LR 44/2008) enforced more stringent limits on dioxin stack

emissions for plants operating in the metal sector. In fact, the existing
Italian emission limits were inadequate to prevent POP accumulation
in the environment and not aligned to relevant regulation already into
force in other European countries (Francois et al., 2000, 2001). The
new limits were set to 2.5 ng I-TE/Nm3 starting from 1st of July 2009
and 0.4 ng I-TE/Nm3 starting from 1st of January 2011 in order to
allow a reasonable, although short, amount of time to adopt technologies on such a large scale, the sinter plant being among the largest
known with a total sinter bed surface of 472 m2.
In addition, and in order to investigate the extent of the contamination, an extensive monitoring plan was set up and performed throughout
the period 20082011 during which time more than 100 atmospheric
deposition monthly samples, 50 soil and groundwater samples were
collected and analysed (Esposito et al., 2010, 2012). As a result of the
monitoring the Local Health Authority enforced the ban on grazing
over wasteland within 20 km from the industrial area and the ban on
the consumption of goat and sheep liver originating from animals
grown in the same area, together with the stamping out of over 2000
sheep and goats.
As an outcome of the above enforcement of legislative and monitoring
actions a signicant reduction of the yearly mass ow of POPs emitted to
the atmosphere as stack exhaust gases was observed, as demonstrated by
the latest emission measurements. Nevertheless, diffuse and fugitive
emissions are arguably contributing to the overall impact on the
surroundings resulting in a measurable POP atmospheric deposition of
both wet matter and dry matter on soils and other urban surfaces
(Esposito et al., 2012).
This paper presents the results of PCDD/F, PCB, and PAH emission
control in stack emissions during a ve-year period with respect to the
enforcement of stricter legislation and adoption of process-integrated
and end-of-pipe techniques.
2. Materials and methods
Stack emission samples were collected according to Method UNI EN
1948-1 (lter condenser method) by using an Isostack apparatus (TCR
Tecora, Corsico Milan, Italy). The lter-condenser method allows sampling of both gas-phase matter and particle-phase matter. The ue gas
enters the sampling train through an electrically heated glass lined
probe. This is connected to a glass lter casing in which a quartz bre lter (Munktell, Baresnstein, Germany) is supported on a PTFE lter holder. The lter casing is inside an electrically heated box. It is followed by a
water cooled coil condenser and a XAD-2 resin (Supelco, Supelpak, St
Louis, MO, USA) lled cartridge. The condensate and the gas pass
through the resin to a round bottomed ask in which the condensate
is collected. Exhaust gases were drawn in isokinetic conditions from
plant stack for a total of 6 h. Sample extraction was performed by Accelerated Liquid Extraction (Dionex, Sunnyvale, CA, USA) with Toluene. Extract aliquots for the determination of PCDD/Fs and PCBs by method EN
1948-2-3-4 were puried/fractionated by means of an automated
clean-up process with a PowerPrep system (Fluid Management System,
Waltham, Massachusetts) using disposable columns (multilayer silica,
alumina and carbon). Extract aliquots for the determination of PAHs
were puried over silica gel. Labelled standards were purchased from
Cambridge Isotope Laboratories (Andover, MA, USA) and used according to Method EN 1948 1-2-3-4 for PCDD/Fs and PCBs and ISO 11338
1-2 for PAHs. PCDD/Fs were separated by high resolution gas chromatography (HRGC) on a DB-5 MS capillary column (60 m 0.25 mm,
0.25 m lm thickness, J&W Scientic, California). Isotope-dilution
high-resolution mass-spectrometry (HRMS) determinations were carried out on a DFS High Resolution system (Thermo Fisher, Bremen,
Germany) at a resolution of 10,000 operating with electron ionisation
(EI) at 45 eV in the selected ion monitoring (SIM) mode. PCBs including
dioxin-like PCBs (dl-PCBs) were separated by HRGC on a HT8 capillary
column (60 m 0.25 mm, 0.25 m lm thickness, SGE Analytical

119

Science, Australia) and determined by HRMS, in the same operating

conditions used for PCDD/Fs. PAHs were separated by HRGC on a DB-5
MS capillary column (30 m 0.25 mm, 0.25 m lm thickness, J&W Scientic, California) and determined by HRMS, in the same operating conditions used for PCDD/Fs. For each batch of seven samples a laboratory
blank and a control sample (certied y-ash from inter-laboratory prociency tests) were analysed. In addition, every sampling campaign included a eld blank, according to UNI EN 1948-1 that was used to
ensure that no signicant contamination had occurred during all steps
of the measurement, and were not subtracted from measured values.
Recovery rates for sampling and extraction labelled standards were in
compliance with UNI EN 1948 requirements (greater than 50%).

Table 1
Results for stack emission measurements at Taranto sinter plant.
Date

12 Jun 07
14 Jun 07
16 Jun 07
26 Feb 08
27 Feb 08
28 Feb 08
23 Jun 08
24 Jun 08
26 Jun 08
21 Jul 09
22 Jul 09
23 Jul 09
17 Nov 09
18 Nov 09
19 Nov 09
11 Jan 10
12 Jan 10
13 Jan 10
1 Feb 10
2 Feb 10
3 Feb 10
16 Feb 11
17 Feb 11
18 Feb 11
16 May 11
18 May 11
19 May 11
14 Nov 11
15 Nov 11
16 Nov 11
12 Dec 11
13 Dec 11
14 Dec 11
18 Jul 12
19 Jul 12
20 Jul 12
15 Oct 12
16 Oct 12
17 Oct 12
13 Dec 12
14 Dec 12
15 Dec 12
17 Jun 13
18 Jun 13
19 Jun 13

PCDD/Fsa

Dioxinlike PCBsb

Total PCBsc

Benzo(a)
pyrene

Sum PAHsd

pg I-TE/Nm3

pg WHO-TE/
Nm3

ng/Nm3

ng/Nm3

mg/Nm3

3421
7192
6022
4443
8344
8082
2670
4215
2428
857
711
1063
1552
1261
2103
3166
778
3591
1138
1057
1243
1639
1700
1966
1159
1019
1884
327
318
264
135
95
136
462
909
677
119
143
251
687
58
339
248
123
149

181
368
346
293
520
478
195
364
226
32
29
38
117
100
132
156
56
230
100
102
105
189
178
194
124
100
176
33
33
38
13
11
16
59
111
72
13
14
28
57
4
30
44
13
16

823
2153
1259
846
1242
1236
1184
1454
1160
633
839
1064
1452
1479
1516
1127
477
794
637
527
488
1074
713
795
309
306
525
110
100
116
73
69
104
191
264
199
73
78
86
205
44
169
178
71
103

611
1480
526
917
1338
2817
539
1299
388
257
268
367
187
250
1120
1074
708
2817
487
363
341
459
1075
748
1063
1324
3086
17
15
17
1.1
3.8
8.1
10
47
62
5.0
7.5
6.3
450
26
93
1.4
1.3
1.4

0.010
0.022
0.018
0.0096
0.019
0.031
0.010
0.021
0.0098
0.0033
0.0029
0.0043
0.0054
0.0064
0.027
0.035
0.017
0.055
0.017
0.013
0.019
0.0093
0.011
0.012
0.0099
0.011
0.024
0.00028
0.00025
0.00030
0.000035
0.000058
0.00019
0.00036
0.0017
0.0020
0.00014
0.00015
0.00024
0.0086
0.00048
0.0014
0.00018
0.00017
0.00032

All data are normalised to 16% O2 content for consistency purposes only and not for
regulatory compliance.
a
Sum of seventeen 2378-chlorine substituted congeners.
b
Sum of twelve non-ortho and mono-ortho PCBs.
c
Sum of all measurable mono- to deca-CB.
d
Sum of selected PAHs as regulated by Italian Legislation: Benzo(a)anthracene,
Benzo(b + k + j)uoranthene, Benzo(a)pyrene, Indeno(123-cd)pyrene, Dibenzo(ah)anthracene, Dibenzo(al)pyrene, Dibenzo(ae)pyrene, Dibenzo(ai)pyrene, and Dibenzo(ah)
pyrene.

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V. Esposito et al. / Science of the Total Environment 491492 (2014) 118122

Fig. 1. a) PCDD/Fs, bold vertical lines represent the legislative deadlines, horizontal lines represent the enforced Emission Limit Values; b) dioxin-like PCBs; and c) PAHs in sinter plant stack
emission relative to the adoption of abatement techniques (ESP = electrostatic precipitator; MEEP = moving electrode electrostatic precipitator).

Toxic equivalent (TEQ) values for PCDD/Fs were calculated

using NATO Toxic Equivalency Factors (I-TEFs, 1989) as required
by Italian legislation on stack emissions and expressed as lowerbound concentrations. Toxic equivalent (TEQ) values for PCBs were
calculated using WHO Toxic Equivalency Factors (WHO-TEFs, 1998).
The laboratory has ISO17025 accreditation.

3. Results and discussion

A total of 42 stack emission samples were collected at the sinter
plant in Taranto over the period 20072013. Results for PCDD/Fs, total
PCBs (mono- to deca-CB), dioxin-like PCBs, Benzo(a)pyrene and other
selected PAHs are presented in Table 1.

V. Esposito et al. / Science of the Total Environment 491492 (2014) 118122

It has to be noted that the enforced legislation requires a 35%

subtraction to be applied to PCDD/F measured values as listed in the
Table 1 in order to take into account measurement uncertainty even
when values are compliant to the emission limit. In addition, O2% in
ue gas is not used to normalise measured values (measured O2 values
ranged from 16% to 18.5%), as the valid Permit does not yet allow O2
normalisation. However, in order to report consistent and coherent
emission values, and to allow comparison with other reported data, a
correction with respect to 16% reference oxygen is applied to measured
values and yearly mass ows. Emission Limit Values (ELV) are intended
as yearly-average of a minimum of nine measurements grouped in a
minimum of three campaigns.
The enforced ELV prompted sinter plant operators to adopt primary
and end-of-pipe abatement techniques that would allow compliance to
the new standards. For the period starting from July 2009 to December
2010 (ELV equal to 2.5 ng I-TE/Nm3) a Urea addition device was used to
add the known organic-nitrogen PCDD/F suppressant to the feed
material (Anderson et al., 2007; Ooi and Lu, 2011) together with the
existing primary electrostatic precipitators (ESP) and moving electrode
electrostatic precipitators (MEEP). The observed PCDD/F concentrations
in stack emission samples while solid urea was added to the sinter mix
as a process-integrated abatement technique ranged from 0.86 to 3.59
ng I-TE/Nm3. PCBs are also known to be present in sinter plant exhaust
emissions (Aries et al., 2006) and a reduction similar to PCDD/Fs was observed for dioxin-like PCBs that ranged from 0.18 to 0.52 ng WHO-TE/
Nm3 prior to urea addition and from 0.029 to 0.23 ng ]WHO-TE/Nm3 during urea addition. On the other hand, a somewhat unexpected high variability of the Sum PAHs was also determined (the sum is dened in
Table 1 and corresponds to the compounds listed in the national legislation). In fact, although the mechanism of urea is not fully known it is speculated that urea could be able to reduce the rate of formation of aromatic
rings, thus affecting PAHs as well (Kuzuhara et al., 2005). Prior to urea addition the Sum PAHs ranged from 9.6 to 31 g/Nm3 and after introducing
urea in the sinter mix the range was enlarged from 2.9 to 55 g/Nm3 with
more evident scattering of the results with an observed consistent reduction only during 2009 that was apparently lost in 2010 while urea was
still added. The latter observation suggests that together with urea some
other process-integrated techniques or operational measures were possibly put in place by plant operators. It has to be noted that measurements
for the year 2010 only cover January and February, thus introducing uncertainty in the estimates.
Starting from January 2011 plant owners switched from urea addition (dismantled) to activated carbon injection ahead of ESP (Francois
et al., 2000) as an end-of-pipe abatement technique, although without
the addition of fabric lters that are usually implemented together
with the adsorbent injection. At the present time, fabric lters are included in the revised Permit and will be installed in the forthcoming
years. Those measures have allowed compliance to the limits, although
up to May 2011 values in excess of 1 ng I-TE/Nm3 were still measured
and oxygen content of exhaust was still high (range 1718.5%, average
17.7%). It has to be noted that carbon injection, in the form of highgrade carbon designed for sorption of pollutants in exhaust gases or
more cost-effective lignite carbon, is often associated with bag of
mesh lter installation. In this case, no additional lters were added
next or in substitution of ESP or MEEP, although the adoption of this
additional abatement technique has been requested by Authorities.
The latest results in emission control covering year 2012 and the beginning of 2013 have shown an additional decrease of PCDD/F concentrations compared with the preceding years with an observed range of
0.058 to 0.91 ng I-TE/Nm3 with an average value of 0.35 ng I-TE/Nm3
although the range is not yet entirely coherent and reproducible having
found some individual values still well above the 0.4 ng I-TE/Nm3 emission limit value.
Fig. 1 illustrates the n = 42 individual values for PCDD/Fs, PCBs, sum
PAHs in stack emissions relative to introduction of process-integrated
and end-of-pipe abatement techniques.

121

Table 2
Estimated yearly mass ow of selected pollutants for Taranto sinter plant. Italics for year
2013 represent partial estimates including only one sampling campaign.
Year

2007
2008
2009
2010
2011
2012
2013

PCDD/F

Dioxin-like PCBs

Total PCBs

Benzo(a)pyrene

Sum PAHs

g I-TE/year

g WHO-TE/year

kg/year

kg/year

kg/year

165
150
37
54
26
12
5.2

8.9
10
2.2
3.7
2.7
1.3
0.7

42
35
35
20
11
4.3
3.5

26
36
12
29
19
2.3
0.041

499
500
246
775
194
50
6.6

It is possible to estimate the impact of stack emissions on the environment and the public as a yearly mass ow considering a ue gas
emission of 3.4 million Nm3/h with a continuous operation of the
plant, maintenance aside, and the average emission values calculated
for each operational year. Results are summarised in Table 2 and, together with the evident reduction of the yearly mass ow for PCDD/Fs,
they show a signicant contribution of dioxin-like PCBs to overall TEQ
(about 1:20) as well as an emission of sum PAHs still in the order of
the tenth of kg/year.
As most regulated primary sources are today adequately characterised
(Breivik et al., 2004; Fiedler et al., 2003) it is possible to compare the
actual estimates provided in Table 2 with other sources and inventories.
Thermal processes are today considered to be the main sources of
PCDD/F release compared to the chemical industry whose impact was
considered to be prevalent in the past. Within combustion processes,
iron ore sintering is at present considered the most relevant source of
PCDD/F emissions to air (Quass et al., 2004). For three sinter plants
operated in the United Kingdom a cumulative annual mass release of
27.8 g I-TEQ/year was estimated for PCDD/Fs and 1.72 g WHO-TEQ/year
for dioxin-like PCBs during the period 20022004 (Aries et al., 2006).
Similarly, four sinter plants in Taiwan have shown a cumulative annual
emission of 44.7 g I-TEQ/year (Wang et al., 2003). Compared to the
above data, the estimated PCDD/F ux for the Taranto plant was actually
very high even in recent years, up to 165 g I-TEQ/y for this single plant in
2010, while emission reduction techniques, both process-integrated or
end-of-pipe, were already available and apparently implemented in
other countries. Under these circumstances the reduction of PCDD/F
ux for the Taranto plant in years 20112012 appears signicant, and
contributes to the overall PCDD/F emission reduction that is generally
observed in Europe for the period 19902011 (EEA, 2013) for both the
industrial and non-industrial sectors, the latter being an important
contributor to the total amount of PCDD/Fs released to air, especially
for solid-fuelled residential heating (Paradiz et al., 2008; Bieser et al.,
2012). The same applies to Benzo(a)pyrene and other PAHs, were gures in the order of 500 kg/year are estimated for the Taranto sinter
plant in 2008 that decreased of one order of magnitude in 2012, although it is known that for an integrated steel plant the major emitter
of Benzo(a)pyrene are coke-oven facilities (Ciaparra et al., 2009).

4. Conclusions
In 2007 stack emission measurements performed by the Apulian
Environment Protection Agency (ARPA) revealed a high PCDD/F emission at a sinter plant. Since then a stringent monitoring programme to
prove the efciency of the new abatement techniques introduced by
plant operators and to assess the compliance to newly introduced Emission Limit Values has been carried out in the period 20082013 and a
signicant reduction of the mass ow PCDD/F, PCBs, as well as PAHs
has been achieved. Studies are still ongoing to evaluate if the improvements in stack emissions are having a concomitant positive effect on
the observed POP levels in the surrounding environment.

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V. Esposito et al. / Science of the Total Environment 491492 (2014) 118122

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