Article

Metal/Carbon-Fiber Hybrid Composites—Damage Evolution

and Monitoring of Isothermal Fatigue at Low and
Elevated Temperatures
Bilal Khatri 1, * , Jan Rehra 2 , Sebastian Schmeer 2 , Ulf Breuer 2 and Frank Balle 1,3

1 Walter and Ingeborg Herrmann Chair for Power Ultrasonics and Engineering of Functional Materials,
Department of Sustainable Systems Engineering (INATECH), University of Freiburg,
79110 Freiburg, Germany; [email protected]
2 Leibniz-Institut für Verbundwerkstoffe (IVW), Technische Universität Kaiserslautern,
67663 Kaiserslautern, Germany; [email protected] (J.R.); [email protected] (S.S.);
[email protected] (U.B.)
3 Freiburg Materials Research Center (FMF), 79110 Freiburg, Germany
* Correspondence: [email protected]

Abstract: Carbon-fiber-reinforced polymers (CFRPs) are the standard lightweight composite material
for structural applications in aviation. The addition of metallic fibers to CFRPs to form metal/carbon-
fiber hybrid composites (MCFRPs) has been shown to improve the elastic and plastic properties and
to enable a non-destructive method for structural health monitoring over the material’s service life. In
this paper, the results from the fatigue experiments on these hybrid composites at −55, 25 and 120 °C
are discussed. Multidirectional CFRP and MCFRP laminates, fabricated using the autoclave method,



were tested and compared under different fatigue loading conditions, while being simultaneously

 monitored for temperature and electrical resistance. Magnetic phase measurements were additionally
Citation: Khatri, B.; Rehra, J.; carried out for the chosen metastable austenitic steel fibers in the MCFRPs. The results show that
Schmeer, S.; Breuer, U.; Balle, F. the improved ductility of the hybrid composite due to the presence of the steel fibers leads to better
Metal/Carbon-Fiber Hybrid
performance under fatigue loads and a less-brittle failure behavior. Based on the chemical composition
Composites—Damage Evolution and
of the metastable austenitic steel fibers, a temperature and plastic deformation-dependent phase
Monitoring of Isothermal Fatigue at
transformation was observed, which could potentially lead to a method for non-destructive structural
Low and Elevated Temperatures. J.
health monitoring of the hybrid composite over its service life.
Compos. Sci. 2022, 6, 67. https://
doi.org/10.3390/jcs6030067
Keywords: hybrid composites; fatigue in composites; structural health monitoring
Academic Editor: Konda Gokuldoss
Prashanth

Received: 31 January 2022

Accepted: 17 February 2022 1. Introduction
Published: 23 February 2022 Carbon-fiber-reinforced polymers (CFRP) have, in the last few decades, evolved to
Publisher’s Note: MDPI stays neutral
become the primary load-bearing material in modern aircraft, comprising over 50 wt.% of
with regard to jurisdictional claims in
the fuselage mass in aircraft, such as the Boeing 787 and the Airbus A350 [1]. Compared to
published maps and institutional affil- lightweight metals, such as aluminum, CFRPs exhibit comparable stiffness with a superior
iations. strength-to-density ratio and a distinctly lower fatigue onset.
At the same time, these composites exhibit limited damage tolerance, impact tolerance
and a brittle failure behavior, as well as poor electrical conductivity opposite to their
metallic counterparts. A number of important aircraft functions, such as lightning-strike
Copyright: © 2022 by the authors. protection, grounding, electromagnetic shielding and signal transfer, can only be realized
Licensee MDPI, Basel, Switzerland. for CFRP-based fuselages by the addition of metallic components, such as copper foils,
This article is an open access article wires and cables, causing an increase in the process complexity and time. Moreover, these
distributed under the terms and additional masses do not contribute to the structural properties and are a limiting factor in
conditions of the Creative Commons
the cumulative strength-to-density ratio of the fuselage.
Attribution (CC BY) license (https://
The majority of these functions depend on the electrical properties of CFRP. Studies
creativecommons.org/licenses/by/
have looked at modifications in the matrix system to improve the electrical conductivity
4.0/).

J. Compos. Sci. 2022, 6, 67. https://doi.org/10.3390/jcs6030067 https://www.mdpi.com/journal/jcs

J. Compos. Sci. 2022, 6, 67 2 of 18

of the composite through the addition of carbon nanotubes [2,3]. A comparable level of
electrical conductivity to that of aluminum fuselages through modifications of the matrix
has thus far not been attained.
Through the integration of metal fibers in CFRPs, the advantages of both metals and
carbon fibers can potentially be combined. Hybrid composites have been demonstrated
in the case of glass-fiber/CF composites [4,5], which show improved ductility. The use
of metallic sheets or foils is established for fiber-metal laminates, such as GLARE [6],
whereas the addition of steel fibers to a polymer matrix has been shown to combine high
stiffness and ductility [7,8], enabling the tailoring of the composites’ constituents to the
mass, stiffness and ductility requirements. A number of studies and reviews from the
past four years have looked at metal/CF hybrid composites as sandwich panels, from
manufacturing and processing [9,10] to their mechanical [11–13] and damage initiation and
evolution [14] characteristics.
By integrating metal fibers and carbon fibers into so-called metal/carbon-fiber hybrid
composites (MCFRPs), the mechanical and electrical properties can be tailored by modi-
fying the laminate layup and through the fiber fraction of the metal and carbon fibers. A
pronounced improvement in the electrical conductivity through the integration of stain-
less steel fibers has been reported in recent studies [15,16]. One of these also analytically
modeled the failure behavior of steel-fiber and carbon-fiber composites [17].
In a preceding study, MCFRPs with integrated stainless steel fibers were analyzed
for their fatigue behavior and failure mechanisms at room temperature [18]. Through
the use of metastable austenitic steel fibers, a potential non-destructive structural health
monitoring (SHM) system was demonstrated. This relies on the deformation-dependent
austenite–martensite phase transformation of the steel fibers, which causes the metal to
respond to plastic deformation through a measurable magnetic response.
This response can, in turn, be correlated with the progressive damage done to the
material under fatigue conditions. This work expands upon the topic by characterizing
the MCFRPs at aviation-grade temperatures, i.e., −55 and 120 °C, while also comparing
the mechanical and electrical characteristics MCFRPs against similarly fabricated CFRP
laminates. The temperature-dependency of the austenite–martensite phase transition due
to plastic deformation under fatigue loading is also presented.

Intrinsic Structural Health Monitoring

Metastable austenitic stainless steel fibers in the MCFRPs can, in addition to improving
the electrical properties of the composite, provide a non-destructive method for gauging
damage due to fatigue over the hybrid material’s service life. Through the combination of
temperature and plastic deformation, the metastable austenitic steel can undergo a phase
transformation into the magnetically responsive martensite. This temperature-dependent,
deformation-driven austenite–martensite phase transformation of stainless steel can be
explained through its Gibbs free energy diagram [19,20], which is illustrated in Figure 1.
Above the thermodynamic equilibrium temperature T0 , the favored structure of a
given stainless steel is γ-austenite due to its lower Gibbs free energy Gγ . With decreasing
temperature, the probability of the martensitic transformation increases, owing to the
increasing free energy difference between Gγ and Gα’, shown in Figure 1 as ∆Gchem . For a
given chemical composition of the steel, the martensite start temperature (Ms ) represents the
γ→α
point below which the temperature-driven martensitic transformation can occur ∆Gmin .
When undergoing plastic deformation, the additional mechanical energy (∆Gmech )
coming into the system results in an increased free energy difference between the deformed
austenite phase (Gγ ’) and that of the austenite phase (Gα ’) at a given temperature. This
greater difference increases the probability of the γ → α0 transformation to occur at a
temperature higher than Ms , referred to here as the martensite deformation temperature Md .
J. Compos. Sci. 2022, 6, 67 3 of 18

Figure 1. The austenite–martensite phase transformation in steels as a function of temperature and

plastic deformation. Adapted from [19,20].

As Ms and Md are both difficult to determine experimentally, the temperature Md30

is defined as the temperature range within which a 50% γ → α0 transformation can occur
for a plastic deformation pl of 30%. The Ms and Md30 temperatures of the stainless steel
fibers used in this study were empirically approximated using the models described by
Eichelmann [21] and Angel [22], respectively, and were compared to those used in preceding
studies [18,23,24], which looked at different stainless steel types for their metastability.

2. Materials and Methods

2.1. Material Properties
The CFRP and MCFRP laminates were fabricated using Tenax® HTS-40 high-tenacity
carbon fibers (Teijin Ltd., Chiyoda, Japan ) in a Cycom 977-2 epoxy matrix (Solvay, Brus-
sels, Belgium, diameter 7 µm, area weight 135 g/cm2 ). Stainless steel fibers of type DIN
1.4301/AISI-304 with a diameter of 75 µm were procured from Beakaert (Zwevegem, Bel-
gium) and made up the metallic part of the MCFRPs. Table 1 summarizes the mechanical
properties of the constituent materials of the composites.

Table 1. Selected properties of the carbon fibers, steel fibers and epoxy matrix.

Carbon Fiber Stainless Steel Fiber Epoxy Matrix

Density [g/cm3 ] 1.77 7.95 ± 0.01 1.31
Tensile modulus [GPa] 239 ± 2.9 190 ± 9.2 3.52
Tensile strength [MPa] 4121 ± 755 762 ± 7.5 81.40
Failure strain [%] 1.55 ± 0.24 32 ± 2.5 n/a
Shear modulus [GPa] 50 67 ± 9 1.30
Poisson’s ratio 0.23 0.30 0.35
Fiber diameter [µm] 7 75 -

The deformation-dependent austenite–martensite transformation is highly dependent

on the chemical composition of the steel, in particular on the carbon, nitrogen, nickel and
chromium content. The constituents of the stainless steel used in this work were determined
through spectral analysis following the ASTM E 1019 and ASTM E 572 standards and are
shown in Table 2.
J. Compos. Sci. 2022, 6, 67 4 of 18

Table 2. The chemical constituents of the 75 µm thick stainless steel fibers.

Element C Si Mn P S Nb Ti
wt.% 0.026 0.32 1.57 0.011 0.009 0.016 0.004
Element Mo Cu Ni Cr V N2 Fe
wt.% 0.336 0.31 10.99 18.33 0.11 0.036 67.9

2.2. Laminate Fabrication

The CFRP laminates were fabricated using 17 unidirectional plies stacked in the
following layup,
[0°/90°/45°/−45°/45°/−45°/90°/0°/90°/0°/90°/45°/−45°/45°/−45°/ 90°/0°].
The CFRP stack was consolidated through a one-hour dwell at 135 °C, followed by a
three-hour cure at 180 °C at a heating and cooling rate of 2 °C/min. A pressure of 6.5 bar
was applied from the start to the end of the curing process. This dwell time causes a decrease
in the resin viscosity to nearly its minimum, leading to better resin distribution through
the stack and allowing longer times for entrapped air to escape. The final dimensions
of the laminate plates were measured at 350 × 350 × 2 mm3 and a CF fiber content of
60 vol.%. Figure 2a shows the layup alongside an image of the longitudinal CFRP sample
cross-section.
The MCFRP laminates were fabricated using the same CF layup except for the two
0°-plies on the periphery. These were replaced by four steel fiber layers on each side
in the [90°/ 90°/ 0°/ 0°] directions. These metallic plies were fabricated in cooperation
with GKD-Gebr. Kufferath AG (Düren, Germany) into quasi-unidirectional weaves with
polyethersulfone (PES) filaments (φ = 90 µm) in the warp direction approximately every
50 mm, as shown in Figure 3a. The weaves were impregnated with the Cycom 977-02 (area
weight: 40 g/cm2 ) resin film.

0°

SF
0°
90° 0°
45° 90°
90°
−45°
45°
45° −45°
−45° 45°

90° −45°
90°
0°

CF
0°
90°
0°
PLACEHOLDER 90°
0°
90°
90°
−45°
−45° 45°
45° −45°

−45° 45°

SF
90°
45° 90°
90° 0°

1 mm
0°
0°
500 µm
(a) (b)

Figure 2. (a) The CFRP laminate layup illustrated schematically next to a light-microscopic image
of a sample in the longitudinal direction. (b) A schematic depiction of the MCFRP laminate layup
alongside a microscopic image of a sample, with the eight peripheral layers composed of stainless
steel fibers (SF).

Figure 3b illustrates the fabrication process for the steel plies. After weaving the PES
filaments, the fibers were fixed onto a frame and stretched to ensure a parallel fiber orien-
tation. The PES fibers were then dissolved by heating to 250 °C, followed by the pressing
and curing of resin films on both sides of the ply at 130 °C. The hardened plies were then
cut to the required size and used on the top and bottom layers using the aforementioned
autoclave process. The MCFRP laminate plates were fabricated in the same lateral size as
that of the CFRP plates, with a thickness of 2.4 mm and CF and steel-fiber (SF) contents of
49 vol.% and 18 vol.%, respectively. The layup and longitudinal cross-section for MCFRP is
shown in Figure 2b.
J. Compos. Sci. 2022, 6, 67 5 of 18

Fabric installed Cleaning and Melting of the

Woven on to a frame stretching PES filaments
areas
250°C

fabric
PES-Filaments
Warp direction
Cutting to the Epoxy resin
Cooling
required size application
Weft direction
−18°C 180°C

Woven
area 350µm
15mm
Steel fiber
(a) (b)
Figure 3. (a) Images of the steel fiber woven with PES filaments in the warp direction. (b) A schematic
depiction of the preparation of the steel-fiber weaves for the fabrication of MCFRPs. The fibers are
stretched on to a frame and heated to 250 °C to melt the PES filaments. After cooling to −18 °C and
cutting to the required dimensions, the plies were impregnated with epoxy at 180 °C.

The laminate plates were cut into dog-bone shaped samples using a Daetwyler Mi-
crowaterjet (Bleienbach, Switzerland), measuring 160 mm in length with a grip-area of
20 × 35 mm as illustrated in Figure 4a. The middle section of the samples (R = 139 mm)
resulted in a width of 5 mm at the center.

Figure 4. (a) A schematic depiction of the dog-bone shaped samples fabricated using CFRP and
MCFRP for this work. All measurements are in mm. The radial central region of the sample resulted
in a width of 5 mm in the middle of the sample. (b) An image of a fully-equipped MCRFRP sample
for fatigue testing. The sample is clamped in the servohydraulic test-machine between (1) and (2).
The setup is additionally equipped with a strain-gauge (3), three thermocouples mounted onto a
holder (4) and a four-point resistance measurement setup (5).

The samples were coated with the SilverDAG 1415 electrically conductive paste (Plano,
Wetzlar, Germany) to reduce the contact resistance for the four-point resistance electrical
measurements. Additionally, 0.5 mm-thick glass-fiber composite tabs were adhered to the
grip area of the samples using epoxy to electrically isolate the sample from the rest of the
test setup and to ensure a uniform clamping force during the experiments.

2.3. Experimental Setup

The CFRP and MCFRP samples were tested under tensile and fatigue conditions at
three different temperatures; –55, 25 (RT) and 120 °C. Tensile tests were used to determine
J. Compos. Sci. 2022, 6, 67 6 of 18

the ultimate tensile strength of the samples, based upon which the fatigue tests were carried
out. Fatigue testing under increasing load–amplitude (ILA) conditions was carried out to
gauge the materials’ response to different loads at different temperatures.
Based on the failure stress amplitude and the plastic material response during the
ILA tests, a set of tests under constant load–amplitude (CLA) were performed to develop
SN-curves for both laminates at each of the aforementioned temperatures. To analyze
the fracture behavior, interrupted constant load–amplitude (iCLA) tests were carried out,
where the samples were microscopically imaged at various fatigue stages to evaluate the
crack initiation and propagation under cyclical loading conditions.
The tensile and fatigue experiments were carried out on the Zwick/Roell HC-25
servohydraulic testing machine (Ulm, Germany). Force and strain measurements were
taken using a 25 kN load cell and a clip-on strain gauge with a ±2.5 mm range. The non-RT
experiments were performed with the samples enclosed inside a temperature chamber
from the same manufacturer. This chamber was heated to 120 °C using its internal heater
or cooled down to −55 °C connected to an external liquid nitrogen (LN2 ) tank, which the
chamber was able to control using a valve.
All fatigue tests were performed at a stress ratio R = 0.1 at a frequency of 5 Hz, except
for the experiments at −55 °C, which were carried out at 10 Hz due to the volume limitations
of the available LN2 tank. For tests at –55 and 120 °C, the samples were held for 30 min
after the test temperature was attained to ensure temperature homogeneity over the whole
sample. Cyclical measurements of force, displacement, stress and strain were recorded
using the testing machine’s software, testXpert R. These yielded the total strain–amplitude
a,t and stiffness trends shown in the results and were recorded for each test up to the
sample failure at the stress-amplitude σa,f and the corresponding loading cycle Nf .
Additional sensors were incorporated into the test setup to measure the sample
temperature and electrical resistance during the experiments. Three type K thermocouples
were used to observe changes in the sample’s surface temperature due to fatigue and
fractures. The difference of the central thermocouple’s (TC2 ) reading, which is situated in
the region undergoing fatigue damage, and the average of the temperature of the upper
and lower thermocouples (TC1 and TC3 , respectively), situated 20 mm from TC2 , yielded
the temperature difference (∆T) of the sample,

TC1 + TC3
∆T = TC2 − . (1)
2
The stiffness degradation of the samples was obtained by taking the normalized ratio
of the upper and lower limits of the applied force F and measured strain e for each loading
cycle N using

Fmax − Fmin Fmax − Fmin

   
Stiffness degradation = − (2)
emax − emin N emax − emin N =0
A four-point resistance measurement setup was realized using two gold-plated clamps
attached to the sample throughout the tests to measure the change in electrical resistance
∆R. For MCFRP, the martensite content was measured and compared before and after the
relevant experiments using the Fischer FMP-30 ferritscope (Helmut-Fischer, Sindelfingen,
Germany). The temperature, resistance and martensite readings were interfaced with an
in-house data-logger developed in the LabVIEW® programming environment.

3. Results and Discussion

3.1. Tensile Tests
The CFRP and MCFRP samples were tested for their monotonic properties at a rate
of 50 N/s at –55, 25 and 120 °C. Five CFRP and MCFRP samples were tested at each
temperature. The measured ultimate tensile strengths are shown in Figure 5.
The CFRP samples in Figure 5a show higher ultimate tensile strengths (UTS) compared
to their MCFRP counterparts. This is a result of the laminate layup difference between
J. Compos. Sci. 2022, 6, 67 7 of 18

the two composites with the CFRP laminate carrying two more 0° CF layers. The UTS
for both laminates can be seen to decrease with increasing temperatures. In Figure 5b, no
pronounced difference in the plasticity and the total strain at failure was observed between
the two laminates. The average UTS values observed for each laminate and temperature
were used as the upper boundary condition for the increasing load–amplitude fatigue tests.

(a) (b)

Figure 5. Results from the quasi-static tests, (a) the ultimate tensile strength (UTS) and (b) the failure
strain, of the CFRP and MCFRP samples at the three test temperatures.

3.2. Increasing Load–Amplitude (ILA) Tests

Increasing load–amplitude tests were performed for both composites at each tem-
perature point using the data obtained from the monotonic experiments. Each ILA test
was carried out at a step-wise increasing stress-amplitude ∆σa of 5 MPa every 5 × 103 to
1 × 104 cycles per step (∆N). The experiments at RT and 120 °C were done at a loading
frequency of 5 Hz, whereas the −55 °C tests were performed at 10 Hz. The upper limit of σa
was set to the ultimate tensile strength (UTS) observed for each material and temperature.
Figures 6 and 7 show the characteristic curves from ILA tests for both laminates. Both
follow a step-wise increase in the stress-amplitude with a corresponding increase in the total
strain–amplitude, indicated in the blue curves, leading to different stiffness degradation
behaviors, shown in yellow. At all three test temperatures, the CFRPs (Figure 6) show
no degradation until after the halfway point of the experiment (N > 0.5 · Nf ), after which
delaminations and fiber breakages cause a sharp decrease in the stiffness, leading to a
brittle failure behavior.
In comparison, the stiffness degradation of the MCFRP (Figure 7) is more reactive
to the step-wise increasing load–amplitudes, leading to a gradual degradation and a less
brittle failure. This is due to the ductility of the steel fibers on the periphery of the MCFRP
samples, which undergo plastic deformation in response to the applied cyclical load. The
stiffness degradation can additionally be seen to be sharper at lower temperatures for
the MCFRPs.
For the experiments at room temperature, the highest temperature increase (∆T) for
both the CFRP and MCFRP samples (Figures 6a and 7a, respectively) can be seen at the
sample failure, as a result of the numerous fiber breakages at this point. Over the course
of the tests, the ∆T for the CFRP exhibits a change of up to 0.5 °C. In contrast, the MCFRP
sample exhibits a progressive temperature increase with increasing load amplitudes, with
∆Tmax reaching 1 °C during the fatigue phase.
For the tests at 120 °C (Figures 6b and 7b) as well as those at −55 °C (Figures 6c and 7c),
the
1
∆T max can be seen to remain within ±1 °C throughout the tests.
The electrical resistance behavior with fatigue, indicated in the green curves in
Figures 6 and 7, confirm the slower fatigue onset of the MCFRPs. For the CFRP, the change
in resistance was dependent on the damage done to the 0° CF-layers at the center and the
J. Compos. Sci. 2022, 6, 67 8 of 18

periphery of the samples (shown in Figure 2a) and can be seen to remain constant up until
fiber breakages right before failure.
The 45° and 90° CF layers did not contribute to the electrical resistance of the sam-
ple, as they provide no direct electrical contact between the terminals of the four-point
resistance measurement setup (see Figure 4b(5)). The steel fibers in the MCFRPs, with
an inherently lower electrical resistance than CF, showed a gradual increase in resistance
while undergoing plastic deformation. At RT and at 120 °C, a pronounced increase prior to
failure can also be observed, arising due to fiber breakages.

(a)

(b)

(c)
Figure 6. Fatigue behavior of the CFRP samples under increasing load–amplitude (ILA) conditions
(a) at room temperature/5 Hz, (b) at 120 °C/5 Hz and (c) at −55 °C/10 Hz.
J. Compos. Sci. 2022, 6, 67 9 of 18

(a)

(b)

(c)
Figure 7. Fatigue behavior of the MCFRP samples under increasing load–amplitude (ILA) conditions
(a) at room temperature/5 Hz, (b) at 120 °C/5 Hz and (c) at −55 °C/10 Hz.
J. Compos. Sci. 2022, 6, 67 10 of 18

3.3. CLA—Constant Load–Amplitude (CLA) Tests

Experiments at constant load–amplitude were performed to investigate and compare
the fatigue behavior, in the form of SN-curves, for both composite materials. At each test-
temperature, the cycles to failure (Nf ) were recorded against the load–amplitude alongside
the temperature, electrical resistance and the pre- and post-failure martensite content.
Figures 8 and 9 show representative results from CLA tests of CFRP and MCFRP samples,
respectively, alongside the simultaneous recording of the change in the sample temperature
(∆T) and electrical resistance (∆R) due to fatigue.
Under CLA conditions, both samples exhibited a three-phase stiffness degrada-
tion behavior. During the first stage, the samples undergo cyclic softening during the
first ≈ 2% cycles. This softening was more pronounced at higher temperatures. The stiff-
ness degradation curves of the CFRP samples (Figure 8a–c, yellow) show a steady decrease
over the course of the tests, whereas the MCFRP samples (Figure 9a–c, yellow) exhibit a
relatively flat region between the fatigue-softening and failure stages.
The strain–amplitude curves (blue) indicate the progressive damage done to the
samples over the course of the tests. Both samples exhibit a more brittle behavior at
lower temperatures, whereas the CFRP samples accumulate damage, arising due to layer
delaminations and fiber breakage in the 45° and 90° layers relatively early when compared
to their MCFRP counterparts (see Section 3.5). These total strain–amplitude and stiffness
degradation trends hold for all three test temperatures and are an indicator for the better
fatigue performance of MCFRPs.
The red curves show the change in temperature over the CLA tests. At 120 °C
(Figures 8b and 9b), the ∆T of both samples remains unchanged throughout the fatigue
stage. At RT and −55 °C, both samples showed a sharp increase in temperature at the start,
followed by a gradual decrease back to the ambient temperature over the course of the
experiment. The initial increase in temperature occurs during the cyclic-softening stage
and is more pronounced at −55 °C due to accumulation of internal stresses during the
cool-down phase before the samples are cyclically loaded.
The electrical resistance (green) curves for both sample types follow the expected
trend seen in the ILA tests. The resistance of the CFRP samples, mainly dependent on the
four 0° CF-layers, remained relatively constant throughout the tests independent of test
temperature, followed by an increase before failure, where fiber breakages start to occur. In
contrast, plastic deformation of the steel fibers of the MCFRPs results in a gradual increase
in ∆R at RT and 120 °C. At −55 °C, the change in resistance occurred chiefly at failure for
both samples.
Figure 10 summarizes the results of CLA tests in form of SN-curves. Both sample
types exhibit the expected inverse σa -N trend up to the run-out (N = 2 × 106 ) as well as
higher fatigue strengths at lower temperatures. The difference in the stress amplitudes
between the CFRP and MCFRP arose due to the lower number of 0° CF layers in the MCFRP
samples. Comparing the −55 °C run-out tests, the CFRP and MCFRP samples showed 30 %
higher fatigue strengths compared to their respective RT counterparts.
J. Compos. Sci. 2022, 6, 67 11 of 18

(a)

(b)

(c)
Figure 8. Representative behavior of the CFRP samples under constant load–amplitude (CLA)
fatigue loading with R = 0.1 , tested at (a) room temperature/5 Hz, (b) at 120 °C/5 Hz and (c) at
−55 °C/10 Hz.
J. Compos. Sci. 2022, 6, 67 12 of 18

(a)

(b)

(c)
Figure 9. Representative behavior of the MCFRP samples under constant load–amplitude (CLA)
fatigue loading with R = 0.1 , tested at (a) room temperature/5 Hz, (b) at 120 °C/5 Hz and (c) at
−55 °C/10 Hz.
J. Compos. Sci. 2022, 6, 67 13 of 18

−55 °C

Figure 10. SN-Curves for the outline CFRP and the solid MCFRP laminates at black, square: RT, blue,
inverted triangle: −55 °C and red, triangle: 120 °C, alongside their respective power-law relationships.
The results shown with arrows did not fail up to 2 × 106 cycles. The annotations next to the −55 °C
MCFRP results indicate the maximum martensite content measured post-failure for the corresponding
experiments. The highest measured Fe-% was 8.2 % for the experiment carried out at σa = 160 MPa.
No martensite content was observed at RT or at 120 °C.

3.4. Metastability of the Steel Fibers

The plasticity-induced martensitic phase transformation was measured for the MCFRP
samples at the three test temperatures. No martensite content could be measured for all
experiments at RT and 120 °C. The measured maximum martensite content observed at
the end of each MCFRP CLA test at −55 °C is annotated in Figure 10. The Fe-% content
measured in the low-cycle fatigue (LCF) regime (Nf ≤ 1 × 104 ) as well as for the run-out
test (N = 2 × 106 ) is significantly lower than that of the high-cycle fatigue (HCF) tests,
indicating a dual-dependency on the magnitude of the applied cyclical stress as well as a
minimum number of cycles to failure.
The cumulative deformation of the CF and SF in the hybrid composite at a given
stress-amplitude is the key factor governing the measured magnetic response. This can
be seen for the sample tested at σa = 130 MPa, which did not fail until the experimental
upper limit of 2 × 106 cycles but exhibited a Fe-% content significantly lower than that of
the experiment performed at σa = 140 MPa. This could be a result of the applied stress-
amplitude not being high enough to cause significant plastic deformation in the steel fibers.
The highest Fe-% was measured at 8.3 % at σa = 160 MPa and Nf = 158,630 cycles.
The room temperature stability of the austenite phase for the steel fibers used in this
work can be explained through the Schaeffler diagram [25]. The steel fibers used here and
in the preceding study [18] fall within the norms of the DIN standards for steels of type
1.4301 (AISI 304-L); however, their metastability was found to be significantly different
at room temperature. Figure 11 illustrates and compares the metastability based on the
measured chemical constituents of the fibers used in both studies.
It can be seen from Figure 11 that, although the steel fibers used in both studies
fall under the constraints of the DIN 1.4301 standard, they differ significantly from each
other in their nickel-equivalent content. This equivalency is dependent additionally on
the carbon, manganese and nitrogen content found in the fibers. The chemical makeup of
the fibers used in the prior study, marked red, lie on the boundary of the austenite and
the martensite+austenite phase, which resulted in their metastability at room temperature
and below. In contrast, the four fiber batches analyzed during this study had higher Ni-
equivalent content and lay on the boundary of the austenite and austenite+ferrite phases.
J. Compos. Sci. 2022, 6, 67 14 of 18

This resulted in a more stable austenite phase at room temperature. The Ms and
Md30 temperatures for the current and preceding studies, based on the empirical models
described by Eichelmann [21] the Angel [22], are compared in Table 3.

Figure 11. A comparison of the steel-fiber equivalent chemical formulations from four batches used
in this work (blue), compared to those used in a preceding study (red) [18], using the Schaeffler
phase-diagram [25]. The area within the red rectangle indicate the tolerances allowed for 1.4301 steel.

Table 3. A comparison of the Ms and Md30 temperatures calculated through the Eichelmann [21]
and Angel [22] empirical models.

Fiber Diameter Ms (Eichelmann) Md30 (Angel)

[µm] [°C] [°C]
Backe et al, 2018 [18] 60 µm −38 47
Current work 75 µm −254 −24

Comparing the Md30 temperatures for both fibers, the metastability and the result-
ing deformation-induced martensitic phase transformation of the steel fibers from the
previous study can be justified. For the fibers used in this work, the Md30 temperature
of −24 °C resulted in a stable austenitic phase at room temperature. For this reason, the
martensitic phase could be observed and measured solely for the tests carried out at −55 °C.
Future investigations can look at tailored steel compositions, which can ensure metastable
characteristics at room temperature.

3.5. Microscopy and Damage Evolution

Interrupted CLA tests were performed to observe and compare the fatigue–failure
mechanisms of the CFRP and MCFRP samples. The sample cross-sections were hand-
polished and imaged at different points under CLA conditions to observe the crack initia-
tion, growth and failure. These experiments were performed at RT using load–amplitudes
of 225 MPa for the CFRP and 100 MPa for the MCFRP samples, with an expected failure in
the high-cycle fatigue (HCF) regime, between N = 2 − 3 × 105 cycles. No additional sensors
were mounted onto the sample during these tests to protect the imaging surfaces of the
samples. Figures 12 and 13 show these results for CFRP and MCFRP, respectively.
J. Compos. Sci. 2022, 6, 67 15 of 18

a) N=0 b) N=0.13 Nf

1 mm 1 mm

d) N=0.37 Nf c) N=0.51 Nf

1 mm 1 mm

e) N=0.75 Nf f) N=0.99 Nf

1 mm 1 mm

Figure 12. Microscopic images showing the damage evolution of a CFRP sample at various fractions
of its fatigue life, indicated as a fraction of the cycles to failure (Nf ). Visible damage is shown using
the white arrows.

The CFRP images shown in Figure 12 confirm the early damage initiation and prop-
agation observed during the CLA tests. During the first stage of fatigue (imaged at
N = 13 % · Nf ), micro-cracks in the matrix can be observed alongside a delamination
of part of the lowermost 0°-CF layer. At N = 37 % · Nf , a delamination of the uppermost
0°-CF-layer can be seen. This is followed by macro-delaminations of the 45° layers at
75 % · Nf . At this point, the effective sample cross-section is significantly reduced and
the failure growth-rate accelerates. Shortly prior to failure (N = 99 % · Nf ), the outermost
0°-layers can be seen to have completely separated and suffered fiber breakage. At Nf , the
core 0°-layers failed due to the highly reduced effective sample cross-section, leading to
very high stresses on the remaining intact layers and a brittle failure.

a) N=0 b) N=0.1 Nf

1 mm 1 mm

c) N=0.57 Nf d) N=0.72 Nf

1 mm 1 mm

e) N=0.88 Nf f) N=0.99 Nf

1 mm 1 mm

Figure 13. Micrographs showing the damage evolution of an MCFRP sample over its fatigue life. The
white and blue arrows indicate damage observed in the carbon-fiber and steel-fiber layers, respectively.

The MCFRP failure behavior can be seen in Figure 13. During the first stage, no
micro-cracks could be observed in the sample cross-section (N = 10 %), which confirms
the significantly lower fatigue softening observed in these samples during the CLA tests.
Visible damage can be observed only after the half-way mark of the fatigue life. This
included CF layer delaminations as well as debonding and expulsion of some 90° steel fiber
layers at N = 72 % · Nf , shown as the blue arrows in Figure 13d. This point also marked
the start of the accelerated damage phase, which resulted in several macro-delaminations
and fiber breakages of the outermost steel-fiber layer as well as for the ±45° and 90° CF
layers at 88 % · Nf (Figure13e). During the final stage before failure, several carbon-fiber
breakages and a complete breakage of one of the 0° steel-fiber layers can be seen.
The damage initiation and propagation differences between CFRP and MCFRP, ob-
served during the tests under constant load–amplitudes can be confirmed in the microscopic
J. Compos. Sci. 2022, 6, 67 16 of 18

images. The damage initiation and propagation occurs significantly later for the MCFRP
due to the ductility of the steel fibers. When comparing the two composites right before
failure (N = 99 % · Nf ), the MCFRPs exhibited greater damage in the form of delaminations
and fiber breakages, which resulted in comparatively less brittle failure behavior.

4. Conclusions and Outlook

In this work, we explored the fatigue behavior of metal/carbon-fiber hybrid com-
posites over a wide range of temperatures and compared the results to conventional
carbon-fiber-reinforced polymers. Both composites were fabricated using the autoclave
method with an identical epoxy matrix material. Tensile tests were performed to gauge the
ultimate tensile strength of each composite, which was the basis for fatigue testing. The
CFRP samples exhibited higher UTS due to more 0° layers in the laminate.
Fatigue experiments were performed at a stress ratio R of 0.1 at 5 Hz at RT and
120 °C as well as at 10 Hz at −55 °C. These included experiments with increasing load–
amplitudes that showed increased strength at lower test temperatures. Both laminates
showed increased cyclic softening at higher temperatures. A series of constant load–
amplitude tests revealed the temperature behavior of the laminates over their fatigue
properties up to 2 × 106 loading cycles.
At −55 °C, the CFRP and MCFRP laminates were found to be, respectively, 30 % and
40 % more resilient compared to the 120 °C experiments. Simultaneous measurement of
temperature on the sample surface enabled the monitoring of temperature evolution due
to fatigue and due to crack initiation and propagation under cyclical loading. Electrical
resistance measurements showed that the plastic deformation and breakage of the steel
fibers in the MCFRPs resulted in a simultaneous decrease in their electrical conductance.
The use of metastable austenitic steel fibers enabled the monitoring of the deformation-
dependent austenite–martensite phase transformation before and after the fatigue tests.
At 120 °C and at room temperature, no martensite content was detected. The samples
tested at −55 °C indicated a load- and fatigue-dependent relationship with the martensitic
transformation, with up to 8.2 % martensite measured in the HCF regime. These results
are dissimilar when compared to the preceding study [18], which reported up to 12 %
martensite content at room temperature.
The difference can be explained through the Cr and Ni-equivalent contents in the
steel fibers through the Schaeffler diagram. Though both steel fibers qualify for the DIN
standard 1.4301/AISI standard 304-L steel, the slightly higher Ni and Cr equivalent content
of the fibers used in this study led to a more stable austenitic phase at room temperature
and higher. To measure and correlate the degree of plastic deformation due to fatigue
with the martensitic content in a practical application, steel fibers with a tailored chemical
makeup, particularly by controlling the Ni, Cr, N and C-content, will be required.

Author Contributions: Conceptualization, S.S., U.B. and F.B.; methodology, S.S. and F.B.; software,
B.K.; validation, J.R. and B.K.; formal analysis, B.K.; investigation, B.K.; resources, S.S., F.B. and U.B.;
data curation, B.K.; writing—original draft preparation, B.K.; writing—review and editing, J.R., S.S.,
F.B. and U.B.; visualization, B.K. and J.R.; supervision, F.B., U.B.; project administration, S.S., F.B. and
U.B.; funding acquisition, F.B. and U.B. All authors have read and agreed to the published version of
the manuscript.
Funding: This research was funded by the Deutsche Forschungsgemeinschaft (DFG), Project BA4073-
6-2 and BR4262/2-1.
Acknowledgments: The authors would like to thank and gratefully acknowledge the financial
support from the Deutsche Forschungsgemeinschaft (DFG), funding number 650202.
Conflicts of Interest: The authors declare no conflict of interest.
J. Compos. Sci. 2022, 6, 67 17 of 18

Abbreviations
The following abbreviations are used in this manuscript:

CF Carbon-fiber
CFRP(s) Carbon-fiber reinforced composite(s)
SF Steel-fiber
MCFRP(s) Metal/carbon-fiber reinforced composite(s)
SHM Structural health monitoring
PES Polyethersulfone
ILA Increasing load–amplitude
CLA Constant load–amplitude
iCLA Interrupted constant load–amplitude
LCF Low-cycle fatigue
HCF High-cycle fatigue
RT Room temperature
TC Thermocouple
LN2 Liquid nitrogen
Gγ Gibbs’ free energy of γ-austenite steel
Gα ’ Gibbs’ free energy of α-martensite steel
∆Gchem Chemical energy difference between Gγ and Gα ’
∆Gmech Mechanical energy difference between Gγ and Gα ’
pl Plastic strain
Ms Martensite start-temperature
Md Martensite deformation temperature
Md30 Martensite deformation temperature for a 50 % transformation at pl = 30 %
σa Stress amplitude
σa,f Stress amplitude at sample failure
a,t Total strain amplitude
R Ratio of the lower and upper loading limits under cyclical loading
N Fatigue loading cycle
Nf Number of cycles at sample failure
∆σa Stress amplitude step
∆T Change in temperature
∆R Change in electrical resistance

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