Composites Part A 29A (1998) 933–938

1359-835X/98/$ - see front matter

q 1998 Elsevier Science Ltd.
PII: S1359-835X(98)00021-9 All rights reserved.

Manufacture of aramid fibre reinforced nylon-12

by dry powder impregnation process

M. Rath, S. Kreuzberger and G. Hinrichsen*

Technical University of Berlin, Institute of Nonmetallic Materials, Polymer Physics,
Englische Straße 20, 10587 Berlin, Germany
(Received 12 September 1997; revised 12 December 1997; accepted 15 January 1998)

The present paper deals with the manufacturing of composites, consisting of continuous aramid fibres and nylon-
12, by applying the so-called dry powder impregnation process. The fibres are pre-impregnated by the deposition
of fluidised powder particles on aramid fibre tows which are consolidated by heat and pressure to form continuous
prepregs. Features of the nylon-12 powders which are important for the dry powder impregnation process are
discussed. Material, tool and processing parameters influencing the achievement of impregnation and therefore
the fibre volume content of the prepregs are outlined. q 1998 Elsevier Science Ltd. All rights reserved.

(Keywords: dry powder impregnation; E. prepreg manufacture; fibre reinforced composite; A. aramid fibre; nylon-12)

INTRODUCTION impregnation should operate well with these materials,

A great variety of unique processing and manufacturing
techniques have been developed for the production of
thermoplastic composite materials1–4. The suitability of
impregnation techniques for the manufacture of specific
fibre–matrix combinations is currently being investigated at
the Technical University of Berlin5–7. Dry powder impreg-
nation is identified in this paper as a suitable technique for
the manufacture of thermoplastic prepreg tapes. This
technique is based on the powder coating technique,
which uses a fine dispersion of polymer particles in the
fibre tow in which the charged powder particles are
electrostatically deposited onto the fibre surface8,9.
In the present study, experimental results are presented on
the influence of various production parameters on the fibre
volume content of aramid fibre reinforced prepregs during
manufacture by the dry powder impregnation process.
Manufacture was conducted with nylon-12 powder in a
mechanically agitated fluidised powder bed.
MATERIALS
The aramid fibre TWARON 1056 is produced by Akzo
Nobel, and the high modulus (HM) type is used in this work.
Owing to the importance of powder size, four nylon-12
powders with different average particle size, commercially
used in the fluidisation coating technique, were taken into
consideration (Vestosint 1111, 1118, 2175, and 3158, Hüls
AG, Marl). Nylon-12 powders were selected because
* Corresponding author
resulting in an approximately fully wetted fibre tow with
low viscosity melts, such as nylon-1210.
Characteristic properties of the materials used are
summarised in Table 110,11.
Fluidisation
A stream of gas is passed upwards through a perforated
bottom plate (distributor) into an impregnation chamber
including a settled powder bed. At a gas velocity u mf high
enough to separate the particles from each other, the
particles become freely supported and behave like a boiling
fluid in the ascending gas. The velocity u mf is called
‘minimum fluidisation rate’12. Helping to disrupt large
clusters of particles formed by interparticle forces and to
realise uniform fluidisation and bed expansion, especially
for cohesive powders which are difficult to fluidise12, it is
important to agitate the powder layer. This procedure is
successfully used in the fluidised bed dip coating technology
and is identified as an effective method for the manufacture
of composites4. The material to be coated is heated beyond
the melting point of the polymer coating compound, then
fully dipped into a bath of fluidised powder particles. The
polymeric material melts and adheres to the surface of the
article which is subsequently transferred to an oven where the
plastics forms a homogeneous coating of constant thickness.
Geldart et al.13 described a simple method to quantify the
flowability of powders by measuring the leakage of powder
particles through an outlet connector as a function of time. A
schematic illustration of the arrangement used to estimate
the flowability of powders is presented in Figure 1.

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Composite production by dry powder impregnation: M. Rath et al.

The expansion ratio (relation between the bed height of thermoplastic composites can be divided into different
the expanded powder, h, and that of settled powder, h 0) for categories, according to the techniques of pre-impregnation
different powder masses in the chamber is dependent on the and consolidation of the prepregs. Reviews and descriptions
gas velocity. The result is shown in Figure 2. The leaked for the different techniques have been provided by various
powder mass as a function of the expansion ratio is authors15,16. One of the earliest references to the powder
presented in Figure 3. impregnation technique using thermoplastic matrices was
As illustrated in Figure 2, with increasing gas velocity the the patent of Price17. The dry powder impregnation
expansion ratio increases in relation to the powder mass in processes can be subdivided into three main categories,
the impregnation chamber. Keeping the gas velocity namely impregnation in:
constant the expansion ratio increases with the inserted
• a settled powder bed
powder mass.
• a fluidised powder bed and
To avoid dust emission during the impregnation process a
• an electrostatic field.
well defined amount of powder is used, because of suitable
expansion ratios at low gas velocities and sufficient flowability
of the agitated powder bed structure (see Figures 2 and 3).
The results presented in Figures 2 and 3 agree with the
observations of the expansion behaviour of flour for
different gas velocities by Brakken et al.14. Figure 3
demonstrates that the powder particle discharge is very
small for expansion ratios h/h 0 , 1.4, because of the
collapsed flowability of the powder particles. Therefore, a
reproducible impregnation of the fibre tow is impossible and
such ratios can not be used for the dry powder impregnation
process of Vestosint 3158.

DRY POWDER IMPREGNATION PROCESS

Techniques for the production of reinforced polymers Figure 2 Powder expansion ratio as a function of the gas velocity for
different powder masses
The impregnation processes used for the manufacture of

Figure 1 Schematic of the basic arrangement for estimation of the

flowability of powders. 1, Fluidization gas; 2, Impregnation chamber; 3,
Oszillation sieve; 4, Diffusor; 5, Fluidized bed of polymer particles; 6,
Outlet connector; 7, Guide plate; 8, Leaked powder particles; 9, Precision Figure 3 Discharged powder mass as a function of the expansion ratio for
balance various observation times

Table 1 Characteristic properties of the materials

Property Twaron HM 1056[11] Vestosint 3158[10]
¹3
Density (g cm ) 1.45 1.02
Melting point (8C) Degradation temperature . 500 172–180
Tensile strength (MPa) 3150 57
Elongation at break (%) 2.0 300
Young’s modulus (GPa) 121 0.98
Filament diameter (mm) 12 –
Filament number 5000 –
Mean powder size (mm) – 12

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 Composite production by dry powder impregnation: M. Rath et al.
Design of the laboratory equipment
The dry powder process developed by us for the
manufacture of prepregs consisting of aramid multifilament
fibre tows and nylon-12 powder is shown schematically in
Figure 4. The fibre tow is continuously unwound from a
fibre spool (1) by a motor (2) using a constant pretension by
which the motor torque is controlled using a speed
controlling device. The fibre tow passes some guide pins
(3) which widen the collimated fibre tow. The guide pins
ensure that the fibre tow is spread to such an extent that each
filament in the tow can be uniformly coated with powder
particles. After passing a force-sensitive device (4)
governed by closed loop controlling unit (5), the fibre tow
reaches the impregnation bath (6) filled with fluidised
powder and the impregnation pin (7) inserted in the
impregnation tool. A stream of gas controlled by a gas
flow counter (8) is passed through a diffusor (9) in a
mechanically agitated powder bed. The gas pressure was
measured below the diffusor using a manometer (10). The
agitation of the powder bed was realised by an oscillating
sieve (11) driven by another motor (12). After leaving the
impregnation bath the pre-impregnated fibre tow passes
through a controlled heating chamber (13, 14), in which the
matrix material is melted. The fibre tow is finally
impregnated and consolidated with pressure rollers (15),
Table 2 Classification of parameters for the dry powder impregnation technique
Tool parameter Processing parameter
Distance of impregnation pins Drawing velocity a
Contact angle Tension of fibre tow a
Number of impregnation pins Gas velocity
Diameter of impregnation pins a
Width of impregnation pins a
Depth of fluidised powder layer above the impreg-
nation pin a
a
Parameters investigated in this paper
Figure 4 Sketch of the dry powder prepreg process. 1, Fibre spool; 2, Motor; 3, Guide pins; 4, Force-sensitive device; 5, Motor torque controlling unit; 6,
Impregnation bath; 7, Impregnation pin; 8, Gas flow counter; 9, Diffusor; 10, Manometer; 11, Oszillating sieve; 12, Motor; 13, Heat controlling unit; 14,
Heating chamber; 15, Roll nip; 16, Tension rolls; 17, Winder
then transported through speed-controlled tension rolls (16)
and wound up (17).
EXPERIMENTAL
Classification of the parameters for the dry impregnation
process
Vodermayer18 defined various tool, material and proces-
sing parameters which influence the fibre volume content in
the continuous production of fibre reinforced polymers
using the aqueous dispersion technique. A synopsis of the
most important parameters for the dry impregnation
technique is shown in Table 2. Some of the parameters
were held constant during all experiments (see Table 3).
In preliminary experiments it was observed that the fibre
volume content remains practically constant, while the
drawing velocity has been varied between 1 and 3 m min ¹1
(Figure 5). Therefore, to determine a reasonable value of the
fibre volume content of the prepregs for constant width of
the impregnation pin the obtained data for the five
investigated drawing velocities were averaged. The drawing
velocity is influenced by the limited torque of the speed-
controlled tension rolls (see Figure 4 (16)).
Material parameter
Filament diameter
Particle size a
Flowability of powders
Expansion behaviour of powders
Powder particle size distribution
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Composite production by dry powder impregnation: M. Rath et al.

Using the rule of mixture the fibre volume content of the constant the fibre volume content increases with the applied
prepregs can be easily determined gravimetrically requiring tension. A fibre volume content in the range of 20–45% can
densities and masses of the two components. be adjusted using an impregnation pin with a diameter of
mF ·rM 10 mm and width in the range 5–100 mm.
vF ¼ (1)
mF ·rM þ (mc ¹ mF )·rF
Table 3 Parameters which have been held constant during manufacturing
where v F is fibre volume content (%), m F is fibre mass per
unit length (g), m C is composite mass per unit length (g), r M Number of impregnation 1
pins
is the density of the matrix (g cm ¹3) and r F is the density of Contact angle (deg.) 180
the fibre (g cm ¹3). Filament diameter of (mm) 12
Twaron HM 1056
Temperature of heating (8C) 300
device
DATA AND RESULTS

Position of the impregnation tool in the fluidised powder

bed
The local position of the impregnation tool within the
fluidised powder bed influences the dispensation of powder
particles in the nip of the impregnation pin. The fibre
volume content as a function of the bed height of the
expanded powder above the impregnation pin is presented
in Figure 6. The chosen position defines the thickness of the
fluidised powder layer between the impregnation pin and the
surface of the powder layer. As can be seen from Figure 6
the fibre volume content decreases with increasing thickness
of the fluidised powder layer above the impregnation pin.
Care must be taken to ensure the powder bed height in the
impregnation chamber is sufficiently high, because a
restricted flowability of the powders for bed heights lower Figure 5 Fibre volume content as a function of drawing velocity for
than 1.0 cm above the impregnation pin leads to irregular different widths of impregnation pin. Roving tension 2 N
dispensation of powder particles, so that an entirely
immersed impregnation pin during the impregnation
process can not be guaranteed.
For a reproducible impregnation process during manu-
facture it is necessary that a fluidised and bubbling powder
layer of 2 cm above the impregnation is realised.

Width of the impregnation pin

A second decisive parameter influencing the fibre volume

content of the prepregs is the width of the impregnation pin.
The function of the impregnation pin is to open up and
spread the fibre tow to as large a volume as possible to
facilitate the penetration of powder particles into the free
space between the filaments, so that powder impregnation
can occur throughout the complete fibre tow. The influence
Figure 6 Fibre volume content as a function of the depth of the fluidised
of spreading on the fibre volume content was investigated powder layer above the impregnation pin
by variation of the width (b i) of the impregnation pin and the
tension of the fibre tow, while the diameter of the pin was
held constant (d ¼ 10 mm). A schematic of the impregna-
tion pin is shown in Figure 7 and the results of the
measurements are presented in Figure 8.
An increase of the width of the impregnation pin in the
range 5–34 mm results in a decrease in the fibre volume
content and levels up to a constant value for pins of 34–
100 mm width. In addition, the tension applied to the fibre
tow also has a remarkable influence on the fibre volume
content of the prepregs. Holding the width of the pin Figure 7 Schematic diagram of the impregnation pin

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 Composite production by dry powder impregnation: M. Rath et al.

Collimated filaments allow fewer particles to penetrate than fluidise because of high interparticle forces and, therefore,
an open fibre tow which includes a greater accessible volume their use for the dry powder impregnation process is
for powder particles, and hence the fibre volume content restricted. On the other hand, impregnation of individual
increases with decreasing width of the impregnation pin. fibres becomes more difficult with larger particles14. In the
It has to be mentioned that the standard deviation of the past, powder particles with diameters in the range 15–
fibre volume content varies with the width of the 150 mm have been successfully applied4. Our experiments
impregnation pin in the range 5–14 mm and levels down were conducted using an impregnation pin of 34 mm width
to about 2% for greater widths, i.e. using small pin widths and 30 mm diameter and five steps of roving tension.
the impregnation process is characterised by considerable In this investigation the average particle size (x 50) of the
fluctuations which cause uncertainties in the fibre volume nylon-12 powders was determined with a Sympatec Helos
content of the prepregs. particle size analyser. The powder was suspended in
aqueous dispersion and stirred to break up aggregates of
powder particles. The results of the size measurements are
Diameter of the impregnation pin
presented in Table 4.
The diameter of the impregnation pin defines the length
on which the fibre tow is in contact with the surface area of
the impregnation pin. A sketch of the impregnation tool is
shown in Figure 9, and the dependence of the fibre volume
content of the produced tapes on the diameter of the
impregnation pin is presented in Figure 10. As can be seen,
the fibre volume content increases monotonically with the
pin diameter; roving tension has a minor but significant
influence on this quantity.
The guide pins open the fibre tow and spread it to a
sufficient width, so that polymer particles are allowed to
penetrate between the filaments.
The period of time for which the fibre tow is in contact
with the impregnation pin rises with increasing impregna-
tion pin diameter, and a certain amount of powder particles
already ‘fixed’ between the filaments are squeezed out and,
therefore, the fibre volume content is increased.

Particle size
It has been pointed out by Iyer and Drzal15 that for
optimum impregnation it is advantageous that the dimen-
sions of the powder particles should be approximately
identical with the diameter of the fibre, which is difficult to
achieve in practice. Particle size is restricted by economic
Figure 9 Schematic diagramm of the impregnation tool. 1, Fluidized
limitations and the cost of the manufacturing method used to powder bed; 2, Impregnation pin; 3, Guide pins; 4, Fibre tow; 5, Distributor;
prepare the powder. Very fine particles are difficult to 6, Oszillating sieve

Figure 8 Fibre volume content as a function of the width of the

impregnation pin. Tension of the roving has been varied in the range 2– Figure 10 Fibre volume content as a function of the diameter of the
10 N impregnation pin. Tension of roving has been varied in the range 2–10 N

937
Composite production by dry powder impregnation: M. Rath et al.
Figure 11 Fibre volume content as a function of the average diameter of
the powder particles. Tension of roving has been varied in the range 2–10 N
Table 4 Average powder particle size
Powder x 50 (mm)
Vestosint 3158 12
Vestosint 1118 31
Vestosint 2175 64
Vestosint 1111 86
As can be obtained from Figure 11, the fibre volume
content decreases with increasing average diameter of the
powder particles. In the region of fine powders (average
particle diameter in the range 12–30 mm) the fibre volume
content remains nearly constant and decreases strongly for
coarse powders (average particle diameter: 64–86 mm)
resulting in a matrix-rich composite.
In the case of a broad distribution of powder particle
diameter one can imagine that the larger particles, which
have penetrated into the roving and are fixed to the
filaments, ‘open’ the fibre tow for smaller particles. This
effect may lead to an additional impregnation of the fibres
which results in a decrease of the fibre volume content15.
The quality of the powder impregnation was evaluated
using an x-ray refraction method developed by Hentschel et
al.19. The set of these results influencing the quality of the
powder impregnation for different diameter of the impreg-
nation pin and powder particle size will be presented in a
further paper.
CONCLUSIONS
• Nylon-12 powders are successfully fluidised by passing a
stream of compressed air in a mechanically agitated
powder bed. The expansion takes place beyond a lower
limit of the gas velocity.
938
• Continuous manufacture of aramid fibre reinforced
nylon-12 prepregs, with different fibre volume contents
in the range 20–50%, can be realised by the developed
dry powder impregnation process.
• Various parameters, such as the width and diameter of the
impregnation pin, tension of fibre tow and average parti-
cle diameter, influence the fibre volume content.
• The production of high performance prepregs consisting
of aramid fibre reinforced nylon-12 can be warranted by
the presented dry powder impregnation process.
ACKNOWLEDGEMENTS
The authors thank Hüls AG, Marl, for supplying the
appropriate nylon-12 powders.
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