Effects of processing induced

microstructure on the fatigue

crack propagation of unfilled and
short fibre-reinforced PA-6
J. KARGER-KOCSIS

(TAURUS Hungarian Rubber Works, Budapest, Hungary)

The microstructure-related fatigue performance of injection-moulded neat

and short glass fibre-reinforced (20 and 30 wt%) polyamide (PA-6) was
investigated. Change in the microstructure both of the neat and reinforced
PA-6 was achieved by alterations in processing variables, ie, mould tempera-
ture (TM) and injection speed (vinj), and studied by light and scanning
electron microscopy (SEM). The microstructure of the composites was char-
acterized by a reinforcing effectiveness parameter, Rc. Fatigue crack propa-
gation (FCP)curves indicated the validity of the Paris power law. The FCP
response both of the neat and reinforced PA-6 was discussed by the micro-
structural efficiency (M) approach. An attempt was made to define a reinforc-
ing effectiveness parameter for the matrix, RM, comprising the morphology
and thus correlate the FCP response with the microstructure.

Key words: crystallinity effects; fatigue crack propagation; failure mecha-

nisms; glass fibre reinforcement; injection-moulding; polyamide-6

Until recently works published on the fatigue perfor-
mance of polyamides (PA) and their short fibre-
reinforced composites were dealing mostly with the
effects of external testin~ conditions, ie temperature,
frequency, wave shape. 1-2 Moderate attention was
paid, however, to the influence of 'internal', material-
related parameters such as processing induced skin-
core morphology of the matrix polymer 3 and fibre
arrangement (alignment and layering) in chopped fibre
filled composites. It is surprising, since the fatigue
response of short fibre-reinforced thermoplastics
strongly depends on the anisotropy caused by
processing. 4-6 Indeed, the effect of processing condi-
tions on the development of fibre layering, 78 ' matrix
morphology 9 and microstructure-related tensile
properties 8 of injection-moulded short glass fibre (GF)
filled PA-6 composites were extensively studied and
reported. However, information is completely missing
as to what extent the fatigue crack propagation (FCP)
can be influenced by the injection-moulding para-
meters. Fatigue characterizations until now were
mainly focussed on GF-PA-6 systems with different fibre
loading2,4,10 or toughened matrix 11'12 rather than on
processing induced effects, which were neglected.
The aim of the present paper is to contribute to this
topic and to establish basic relationships between
0010-4361/90/050243-12 © 1990 Butterworth & Co (Publishers) Ltd
COMPOSITES. VOLUME 21 . NUMBER 3. MAY 1990
processing induced microstructure and fatigue response
both for neat and GF-filled PA-6.
EXPERIMENTAL
Materials and processing
Commercially available neat PA-6 (Danamid E,
Magyar Viscosagyar, Hungary) and its 30 wt% (= 16
vol%) coupled GF reinforced Composite (Danamid
FGF-30) were used in this study. Another composite
grade with 20 wt% (= 10 vol%) GF content was
injection-moulded directly from a proper granulate
mixture of the above grades. It has been previously
reported 13 that the main processing variables affecting
the fibre structuring and thus the mechanical perfor-
mance are melt (Tm) and mould (TM) temperatures and
injection speed (Vinj). Therefore in this study both TM
(25 ° and 80°C) and Vinj (10 and 30 mms -1) were varied
giving four processing conditions for a given material.
Film gated plaques of 82 x 82 x 4 mm 3 dimension were
moulded using a 650 MN clamping force Netstal-
Neomat 150/75 type reciprocating screw injection-
moulding machine under the following conditions:
Tm = 270oc
TM = 25 ° and 80°C (variable)
243
 Screw rotation = 90 min-1
1;inj = 10 (slow) and 30 (fast) mm s-1 (variable)
Injection pressure = 135 MPa
Pressure in the mould = 55 MPa
Back pressure = 5 MPa
Mould filling time = - 5 s (depending o n k'inj)
Cooling time = 45 s
The injection-moulding machine operated under
closed-loop Control (Laokon-Cosy-GAMF system) :
the injection speed profile was defined in function of
screw movement, while pressure steps in the mould
were regulated by time.
Microstructural characterization
The skin-core morphology and spherulite size in the
core was studied by light microscopy on thin micro-
tomed slices. Crystallinity was evaluated by differential
scanning calorimetry (DSC) using a Heraeus TA 500 S
device at 10°C min -1 heating rate. For the melt enthal-
z beam. The FCP rates (da/dN) were read as the slopes of
x / [ ~ -'"
if,- / F" t
a =
MFD
,•_B=3-4mm B
-y
(ram)
Fig. 1 (a) Sectioning for light (position c) and scanning electron
microscopic (positions a-c) investigations to establish the
skin-core morphology of the matrix and fibre layering and
alignment in the surface and central layers of the composites;
(b) specimens machined from injection-moulded plaques
schematically and the geometry of the CTspecimen used. B,
plaque thickness; MFD, melt flow direction (mould filling
direction); S, skin and surface layer for the matrix and
composite, respectively; C, core and central layer for the matrix
and composite, respectively. Note: distinction between skin and
surface, as well as between core and central layers is necessary,
since their thickness do not agree with each other (Figs 2 and 3).
It is due to the different flow and thermal behaviour of the
matrix and related short GF-filled composite.
244 COMPOSITES. MAY 1990
phy of the 100% crystalline PA-6 175 J g-i was
accepted. 14
The processing induced fibre orientation and layering
were studied on metallographically polished sections
cut from the moulded plaques in the scanning electron
microscope (SEM). Prior to SEM investigations in a Leitz
1600 T microscope the polished sections were gold
sputtered. Sectioning of the moulded plaque for
microscopic investigations is shown schematically in
Fig.l(a).
Fatigue crack propagation measurements
Compact tension ( C T ) specimens were machined from
the injection-moulded plaques and notched either
parallel (longitudinal or L-notch) or perpendicular
(transverse or T-notch) to the mould fill direction
(MFD) as shown schematically in Fig. l(b). FCP mea-
surements were carried out on a Schenck PSA
10 kN closed-loop servohydraulic testing machine in
tension-tension mode with a minimum to maximum
load ratio of R = 0.2 (cf. ASTM E 647 standard).
Fatigue tests were performed at room temperature ( R T )
in air under load control using a sinusoidal wave
function o f f = 5 Hz frequency. Prior to the measure-
ments the saw cut notches of the CT specimens were
sharpened by a razor blade. Crack growth was
measured without test interruption using a travelling
microscope. The crack was visualized both by direct
and transmitted light using a flexible optic fibre light
crack growth vs. number of cycles (Aa-N) curves. The
corresponding stress intensity factor range (A K) was
calculated by:
AK, AF
.a i (1)
B.W \W/
where:
A F = F m a x - F m i n is the load amplitude; B = specimen
thickness (~-3-4 mm); W = specimen width (29 mm)
(see Fig. l(b) ); a i = a + Aa i is the actual crack length
(a, initial value (Fig. l(b) ) Aai, the crack extension at
a given fatigue cycling) ;f(ai/W) is the shape factor
(ASTM E399 standard)
Fractography
Topology of the fatigue fracture surface was studied
after gold coating by SEM. Any further details related
to the experimental section can be taken from previous
papers.3,5,6,12,15
RESULTS
Microstructure
1. Matrices
Change in the skin-core morphology of the PA-6 matrix
due to TM is depicted in Fig. 2. Increasing TM results in
a very effective reduction of the skin layer (from about
170 to 25 ~tm) and in a slightly greater average spheru-
lite diameter (from about 15 to 19 Ixm). The absence of
Table 1. Microstructural characteristics of the injection-moulded unfilled PA-6

Processing conditions Relative layer Average spherulite Crystallinity

thickness of the diameter in the core (DSC)
skin layers Skin(S) Core(C)
(%) (~m) (%)

TM=25°C
Vinj=10 mm s -1 11.2 15 8 42
vinj=30 m m s -1 10.6 13 5 34

TM=80°C
Vinj=10 mm S-1 1.7 19 30 49
Vinj=30 m m s -1 1.3 17 25 43

[~ Skin ~I Core N
E N(dpi).cos2(~i
~c0s2(~ =i=1 (2b)
N
~.~ N(~pi)
i=1

Fig. 2 Effect of m o u l d t e m p e r a t u r e , TM, on the skin-core
m o r p h o l o g y of the PA-6 matrix. (Light microscopic pictures
taken b e t w e e n crossed-polars). Processing conditions: (a) TM =
25°C; v~.i = 10 m m s - t ; (b) mM = 80°C; Vlnj 10 m m s
=
shear zone is rather peculiar for injection-moulded
PA-6.16 Based on the DSC traces the skin proved to be
highly amorphous, whereas the core exhibited usual
crystallinity values. The results on the matrix micro-
structure are summarized in Table 1.
2. Composites
On the composed SEM micrographs (Fig. 3) taken in
the z-x plane (specimen thickness, B, vs. mould filling
direction, MFD), the surface (S) and central (C) layers
could be distinguished based on the fibre orientation
patterns in the y-x plane. For this purpose sections
were taken from the plaque according to Fig. l(a) and
visualized by SEM after polishing. The average planar
fibre orientation (fo) in the y-x plane was calculated by
use of a modified ~ermans orientation factor. 5 ' 15 "17
The latter reflects the angle between individual fibres
at a reference direction:
fp=2<COS2q~> - 1 (2a)
where:
q~ is the angle between individual fibres and MFD, and
N(q~i) is number of fibres inclined at %.
Moulding by slow injection speed led to the formation
of a 5- (splitting of the S layers), while fast injection
speed favoured the development of a 3-layer laminate
structure. Their formation can be explained by changes
in the velocity profile of the melt front in the cavity
during mould filling. The front of the advancing melt is
strongly affected by the processing variables which
cause alterations in the shear and elongational flow
fields which are of crucial importance for fibre align-
ment and layering. The formation of the outer skin (S 1
in Fig. 3) in the plaques moulded by slow Vin)should be
connected with a change in the velocity profile of the
advancing melt front. The unexpected high fp values
found in this layer may also indicate a pronounced fibre
alignment into MFD at the sprue and gate before cavity
entrance. 18 Table 2, in which microstructural parame-
ters of the composites are summarized, clearly indicates
that both C/B (cf. Fig. 3) and absolute value offp in the
S and C layers, [(p(S)[, [(p(C)l, increase with increasing
fibre volume fraction (vv) in accordance with predic-
tions and findings. ]9.20
Table 2 also contains the main values of the fibre length
distribution curves, namely those of the peak (/max), the
number-(/N) and weight-average (/w) fibre length.
Comparing the above values with those of the virgin
granules of the 30 wt% GF-PA-6 (lmax=400, lN=560 and
/w=640 ~*m)one can conclude that its processing in
'diluted' form (by adding matrix to set the 20 wt%
GF-filling) does not affect these fibre characteristics.
Increasing vv, however, shifts the fibre length distribu-
tion curves toward lower length (ie/max and thus the
average aspect ratio, lmax/d, decreases) which is a
general trend in short fibre-reinforced injection-
moulded themoplastics. 19.zoTable 2 also contains the
fibre reinforcing effectiveness values of the composites
(Rc) determined by:iS

COMPOSITES . MAY 1990 245

Table 2. Microstructural characteristics of the injection-moulded GF-reinforced PA.6 composites. (All values
are dimensionless; Rc calculated according to Equation 3)

Reinforcing
Material Fibre layering and orientation Fibre length effectiveness
processing conditions characteristics Rc

C/B fp,c fp,sl fp,S2 /max/d (/W//N) L T

PA-6 + 20 wt% GF
TM=25°C
v~nj=10 mm s -1 0.19 -0.56 0.88 0.58 =38 1.2 0.6 2.1
vi.j=30 mm s -1 0.28 -0.58 0.60 =36 1.3 0.7 2.1
TM=80°C
Vinj= 10 mm s -1 0.17 -0.63 0.86 0.56 =37 1.2 0.7 1.9
Vinj=30 mm s -1 0.25 --0.70 0.74 =36 1.3 0.9 2.0

PA-6 + 3 0 w t % GF
TM=25°C
Vinj=10 mm s -1 0.28 -0.79 0.42 0.63 =28 1.2 1.0 2.4
Vinj=30 mm s -1 0.34 -0.87 0.55 =28 1.3 1.3 2.9
TM=80°C
Vinj=10 mm s -1 0.28 -0.86 0.41 0.77 =25 1.3 0.9 2.2
vi,i=30 mm s -1 0.29 -0.70 0.39 0.76 =24 1.3 1.0 2.1

Vin j {mm s-1} 10 30 10 30 direction, fibre volume fraction, fibre aspect ratio and
Tmot t o ~ . . . . 80 on its distribution. 15
The effects of processing conditions on the composites'
microstructure could be summarized by the following
trends (cf. Table 2):
1) C/B slightly decreases by increasing TM and
increases with increasing vi,j. Analogous chan~e can
be predicted for Lfplboth in the S and C layers ~U
2) the average fibre length slightly decreases with
faster injection and is practically unaffected by
mould temperature. It should be noted here, that
pronounced fibre breakage during injection-
moulding of GF-PA-6 occurs above 80 mm s -1
injection speed, 22 which is, however, not used in
practice.
x (=MFD)
Fig. 3 Fibre layer structuring caused by processing on the
e x a m p l e of 20 w t % GF-PA-6
Fatigue crack propagation
2 1. Matrices
(3) In Fig. 4 the FCP curves of the skin and core layers of
tN the unfilled PA-6 are shown. It succeeded in distinguish-
ing between the skin and co,re by establishing the crack
where: growth at the specimen surface and in the bulk by
direct and transmitted illumination. 3 Until now the
d = fibre diameter;fo ~a s andfo ~ff c give the effective
only reference 23 for the effect of skin-core morphology
fibre orientation in tl~e S' and C ~ayer, respectively. [Its
value varies between 0 (fibres Oriented perpendicular on FCP of PA reported that the crack length of wet
to the load direction) and 1 (fibres fully aligned into the samples 'at the mid thickness extended as much as
load direction) and can be obtained from a graph fp vs several millimetres further than the corresponding
fp,~ffgiven in Reference 21] (all the other terms were crack position at the two free surfaces'. Fig, 4 illustrates
defined above.) the fatigue crack acceleration in the skin layer. If one
takes into consideration that the skin layer is under
This R c term describes the microstructure of the compression, whereas the core lays under tensile
composites since it takes into consideration the fibre stresses due to the solidification process during
layering and alignment with respect to the loading moulding, 24 this internal stress field should result in FCP

246 COMPOSITES . MAY 1990

deceleration in the S layer. However, this effect was 5x10-3
negligible in the present case, since the relatively low PA-6

melt viscosity of the PA-6 applied allows a rapid stress L~ T notch

relaxation of the macromolecules during the cooling £K=2.5 MPa m½
phase. 25 The relatively low melt viscosity refers to a • Experimental
moderate molecular weight which is characteristic for O Calculated
PA-6 produced by hydrolitic polymerization of
I0
e-caprolactam. The very simple skin-core structure
>.
observed (Fig. 2) should be connected to the above U

facts. Instead of FCP deceleration the opposite occurs in E

the skin when the corresponding F C P curves (Fig. 4) are 3 10-3 m

compared. The observed run can only be attributed to "U

o
changes in the crystallinity. Indeed, da/dN values taken t~
"13
z • •
o
at constant A K level, da/dN(AK=const), and plotted o •
against the DSC crystallinity can be approximated by a 5xi0 -4 • o
straight line (Fig. 5). The scatter range of this single o
logarithmic plot in Fig. 5 may refer to orientation and
spherulite arrangement (type and size), as well as
residual stress effects. Results obtained from T-and
L-cracked specimens do not differ from each other
practically when compared with the Paris constants
(A - preexponential, m-exponential term) derived from
the FCP plots in double logarithmic scale (Table 3). This
fact can be attributed again to the simple skin-core
structure observed and to a negligible internal stress 10-4 I I I I
state in the moulding as assumed. The exponential 0 10 20 30 40 50
constant (m) of the Paris Equation decreases with DSC crystallinity (%)
Fig. 5 FCP rates at constant ~ K level ( A K = 2,5 MPa m 1/~)
plotted against Dsc crystallinity. O, Experimental; ©, calculated
10-1
by the Paris Equation using the constants reported in Table 3
PA-6
T-direction increasing mould temperature, ie increasing crystallin-
Tm = 270oc; TM= 25oc ity. For the CT specimens cut from the plaques moulded
at high TM only a small difference, if at all, could be
Vin j (mm s -1 )
resolved by comparison of the FCP curves for the skin
10-2
10 (slow) and core, respectively. It means that the highly
30 (fast) stretched, curved crack front profile observed for the
less crystalline specimens becomes more and more
/ right-angled. It involves that increasing TM and thus
J
crystallinity, promotes a transition from plane stress
toward plane strain. The same effect in FCP behaviour
10-3
IO was observed due to postcrystallization and annealing
>. treatments on the example of polyetheretherketone
L)
E (PEEK) as reported recently. 2~ Fig. 5 demonstrates,
E however, that fatigue response of unfilled PA-6 and
skin thus FCP behaviour of other semicrystalline thermoplas-
"o

lO-q -
,'/// tics depends mostly on crystallinity.

2. Composites
FCP curves of the composites can be seen in Fig. 6
which demonstrates that increasing vr results in FCP
deceleration. This effect was observed and reported for
10-5 -- many short fibre-reinforced composites.- .6. .12719
. . 20 27
The effect of crack direction is also obvious in Fig. 6,
since T-cracked CT specimens exhibit higher FCP
resistance. It is due to the layering shown by Fig. 3
since for the composite plaques investigated the
following relation is valid:
10-6 I I I I I I
1.0 1.5 2.0 2.5 3.0 3.5 4.0 5.0 2
_c<<2 Es,
Z~K (MPa rn½) B B i=l
Fig. 4 FCP rates in the skin and core regions of the neat PA-6
injection-moulded at TM = 25°C with different plunger speed. In T-cracked specimens fibre orientation in the S layers
--, V i n j = 10 mm s - t ; - - - , V i n j : 30 mm s -~

COMPOSITES . MAY 1990 247

Table 3. Consta nts (A,m) and validity interval ( A K) of the Paris p o w e r law, dald N=A. ( A K) m, for the FCP
response of the neat PA-6

Processing conditions Notch A /7/ AK

Skin Core Skin Core (MPa m 1/2)

TM=25°C
V i n j = 10 m m S-1 L 3.3x 10 -6 4.3x 10 -6 6.3 4.9 1.6-3.4
T 5.4x 10 -6 4.7 x 10 -6 5.8 4.6 1.5-3.5
Vinj=30 m m S-1 L 5.3x 10 . 6 6.0X 10 -6 6,2 5.2 1,5-3,0
T 9.5 x 10 -6 7.2 x 10 -6 5.4 4.8 1.5-3.0

TM=80°C
V i n j = 10 m m s -1 L 2.2 x 10-5 2.3x 10 -5 3.7 3.2 1.6-2.8
T 2.0 x 10 -5 2.9 × 10 -5 3.2 2.4 1.5-2.5
Vinj=30 mm s -1 L 2.5x 10 -5 2.5× 10 -5 3.8 3.4 1.5-2.5
T 2.3x 10 -5 3.1 x 10 -s 3.6 2.8 1.5-2.5

agrees mainly with that of the load (cf. Figs l(b) and 3) The constants of the Paris power law for the GF-
which implies a greater load bearing and thus greater composites are summarized in Table 4. The results
resistance against crack propagation. 3'5'6'15'19'2°'27 demonstrated in Fig. 6 and listed by Table 4 compared
Higher reinforcing effectiveness values (Rc) of T- with those of the matrices (Fig. 4 and Table 3) could be
cracked specimens in Table 2 account for this effect. summarized as follows:
10-1 10-I

- PA-6 + GF -- PA-6 + GF

L / T directions L/ T directions
TM=25°C; Vinj= 10mrn s -1 TM= 80oC; Vinj = 10rams -1

10-2 VF(VOl%) 10-2 v F (vol %)

10 ..... 10
16 ~ 16
/
/
/
/
10-3 -- / 10-3 k
I
/ /
u
u
E i/I .,~///
E E

-ro
E

"o
/
"O
10-4 -- "o 10-4
/ ///

10-5 -- 10-5 '¢/

lO-6 I I I I I I lO-6 I I I I I I
1.0 1.5 2.0 2.5 3,0 3.5 4.0 5.0 .0 1.5 2.0 2.5 3.0 3.5 4.0 5.0
a &K (MPa m½) b &K (MPa m'})

Fig. 6 FCP curves of the GF-PA-6 composites notched in L- and T-direction, respectively. Processing conditions: (a) TM25°C; V i n j = 10
m m s - l ; (b) TM=80°C; vi.i= 10 m m s -1. -----, Fibre volume fraction, VF=0.10 (=20 w t % ) ; - - , fibre volume fraction, VF=O.16 (=30 w t % )

248 C O M P O S I T E S . M A Y 1990
Table 4. Constants (A,m) and validity interval (A K) of the Paris-type relationship for the short glass
fibre-reinforced PA-6 composites

VF A m A K ( M P a m v')
Material
processing conditions (vol %) L T L T L T

TM=25°C
Vinj=lOmm s -1 10 5.0x10 -8 1.4x10 -6 9.1 5.8 1.7-3.5 2.0-4.0
16 5.4x10 -7 2.5x10 -7 5.0 4.8 1.8-3.5 2.0-4.5
Vinj=30 mm S- 1 10 2.2x10 -8 1.1x10 -7 10.1 6.4 1.7-2.7 2.0-4.5
16 9.9x10 -8 1.1x10 -7 6.4 5.7 1.8-4.0 2.1-5.0
TM=80°C
-1
V i n i = 10 m m S 10 8 . 4 x 10 -9 4.1x10 -8 10.9 7.5 1.9-3.0 2.0-3.5
16 2 . 1 x 1 0 -7 2.0x10 -8 8.7 7.3 2.0-3.5 2.3-5.0
Vini=30 m m s -1 10 2 . 3 x 1 0 -7 9.3x10 -8 6.9 6.7 1.9-2.6 2.0-4.0
16 2 . 7 x 1 0 -8 2.9x10 -9 8.4 9.2 2.0-3.6 2.5-4.0

1) The threshold stress intensity amplitude below results also in a change from plane stress toward plane
which no fatigue crack growth takes place (AKth) is strain condition. Improved bond quality is, however,
shifted to higher A K values due to fibre loading. not always accompanied with a further increase in
This is obvious from the much smaller preexponen- resistance against fatigue crack growth. In a composite
tial constant 'A' for the composites ('A' values in with poor fibre/matrix bonding the crack path follows a
Tables 3 and 4) zig-zag route due to fibre debonding and related matrix
2) Values of 'm' for the composites are slightly higher deformation processes. For polyamide and linear
than those of the matrix (Tables 3 and 4) polyester based composites of good fibre/matrix
3) The exponential constant of the composites interfacial adhesion the crack profile proved to be more
decreases with increasing v v and a change from L- straight, which may involve less hindrance against crack
to T-notching of the specimens results in an analo- growth and thus FCP acceleration. ~9The fibre/matrix
gous trend (Table 4). bond quality was, however, not characterized in this
case.
Changes listed under (2) and (3) are connected with a
pronounced development of plane strain conditions. It In the first approximation AK(d,~/aN=c,,,,st) VS. Rc
should be noted here that stronger fibre/matrix bonding function, provided that values of the former term are

10-2

[3

5 D D • [] 1o 3 _

do/dN = 10-3mmcy

2
°~o i 10 -5 --
-

(.'i
L PA-6 + G F _
1 d o / d N = const

oI I I I I I lO-6 I I I I I I
0 0.5 1.0 1.5 2.0 2.5 3.0 1.0 1.5 2.0 2.5 3.0 3.5 LI.O 5.0

a RC (-) b AK (MPa m½)

Fig. 7 (a) (AK)damN=const values plotted against R c for the GF-reinforced PA-6 composites. The ordinate section of these regression
lines, (AK)Rc = o served for the construction of a hypothetical FCPcurve of the matrix (Fig. 7b). Note: scatter range increases with
increasing FCP rate. (b) Comparison of the FCP b e h a v i o u r of the neat PA-6 established e x p e r i m e n t a l l y for the core (scatter band indicates
for processing effects) with the extrapolated values of Fig. 7a (D)

COMPOSITES . M A Y 1990 249

taken from the range where the Paris power law is
valid, is linear (Fig. 7(a) ). This Figure shows that
fatigue response of the GF-PA-6 composites mostly
depends on the fibre reinforcing effectiveness, R c. This
is, however, rather a phenomenological description
than a causalistic one. The latter, namely, FCP rate in
function of the microstructural efficiency factor21 is
discussed below, in the concluding paragraph. From
the ordinate section (Re=0) of the straight lines fitted
for the/k K ( d a / d N _ c o n s t ) -- R C point pairs a hyl~othetical
FCP curve for the-matrix can be constructed. 1~Its run
agrees very well with those of the core layers found for
the unfilled PA-6 (Fig. 7(b) ).

Fractography
1. Matrices
Fig. 8 shows the fracture surface topology of the neat
PA-6 moulded at low TM and Vini. In both SEM pictures
of Fig. 8 the skin and core layers can clearly be distin-
guished due to their different failure manners. At the
beginning of stable FCP characteristic failure mode in
the core is a microductile one with primary and second-
ary cracking. It still remains dominant until the end of
the stable FCP, however, strongly increases its ductile
appearance. This effect is connected with the adiabatic
heating during fatigue at the crack tip which can easily
reach the glass transition temperature (Tg) of the PA-6.
In the bottom of the craters formed by secondary crack
propagation extensive crazing could be resolved (Fig.
Fig. 9 (a) Craters caused by secondary cracking phenomena in
the core region showing extensive crazing at their bottoms; (b)
striation bands on the shear lip (skin region)

9(a) ). It suggests that the amorphous interlayer

between the spherulites and crystalline lamellae - -
which determines the deformability of a given
morphology - - may influence the FCP behaviour
considerably. 26'28The main role in this respect should
be attributed to the tie-molecules connecting the
neighbouring morphologic arrangements and acting as
Spo
nuc load transfer chains. The skin fails highly ductilely at
the early stage of fatigue (rib-like pattern of Fig. 8(a) )
/
zon,
and favours shear lip formation at the end stage (Fig.
IP Core 8(b) ). In the latter, SEM picture striation bands (fatigue
advance by one loading cycle) can also be evidenced.
These striations are depicted on a higher magnification
SEM microphotograph in Fig. 9(b).
The shear lip formation is restricted considerably for
the specimens moulded at high TM due to the very thin
skin layers involved. In this case final breakdown
(unstable or fast fracture) at the end of stable FCP
occurs mostly by normal plane fracture, ie without
formation of shear lip and without 'stretching' of the
advancing crack front profile. It is a clear evidence that
the more amorphous, and thus more deformable the
skin, the stronger the contribution to the formation of a
plane stress state. In Fig. 2 between the skin and core
an interlayer, composed from sporadic nucleated
spherulites, can be observed which appears as a white
Fig. 8 Fatigue fracture surface of the neat PA-6 (T M = 25°C,
v~ni= 10 mm s -1) a t t h e beginning (near to the razor notch; (a))
zone due to strongly crazed secondary cracking in Fig.
and at the end (before final fast fracture occurs; (b)) of the 8(a). This supports the previous statement about the
stable FCPrange role of tie molecules, namely their density here should

250 C O M P O S I T E S . M A Y 1990

Fig. 10 Fatigue fracture surface of the 30 wt% GF-PA-6at the
beginning (a) and end (b) of the stable FCP range. Note: ductility
of the matrix increases with increasing da/dNor AK
be much higher than in the core. Fig. 8 gives general
impressions for the different failure mechanisms in the
skin and core, closely related with the resistance of the
given morphology which explains the FCP behaviour
observed.
2. Composites
Fig. 10 indicates that the higher A K or FCP rate the
more pronounced is the ductile failure manner of the
matrix. At the beginning of stable FCP the matrix fails
microductilely. Here 'steps' on the fracture surface due
to matrix parts broken off are caused by interaction
between matrix crazing and fibre debonding as
depicted schematically in Fig. ll(a). The bare fibres
present illustrate a rather poor matrix/fibre bonding
which supports the validity of the failure mode
proposed (Figs 10(a) and ll(a)). The failure manners
(fibre/matrix debonding, crazing, shear banding)
observed cause an extensive deviation of the crack
plane which improves the fatigue resistance. In com-
posites of better bonding between fibre and matrix the
debonding process and matrix deformation is highly
restricted which may result in FCP acceleration.
At the end of the stable FCP the matrix fails again very
ductilely due to crack tip heating effects. It leads at the
same time to changes in the microscopic breakdown
processes. In this higher A K range fibre/matrix separa-
tion dominates among the fibre-related micromecha-
a
T. ]~=-- -- -
_ II n
Fig. 11 Schematic fatigue failure micromechanisms of short
fibre-reinforced themoplastics (a) at the beginning; (b) at the
end of stable FCPrange. Dotted line indicates for possible crack
path
nisms. The high FCP rate in this region can be attributed
to a secondary cracking phenomenon of the matrix,
which is induced by tips of pulled out fibres (model in
Fig. 1l(b)). The higher FCP rates revealed at the end of
stable FCP can also be attributed to a deterioration in
the E-modulus of the composite due to thermal soften-
ing which contributes to FCP acceleration. 29
Fibre fracture events at the beginning of stable FCP are
caused rather by the stress field during 'step-bridging'
(Figs 10(a) and 1 l(a) ) in a relative stiff matrix than to
compressive forces acting on partially pulled out fibres
during the unloading cycle part as recommended by
Lang et al. 30 The latter failure mode is, however, more
probable at the end of stable FCP where crack closure
may take place (cfbroken fibres in Fig. 10(b)).
CONCL USIONS
Microstructure-related fatigue of the matrix
Based on this study the effects of the microstructural
parameters of the matrix: crystallinity and average
spherulite diameter, on the run of FCP curve are
summarized in Fig. 12. It should be emphasized here
that the trends indicated in Fig. 12 strictly relate' to this
case. It is highly probable that FCP resistance goes
through a maximum both in function of crystallinity
and spherulite size. Based on the run of stress intensity
C O M P O S I T E S . M A Y 1990 251

AKmax
II
II
/I
/ simplified in the present case based on the following
'o
~ h spherulite size
I at Vcr=0 and 1 at Vcr=l
/ with crystallinity
! /
I I/
I I!
I II
I I I
AKth
AK
Fig. 12 Effects of crystallinity and spherutite size on the FCP
response of the matrix, schematically. Note: AK,,,a× is closely
matched to the critical stress intensity factor or fractu re
toughness (K~) derived from static loading measurements. Its
value is practically unaffected by crystallinity and spherulite
size. The threshold z~g value, lXKth, connected with the onset of
crack propagation, on the other hand, slightly increases with the
above morphological parameters
factor (Kc) derived from static loading measurements
as plotted against these morphology parameters for
other semicrystalline thermoplastics, such as
polypropylene,31,3e this effect would be expected.
Considering the microstructure of an injection-
moulded semicrystalline thermoplastic as a layered
laminate (skin-core structure) one can define a
morphology-related effectiveness parameter for the
matrix, RM, by the following Equation:
gM= ~lTi.vcr,i.fcr,eff, i +~,drj.Varn,j.fam.eff.j
where:
Ti, = normalized layer thickness of the crystalline (cr)
layer, T i = normalized layer thickness of the amor-
phous layer (am) (normalization is based on specimen
thickness, B, in both cases) E Ti + E Ti = 1;
vcr.i = crystalline volume fraction in the i-layer,
V~mj = amorphous volume fraction in the j-layer.
fer e~ i and fam elf j are terms of relative morphology
effec{iveness, "the former takes into consideration the
spherulite size, type, deformability and the internal
stress state, (in relation to the loading direction) and
the latter involves the amorphous layer orientation,
deformability and internal stress state. The value of
both parameters varies between 0 and 1 and should be
determined experimentally. Under deformability,
possible morphological rearrangements, such as,
spherulite-fibrillar transition, recrystallization in the
crystalline layers, strain-induced crystallization,
disentanglement in the amorphous layers and morpho-
logical alterations in both phases due to tie-molecules,
during fatigue are considered.
It should be noted here, that the distinction between
amorphous (j) and crystalline layers (i) and fractions is
252 COMPOSITES. MAY 1990
rather arbitrary. This morphology effectiveness param-
eter in such a way takes into consideration the initial
morphology as well as its change during cyclic loading,
since both of them affect the fatigue response consider-
ably.
The complex function of Equation (4) can be strongly
assumptions:
1) no amorphous layer exists
2) crystalline fractions agree with the DSC crystallini-
ties
3) fcr,eff,idepends only on crystallinity and changes
linearly with it. The value of this term is therefore 0
2S
RM = ~ Ti. Vcr,i. fcr,eff,i = + C v2 (5)
i F-
whe re:
VDSC,S(C)are crystalline fractions of the skin and core,
respectively, from DSC measurements.
The RM values calculated according to the above route
are summarized in Table 5. Plots of the A K values
taken at a constant FCP rate, (A K)da/dN=const , a s a
function of R M resulted in straight lines (Fig. 13). This
is in close analogy with the results in Fig. 7(a), from
which the microstructure-related fatigue performance
of the composites can be read. The interceptions of the
ordinate with the regression lines,
(/k K)daldN=const,RM=O,may be used again for the
construction of a hypothetical FCP curve (see Fig.
7(b) ). In the present this curve represents the FCP
behaviour of a fully amorphous PA-6. The extrapolated
values are indeed in a very good agreement with the
FCP response for the skin of the specimens of lower
crystallinity (Fig. 4; Table 3). These findings indicate
that the microstructural efficiency concept elaborated
for chopped fibre composites 5621' • can adequately be
modified and thus extended for unfilled plastics, too.
(4)
Microstructure-related fatigue of the composites
It was demonstrated in previously5"6that the FCP rate at
a constant A K level, (da/dN) AK=const,plotted against
the microstructural efficiency factor of the composites,
Mc, in a double logarithmic representation can be
described by a linear function. The microstructural
efficiency of the composite, M c, is given by the follow-
ing semiempirical Equation: el
Table 5. Morphology effectiveness parameter of
the matrix, RM. RM calculated by Equation (5) using
the microstructural parameters reported in Table I
Processing conditions RM
TM = 25°C
Vinj=10 m m s -1 0.16
Vinj=30 m m s -1 0.10
TM=80°C
Vin j = 10 m m s - ~ 0.24
Vinj=30 mm s -~ 0.18
 3
KQ,c = M c = a + n . R c (6)
KQ,M
where:

1o .4 "I- -r i KQ,c = stress intensity factor of the composite and

d o / d N = 5 x10-5 mm cycle -1
PA-6
d a / d N = const
KO,M = stress intensity factor of the matrix, (derived
from static fracture); M c = microstructural efficiency of
the composite; a = matrix stress condition factor; n =
energy absorption ratio; and Rc = reinforcing
effectiveness of the composite (see Table 2)

I I 1 I Based on the results of static fracture measurements

0.05 0.1 0.15 0.2 0.25 carried out on the same CT specimens at T = R T and at
Rk~ (-) a cross-head speed of 10 ° mm rain -1, a = 0.9 and
n = 0.22 values were established for the composites.
Fig. 13 (AK)daldN=cons t VS. R M function for the neat PA-6. Note:
(~K)da/dN=constvalue refers for an average calculated by using The FCP rates at a given A K level plotted against this
the c o r r e s p o n d i n g values established for the skin and core M c term (calculated by Equation (6) using the above
regions. Scatter bars indicate experimental deviations o b s e r v e d mentioned 'a' and 'n' as well as R c values from Table 2)
on T- and L-notched CT s p e c i m e n s yield straight lines with fair correlation (Fig. 14). Such
a regression was observed for other short and long
GF-reinforced thermoplastic matrix composites as
published recently. 5'6'19 The correlation found in this
10-3
case suggests that the effects of processing conditions
are of secondary importance in respect of the fatigue
performance of the composites, ie the microscopic
fibre- and matrix-related breakdown processes practi-
cally do not change with the processing conditions, at
least at the A K level chosen. At higher A K levels due
to the crack tip heating and related changes in failure
(3D manners shown and discussed above, it is reasonable to
use other 'a' and 'n' values. Their values can be deter-
mined from low speed static fracture measurements
carried out at a testing temperature which may arise in
10-4 D the crack tip during fatigue. It is worth mentioning that
i
a remarkable change in the values of both 'a' and '11"
occurs at the Tg region of the matrix. 33
Considering the FCP results published for short and
>. I
L) long GV-reinforced injection-moulded PA
E o
composites, °1219 the effects of the microstructural
E
parameters on the FCP response can be summarized
-O i according to the scheme in Fig. 15. Comparing the

&Kma x
10-5 - -

Ma Composite
PA-6 + GF -O

A K = 2 . 5 MPa m ½ "O

i0-6 I I I I 1 I I I
/
0.9 1.0 1.1 1.2 1.3 1.4 1.5 1.6 1.7 1.8

MC (-)

Fig. 14 FCP rates of the c o m p o s i t e s at a constant stress intensity

amplitude, (da/dN)±K~2 5 Mea mv2, plotted against the microstruc-
tural efficiency factor, M c. Note: this straight line shifts m o r e or
i
AKth
/i' AK
less parallel to itself t o w a r d higher or lower FCP rates w h e n
d a / d N v a l u e s at higher or l o w e r A K level are considered. In this Fig. 15 Effects o f fibre loading (VF) and fibre aspect ratio (1/d)
case A K = 2 . 5 MPa m 1/2 was chosen because it b e l o n g s to the on the FCP r esponse of d i s c o n t i n u o u s f i br e- r ei nf or ced p o l y a m i d e
valid FCP range f o r all samples composites, schematically

COMPOSITES . MAY 1990 253

schemes given for the matrix and composites (Figs 12
and 15), one can conclude analogies with respect to the
change in FCP response between crystallinity and fibre
loading and between spherulite size and fibre aspect
ratio.
ACKNOWLEDGEMENT
The author would express his thanks to the Alexander
von Humboldt Foundation for granting him a fellow-
ship at the Technical University Hamburg-Harburg
(TUHH). He is also indebted to Dr I. Csikai (GAMF,
H-6000 Kecskem6t, Hungary) for supplying the
injection-moulded plaques investigated. Information
about the Laokon-Cosy-GAMF processing control
system for injection moulding is available from Dr I.
Csikai.
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AUTHOR
Dr J. Karger-Kocsis is with the Polymer and Composite
Group of the TU Hamburg-Harburg, D-2100 Hamburg
90, PO Box 901403 FRG. He is on leave from the
TAURUS Hungarian Rubber Works, Technical
Rubber Division, H-1475 Budapest, Hungary,