Long glass fiber thermoplastics - Fiber Reinforced Polymer

Long glass fiber thermoplastics - Fiber Reinforced Polymer Long glass fiber thermoplastics - Fiber Reinforced Polymer

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Long glass fiber thermoplastics Material classification and characterisation 1. Introduction There has been a rapid and steady growth in the use of long fiber reinforced plastics in recent years. This has been achieved due to their potential of combining high performance / price ratios - such as reduced weight, corrosion resistance, great design and styling flexibility - with rapid clean processability and the attraction of their intrinsic recyclability. Since the early 80ties thermoplastic composites (TC) in structural applications have played a greater role in the automotive industry. The combination of high volume processing, and high end-use properties and lower system costs, is a strong driving force for further applications. Furthermore their high integration potential - the consolidation of various parts into one single component - is rapidly being recognised as a major advantage in comparison to traditional materials. Typical automotive applications are dashboard carriers, technical front-ends, seat shells, bumber carrier, battery trays, spare wheel dwells and – as one of the most rapid growing markets - complete underfloor systems. 2. New material and process developements For a long time, the main driving force for new thermoplastic composite applications, was represented by Glass Mat reinforced thermoplastics (GMT). Random in-plane fiber reinforced GMT-sheets can be prepared by melt impregnation of non-woven glass mats (dry process), or by mixing chopped fibers with polymer powder in a fluid medium, followed by straining, drying and consolidation (wet process). GMT sheets were heated up in an oven system and pressed to complex parts in a press forming process. Although the GMT process is an established and well known technology, it´s role of a ´trailblazer´ for new and innovative applications is being challenged. Caused by the necessity of massive cost savings - a clear demand especially from the automotive industry - a number of alternative materials and processes has been developed in the last years. Long fiber reinforced granulates (LFG), pellets and chips (STC), prepared by wirecoating, crosshead extrusion or several pultrusion techniques were introduced 10 years ago, recent developments in this area are based on commingling and powder impregnation techniques. These long fiber granulates are suitable both for the classic injection moulding process (IM) and the injection compression moulding process (ICM) as well as for the extrusion compression moulding process (ECM). Common to all these processes is a plastification unit in form of an injection or extrusion screw which is the mainspring for the process intrinsic deficit - an apparent fiber length degradation in the finished part /1-4/.

<strong>Long</strong> <strong>glass</strong> <strong>fiber</strong> <strong>thermoplastics</strong><br />

Material classification and characterisation<br />

1. Introduction<br />

There has been a rapid and steady growth<br />

in the use of long <strong>fiber</strong> reinforced plastics in<br />

recent years. This has been achieved due to<br />

their potential of combining high performance<br />

/ price ratios - such as reduced weight,<br />

corrosion resistance, great design and styling<br />

flexibility - with rapid clean processability<br />

and the attraction of their intrinsic recyclability.<br />

Since the early 80ties thermoplastic composites<br />

(TC) in structural applications have<br />

played a greater role in the automotive industry.<br />

The combination of high volume<br />

processing, and high end-use properties<br />

and lower system costs, is a strong driving<br />

force for further applications. Furthermore<br />

their high integration potential - the consolidation<br />

of various parts into one single component<br />

- is rapidly being recognised as a<br />

major advantage in comparison to traditional<br />

materials. Typical automotive applications<br />

are dashboard carriers, technical front-ends,<br />

seat shells, bumber carrier, battery trays,<br />

spare wheel dwells and – as one of the<br />

most rapid growing markets - complete underfloor<br />

systems.<br />

2. New material and process developements<br />

For a long time, the main driving force for<br />

new thermoplastic composite applications,<br />

was represented by Glass Mat reinforced<br />

<strong>thermoplastics</strong> (GMT). Random in-plane<br />

<strong>fiber</strong> reinforced GMT-sheets can be prepared<br />

by melt impregnation of non-woven<br />

<strong>glass</strong> mats (dry process), or by mixing<br />

chopped <strong>fiber</strong>s with polymer powder in a<br />

fluid medium, followed by straining, drying<br />

and consolidation (wet process). GMT<br />

sheets were heated up in an oven system<br />

and pressed to complex parts in a press<br />

forming process. Although the GMT process<br />

is an established and well known technology,<br />

it´s role of a ´trailblazer´ for new and<br />

innovative applications is being challenged.<br />

Caused by the necessity of massive cost<br />

savings - a clear demand especially from<br />

the automotive industry - a number of alternative<br />

materials and processes has been<br />

developed in the last years.<br />

<strong>Long</strong> <strong>fiber</strong> reinforced granulates (LFG), pellets<br />

and chips (STC), prepared by wirecoating,<br />

crosshead extrusion or several pultrusion<br />

techniques were introduced 10 years<br />

ago, recent developments in this area are<br />

based on commingling and powder impregnation<br />

techniques.<br />

These long <strong>fiber</strong> granulates are suitable<br />

both for the classic injection moulding process<br />

(IM) and the injection compression<br />

moulding process (ICM) as well as for the<br />

extrusion compression moulding process<br />

(ECM).<br />

Common to all these processes is a plastification<br />

unit in form of an injection or extrusion<br />

screw which is the mainspring for the<br />

process intrinsic deficit - an apparent <strong>fiber</strong><br />

length degradation in the finished part /1-4/.


This typical reduction of the <strong>fiber</strong> length is<br />

irrespective of massive ameliorations in the<br />

field of the plastification systems (screw<br />

geometrie, mixing zones, etc.), and optimised<br />

process parameters (screw speed,<br />

injection speed, back pressure, etc.).<br />

av. <strong>fiber</strong> length lm [mm]<br />

25<br />

20<br />

15<br />

10<br />

5<br />

0<br />

basis length<br />

zone 46<br />

zone 32<br />

zone 27<br />

Picture 1: Typical degradation of the average<br />

<strong>fiber</strong> length, found in ECM-process (PP-<br />

LFG25mm, 40% <strong>glass</strong> content)<br />

Specifically in closed mould operation – like<br />

in the injection moulding process - the additional<br />

<strong>fiber</strong> length reduction in the nozzle,<br />

the gating system and the mould itself<br />

(geometrie, radii. etc.) must be taken into<br />

consideration to minimize <strong>fiber</strong> breaking and<br />

nonuniform physical properties in the finished<br />

part /1-5/.<br />

A real breaktrough in thermoplastic composites<br />

was the idea of combining the compounding<br />

of a long <strong>fiber</strong> reinforced thermoplastic<br />

material directly with the final part<br />

production process. The reinforcing <strong>fiber</strong>s<br />

were incorporated and impregnated with the<br />

PP-matrix directly during the compounding<br />

and plastification process of the thermoplastic<br />

composite (DIF-process). The leaving<br />

out of semifinished products, like blanks<br />

zone 16<br />

screw zone<br />

zone 1<br />

extruder<br />

head<br />

plastificat<br />

part<br />

or pellets, leads to a clear benefit concerning<br />

to the material and process costs.<br />

The main developments were performed in<br />

the area of extrusion compression moulding.<br />

These process technologies could be differentiated<br />

by different compounding methods<br />

(single or double screw extruder), impregnation<br />

methods (direct feeding or accessory<br />

systems), reinforcing material basis<br />

(chopped or endless <strong>fiber</strong>s), matrix material<br />

(PP in form of granulats, powder or water<br />

dispersion) /6-13/. Although the development<br />

of modified injection moulding processes<br />

was started almost 10 years ago, a<br />

broad industrial introduction of these systems<br />

is expected previously for the next<br />

years /14-18/. But the cut off of the semifinished<br />

material step also has some drawbacks<br />

- the part producer is not only responsible<br />

for the final production but additionally<br />

for the homogenisation and preparation<br />

of the raw materials and the material<br />

classification and quality. Furthermore is<br />

has to be noted that an in line compounding<br />

system needs higher investment costs and<br />

skilful service personal.<br />

Regarding all these developments on the<br />

field of new materials and different processes,<br />

the part producer is confronted with<br />

the question which kind of process and<br />

which kind of material is the right decision.<br />

On the one hand he has to fulfill the demands<br />

and requirements of his customer for<br />

a specific part - on the other hand he has to<br />

produce on a cost level which is accepted<br />

by the market.


One of the main tasks in future projects<br />

could be the qualified comparison of different<br />

types of materials in one and the same<br />

application, the assessment of different processes<br />

and the efficiency of process parameters.<br />

Therefore a basic understanding<br />

of the general influencing factors by the designers<br />

and the engineers is a very important<br />

condition for a better understanding of<br />

the performance, the advantages and the<br />

limitations of long <strong>fiber</strong> reinforced <strong>thermoplastics</strong>.<br />

3. Material basics of long <strong>fiber</strong> reinforced<br />

<strong>thermoplastics</strong><br />

The mechanical properties of a part made of<br />

reinforced <strong>thermoplastics</strong> are defined by the<br />

matrix system, the <strong>fiber</strong>s, the <strong>fiber</strong> content<br />

and most of all by the orientation of the reinforcing<br />

<strong>fiber</strong>s. High performance levels<br />

can only be obtained from a composite part<br />

with high <strong>fiber</strong> concentrations and if the reinforcing<br />

<strong>fiber</strong>s in the final product have a<br />

sufficiently high aspect ratio - which defines<br />

the length to diameter relation of a single<br />

<strong>fiber</strong>. Mainly affected on different, flow induced<br />

<strong>fiber</strong> orientations, it is usual that a<br />

great variation of properties could be found<br />

over a part. The orientation and the length<br />

of the <strong>fiber</strong>s are distinctly influenced by the<br />

production process and the variation of process<br />

parameters. This is the reason why<br />

different mechanical values may be found<br />

on identical parts produced by different<br />

technologies and why a comparison of different<br />

materials is rather difficult although<br />

the part geometry is the same. Even in the<br />

same zone a difference of the mechanical<br />

properties as a function of the traction angle<br />

applied, may be found /19/.<br />

It is obvious that measuring or indicating<br />

single values – wheater it is a young´s module,<br />

a tensile strength or a charpy impact<br />

energy – which is often required and practiced<br />

- is no sufficient method to handle the<br />

complexity of these kind of materials.<br />

3.1 Influence of the <strong>fiber</strong> orientation and<br />

the <strong>fiber</strong> length on the mechanical properties<br />

relative quantity [%]<br />

9,00<br />

8,00<br />

7,00<br />

6,00<br />

5,00<br />

4,00<br />

3,00<br />

2,00<br />

1,00<br />

0,00<br />

Modulus [Mpa]<br />

-90°<br />

0°<br />

-80° -60° -40° -20° 0° 20° 40° 60° 80°<br />

traction angle [°]<br />

6000<br />

5000<br />

4000<br />

3000<br />

2000<br />

1000<br />

Picture 2: Prediction of the tensile modulus<br />

for a flow orientated 40%-GMT (below)<br />

based on X-ray testing (on top) and orientation<br />

related quantification by picture analysis<br />

(middle)<br />

0<br />

90°<br />

10 mm<br />

10 mm<br />

-90 -80 -70 -60 -50 -40 -30 -20 -10 0 10 20 30 40 50 60 70 80 90<br />

traction angle [°]


���� [ - ]<br />

Normalized Properties<br />

With models, founded on the theory of Halpin<br />

& Tsai it is possible to predict the stiffness<br />

of long <strong>fiber</strong> reinforced materials with a<br />

sufficient accuracy /20-21/. Although a<br />

number of models for the prediction of composite<br />

strength and impact properties exist,<br />

there is no appropriate simulation method<br />

for the practice /22-25/.<br />

Recent methods are based on X-ray analysis<br />

of test plates and cut out sections of real<br />

parts. With powerful picture analysis programs<br />

a complete functionality between<br />

modulus and load angle can be plotted,<br />

picture 2. Only a few references are handling<br />

the relation between <strong>fiber</strong> length, orientaton<br />

and strength. But most of the scientific<br />

work done on this topic are more or less<br />

theoretical and could be verified only on test<br />

plates in an adequate state /24-26/. The<br />

qualitative relation between the <strong>fiber</strong> length<br />

and the mechanical properties of a <strong>glass</strong><br />

<strong>fiber</strong> reinforced PP is shown in picture 3.<br />

1.0<br />

0.8<br />

0.6<br />

0.4<br />

0.2<br />

0<br />

0.1<br />

modulus<br />

strength<br />

impact resistance<br />

<strong>Fiber</strong> diameter d F: 10 µm<br />

1<br />

<strong>Fiber</strong>length l [mm]<br />

10 100<br />

Picture 3: Qualitative relation between the<br />

normalized mechanical properties and the<br />

<strong>fiber</strong> length of a <strong>glass</strong> <strong>fiber</strong> reinforced PP<br />

(based on /26/)<br />

It could be determined that the stiffness of<br />

the composite couldn´t be boosted over a<br />

significant level by using longer <strong>fiber</strong>s.<br />

But the maximum strength and the impact<br />

properties could be increased distinctly by<br />

raising the <strong>fiber</strong> length. This is the reason<br />

why the crash performance of complete<br />

parts could be improved significantly by the<br />

utilisation of longer <strong>fiber</strong>s. Despite the fact<br />

that these theoretical relations between <strong>fiber</strong><br />

length and impact performance could be<br />

verified on principle in the reality, there is a<br />

lack of profound work on real parts and examinations<br />

considering the specific circumstances<br />

of real production processes.<br />

Moreover evident is the lack of comprehensible<br />

and accessible data relating <strong>fiber</strong> content<br />

and <strong>fiber</strong> length distribution with impact<br />

properties. One of the difficulties is the correct<br />

and reproducable measurement of <strong>fiber</strong><br />

length distributions in real parts.<br />

1 mm<br />

Picture 4: Optical determination of the <strong>fiber</strong><br />

length on injection moulded parts<br />

left) short <strong>fiber</strong> PP right) long <strong>fiber</strong> PP<br />

The existing analytical methods for the<br />

measurement of the <strong>fiber</strong> length - like different<br />

sieving, filtering or optical methods - are<br />

very large-scaled, expensive and time consuming.<br />

Furthermore these methods allows<br />

no indication on the efficiency of the <strong>fiber</strong>


coupling and the interphase properties of a<br />

<strong>fiber</strong>, pictures 4 and 5.<br />

amount of <strong>fiber</strong>s [%]<br />

20<br />

18<br />

16<br />

14<br />

12<br />

10<br />

8<br />

6<br />

4<br />

2<br />

0<br />

0-1<br />

1-2<br />

2-3<br />

3-4<br />

4-5<br />

5-6<br />

6-7<br />

Picture 5: Typical <strong>fiber</strong> length distribution in<br />

an injection moulded part (PP-LFG 15mm,<br />

30% <strong>glass</strong> content)<br />

4. A new practical approach for the characterisation<br />

of orientation and <strong>fiber</strong><br />

length on the mechanical properties<br />

Due to the absence of easy, practise oriented<br />

test methods for the characterisation<br />

and determination of the <strong>fiber</strong> length distribution<br />

in a part, large-scale and cost intensive<br />

component tests are commonly used.<br />

Based on this unsatisfying situation a systematic<br />

investigation of the relations between<br />

different materials, processes and<br />

geometries was performed /27/. With the<br />

use of a typical press moulded GMT part<br />

for representation, it is shown that with a<br />

simple test procedure the relation between<br />

<strong>fiber</strong> orientation, stiffness and strength could<br />

be determined. By cutting specimen out of<br />

the complete part surface, the whole variety<br />

of flow induced <strong>fiber</strong> orientations in the part<br />

can be considered. After the flexural specimen<br />

is tested in a standardized bending test<br />

(ISO178), the influence of the <strong>fiber</strong> orienta-<br />

7-8<br />

8-9<br />

<strong>fiber</strong> length [mm]<br />

9-10<br />

10-11<br />

11-12<br />

12-13<br />

13-14<br />

14-15<br />

tion can be visualized by plotting the flexural<br />

strength and the related stiffness in one<br />

diagram. A linear connection between the<br />

maximum flexural strength and the flexural<br />

modulus could be found, picture 6.<br />

Under the assumption that the <strong>fiber</strong> length<br />

distribution in a mat based GMT is quite<br />

narrow, this outcome points out that in this<br />

case the <strong>fiber</strong> orientation is the main factor.<br />

Well oriented <strong>fiber</strong>s lead to higher stiffness<br />

and higher strength values, specimen containing<br />

<strong>fiber</strong>s oriented in a perpendicular<br />

way to the load shows poor values.<br />

Flexural strength [Mpa]<br />

200<br />

175<br />

150<br />

125<br />

100<br />

75<br />

50<br />

25<br />

0<br />

GMT 30<br />

1500 2500 3500 4500 5500 6500 7500 8500<br />

Flexural Modulus [MPa]<br />

GMT 40<br />

Picture 6: Linear relation between the<br />

maximum flexural strength and the flexural<br />

modulus (30% and 40% mat reinforced<br />

GMT)<br />

Whereas this outcome is a rather simple<br />

and a well-known phenomenon in the daily<br />

testing practise of long <strong>fiber</strong> reinforced materials,<br />

the acquired experience of these<br />

experiments is building the root for a connection<br />

between the static and the impact<br />

behaviour.<br />

The next step was just a slight extension of<br />

the commonly used charpy impact test.<br />

Cut out and prepare of specimen<br />

(15�80�thickness, accord. ISO 3167) in dif-


ferent positions of the part, at least about 15<br />

samples with different flow orientations. The<br />

specimen were tested in a bending trial<br />

(ISO178) without rupture within linear elasticity<br />

(max 2 mm deflection, 23°C) and the<br />

flexural modulus is measured. After that the<br />

same specimen were used for the charpy<br />

impact test (ISO 179eU) and the impact<br />

strength is measured. The two valuescharpy<br />

impact energy and flexural modulus -<br />

are drawn in one plot, picture 7.<br />

Represented for GMT with three different<br />

<strong>fiber</strong> percentages (20, 30 and 40%) it is obvious<br />

that a linear relation between the<br />

charpy impact energy and the stiffness exists.<br />

Charpy Impact [KJ/m²]<br />

70<br />

65<br />

60<br />

55<br />

50<br />

45<br />

40<br />

35<br />

30<br />

25<br />

20<br />

15<br />

10<br />

GMT 20<br />

GMT 30<br />

1500 2500 3500 4500 5500 6500 7500 8500<br />

Flexural Modulus [MPa]<br />

GMT 40<br />

Picture 7: Linear relation between the<br />

charpy impact energy and the flexural<br />

modulus of 20, 30% and 40% mat reinforced<br />

GMT materials<br />

The most interesting outcome is the slope of<br />

the charpy / modulus-ratio, which is nearly<br />

identical for the three different <strong>fiber</strong> contents.<br />

It was shown that the flexural modulus<br />

the flexural strength and the charpy impact<br />

energy are direct related to the <strong>fiber</strong> orientation<br />

in the part.<br />

The real benefit of this new testing approach<br />

could be displayed by the investigation of<br />

different processes and materials. Represented<br />

in picture 8 is the flexural strength to<br />

modulus behaviour of specimen from parts<br />

with 30% <strong>glass</strong> <strong>fiber</strong> content, but produced<br />

with three different processing technologies.<br />

Flexural strength [Mpa]<br />

175<br />

150<br />

125<br />

100<br />

75<br />

50<br />

25<br />

0<br />

all Materials: PP - 30 % GF<br />

2000 3000 4000 5000 6000 7000<br />

Flexural Modulus [MPa]<br />

LFG - ICM<br />

LFG - IM<br />

SFG - IM<br />

Picture 8: Influence of the <strong>fiber</strong> length on the<br />

linear relation between the maximum flexural<br />

strength and the flexural modulus (30%<br />

<strong>glass</strong> reinforced PP materials)<br />

The specimen made with long <strong>glass</strong> <strong>fiber</strong><br />

granulates in an injection compression<br />

moulding process (LFG-ICM) – which diminish<br />

the <strong>fiber</strong> breakage - exhibit the highest<br />

strength and stiffness values. The<br />

specimen cut out of parts produced with the<br />

identical granulate type, but in a common<br />

injection moulding process (LFT-IM), are<br />

showing mediocre values and at least the<br />

specimen from parts injected with normal<br />

short <strong>fiber</strong> granulates (SFG-IM) are manifesting<br />

the lowest stiffness and strength<br />

values. This outcome points out that – beneath<br />

the <strong>fiber</strong> orientation – a second influence<br />

is taking effect – the <strong>fiber</strong> length, here<br />

as the result of different production tech-


Charpy Impact [KJ/m²]<br />

nologies. As described in the literature the<br />

stiffness and the strength is directly related<br />

to the <strong>fiber</strong> length. The efficiency of the <strong>fiber</strong><br />

length could be directly evaluated by the<br />

slope of the strength / stiffness-ratio, which<br />

is raising significantly towards longer <strong>fiber</strong>s.<br />

How easily and comprehensibly the method<br />

could be used to draw clear distinctions<br />

between the described process technologies<br />

for long <strong>fiber</strong> reinforced <strong>thermoplastics</strong><br />

is shown in picture 9. When the charpy impact<br />

values of the different specimen is<br />

plotted over their related stiffness the three<br />

processes could be distinguished very well.<br />

The increase of the <strong>fiber</strong> length leads to a<br />

significant increase of the charpy / modulusratio.<br />

35<br />

30<br />

25<br />

20<br />

15<br />

10<br />

5<br />

0<br />

all Materials: PP - 30 % GF LFG - ICM<br />

LFG - IM<br />

SFG - IM<br />

2000 3000 4000 5000 6000 7000<br />

Flexural Modulus [MPa]<br />

Picture 9: Influence of the <strong>fiber</strong> length on the<br />

linear relation between the charpy impact<br />

energy and the flexural modulus (30% <strong>glass</strong><br />

reinforced PP materials)<br />

Whereas the slope of the charpy / modulusratio<br />

for the injection moulded short <strong>fiber</strong> PP<br />

is almost zero, a distinct difference could be<br />

noticed for the LFG-IM and the LFG-ICM<br />

process. With increasing <strong>fiber</strong> length you will<br />

increase the charpy / modulus-ratio as<br />

shown.<br />

5. Outlook<br />

With a rather simple mechanical test procedure<br />

fundamental relations between the<br />

<strong>fiber</strong> length and the <strong>fiber</strong> orientation of long<br />

<strong>glass</strong> <strong>fiber</strong> reinforced composites with polypropylene<br />

matrix can be determined and<br />

visualized. With a slight extension of the<br />

charpy impact test – which is in any case<br />

part of the normal testing program for thermoplastic<br />

composite parts – it is possible to<br />

obtain a lot more information and correlations<br />

about the material performance, as if<br />

common single point testing methods were<br />

used.<br />

With this practise oriented measuring<br />

method, the producer of TC-parts is enabled<br />

to optimise process parameters, to compare<br />

different kinds of materials and to classify<br />

different kinds of production processes.<br />

6. References<br />

1. Schweizer, R.A. : Glass <strong>fiber</strong> length degradation<br />

in <strong>thermoplastics</strong> processing, Proc.<br />

36 th Ann. SPI Conf., Session 9A, p 1-4<br />

(1981)<br />

2. Schmid, B. : Spritzgießen von langfaserverstärkten<br />

Thermoplasten, Kunststoffe 79<br />

(1989) 7, p 624-630<br />

3. Sanschagrin, B. ; Ehrhardt, P. ; Fisa, B. :<br />

<strong>Fiber</strong> length degradation of long <strong>glass</strong> <strong>fiber</strong><br />

reinforced Polypropylene during injection<br />

molding, Proc. 46 th Ann. SPI Conf., Session<br />

9A, p 1-10 (1991)<br />

4. Wolf, H.-J. : Faserverkürzung beim Verarbeiten<br />

langfasergefüllter Thermoplaste,<br />

Kunststoffe 83 (1993) 1, p 69-72<br />

5. Hafellner, R., Pichler, M. ; Wörndle, R. ;<br />

Steinbichler, G. ; Egger, P. : Lange Fasern<br />

spritzgießen, Kunststoffe 90 (2000) , p 44-48


6. Hawley, R. C. : Extruder Apparatus and<br />

Process for Compounding Thermoplastic<br />

Resin and <strong>Fiber</strong>s, U.S. Patent Number<br />

5,165,941 (4 Nov. 1992), to Composite<br />

Products, Inc. (CPI)<br />

7. N.N.: http://www.compositeproducts.com<br />

8. N.N.: http://www.lawtonmachinery.com<br />

9. Holzki, R. : Träger für Armaturentafeln aus<br />

glasfaserverstärktem PP im Naß-<br />

Anformprozeß, 27. AVK Jahrestagung Baden<br />

Baden1996, A 2 S1-6,<br />

10. Brüssel, R. ; Kühfusz, R.: Ein Jahr Serienproduktion<br />

von Menzolit-Fibron Lang-<br />

Faserverstärktem-Thermoplast mit dem Direkt-Verfahren,<br />

1. AVK-TV Jahrestagung<br />

Baden Baden1998, A2<br />

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