Review Articles
Review Articles
Bromine in Waste Incineration
Partitioning and Influence on Metal Volatilisation
Jürgen Vehlow*, Britta Bergfeldt, Hans Hunsinger, Helmut Seifert and Frank E. Mark1
Forschungszentrum Karlsruhe GmbH, Institute for Technical Chemistry, Karlsruhe, Germany
1 Dow Europe, Horgen, Switzerland
* Corresponding author (vehlow@itc-tab.fzk.de)
DOI: http://dx.doi.org/10.1065/espr2003.02.147
Abstract
Intention, Goal, Scope, Background. The halogen bromine is
far less abundant than chlorine, but it can be found at high
concentrations in special materials like flame retarded plastics.
The fate and effects of Br in waste incineration are not well
understood. It may have similar implications like Cl for the
volatilisation of heavy metals and the formation of low volatile
organic compounds. Due to its lower oxidation potential, there
is a risk of formation of elementary Br2 in the offgas.
Objective. Co-combustion tests of different types of Br contain-
ing plastic waste materials (up to 22%) and MSW in the
TAMARA pilot plant for waste incineration were conducted to
investigate the Br partitioning and the influence of Br on metal
volatilisation.
Methods. The Br inventory of the fuel mix was elevated to approx.
1 wt-%. All input and output mass flows of the furnace have been
sampled and the partitioning of Cl, Br, S, and a number of heavy
metals, has been calculated on the basis of closed mass balances.
Results and Discussion. Organically-bound Br was typically re-
leased to more than 90% into the raw gas. Elementary Br2 was
detected at high Br levels. Its presence was always analysed when
all SO2 in the raw gas was oxidised to SO3. Br enhances the
volatilisation of metals like K, Zn, Cd, Sn, Sb, and Pb out of the
fuel bed principally in the same way as Cl. The tests gave strong
indication that the promoting influence of the halogens on metal
volatilisation is more pronounced than that of the fuel bed tem-
perature. The volatilised metals are condensated on the fly ashes
and are discharged along with the filter ashes.
Conclusions. As long as a surplus of SO2 is present in the raw
gas no Br2 is formed. Although the halogen induced transfer out
of the fuel bed causes high concentrations of volatile metals in
the filter ashes, a recovery is not economically feasible for the
time being. The volatilisation gives no rise to metal emission
problems as long as efficient dedusting is achieved.
Recommendation and Outlook. If there is a risk of Br2 forma-
tion, in wet scrubbing a reducing agent has to be added to the
neutral scrubber for efficient abatement. Filter ashes should be
disposed of in a way that enables access for recovery in the fu-
ture. The exact volatilisation characteristics of the various metals
have to be studied in future using specifically tailored experiments.
Keywords: Bromine; chlorine; co-combustion; heavy metals; par-
titioning; plastic waste; volatilisation; waste from electrical and
electronic equipment; waste incineration
ESPR – Environ Sci & Pollut Res 10 (5) 329 – 334 (2003)
© ecomed publishers, D-86899 Landsberg, Germany and Ft. Worth/TX • Tokyo • Mumbai • Seoul • Melbourne • Paris
Bromine in Waste Incineration
Introduction
Bromine is the third element in the group of halogens and
its chemical properties are similar to those of the by far more
abundant chlorine. It is used for its chemical and biological
activity in special applications like photographic chemicals
and pharmaceuticals. Major Br products are flame retard-
ants and, hence, it is found in high concentrations, in part,
in some textiles and primarily in engineering plastics in the
electrical and electronic, as well as in the building industry.
End-of-life products from these sectors are main Br sources
in municipal solid waste.
There is not much valid information found in literature on
the effects of Br in waste incineration. The main reason for
this lack of knowledge is its low concentration in municipal
solid waste (MSW). However, since the disposal and espe-
cially the incineration of chlorine containing plastic waste is
of high public concern due to suspected dioxin formation, it
is no surprise to see this discussion being extended to waste
fractions with a higher Br inventory. Other potential effects
are the formation of elementary Br2 in the offgas and the
volatilisation of some toxic heavy metals, both in view of
emission implications.
Consequences could be expected for the disposal of plastic
waste from electrical and electronic equipment (WEEE), since
about 11% of the plastic material is flame retarded and some
applications make use of brominated organic compounds.
Other waste streams with a significant Br level due to their
flame retardancy are rigid polyurethane (PUR) and extruded
polystyrene foams (XPS) from the building sector.
The Forschungszentrum Karlsruhe and industrial project
groups under the umbrella of APME, the Association of
Plastics Manufacturers in Europe, have conducted semi-
technical tests on the behaviour of various fractions of Br-
containing end-of-life plastic materials in co-combustion
with municipal solid waste (MSW) (Mark 2000, Vehlow et
al. 1995, 2000, 2002). The tests were performed in the
TAMARA pilot plant for waste incineration located at the
Institute for Technical Chemistry in Karlsruhe, Germany.
The most important findings concerning the Br partition-
ing and the influence of Br on metal volatilisation are de-
scribed in this paper.
329
Bromine in Waste Incineration
1 Experimental Methods and Materials
All experimental investigations have been performed in the
Karlsruhe TAMARA pilot plant for waste incineration.
TAMARA is a scaled-down model of a grate combustion
furnace equipped with a boiler, a fabric filter and a two-
stage wet scrubbing system. The geometry of the combus-
tion chamber can be varied between a contra, centre and
parallel flow configuration by installation of variable roof
elements. All configurations have been used during the tests.
The thermal capacity of TAMARA is 0.5 MW at a through-
put of 200–300 kg/h. The basic fuel comprises typically 75
wt-% of shredded and homogenised residential waste and
25 wt-% of pelletised refuse derived fuel (RDF). This fuel
mix well represents today's Central European municipal solid
waste without separating or pre-sorting activities.
The investigation of Br partitioning and the effects of Br on
metal volatilisation were major topics of the co-combustion
trials with Br containing plastic waste fractions. The test
programmes in TAMARA hence comprised an extensive
sampling and analysis programme in order to establish bal-
ances not only for halogens, but also for metals. Samples
were taken from all input and output mass streams follow-
ing the recommendations of the International Ash Working
Group (International Ash Working Group 1997). Fly ashes
were not taken from the fabric filter discharge flow, but
isokinetically sampled in a gas duct downstream of the boiler.
From industrial waste incineration, it is known that, at high
Br concentrations in the fuel, elementary Br2 may be found in
the raw gas. Br2 is insufficiently absorbed in wet scrubbing
systems if no reducing agent is added to the neutral scrubber.
For the species-specific analysis of the total Br concentration
in the raw gas, hence, a special sampling train was used. The
train comprised a condenser, a first acidic scrubber for HBr
absorption, and a second neutral scrubber with the addition
of Na2S2O3 for the absorption of elementary Br2.
In two research programmes, plastic foams from the building
sector (PUR and XPS), flame retarded by brominated organic
compounds like HBCD and brominated polyols, were co-
combusted (Vehlow and Mark 1995). The addition of foams
was limited to 3 wt-% which accounted for approx. 20–30
vol-% of the input due to the low density of the material.
Various types of WEEE were subject of two further test pro-
grammes (Vehlow and Mark 2000). In the first programme,
up to 12 wt% of 3 plastic materials from the consumer (small
appliances, kitchen machines, PC, TV), commercial (medium
size parts, PC, fax machines), and industrial sector (mix of
electrical housings, printed circuit boards, main frame com-
puters) were added to the basic fuel. A fourth synthetic mate-
rial simulated the composition of the average European poly-
mer mixture for this sector today. The maximum Br inventory
in the fuel mix during this campaign was approx. 0.25 wt-%.
A second WEEE test campaign was conducted with an ad-
dition of other end-of-life flame retarded plastic materials.
This time up to 22 wt% of the plastic waste were added to
the reference waste fuel in order to increase the Br inventory
of the fuel mix up to 1 wt% and to check for the option of
Br recovery from the effluents of wet scrubbing systems
330
Review Articles
(Vehlow et al. 2002). The materials used were mixed WEEE
shredder residue (2 types), shredded television back and front
plates (2 types), and shredded printed wiring boards.
2 Parameters Controlling Element Volatilisation
All waste fractions contain metals. Their concentration varies
and so does their speciation. All different species from pure
metals to even rare compounds may be analysed. In plastic,
metals serve various purposes: they are used as catalysts, fill-
ers, flame retardants, or pigments, depending on their field of
application. Some plastic waste fractions, like Automotive
Shredder Residues (ASR), may contain pure metals as well as
inorganic and organic metal compounds (Mark 1998).
Metals of concern are Cu, Zn, Cd, Sn, Sb, Hg, and Pb. The
emission of these metals is subject to most legislative regula-
tions of air emission from waste incineration. That is why
the volatilisation of these metals into the raw gas was an
important topic to be investigated in the co-combustion tests.
The extremely volatile Hg was omitted, since it was only
present in traces in the co-combusted plastics.
The partitioning of elements in waste incineration is con-
trolled by a number of parameters:
• their speciation in the fuel,
• the total chemical composition of the fuel, that is the concentra-
tion and the speciation of major potential reactants with the ele-
ment in question,
• the temperature they are exposed to in the fuel bed on the grate
and
• the time of this exposure.
The fate of an element in a well defined, closed and homo-
geneous chemical system can in principle be predicted by
calculation of the thermodynamic equilibrium (Alvin 1977,
Frandsen 1994). The preferentially formed compounds are
characterised by negative free formation enthalpies. Ther-
modynamic data for many systems are available meanwhile
and commercial programmes can also be found for such
calculations (Barin 1996).
In the case of waste incineration, however, the chemical sys-
tem cannot be sufficiently defined, it is not homogeneous
nor closed. The chemical speciation of elements in the waste,
the temperature in the fuel bed, and the respective residence
time are widely unknown. Thermodynamic calculations are
therefore not meant to deliver precise transfer numbers for
a specific element in waste combustion. Such calculations,
nevertheless, supply valuable information concerning which
compounds are most likely formed, and thermodynamic
modeling is a useful tool to establish overall strategies for
the control of element fluxes.
Experimental investigations in waste incineration plants also
need to consider a number of factors which may limit their
accuracy:
• the waste fuel is rather inhomogeneous, even if its input is well
controlled by the crane operator,
• the mass flow of the solid residues like the grate ashes in full-
scale plants is mainly taken from long-term averages and its
error can be estimated to exceed 10%,
ESPR – Environ Sci & Pollut Res 10 (5) 2003
Review Articles
• the sampling and sample pretreatment – again first of all for the
inhomogeneous solids – may cause errors of more than 20%,
• the fuel bed temperature is unknown in full-scale plants, and
even in TAMARA it is only measured at 8 central positions along
the grate length.
The analytical error, in most cases, can be kept <1% and can
– compared to these major sources of error – be neglected.
Taking these impediments into account, the total error of the
inventory of homogeneously distributed major constituents
of the waste fuel like Cl is estimated to be at least ± 10%. The
determination of metals like Cu or Pb, which may partly be
present as metallic species in the input and in the grate ashes,
will suffer from higher errors and be on the order of ± 20%
and more. Hence, the following discussion of correlations be-
tween metal partitioning, halogens, and temperatures can only
provide indications and further theoretical as well as experi-
mental work is needed to establish a more exact description
of the interdependencies of the various parameters control-
ling the fate of elements in waste incineration.
A number of experimental results of element partitioning
derived from sampling experiments in full-scale plants have
been published (Brunner 1986, Schneider 1986, Reimann
1989, Angenend 1990, Belevi 2000). The data obtained re-
veal a significant correlation between the Cl inventory of
the fuel and the volatilisation of a number of metals. The
same correlation was found in the TAMARA pilot plant
which can be operated under much more defined conditions
than a full-scale waste incinerator (Vehlow 1996). The pro-
moting effect of Cl on metal volatilisation is easily explained
by the fact that the chlorides typically have lower boiling
points and higher vapour pressures than most other metal
compounds. Furthermore, the formation of chlorides is very
likely in the fuel bed in a waste incinerator, due to the rather
high Cl concentration of 0.5–1 wt-% in MSW.
According to its close chemical relationship, Br should have
the same effect as Cl for most volatile metals. In fact, the
Table 1: Boiling points of selected halogenides
Compound b.p. in °C
KCl 1407
KBr 1380
FeCl2 1012
FeBr2 967
Cu2Cl2 1367
Cu2Br2 1345
ZnCl2 732
ZnBr2 650
CdCl2 960
CdBr2 863
SnCl2 652
SnBr2 620
SbCl3 283
SbBr3 280
PbCl2 950
PbBr2 916
ESPR – Environ Sci & Pollut Res 10 (5) 2003
Bromine in Waste Incineration
boiling points of the bromides of the above mentioned met-
als are slightly lower then those of the respective chlorides,
as is documented in the compilation in Table 1. In MSW
incineration, no specific influence of Br will be detected, since
the Br level in MSW is typically lower than that of Cl by a
factor of 50–100 and the formation of bromides can be ne-
glected. However, it must be expected that, at an elevated
Br inventory of the fuel, those compounds are formed and
are to a great extent volatilised out of the fuel bed.
A comparison of chemical effects needs to be based on the
molar rather than on the mass concentration of the halo-
gens. The atomic weight of Br is approx. 80 amu compared
to approx. 35.5 amu of that of Cl. This fact, furthermore, is
impeding the evaluation of the influence of Br against that
of Cl on the volatilisation of metals.
3 Results and Discussion
3.1 Partitioning of Br
The prevailing combustion products of halogens in MSW
incineration are their hydrides (e.g. HCl, HBr), which are
released into the gas phase. The transfer of Cl into the raw
gas is approx. 80–90% of its inventory in the fuel (Interna-
tional Ash Working Group 1997). Br seems to stay in the
bottom ashes to a greater extent. Its balance is depicted in
Fig. 1 for the co-combustion of XPS foams at 950°C. The
partitioning found here is typical for all co-combustion tests
with Br containing plastics. It indicates that Br bound in or-
ganic matrices is almost totally transferred out of the fuel bed.
This can be explained by the fact that halogen containing or-
ganic compounds already decompose at lower temperature in
the pyrolysis and gasification zone on the grate, and release
halogen hydrides or short chain halogen containing organic
compounds into the gas phase (Lenz 1979). Inorganic halo-
gen compounds are typically decomposed or evaporated at
much higher temperature and hence have a greater tendency
to stay in the bottom ashes (Hunsinger 1994).
The total Br concentration measured in the raw gas during
the first WEEE campaign reached approx. 250 mg/m3. Up
to this level, HBr was the only detected Br species. In the
Fig. 1: Balance of Br during XPS co-combustion at 950°C
331
Bromine in Waste Incineration
Fig. 2: Partitioning of Br in the raw gas of the 2nd WEEE campaign
second campaign, the respective concentration was much
higher with a maximum of almost 1000 mg/m3. The parti-
tioning of Br between the residue compartments was the
same as obtained in the former test campaigns. At total Br
concentrations exceeding some 300 mg/m3, however, elemen-
tary Br2 was analysed in the raw gas. The raw gas Br
speciation in Fig. 2 documents that the share of this species
reached approx. 50% at high Br loads.
With increasing Br concentration in the raw gas, a decrease
of the SO2 concentration, and along with this the appear-
ance of SO3, was observed. The speciation of sulphur in the
raw gas is depicted in Fig. 3, again as a function of the total
Br concentration in the gas phase. Comparing both graphs,
it becomes obvious that elementary Br2 is detected as soon
as SO2 is no longer present in the gas phase.
This finding is explained by the overall redox reaction
Br2 + SO2 + H2O 2 HBr + SO3
Br2 has a high oxidation potential and oxidises SO2 rapidly
to SO3 by forming HBr. The presence of SO3 prior to the
observation of Br2 indicates most likely its intermediate for-
Fig. 3: Partitioning of S in the raw gas of the 2nd WEEE campaign
332
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mation already at lower total Br concentrations. To sup-
press the presence of Br2 in the gas phase, it is recommended
to care for a surplus of approx. 100 mg/m3'of SO2 (approx.
50 mg/m3 of S) in the raw gas which is normally reached in
MSW incineration.
During all experiments, at a high Br input, the second (neu-
tral) scrubber of the air pollution control system was oper-
ated with the addition of Na2S2O3. Under these conditions,
an emission concentration of Br in the order of 1 mg/m3
could be maintained.
3.2 Influence of Halogens and Fuel Bed Temperature on Metal
Volatilisation
In the following, the term volatilisation will be defined as the
fraction of the inventory of an element which is transferred
into the fly ash. The boiler ashes are excluded, since there is
always a risk of tailing effects from former experiments. The
gas phase is not taken into account, since no other metals than
Hg could be detected in the gaseous state at the filter tempera-
ture of the isokinetic sampling train of 180°C.
The results of the first tests of Br containing plastic waste
fractions in TAMARA (Vehlow 2000) gave an indication of
a promoting effect of Br on metal volatility. The volatilising
effect of Cl and an expected influence of the fuel bed tem-
perature, however, were difficult to be separated. The broader
range of Cl, Br, and temperature established in the later ex-
periments gave hope for better results.
If the assumption of a similar action of Cl and Br in view of
metal volatilisation is right, there should be a correlation
with the sum of the halogens and the temperature the fuel
was exposed to on the grate. For such evaluations,
volatilisation data from all plastic co-combustion tests were
plotted versus the accumulated halogen inventory of the fuel
and the maximum fuel bed temperature.
(1) The three-dimensional plots in Fig. 4 and Fig. 5 show a dis-
tinct correlation of the transfer of the volatile heavy metals
Cd and Sn with the accumulated halogen inventory. The
fuel bed temperature under these conditions seems to have
only a minor or even no effect. From this finding, it would
Fig. 4: Volatilisation of Cd as a function of the accumulated Cl+Br concen-
tration and the maximum fuel bed temperature
ESPR – Environ Sci & Pollut Res 10 (5) 2003
Review Articles Bromine in Waste Incineration

Fig. 5: Volatilisation of Sn as a function of the accumulated Cl+Br concen- Fig. 7: Volatilisation of Sn as a function of the Cl and Br inventory of dry fuel
tration and the maximum fuel bed temperature

appear that the probability of formation of metal halogenides

in the fuel bed is mainly controlling the volatilisation and over-
rules the expected strong influence of the fuel bed tempera-
ture on the evaporation of these compounds. Other metals
like K, Cu, Zn, Sb, and Pb show similar results with the halo-
gen influence by far overruling the temperature effect.

3.3 Separation of Cl and Br Influence

The broad range of variation of the Cl (0.2–1 mol/kg) and

Br (<0.001–0.12 mol/kg) inventory in the waste fuel mix
gave rise to look for the separate influence of the two halo-
gens on the volatility of selected heavy metals which has
been done in the diagrams of Fig. 6 to Fig. 9.
The highly volatile Cd (Fig. 6) shows a strong increase of its Fig. 8: Volatilisation of Cu as a function of the Cl and Br inventory of dry fuel
transfer into the fly ash already at low Cl concentrations. It
seems that in at an inventory of approx. 0.4 mol/kg – equiva-
lent to about 1.4 wt-% – almost all Cd is volatised. The
residual fraction staying in the bottom ash consists presum-
ably of silicates or other non-reactive Cd compounds. The
influence of Br is also rather high.
In the case of Sn (Fig. 7), the promoting influence of Cl is
more pronounced than that of Br, whereas for the moder-
ately volatile Cu (Fig. 8) the activity of Br seems to be much
higher than that of Cl. The low volatile Mo revealed only a

Fig. 9: Volatilisation of Mo as a function of the Cl and Br inventory of dry fuel

low effect of Cl, but a rather high effect of Br. Although Mo

Fig. 6: Volatilisation of Cd as a function of the Cl and Br inventory of dry fuel
is mainly forming MoO3 and molybdates during waste com-
bustion, there is a chance for the high temperature forma-
tion of chlorides as well (Strafford 1991) and it can be ex-
pected that this is also true for bromides (Fig. 9).
Similar results were obtained for K, Zn, Sb, and Pb, the
scattering of data, however, obscured a clear separation of
effects for some of these metals. A surprisingly well docu-
mented promotion effect of both halogens could even be
observed on the almost lithophilic Fe.

ESPR – Environ Sci & Pollut Res 10 (5) 2003 333

Bromine in Waste Incineration
4 Conclusions
Co-combustion tests of different types of Br containing plastic
waste materials and MSW in the TAMARA test incinerator
were performed looking for real effects in a modern waste
combustor. Up to 3 wt-% of plastic foams and 22 wt-% of
WEEE were added to pre-treated MSW as basic fuel. The Br
inventory of the waste fuel mix was thus increased up to
almost 1 wt-%. In view of the fate of Br and its effects on
metals, the following conclusions can be drawn from the
results obtained:
• Organically bound Br is almost totally released out of the fuel
inside the combustion chamber. The major fraction is staying in
the gas phase. This enables an easy recovery of a high fraction
of the Br inventory from the scrubber effluents.
• As long as a surplus of SO2 as a reducing agent is present, HBr
is the only species in the raw gas; otherwise elementary Br2 is
formed.
• The volatilisation of a number of metals is more dependent on
the inventory of Cl and Br in the fuel than on the fuel bed tem-
perature.
• Attempts to separate the effect of Br on the metal volatilisation
from that of Cl gave a strong indication that Br has a promoting
influence on the transfer of K, Fe, Cu, Zn, Mo, Cd, Sn, Sb, and Pb.
5 Recommendations and Outlook
The tests revealed a formation of elementary Br2 in the flue
gas at high Br concentrations in the waste fuel. Such forma-
tion can be prevented if care is taken to establish a SO2 sur-
plus in the raw gas. To prevent any emission problems if Br2
formation cannot be excluded, the addition of a reducing
agent to the neutral scrubber is strongly recommended in
the event of wet scrubbing.
The experiments corroborated the theoretical assumption that
Br has a similar promoting effect as Cl on the metal mobility
in the waste combustion process. The obtained indications
will be subject to detailed thermo-gravimetric investigations.
At a second stage, further pilot plant tests are planned with
more precisely adjusted combustion parameters.
Acknowlegement. The described projects have been supported by
the following associations: APME (Association of Plastics Manufactur-
ers in Europe), BFRIP (Brominated Flame Retardant Industry Panel),
EBFRIP (their European equivalent), EFRA (European Flame Retard-
ant association), FIEE (Fédération Française des Industries Electriques
et Electronics), FZK (Forschungszentrum Karlsruhe), ZVEI (Zentralver-
band der Elektro- und Elektronikindustrie).
A number of people from different companies have contributed to the
performance of the project: H. Geisert, H. Gramling, R. Härtel, H. Reis,
R. Siegel (FZK), H. Fisch, R. Martin (APME), L. Tange (Eurobrom B.V.
DSBG), D. Drohmann (Great Lakes Chemical), A. Jean (Elf Atochem),
J.M. Falguière (Du Pont), W. Pauli (ABB), M. de Poortere (EBFRIP/
BFRIP/EFRA), M. Rohr (Bayer). The authors are very grateful for all of
these contributions.
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Received: July 19th, 2002
Accepted: February 3rd, 2003
OnlineFirst: February 4th, 2003
ESPR – Environ Sci & Pollut Res 10 (5) 2003