Fuel 81 (2002) 18271833

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Gasication process of wastes containing PVC q

C. Borgianni a, P. De Filippis a, F. Pochetti a,*, M. Paolucci b
a

Department of Chemical Engineering, University of Rome La Sapienza, Via Eudossiana 18, 00184 Rome, Italy
b
Department of Physics, University of Rome Roma Tre, Via della Vasca Navale 84, 00146 Rome, Italy
Received 7 December 2001; revised 6 March 2002; accepted 13 March 2002; available online 19 April 2002

Abstract
Solid waste, in dealing with the growing presence of organic compounds, especially plastics, can be considered an important source of
energy since they are inexpensive and easily obtainable materials. However, the presence of polyvinyl chloride (PVC) in the waste can result
in a recycling problem when thermal treatment is involved.
This work shows the possibilities of recovering energy from waste containing PVC by a gasication process without additional dechlorination facilities.
Experimental data obtained in a bench scale two-stage reactor indicate that the addition of Na2CO3 in a blend containing refuse-derived
fuel (RDF) and PVC is efcient in eliminating chlorine from the produced off-gas. On the contrary, the less expensive calcium compounds do
not show a satisfactory chlorine removal. A thermodynamic simulation of the process substantially leads to the same results.
Starting from this study, the working conditions for gasifying waste blends containing PVC in a scaled-up two-stage reactor can be
predicted. According to the simulation, the obtained syngas shows that the polluting compounds content is lower than the Italian law limit. As
a consequence, it can be used directly to obtain electric power and/or local heating. q 2002 Elsevier Science Ltd. All rights reserved.
Keywords: Gasication; PVC; Gas dechlorination; Energy recovery

1. Introduction
The problem of disposal of municipal wastes due to
declining landll capacity, together with the increasing
cost of petroleum products, has encouraged research on
the possibility of their conversion into useful forms of
energy or chemical products. Solid waste, in fact, in dealing
with the growing presence of organic compounds, especially plastics, can be considered an important source of
energy since they are inexpensive and easily obtainable
materials. Among plastics, polyvinyl chloride (PVC) gives
an important contribution. PVC, in fact, due to its chemical
and mechanical characteristics, is widely used in building,
transport, packaging, electrical/electronic and healthcare
applications [1] and, with an annual world output of 19
millions tons, is second only to polyethylene for the
volumes of thermoplastic materials produced [2]. The
simplest and most effective method for recovering energy
from solid wastes is incineration. This process can utilise a
wide variety of materials, but the presence of PVC can result
in a recycling problem. PVC, in fact, due to its high chlorine
* Corresponding author. Tel.: 139-644-585566; fax: 139-644-585416.
E-mail address: fausto.pochetti@uniroma1.it (F. Pochetti).
q
Published rst on the web via Fuelrst.comhttp://www.fuelrst.com

content, causes pollution problems, mainly hydrochloric

acid, chlorine gas and dioxins, when thermal treatment is
involved [3,4]. As a result, it becomes mandatory to clean
the chlorine-containing gases.
An alternative to solid waste incineration is pyrolysis or
gasication. Pyrolysis has been extensively studied, but the
production of large amounts of char and tar, which are difcult to handle, limits its application. The gasication of solid
waste, on the contrary, can be considered as an extension of
the well-known technology of coal gasication. Although
its feasibility has been demonstrated for several years [57],
only recent studies have been carried out to develop
processes for energetic waste utilisation. The two gasication processes that involve PVC are those developed by
Akzo Nobel and Linde KCA. Both require facilities to
treat chlorine compounds [8,9].
The aim of this work is to demonstrate the possibilities of
recycling PVC by gasication processes without additional
dechlorination facilities. The feasibility of this process is
examined through a bench scale two-stage reactor. To
increase PVC heating value and to prevent the agglomeration of particles and adhesion to the inner wall of the feeder,
PVC has been blended with refuse-derived fuel (RDF)
and other chlorine-reacting substances forming inert
compounds.

0016-2361/02/$ - see front matter q 2002 Elsevier Science Ltd. All rights reserved.
PII: S 0016-236 1(02)00097-2

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C. Borgianni et al. / Fuel 81 (2002) 18271833

Table 1
Physical and chemical characteristics of the used RDF
Physical properties
Humidity
Volatile substance (dry basis)
Fixed carbon (dry basis)
Ash (dry basis)
Size
HHV

3.67% mass
73.06% mass
13.16% mass
13.78% mass
, 1 mm
17.50 MJ/kg

Chemical analysis (mass % dry basis)

Carbon
Hydrogen
Nitrogen
Oxygen
Sulphur
Chlorine

47.80
6.80
1.87
29.75
, 0.1
, 0.1

The thermal treatment of this blend should guarantee:

an overall blend conversion;

a gas with great heating value;
the absence of tar;
a reduced amount of unburned stuff;
the absence of chlorine-containing substances in the gas
coming from the reactor.

The results of the work were also used to test a simple

thermodynamic model useful for predicting the performance of a scaled-up two-stage gasication reactor.
2. Experimental
2.1. Materials
The RDF used in the gasication tests was supplied by
AMA (Municipal Environment Company of Rome). Prior to
use, the RDF was ground and mixed in order to obtain a
homogeneous mixture with a grain size suitable for feeding
the bench scale apparatus. The physical and chemical
characteristics of the used RDF were determined.
The physical properties measured included ash content,
humidity, volatile matter, xed carbon and the higher
heating value (HHV). The chemical analysis included the
determination of the elements C, H, N, O, S and Cl. The
results of these analyses are presented in Table 1. PVC high
molecular weight (MW approximately 200,000), supplied by
BDH, Na2CO3, CaO and Ca(OH)2, supplied by Aldrich,
were also used.
2.2. Apparatus and operative conditions
The gasication process, shown schematically in Fig. 1, is

Fig. 1. Schematic diagram of the bench scale gasication unit.

C. Borgianni et al. / Fuel 81 (2002) 18271833

composed of two main sections: reaction and product

collection.
The reaction section consists of two vertical stages in
series. Stage one is constructed from a 50 mm i.d. by
500 mm length quartz tube equipped with a quartz frite on
the bottom side. Stage two is a 30 mm i.d. by 700 mm length
quartz tube lled with 4 mm diameter alumina spheres.
Each stage reaches the desired working temperature by
means of electrical resistances. The temperature of the
two stages is measured through two thermocouples placed
inside the quartz tubes. The apparatus for feeding the reactor
is in between the two stages.
The RDF, or the RDF blend, was fed into the reactor by
gravity at a uniform volumetric rate supplied by an adjustable feed rate screw feeder. The amount of sample fed in
each run was about 25 g. The small amount of material
sticking to the screw-feeder, hopper and feed connection
was neglected.
The charge, once introduced into the reactor, is immediately pyrolysed. Due to gravity, char goes to the bottom of
stage one and meets the gasifying mixture consisting of
steam and oxygen, introduced through the quartz frite at
the bottom of stage one. The mixture, which mainly consists
of hydrogen, carbon monoxide, carbon dioxide, gaseous
hydrocarbons, volatile and non-volatile substances, ows
up to stage two. In this stage, tar, liquid and heavy
hydrocarbons, trapped in the package, increase their
residence time allowing for complete gasication and
reforming in accordance with the following reactions:

1829

both a kinetic and a thermodynamic point of view, avoiding

the presence of C2 or higher hydrocarbons.
The off-gas from stage two was cooled in a water-cooled
exchanger. The resulting condensed steam was collected in
a receiver, and weighed and analysed for determining the
chlorine content. The gas was then passed through two
sodium hydroxide traps in order to collect all the chlorine
eventually present and dried with a calcium chloride trap.
The amount of gas produced was measured with a dry
meter; at pre-xed times, samples of the produced gas
were drawn out down to the calcium chloride traps and
their composition analysed by a gas-chromatography
equipped with a thermal conductivity detector.
At the end of each test, ashes in the frite were analysed to
determine the carbon and chlorine content.
The reactor operated at atmospheric pressure. To assure
safe working conditions, the charge blend was introduced
before starting the oxygen injection. This way, the blend
undergoes immediate pyrolysis, producing char that in
turn goes to the bottom of stage one and reacts with the
oxygen when introduced. This avoids the formation of
explosive mixtures in the gas phase.
CaO, Ca(OH)2, and Na2CO3, when used, were mixed with
the charge before the introduction in the reactor.
3. Results and discussion
Preliminary gasication tests, conducted with only RDF
as feed, were carried out in order to investigate the inuence
of the operating conditions with respect to the amount of
unreacted material in the residue and to the off-gas heating
value. The parameters investigated were: injected oxygen/
charge ratio ranging from 0.035 to 0.149 kgO2/kgRDF;
steam ow-rate of 70 and 160 L(STP)/h; stage one temperature of 500, 600 and 700 8C, while the stage two temperature
was kept constant and equal to 1000 8C. Stage one temperatures lower than 500 8C were not considered because they
did not assure complete pyrolysis of the RDF used. The
main results are reported in Tables 2 and 3.
Table 2 shows the positive effect of the increase of steam
and oxygen injection in reducing the unreacted materials in

Cs 1CO2g ! 2CO
Cs 1H2 Og ! COg 1H2
COg 1H2 Og ! CO2g 1H2
Cn H2m 1 nH2 O ! nCO 1 m 1 nH2
Cn H2m 1 nCO2 ! 2nCO 1 2mH2
The working conditions of this stage are chosen in order to
support the reforming reactions of all hydrocarbons from
Table 2
Effect of oxygen injection and steam ow-rate on the off-gas characteristics
Run no.

Stage one temperature (8C)

Steam ow rate (L(STP)/h)
Injected O2 (kgO2/kgRDF)
H2 (%vol.)
CO (%vol.)
CO2 (%vol.)
CH4 (%vol.)
3
Yield in dry gas (m(STP)
kg)
3
Heating Value (MJ/m(STP)
)
Unreacted material in the
residue (% mass)

500
160
0.035
74.66
8.87
10.98
5.49
0.80
11.15
50.6

500
70
0.060
75.85
10.12
5.19
8.84
1.13
12.64
31.1

500
160
0.065
76.37
10.12
6.31
7.20
1.32
12.11
19.6

500
70
0.115
75.75
9.68
5.91
8.66
1.23
12.51
25.5

500
160
0.116
74.62
10.81
6.02
8.56
1.27
12.49
16.8

500
160
0.149
74.66
8.87
10.98
5.49
1.42
10.59
11.05

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C. Borgianni et al. / Fuel 81 (2002) 18271833

Table 3
Percentage of unreacted material in the residue as a function of stage one
temperature
T (8C)

Steam ow
rate (L(STP)/h)

Injected O2
(kgO2/kgRDF)

Unreacted material in
the residue (% mass)

500
500
600
600
700
700

160
160
160
160
160
160

0.035
0.116
0.035
0.116
0.035
0.116

50.6
16.8
13.7
4.5
4.2
0.2

the residue, while the gas composition does not change

extensively. This is normal behaviour for a two-stage
reactor, where the gas composition mainly depends on the
characteristics of the charge and the temperature of stage
two. However, when the amount of injected oxygen
increases too much, i.e. the injected oxygen charge ratio is
higher than 0.116 (run 6), the rise observed in the CO2 value
indicates that the reactor is near the condition of RDF
combustion. Moreover, the data in Table 3 show, as
expected, that the higher the stage one temperature, the
lower is the unreacted material in the residue.
From the analysis of the reported data, the chosen operative
conditions for the gasication of the RDFPVC blend were:
1. steam ow-rate 160 L(STP)/h,
2. injected oxygen 0.116 gO2/g of charge fed,
3. total oxygen 0.41 gO2/g of blend, considering that
0.29 gO2/g of blend are already in the sample,
4. rst stage temperature 600 8C,
5. second stage temperature 1000 8C.
The addition of PVC to the RDF has as a consequence an
unexpected increase of unreacted materials in the residue
and a reduction of the heating value of the gas produced.
These effects are attributed to the presence of chlorine

compounds, well known for slowing the combustion [10].

On the contrary, the addition of alkaline compounds to the
blend has a positive effect on the amount of unreacted materials in the residue. The effect is remarkable when Na2CO3 is
used. This is in accordance with the known effect of alkaline
substance in coke gasication, where it acts as a catalyst,
increasing the Boudouard reaction rate [11,12].
Table 4 reports a comparison of typical gasication
results when only RDF, RDF 1 10%wt PVC and
RDF 1 10%wt PVC 1 Na2CO3 were used as reactor charge.
In order to check the efciency of alkaline compounds in
chlorine removal from the produced syngas, various
amounts of CaO, Na2CO3 and Ca(OH)2 were added and
mixed with the RDFPVC blend. The obtained results in
Table 5 show that CaO does not permit a satisfactory level
of chlorine removal, even if a double amount is added in
respect to the stoichiometry. Ca(OH)2 shows similar results
to CaO. On the contrary, sodium carbonate is efcient even
if only 1.2 times the stoichiometry is added. With this addition, an efcient chlorine removal is obtained even when the
PVC percentage in the blend is 20%.
The different efciency observed between calcium and
sodium compounds justies the use of the more expensive
sodium carbonate in chlorine removal operations.

4. Thermodynamic model and data comparison

The model is based on the heat and mass balance carried
out taking into consideration that CO, CO2, H2, CH4 and
H2O are present at the exit of each stage at a concentration
predicted by the water-gas shift and reforming equilibrium.
It was supposed that the thermal cracking reactions occurring in stage one are very fast and the rate-determining step
was considered to be the reaction between char and oxidising compounds. This is supported by the presence of
unburned char. The reactions occurring at the gaseous
state were considered to be at their chemical equilibrium.

Table 4
Comparison of typical gasication results
Working condition and
obtained results
Steam feed rate (L(STP)/h)
Injected oxygen/charge
ratio (kg/kg)
Stage one T (8C)
Stage two T (8C)
Unreacted materials in
residue (%)
H2 (%vol.)
CO (%vol.)
CO2 (%vol.)
CH4 (%vol.)
3
Heating value (MJ/m(STP)
)
Yield in dry gas (Nm 3/kg)
Tar dragged by the gas

RDF

RDF 1 PVC

RDF 1 PVC 1 Na2CO3

160
0.116

160
0.116

160
0.116

600
1000
4.5 ^ 1

600
1000
28.5 ^ 3

600
1000
9.9 ^ 2

73.04
8.89
9.77
8.30
11.99
1.55
Absent

69.6
11.4
13.5
5.5
10.92
0.697
Absent

71.7
10.0
12.4
5.9
11.13
1.19
Absent

C. Borgianni et al. / Fuel 81 (2002) 18271833

1831

Table 5
Alkaline compound efciency in chlorine removal during RDF 1 PVC gasication
PVC (mass %)

Reagent type

PVC/reagent ratio

Steam (L(STP)/h)

Feed Cl (g)

Cl in syngas (g)

Cl in ash (g)

10
10
10
10
10
10
10
10
10
10
10
20

CaO
CaO
Ca(OH)2
Ca(OH)2
Na2CO3
Na2CO3
Na2CO3
Na2CO3
Na2CO3
Na2CO3
Na2CO3

Stoichiometric
2 stoichiometric
Stoichiometric
2 stoichiometric
Stoichiometric
Stoichiometric
Stoichiometric
2 stoichiometric
1.2 stoichiometric
1.2 stoichiometric
1.2 stoichiometric

160
160
160
170
180
160
190
190
190
160
190
170

1.43
1.32
1.32
1.35
1.33
1.36
1.34
1.33
1.39
1.34
1.34
2.84

1.28
0.27
0.25
0.38
0.30
0.11
0.25
0.21
. 0.01
. 0.01
. 0.01
. 0.01

0.14
1.05
1.07
0.97
1.03
1.25
1.09
1.12
1.39
1.34
1.34
2.84

In the simple case where only oxygen is injected, and

impurities such as sulphur and chlorine are not taken into
account, the model equations are:
1
nCO 1 nCO2 1 nCH4 nC
nH2 1 nH2 O 1 2nCH4 nH

0:5nCO 1 nCO2 1 0:5nH2 O nO

nCO2 nH2 =nCO nH2 O Kw

P2 n2t nCO n3H2 =nCH4 nH2 O Kr

nt nCO 1 nCO2 1 nCH4 1 nH2 O 1 nH2 nC 1 nH 2 2nCH4

6
where nO nOw 1 nOj ; n number of kmoles of the
chemical species indicated in the footnote; nt number of
total kmoles at the gaseous state; nOw number of oxygen
kmoles contained in the waste; nOj number of kmoles of
injected oxygen; Kw value of the equilibrium constant of
the water-shift reaction at the test temperature; Kr value
of the equilibrium constant of the reforming reaction at the
test temperature; and P exercise pressure (bar). The
system of six equations and six unknowns, namely nCO,
nCO2 , nCH4 , nH2 O , nH2 and nt, was solved using the conventional Newton method.
In assessing the carbon mass balance, the char that

experimental data show in the residue was considered as

unreacted carbon. If desulphurisation and dechlorination
reactions, indicated as deS and deCl, are taken into account,
the reaction of the formation of HCl and H2S from the blend
during its cracking is considered very rapid, together with
the deCl and deS reactions with Na2CO3 and CaCO3,
respectively. As a consequence, the equilibrium values
have been considered. The relevant thermodynamic data
are taken from the Barin compilation [13].
Table 6 shows the comparison between experimental data
and thermodynamic predictions when a blend containing
10% of PVC is gasied. The prediction and the experimental data are related to the off-gas from stage two.
As experimental data show, due to the absence of an
appropriate catalyst, the reforming reactions are far from
the equilibrium (as supported by the presence of methane
in the produced syngas), and this does not allow for a
completely correct thermodynamic prediction. A better
prediction can be obtained considering only the watershift equilibrium. Table 6 shows that, in this case, the agreement between predicted and experimental data is rather
satisfactory, especially if hydrogen and yield in dry gas
are considered.
As reported in Table 7, the thermodynamic prediction
obtained for chlorine, both in the case of sodium and
calcium compounds, is also in good agreement with the
experimental results.
The chlorine calculations were performed considering the

Table 6
Comparison between experimental data and thermodynamic predictions in a blend containing 10% of PVC
Dry gas composition

H2 (%vol.)
CO (%vol.)
CO2 (%vol.)
CH4 (%vol.)
3
Yield in dry gas m(STP)
/kg

Experimental

69.61
11.38
13.38
5.53
0.697

Thermodynamic predictions
Reforming and
water-shift reaction

Water-shift reaction

68.36
23.55
6.29
0.00
0.741

65.74
20.70
8.36
3.29
0.683

1832

C. Borgianni et al. / Fuel 81 (2002) 18271833

Table 7
Comparison between experimental and calculated value of Chlorine
removal using sodium (1.2 times the stoichiometry) and calcium
compounds (2 times the stoichiometry)

ing gases is extremely low. Conversely, CaO is able to lower

the sulphur content of syngas below the law limit under
every gasication condition.

Cl removal (%)

Na2CO3
CaO
Ca(OH)2

Experimental

Calculated

. 99.9
81.1
77.4

100
83
79

conditions of stage one where the deCl reaction occurs. Both

experimental data and predictions refer to the amount of
chlorine derived from the HCl present in the syngas,
neglecting the presence of NaCl, which indeed is increasingly important for temperatures higher than 873 K.
The results of Table 7 imply that the assumption of a very
fast deCl reaction is correct. Fig. 2 shows that deCl grows
higher when decreasing the injected oxygen amount. Higher
oxygen means higher CO2 and H2O in the gas phase, and
that makes the reaction more difcult. Fig. 2 also shows the
efciency of CaO in deCl; the calculations were performed
taking into account that CO2 lowers the CaO activity at
873 K (600 8C). In agreement with the experimental results,
the addition of CaO is not satisfactory to obtain acceptable
residual chlorine content of syngas, except when the
reaction is performed under strong reducing conditions. In
accordance with Fig. 2, the worse behaviour of Ca(OH)2 in
respect to CaO is easily explained considering that, at the
reaction temperatures, hydroxide is completely transformed
in oxide releasing H2O with the effect of hindering the deCl
reaction.
On the contrary, thermodynamic predictions for deS, as
reported in Fig. 3, show that Na2CO3 is not able to lower the
sulphur content of syngas below the limit of the present
Italian law, i.e. 2 mg/m, unless the concentration of oxidis-

5. Demonstrative plant simulation

Using the described thermodynamic model, the working
conditions for a scaled-up reactor able to gasify important
amounts of RDFPVC blends, can be predicted.
On the basis of the experimental data, the thermodynamic
simulations have been performed considering two blends,
namely 10% and 20% PVC and an amount of Na2CO3 equal
to 1.2 times the stoichiometric amount. The work pressure
was assumed equal to1 bar.
The reactor considered is a two-stage reactor, fed with a
blend of RDF, PVC, Na2CO3 and eventually CaCO3. The
oxygen and steam necessary for gasication and for reaching the desired stage temperature, are injected at the bottom
of stage one, while an additional oxygen injection is also
given at the bottom of stage two.
The stage one temperature should be about 600 8C,
because experimental data show that the lower the temperature, the higher the amount of unburned char, even if
Na2CO3 was present. On the contrary, higher temperatures
involve an important NaCl evaporation that could originate
corrosion problems.
To predict the temperature of each stage, the HHV of RDF
has been considered to be equal to that found experimentally,
namely 17.5 MJ/kg, while a value of 9.5 MJ/kg is taken into
account for PVC. The thermal loss through the reactor wall
has been estimated to be 10% of the involved overall heat,
while ash and NaCl go out at the temperature of stage one.
The stage one temperature, i.e. 600 8C, is reached by
3
injecting 0.5 m(STP)
O2/kgblend. The amount of Na2CO3
added is 1 kg/kg PVC. Provided that Na2CO3 is not able

Fig. 2. Effect of CO2 and H2O on deCl (T 873 K; P 1 bar)

C. Borgianni et al. / Fuel 81 (2002) 18271833

1833

Fig. 3. Effect of CO2 and H2O on deS (T 873 K; P 1 bar)

to reduce the sulphur in syngas under the actual conditions

in an efcient manner, a contemporaneous addition of
CaCO3 in an amount double that of the stoichiometric is
necessary if sulphur is present.
In order to reach a stage two temperature of at least
3
850 8C, an injection of 0.150 m(STP)
O2/kgblend is necessary.
A syngas temperature of 850 8C is, in fact, the lowest
temperature necessary to assure the reaching of the chemical equilibrium of the water shift reaction [14]. Under these
conditions, the resulting syngas is characterised by a H2/CO
ratio and (CO 1 H2) equal to 1.75 and 54.73%, respectively,
and therefore it is useful for producing local heating and/or
electric power.
The calculated overall chlorine content of syngas
3
(NaCl 1 HCl) is 3.2 and 3.7 mg/m(STP)
for 10% PVC and
20% PVC, respectively. These data are lower than those of
the Italian law, namely 5 mg/m 3 (STP). Dioxins and NOx,
are well under the law limits.
Simulations performed considering a work pressure of
10 bar indicated a worsening of the deCl ability of
3
Na2CO3 (12.1 mg/m(STP)
against 3.2), due to the higher
percentage of CO2 present at stage one.

6. Conclusions
Experimental data obtained with a bench scale two-stage
reactor indicate that Na2CO3 is efcient in eliminating chlorine evolving from blends consisting of RDF and PVC and
containing up to 20% of the latter. On the contrary, the less
expensive calcium compounds do not show a satisfactory
chlorine removal.
The data indicate also that stage one temperature, O2/
charge ratio and Na2CO3 addition act positively on the
amount of unburned char. Stage two temperature at

1000 8C is sufcient to avoid the presence of tar in the

exhausting syngas.
A thermodynamic simulation of the process substantially
leads to the same results.
Starting from these results, the working conditions for gasifying blends with PVC in a demonstrative two-stage reactor
have been predicted. According to the simulation, the obtained
syngas shows a polluting compounds content lower than
that of the Italian law limit. As a consequence, it can be
used directly to obtain electric power and/or local heating.
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