Polymers 14 02194

polymers
Article
Carbon Fiber/PLA Recycled Composite
Salem Al Zahmi 1,2, * , Saif Alhammadi 1 , Amged ElHassan 3 and Waleed Ahmed 4
1 Department of Chemical & Petroleum Engineering, United Arab Emirates University,

Al Ain P.O. Box 15551, United Arab Emirates; 201770302@uaeu.ac.ae
2 National Water and Energy Center, United Arab Emirates University,
Al Ain P.O. Box 15551, United Arab Emirates
3 Department of Mechanical and Aerospace Engineering, United Arab Emirates University,
Al Ain P.O. Box 15551, United Arab Emirates; 201450104@uaeu.ac.ae
4 Engineering Requirements Unit, United Arab Emirates University,
Al Ain P.O. Box 15551, United Arab Emirates; w.ahmed@uaeu.ac.ae
* Correspondence: s.alzahmi@uaeu.ac.ae
Abstract: Due exceptional properties such as its high-temperature resistance, mechanical charac-
teristics, and relatively lower price, the demand for carbon fiber has been increasing over the past
years. The widespread use of carbon-fiber-reinforced polymers or plastics (CFRP) has attracted many
industries. However, on the other hand, the increasing demand for carbon fibers has created a waste
recycling problem that must be overcome. In this context, increasing plastic waste from the new 3D
printing technology has been increased, contributing to a greater need for recycling efforts. This
research aims to produce a recycled composite made from different carbon fiber leftover resources
to reinforce the increasing waste of Polylactic acid (PLA) as a promising solution to the growing
demand for both materials. Two types of leftover carbon fiber waste from domestic industries are
handled: carbon fiber waste (CF) and carbon fiber-reinforced composite (CFRP). Two strategies are
adopted to produce the recycled composite material, mixing PLA waste with CF one time and with
CFRP the second time. The recycled composites are tested under tensile test conditions to investigate
the impact of the waste carbon reinforcement on PLA properties. Additionally, thermogravimetric
Citation: Al Zahmi, S.; Alhammadi,
analysis (TGA), X-ray diffraction (XRD), and Fourier-transformed infrared spectroscopy (FTIR) is
S.; ElHassan, A.; Ahmed, W. Carbon
carried out on composites to study their thermal properties.
Fiber/PLA Recycled Composite.
Polymers 2022, 14, 2194. https://
Keywords: carbon fiber-reinforced polymer composites; pure carbon fiber; mechanical treatment;
doi.org/10.3390/polym14112194
tensile strength
Academic Editor: Victor
Tcherdyntsev
Received: 5 May 2022

Accepted: 24 May 2022 1. Introduction
Published: 28 May 2022 Plastic consumption has increased rapidly in several fields. As a result, waste genera-
tion has increased during the last century. The generation of waste is not only a challenge
Publisher’s Note: MDPI stays neutral
with regard to jurisdictional claims in
for humanity but also a major issue for the stability of the whole ecosystem [1]. Therefore,
published maps and institutional affil-
researchers are encouraged to work on environmental solutions to the problem of collecting
iations. and increasing waste of polymeric materials to protect the earth’s natural resources and to
develop a sustainable society. Several suggestions have arisen in response to studies by
researchers including curbing the use of plastics, applying bio-degradable plastic materi-
als, shifting towards non-plastic materials, etc., according to the needs of the society [2].
Copyright: © 2022 by the authors. Proposals for a sudden shift to remove plastics from the world, however, is criticized by
Licensee MDPI, Basel, Switzerland. many sectors, including products and services, because a drastic shift may cause economic
This article is an open access article instability in the world due to the linkage of a wide variety of economic and social strings
distributed under the terms and with the plastic industry [3].
conditions of the Creative Commons Therefore, the application of biodegradable plastics has been presented as the most
Attribution (CC BY) license (https:// viable solution according to the current situation by both researchers and industrialists [4].
creativecommons.org/licenses/by/
This nod by the main stakeholders and interest of the public towards the conservation of
4.0/).
Polymers 2022, 14, 2194. https://doi.org/10.3390/polym14112194 https://www.mdpi.com/journal/polymers

Polymers 2022, 14, x FOR PEER REVIEW 2 of 19
Polymers 2022, 14, 2194 2 of 19
of a healthy environment with less plastic usage in daily life has increased the research on
a healthy environment
biodegradable with less plastic usage in daily life has increased the research on
polymers [5].
biodegradable polymers [5].
1.1. Polylactide (PLA)
1.1. Polylactide (PLA)
Polylactide (PLA), one of the bio-based polymers used as shown in Figure 1, is a bi-
Polylactide
odegradable (PLA),
polymer one in
utilized ofathe
widebio-based
range of polymers
applicationsused as shown
including in Figurepack-
automation, 1, is a
biodegradable polymer utilized in a wide range of applications including
aging, and 3D printing. Because it is easily available and convenient, polylactic acid PLAautomation,
is packaging, and 3Dfor
an ideal candidate printing. Because
a polymeric it is easily
material; yet itavailable and convenient,
lacks thermal polylactic
and mechanical acid
stability.
PLA is an ideal candidate for a polymeric material; yet it lacks thermal and mechanical
PLA is predicted to break down at a temperature of around 400 degrees Celsius. However,
stability. PLA is predicted to break down at a temperature of around 400 degrees Celsius.
because of its limited thermal stability, recycling the material and extracting valuable com-
However, because of its limited thermal stability, recycling the material and extracting
ponents from the matrices is time-consuming [6].
valuable components from the matrices is time-consuming [6].
Figure 1. 1.
Figure Chemical Structure
Chemical ofof
Structure Polylactide Acid.
Polylactide Acid.
Polylactic
Polylactic acid
acid (PLA)
(PLA) is is
anan aliphatic
aliphatic polyester.Carothers
polyester. Carothers DuPont
DuPont discovered
discovered PLA
PLA inin
1932bybyheating
1932 heatinglactic
lacticacid
acidunder
undera avacuum.
vacuum.PLA PLA hashas piqued
piqued the
the interestofofresearchers
interest researchers
over
over the
the last
last twotwo decades
decades due
due toto
itsits superior
superior processability
processability andand characteristics
characteristics when
when com-
com-
pared to other biodegradable polymers. Pre-preg is a composite material composed ofof
pared to other biodegradable polymers. Pre-preg is a composite material composed
“pre-impregnated”fibers
“pre-impregnated” fibersandandpartly
partlycured
curedpolymer
polymermatrices,
matrices,including
including epoxy
epoxy oror epoxy
epoxy
resins, or a thermoplastic combined with fluid elastomers or
resins, or a thermoplastic combined with fluid elastomers or resin [7,8]. PLA has been resin [7,8]. PLA has been
widely electrospun—pure PLA, PLA blends, and their nanocomposites
widely electrospun—pure PLA, PLA blends, and their nanocomposites created with met- created with metals,
metal
als, metaloxides,
oxides, andandcarbon
carbon nanotubes—to
nanotubes—to control its its
control functionality
functionalityconcerning
concerningendendpurposes,
pur-
making it superior to petroleum-based polymers such as polyethylene
poses, making it superior to petroleum-based polymers such as polyethylene (PE), poly- (PE), polypropy-
lene (PP), polystyrene (PS), polycarbonate (PC), and polyethylene terephthalate (PET) [9].
propylene (PP), polystyrene (PS), polycarbonate (PC), and polyethylene terephthalate
Due to the substantially inadequate mechanical performance of pure thermoplastic ma-
(PET) [9]. Due to the substantially inadequate mechanical performance of pure thermo-
terial like PLA [10], the mechanical properties can be improved by adding reinforcement
plastic material like PLA [10], the mechanical properties can be improved by adding rein-
material such as continuous carbon fiber (CCF) to the thermoplastic matrix to form a
forcement material such as continuous carbon fiber (CCF) to the thermoplastic matrix to
continuous carbon fiber reinforced polymer composite (CCFRPC), which could be used
form a continuous carbon fiber reinforced polymer composite (CCFRPC), which could be
in different engineering applications, such as 3D printing. The reinforcement of natu-
used in different engineering applications, such as 3D printing. The reinforcement of nat-
ral fibers with biopolymers is an efficient technique to develop composites that are fully
ural fibers with biopolymers is an efficient technique to develop composites that are fully
biodegradable [11], by incorporation of various percentages of untreated and alkali-treated
biodegradable [11], by incorporation of various percentages of untreated and alkali-
Coir Fibers (CF) and pineapple leaf fibers (PALF) in PLA biocomposites and characteri-
treated Coir Fibers (CF) and pineapple leaf fibers (PALF) in PLA biocomposites and char-
zations of flexural, morphological, and dynamic mechanical properties that will provide
acterizations of flexural, morphological,
attractive consideration of these hybrid and dynamic mechanical
biocomposites properties
for various that will
lightweight pro-
uses in a
vide attractive consideration of these hybrid biocomposites for various
broad selection of industrial applications. Unidirectional flax fabrics were used to reinforce lightweight uses
inpoly(lactic
a broad selection
acid) (PLA).of industrial
Flax/PLAapplications.
composites were Unidirectional
produced byflax fabrics were usedusing
thermo-compression to
reinforce
as-receivedpoly(lactic acid)
flax fibers and(PLA). Flax/PLA
titanium dioxide composites wereflax
(TiO2 ) coated produced by thermo-com-
fibers [12], to investigate
pression using as-received flax fibers and titanium dioxide
the effect of annealing temperature and time, under quiescent or mechanical (TiO2) coated flax fibers
stress [12],
condi-
totions,
investigate the effect of annealing temperature and time, under quiescent
on the microstructure, interfacial adhesion, crystallization, and mechanical properties or mechanical
stress conditions, on the microstructure, interfacial adhesion, crystallization, and mechan-
of composites.
ical properties of composites.
The development of creative ways for generating sustainable solutions for manufac-
The items
turing development
with high of creative
durability, ways for generating
longer sustainable
shelf-life, and solutions for
quality retention aftermanufac-
recycling
turing items with
is required by thehigh durability,
goal longereconomy.
of the plastic shelf-life, and quality retention
Additionally, after recycling
the effective recyclingisof
required by the
the plastics andgoal
the of the plasticplastics
multi-layer economy. Additionally,
is considered the effective
challenging due torecycling of the
their composite
nature [13]. For such cases, mechanical recycling is more resource-efficient; however, it is
Polymers 2022, 14, 2194 3 of 19

plastics and the multi-layer plastics is considered challenging due to their composite na-
ture [13]. For such cases, mechanical recycling is more resource-efficient; however, it is
limitedtotoexposure
limited exposuretotoharmful
harmfulsubstances
substances included
included in in
thethe recycling
recycling process
process as compared
as compared to
to incineration and chemical recycling. To reuse the recycled
incineration and chemical recycling. To reuse the recycled materials, 3D printing materials, 3D printing
can can
be
be used
used [14].[14].
CommercialPLA
Commercial PLAdegrades
degrades slowly
slowly under
under natural
natural settings
settings because
because itsits continued
continued ex-ex-
istence may
istence may harmharm the the ecosystem.
ecosystem.Moreover,
Moreover, discarding
discarding thethe
PLA duedue
PLA to slow natural
to slow deg-
natural
radation is not
degradation a wise
is not choice
a wise choiceduedue
to the lossloss
to the of many
of many useful compounds
useful compounds such as the
such hy-
as the
droxyl group [15]. Therefore, customized settings of the important
hydroxyl group [15]. Therefore, customized settings of the important parameters in this parameters in this re-
gard are necessary for the degradation of PLA [16]. Furthermore,
regard are necessary for the degradation of PLA [16]. Furthermore, throwing out PLA can throwing out PLA can
resultin
result inthe
theloss
lossofofessential
essentialcomponents
componentssuch suchasashydroxyl
hydroxylgroups.
groups.As Asaaresult,
result,recycling
recycling
PLAisiscrucial
PLA crucialto tolimiting
limitingthetheuse
useofofrenewable
renewableresources
resourcesfor forsuch
suchmonomers
monomers[17]. [17].
PLArecycling
PLA recyclingisisgreatly
greatlydesired
desiredbecause
becauseititmaymaybe beused
usedtotogenerate
generateenvironmental
environmental
compatibilizersthat
compatibilizers thatcan
canbebeutilized
utilizedtotoimprove
improve composite
composite products
products made
made from
from PLA,
PLA, pre-
pre-
serving the
serving the material’s eco-friendliness.
eco-friendliness.PLA-based
PLA-basedcomposites
composites with
withnatural
naturalfiber have
fiber nu-
have
merous applications due to their easy processing,
numerous applications due to their easy processing, low toxicity, low toxicity, high mechanical strength,
strength,
etc.,making
etc., makingthe theneed
needforforsustainable
sustainablerecycling
recycling of ofthese
thesematerials
materials anan effective
effective need
need ofofaa
sustainable environment
sustainable environment [17]. [17]. Furthermore,
Furthermore, because
because PLA PLA isis substantially
substantially heavier
heavier than
than
other
other commodity
commodity polymerspolymers (e.g.,
(e.g.,high-density
high-density polyethylene
polyethylene (HDPE)),
(HDPE)), andandlow-density
low-density
polyethylene
polyethylene(LDPE),(LDPE),it itcan
canbebe
easily separated
easily separated based
basedonondensity, making
density, makingpolymer
polymerretention
reten-
very
tion useful [18]. [18].
very useful
1.2.
1.2.Carbon
CarbonFiber
FiberReinforced
ReinforcedPolymers
Polymers(CFRP)
(CFRP)
Carbon
Carbon fiber reinforced polymersor
fiber reinforced polymers orplastics
plastics(CFRP)
(CFRP)arearegaining
gainingpopularity
popularityowing
owingtoto
their wide range of applications in industries such as aviation, military, vehicle
their wide range of applications in industries such as aviation, military, vehicle manufac- manufac-
turing,
turing,transportation,
transportation,architecture,
architecture,sports
sportsindustries,
industries,and
andmedicine
medicine[19,20].
[19,20].Carbon
Carbonfibers
fibers
were
were initially created in the 1960s, and by 2006, almost 27,000 tons of carbonfibers
initially created in the 1960s, and by 2006, almost 27,000 tons of carbon fiberswere
were
being
beingproduced
producedworldwide,
worldwide,with
withthat
thatfigure
figureexpected
expectedto torise
rise to
to 140,000
140,000 tons
tons by
by 2020
2020 [21].
[21].
Carbon
Carbon fiber demand has increased by 15% each year over the last few years, as shownin
fiber demand has increased by 15% each year over the last few years, as shown in
Figure 2. Therefore, the increasing demand for Carbon Fiber Reinforced Polymers (CERP)
Figure 2. Therefore, the increasing demand for Carbon Fiber Reinforced Polymers (CERP)
is also considered necessary due to the increasing consumption of plastic, which leads
is also considered necessary due to the increasing consumption of plastic, which leads to
to increased plastic waste, thereby resulting in the growing demand for better and more
increased plastic waste, thereby resulting in the growing demand for better and more ef-
efficient recycling [22–26].
ficient recycling [22–26].
Figure2.2.Increasing
Figure IncreasingCarbon
CarbonFiber
Fiberdemand
demandover
overthe
theYears
Years[11].
[11].
Furthermore,
Furthermore,no noexpensive
expensiveequipment
equipmentor orconsumables
consumablesare
areneeded,
needed,andandlow-skilled
low-skilled
labor is sufficient to manufacture the parts, further reducing costs [27,28]. As a result,
labor is sufficient to manufacture the parts, further reducing costs [27,28]. As a result, due
due to high material and manufacturing costs, upcycling waste core material has the
to high material and manufacturing costs, upcycling waste core material has the potential
potential to expose new products, processes, and markets for composites that were formerly
to expose new products, processes, and markets for composites that were formerly unat-
unattainable to virgin composites. To counter this, the extrusion process is presented
tainable to virgin composites. To counter this, the extrusion process is presented as a via-
as a viable solution that assists in the degradation of polythene, making its recycling
ble solution that assists in the degradation of polythene, making its recycling more feasible
more feasible [28]. The suggested techniques may easily generate a range of flat and
[28]. The suggested techniques may easily generate a range of flat and curved product
curved product shapes from scrap prepreg, and demonstrator components back up this
shapes from scrap prepreg, and demonstrator components back up this assertion [29].
assertion [29].
The parts include a curved section, a prototype RSRF prosthetic ankle/foot, and a typ-
ical hat stiffening panel [30]. Additional demonstration parts, including tubes, flat panels,
Polymers 2022, 14, 2194 4 of 19
and sandwich panels, have been created in the lab of United Arab Emirates University
under the Department of Chemical and Petroleum Engineering [31,32].
Scrap prepreg can be used to make structural design parts that can be used to construct
larger structures. Thin and thick panels, cylinders, sandwich structures with honeycomb
or foam cores, hat stiffeners, and even scrap prepreg with a variety of types of fiber and
resins, such as glass, carbon, and Kevlar fibers with diverse composites, have all been
combined in the same part [33]. The components based on CF/epoxy have maximum
expected application in the construction, both indoor and outdoor furnishing, and building
structures due to their durability against humidity and the least vulnerability to insect
invasion [34]. The CF/epoxy’s components are durable in the presence of humidity, and it
is a great material for interior and external furnishings, as well as a basic building element
because it has a low insect invasion. Container ships, which are currently composed of
denser materials such as aluminum, worn steel, and wood, could benefit from the usage of
prepreg trash [35].
Green environmental legislation and worldwide regulations have compelled researchers
to investigate several strategies for recycling CFRP trash. However, this is difficult because
the heat-stable matrices of CFRP do not melt with heating. The techniques other than
heating are considered less viable due to their complex procedures. Thermo-mechanical
recycling, therefore, is investigated by many researchers all around the globe as the opti-
mum method in such a scenario [36]. Thermoset polymers are employed as matrices in
structural CFRPs, accounting for about 80% of polymer composites. Mechanical strength,
durability, chemical, and thermal resistance, and dimensional stability are all advantages
of this material. However, because processed thermoset polymers are crosslinked, re-
covering the fibers is challenging as they cannot be easily heated, shaped, processed, or
re-crosslinked following treatment [37]. Recycling CFRP trash reduces greenhouse-gas
emissions associated with CFRP waste while also providing an inexpensive option to make
high-value carbon fibers. By 2030, 6000–8000 business-related aircraft will have reached
the end of their useful lives. As a result, there is an urgent need to create effective and
sustainable waste management and recycling techniques for CFRPs [38].
1.2.1. Recycling Techniques

CFRP trash is disposed of and burned at landfills. Different techniques such as
incineration, laser-based burning, etc., are employed by different public and private sectors
according to the quantity of disposal, resources available, and the applications desired [39].
Several nations have adopted landfill taxes in an attempt to reduce trash disposal, as well
as material recycling, such as CFRP waste. CFRP waste recycling entails not only recycling
carbon fiber but also using recovered carbon fibers (rCFs) in the manufacturing of new
material. Therefore, the quality alongside the quantity of the recovered or recycled carbon
fiber is required as an important parameter not only for the process of recycling but also for
the further application of the recycled product [40].
According to an article published in 2005 by Keiji Ogi, “As far as the authors know,
products employing recycled CFRP have not been disclosed although some research may
be undertaken in laboratories. As a result, no recycling system for CFRP wastes has been
built around the globe thus far.” However, several uses have been developed since that
time to properly utilize CFRP waste. Generally, recycling CFRP is divided into two stages:
first, reclamation of carbon fibers from CFRP waste, then production of rCF reinforced
polymer (rCFRP) as demonstrated in Figure 3 [41,42].
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Figure 3. Recycling Process from Virgin Carbon Fiber to CFRP.

Figure 3. Recycling Process from Virgin Carbon Fiber to CFRP.
1.2.2.Mechanical
1.2.2. MechanicalMethod
Method
Mechanicalrecycling
Mechanical recyclingisisthe
themost
mostcommon
commonmethodmethodof ofrecycling
recyclingCFRP
CFRP[43].
[43].This
Thisap-
ap-
proachconsists
proach consistsofofmultiple
multipleprocedures
proceduresfor forreducing
reducingwaste
wastequantity.
quantity.Initially,
Initially,the
theCFRP
CFRPisis
choppedtotoaasize
chopped sizeofof50–100
50–100mm, mm,andandthen
thenadditional
additionalgrinding
grindingisisemployed
employedtotoprovide
provideaa
range
rangeofofproperties
propertiesranging
rangingfrom
fromash
ashtotofibrous
fibrous[44,45].
[44,45].Damage
Damagetotoprocessing
processingequipment
equipment
caused
causedby byCFRP
CFRPrecycling
recyclingprocedures
proceduresraises
raisesrecycling
recyclingoperating
operatingcosts,
costs,reducing
reducingthe theeco-
eco-
nomic
nomicmargin
marginofofrecycling
recyclingproducts.
products.The Themechanical
mechanicalprocedure
procedureisisrisk-free
risk-freeandandmaymaybe be
finished
finishedatatroom
roomtemperature.
temperature. This method
This method cancan
hold debris
hold up to
debris up50tomm
50 mmand and
attainattain
50–65%50–
of65%
theoftensile strength
the tensile of fresh
strength carbon
of fresh fibers.fibers.
carbon The most serious
The most risk for
serious riskthis
formethod is theis
this method
dust generated by the recycling mechanism [46–57].
the dust generated by the recycling mechanism [46–57].
Fused
FusedFilament
FilamentFabrication
Fabrication (FFF) is considered
(FFF) is consideredoneone
of the latest
of the and and
latest mostmost
effective Ad-
effective
ditive Manufacturing
Additive Manufacturing techniques withwith
techniques highhighexpectations of sustainable
expectations manufacturing,
of sustainable manufacturing, but
the
butmechanical properties
the mechanical of polymers
properties manufactured
of polymers usingusing
manufactured this method are considerably
this method are consider-
lower than those
ably lower thanmanufactured by the traditional
those manufactured methods.methods.
by the traditional Therefore,Therefore,
mechanical methods
mechanical
ofmethods
recycling can be used for such processes [58].
of recycling can be used for such processes [58].
1.2.3. Pyrolysis
1.2.3. Pyrolysis
Pyrolysis is the thermal breakdown of polymers in the absence of oxygen in the atmo-
Pyrolysis is the thermal breakdown of polymers in the absence of oxygen in the at-
sphere (300 ◦ C to 800 ◦ C), allowing the fibers to rebound with a high modulus. A greater
mosphere (300 °C to 800◦ °C), allowing the fibers to rebound with a high modulus. A
temperature (around 1000 C) can be employed, but this would result in mechanical prop-
greater temperature (around 1000 °C) can be employed, but this would result in mechan-
erty degradation. Carbon fibers derived from pyrolysis retained 90 percent of their original
ical property degradation. Carbon fibers derived from pyrolysis retained 90 percent of
mechanical strength, according to studies. Pyrolysis is also used for the investigation of
their original mechanical strength, according to studies. Pyrolysis is also used for the in-
the types of binding materials used in the polymeric materials available in modern paints
vestigation of the types of binding materials used in the polymeric materials available in
as implemented in the research of multi-analytical analysis of the “Orange Car Crash”
modern paints as implemented in the research of multi-analytical analysis of the “Orange
study [59]. Furthermore, the polymeric framework has the potential to be utilized as oil
Car Crash” study [59]. Furthermore, the polymeric framework has the potential to be uti-
droplets of liquid hydrocarbons. The pyrolysis method is recognized as a long-term CFRP
lized as oil
recycling droplets
process of liquid hydrocarbons. The pyrolysis method is recognized as a long-
[60].
term CFRP recycling process [60].
1.2.4. Chemical Method
1.2.4. Chemical Method
Several solvents are used in the chemical process to break down polymer resin and
Several
separate it from solvents
carbonare usedChemical
fibers. in the chemical
recyclingprocess to break
can recover down polymer
high-quality resin
carbon-6 and
fibers
separate it from carbon fibers. Chemical recycling can recover high-quality
with a tensile strength of 98.9%. According to the latest stats, recycling CFRP with the carbon-6 fibers
with a tensile
chemical techniquestrength
consumesof 98.9%. According
38.4 MJ/kg to the which
of energy, latest is
stats, recycling
nearly CFRP
equivalent to with
10–30% the
ofchemical
the totaltechnique consumes
energy required to 38.4 MJ/kg of energy,
manufacture which
new fibers. is nearly[61–65]
Although equivalent
the to 10–30%
chemical
of the total
approach energy required
is feasible, to manufacture
the treatment temperature, new fibers. Although
solvents, [61–65]
and equipment thenegative
have chemical
approach is feasible,
environmental the treatment temperature, solvents, and equipment have negative
consequences.
environmental
The objective consequences.
of this investigation is to handle two different wastes, PLA and different
carbonThefiberobjective of this
leftovers, investigation
domestically is to handle
to produce two different
and characterize wastes, PLA
composite and differ-
material as an
attempt to find
ent carbon fibera leftovers,
solution todomestically
the increasing industrial
to produce andwastes. Different
characterize experimental
composite materialtestsas
an attempt to find a solution to the increasing industrial wastes. Different experimental
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tests
testshave
havebeen
beencarried
carriedout outto
tostudy
studythetheimpact
impactof ofusing
usingcarbon
carbonwaste
wasteas asreinforcement
reinforcementto to
have
the PLAbeen
on carried
the out to study
properties of the the impactcomposites.
processed of using carbon waste as reinforcement to the
the PLA on the properties of the processed composites.
PLA on the properties of the processed composites.
2.2.Materials and Methods
2. Materials
Materials andand Methods
Methods
Assorted
Assorted leftover PLA from 3D printing was collected from the prototyping labs of
Assorted leftover PLA
leftover PLA from
from 3D3D printing
printing was
was collected
collected from
from thethe prototyping
prototyping labs labs of
of
the
the university, sorted
university,sorted based
sortedbased on color,
basedononcolor,
color, and
and then
then shredded.
shredded. Two kinds of materials have
the university, and then shredded. TwoTwo kindskinds of materials
of materials have havebeen
been
been used: CF-Prepreg sheets (CFRP) and
andcarbon fiber
fibersheets (CF), asasshown in Figure 4.4.
used:used: CF-Prepreg
CF-Prepreg sheetssheets
(CFRP)(CFRP)
and carbon carbon
fiber sheets sheets
(CF), as(CF),
shown shown
in Figurein4.Figure
Scissors
Scissors
Scissors were
were used
used to cut both
to materials materials
cut both materials into small pieces as shown in Figure 5.5.InInthe
were used to cut both into smallinto small
pieces pieces as
as shown shown 5.
in Figure inInFigure
the shredding the
shredding
shredding process,
process, a astrong
strong DIY
DIY shredding
shredding with
with stainless
stainless steel
steelblades
blades as
as illustrated
illustrated in
in Fig-
Fig-
process, a strong DIY shredding with stainless steel blades as illustrated in Figure 6 was
ure
ure 66was
was utilized to tobreak down
downthe residual waste material into little bits that
thatmay be
utilized to utilized
break down break
the residual the residual
waste materialwaste
intomaterial
little bitsinto
thatlittle
may bitsbe used may
to be
shred
used
used to shred hard plastics and prepreg carbon fiber waste, whereas twin extruder (Figure
hard to shred and
plastics hardprepreg
plasticscarbon
and prepreg carbonwhereas
fiber waste, fiber waste,
twinwhereas
extrudertwin extruder
(Figure 7) is (Figure
used to
7)7)isisused
used to process
processthe
tomaterial thematerial
material[65–68].
[65–68].
process the [65–68].
Figure
Figure4.4.
Figure 4.The
Theoriginal
The originalshape
original shapeofof
shape ofthe
thesamples
the samples(a)
samples (a)CFRP,
(a) CFRP,(b)
CFRP, (b)CF.
(b) CF.
CF.
Figure
Figure5. Samples after the cutting (a) CFRP, (b)
(b)CF.
Figure 5.
5. Samples
Samples after
after the
the cutting
cutting (a)
(a) CFRP,
CFRP, (b) CF.
CF.
The shredded material was subsequently broken down into smaller bits with a heavy-
duty mixer designed for hardwoods, as the shredded material did not include shredder
residue [65]. Since the plastic waste came from lab sources, the initial stage of the shredding
process was carefully performed to break down the residual waste material. The process of
shredding is important and equally critical so that the Crystal-kinetic properties are linked
with the process [69]. Therefore, this process is carried out with utmost care and control.
The color of the original samples is purplish black. A schematic diagram of the formation
process of the waste PLA/CF composite is shown in the figure below.
Polymers 2022, 14, 2194 7 of 19
Figure 5. Samples after the cutting (a) CFRP, (b) CF.
Figure 6. High speed grinder.

Figure 6. High speed grinder.
Samplesof
Figure7.7.Samples
Figure of(a)
(a)CFRP,
CFRP, (b)
(b) PLA,
PLA, (c)
(c) CF,
CF, (d)
(d) twin-screw
twin-screw extruder.
extruder.
Different
The percentages
shredded of both
material was materials (CF and
subsequently CFRP)
broken mixed
down with
into PLA polymer
smaller were
bits with a
melt-blended into a composite material in a twin-screw extruder (MiniLab Rheomex CTW5,
heavy-duty mixer designed for hardwoods, as the shredded material did not include
HAAKE, Karlsruhe, Germany). The melt blending technique used a closed-loop cycle
shredder residue [65]. Since the plastic waste came from lab sources, the initial stage of
with a rotating speed of 140 rpm and a temperature of 190 ◦ C for 5 min. The blended
the shredding process was carefully performed to break down the residual waste material.
material was extruded via a valve at the extruder’s outlet to collect the composite material
The process of shredding is important and equally critical so that the Crystal-kinetic prop-
for the compression molding stage after the closed-loop cycle. Figure 8 shows the material
erties are linked with the process [69]. Therefore, this process is carried out with utmost
preparation and extrusion process.
care and control. The color of the original samples is purplish black. A schematic diagram
The extruded sample was cut into small pieces and thermally compressed under
of the formation process of the waste PLA/CF composite is shown in the figure below.
5000 psi and at the same extrusion temperature and time using a Carver’s press (CarverTM
Different percentages of both materials (CF and CFRP) mixed with PLA polymer
Lab Presses, 1569 Morris Street, PO Box 298 Wabash, IN 46992-0298 USA). This procedure
were melt-blended into a composite material in a twin-screw extruder (MiniLab Rheomex
was followed for each polymer’s extruded samples with the required filling ratio. The pro-
CTW5, HAAKE, Karlsruhe, Germany). The melt blending technique used a closed-loop
cedure was followed for the extruded samples so that the dimensional coherency would be
cycle withfor
achieved a rotating speed of
the composite 140 rpm
samples and by
made a temperature of 190process,
the compression °C for 5which
min. The
willblended
produce
material was extruded via a valve at the extruder’s outlet to collect the composite
thin sheets that will be examined to investigate the mechanical and thermal properties to material
for the compression
explore the potentialmolding
for usingstage afterwaste
different the closed-loop cycle.
carbon fibers Figure 8 the
to enhance shows the material
properties of the
preparation and extrusion process.
heavy-duty mixer designed for hardwoods, as the shredded material did not include
shredder residue [65]. Since the plastic waste came from lab sources, the initial stage of
the shredding process was carefully performed to break down the residual waste material.
The process of shredding is important and equally critical so that the Crystal-kinetic prop-
Polymers 2022, 14, 2194
erties are linked with the process [69]. Therefore, this process is carried out with utmost
8 of 19
care and control. The color of the original samples is purplish black. A schematic diagram
of the formation process of the waste PLA/CF composite is shown in the figure below.
Different percentages of both materials (CF and CFRP) mixed with PLA polymer
recycled PLA. This analysis
were melt-blended was helpful
into a composite for the
material in determination of a proper
a twin-screw extruder understanding
(MiniLab Rheomex
of material performance under mechanical and thermal characterization [70]. The samples
CTW5, HAAKE, Karlsruhe, Germany). The melt blending technique used a closed-loop
obtained as a result of this technique were thin sheets of composite material that were
cycle with a rotating speed of 140 rpm and a temperature of 190 °C for 5 min. The blended
examined for mechanical and thermal properties. Many researchers have evaluated the
material was extruded via a valve at the extruder’s outlet to collect the composite material
effectiveness of the recycling process experimentally to demonstrate the potential of using
for the compression molding stage after the closed-loop cycle. Figure 8 shows the material
fiber waste as a reinforcement to enhance recycled plastics [71–81].
preparation and extrusion
Figure 8. formation of PLA/CFprocess.
composite.
The extruded sample was cut into small pieces and thermally compressed under 5000
psi and at the same extrusion temperature and time using a Carver’s press (CarverTM Lab
Presses, 1569 Morris Street, PO Box 298 Wabash, IN 46992-0298 USA). This procedure was
followed for each polymer’s extruded samples with the required filling ratio. The proce-
dure was followed for the extruded samples so that the dimensional Tensile Test coherency would be
Hot Press to
achieved
Carbon Fiberfor theCFcomposite
Shredding samples
Mixing PLAmade
with by the compression
prodcude a process,
samples by which will
Mechanical andproduce
wate (CF) process CF shreds punch and die ThermalTesting
thin sheets that will be examined to investigatesheet the mechanical and thermal properties to
cutting device
explore the potential for using different waste carbon fibers to enhance the properties of
the recycled PLA. This analysis was helpful for the determination of a proper understand-
ing of material performance under mechanical and thermal characterization [70]. The
samples obtained as a result of this technique were thin sheets of composite material that
were examined for mechanical and thermal properties. Many researchers have evaluated
the effectiveness of the recycling process experimentally to demonstrate the potential of
Figure 8. Formation of PLA/CF composite.
using fiber waste as a reinforcement to enhance recycled plastics [71–81].
Furthermore,several
Furthermore, severalproblems
problemsoccurredoccurredduring
duringthe theexperiments.
experiments.The Thefirst
firstobstacle
obstacle
was with the high-speed grinder used to turn the samples
was with the high-speed grinder used to turn the samples into powder. The high-speed into powder. The high-speed
grinderoperation
grinder operationduration
duration is is
oneone minute,
minute, while
while thethe remainder
remainder of the
of the cooling
cooling down down timetime
is
is five
five minutes,
minutes, resulting
resulting in ain a lengthy
lengthy wait.wait. However,
However, to save
to save time, time,
twotwo high-speed
high-speed grind-
grinders
ers were
were utilized utilized
at theatsame
the same
time,time,
one for oneeach
for specimen.
each specimen. The other
The other difficulty
difficulty was with
was with the
themelt
Hot Hot extrusion
melt extrusion
(HME) (HME)
process process
because because five distinct
five distinct samples samples were produced
were produced separatelysep-
inarately in a sequential
a sequential processprocess whichlead
which could couldtolead to a possible
a possible discrepancy
discrepancy in theinproperties
the properties of
of the tested samples. The cleaning time was around 30 min,
the tested samples. The cleaning time was around 30 min, while the operation time was while the operation time was
approximately1010min.
approximately min.
ToToinvestigate
investigatethe theinfluence
influenceofofCFRP CFRP andand CFCF reinforcement
reinforcement onon polymer/composite
polymer/composite
samples,researchers
samples, researchersuseduseda auniversal
universaltesting
testingmachine
machine(UTM, (UTM,Shimadzu,
Shimadzu,Kyoto, Kyoto,Japan).
Japan).
The
Thetensile
tensiletesttestsamples
sampleswere wereprepared
preparedusing usingthethethin
thincomposite
compositesheets sheetsresulting
resultingfrom fromthethe
compression
compressionmolding moldingstage,
stage,asasshown
shownininFigure
Figure9,9,according
accordingtotothe theAmerican
AmericanSociety
Societyfor for
Testing and Materials (ASTM)-D 638 [82] guidelines. This was
Testing and Materials (ASTM)-D 638 [82] guidelines. This was to determine the mechani- to determine the mechanical
modulus
cal modulus of elasticity, yieldyield
of elasticity, strength, ultimate
strength, strength,
ultimate and strain
strength, at theatfailure
and strain point.point.
the failure
Figure9.9.Dimensions
Figure Dimensionsofofthe
theSpecimen.
Specimen.
AAunique
uniquemanual
manual blanking machine machinewas wasused
usedtotoacquire thethe
acquire specific dimensions
specific dimensions(Ex-
(Exacta Model-JFP, Bengaluru, India). The
acta Model-JFP, Bengaluru, India). The blanking machineblanking machine was used to make dumbbell-
to make dumbbell-
shaped
shapedtensile
tensiletest
testspecimens
specimensasasshown shownininFigure
Figure10a.
10a.Each
Eachpair
pairofofcomposite
compositesamples’
samples’
dimensions
dimensions(thickness
(thickness(t))(t))are
arelisted
listedininTable
Table1.1.The
Theaccompanying
accompanyingmechanical
mechanicalproperties
properties
were
wereinvestigated
investigatedusing usinga a1010kN kNload
load cell with
cell a 5-mm/min
with a 5-mm/mincrosshead
crossheadmovement.
movement.TheThe
blanking
blankingtechnique
techniqueisisdepicted
depictedininFigure
Figure10b.
10b.Each
Eachsample
samplehadhadthree
threeweights,
weights,each
eachwith
with
three
threetrails,
trails,for
fora atotal
totalofof1515tests
teststotoachieve
achievehigher
higheraccuracy,
accuracy,which
whichareareshown
shownasasstandard
standard
deviations (SDs) in the results plots. The average gauge length and width of the samples
are 17.02 mm and 2.69 mm, respectively. The result of the tensile test was obtained. The
tensile testing machine is shown in Figure 11.
Polymers 2022, 14, 2194 9 of 19
deviations (SDs) in the results plots. The average gauge length and width of the samples
are 17.02 mm and 2.69 mm, respectively. The result of the tensile test was obtained. The
tensile testing machine is shown in Figure 11.
Figure10.
Figure (a)Blanking
10.(a) Blankingmachine,
machine,(b)
(b)Dumbbell
Dumbbellshape
shapesamples
samplesafter
afterblanking.
blanking.
Table 1. Dimensions of the prepared tensile test specimens.
Samples Length mm Width mm Thickness mm

CF-Prepreg 10% + PLA 0.28
CF 10% + PLA 0.20
CF-Prepreg 20% + PLA 17.02 2.69 0.24
CF 20% + PLA 0.26
Figure 10. (a) Blanking
Pure-PLAmachine, (b) Dumbbell shape samples after blanking. 0.27
Figure 11. Tensile testing machine with a sample.
Table 1. Dimensions of the prepared tensile test specimens.
Samples Length mm Width mm Thickness mm

CF-Prepreg 10% + PLA 0.28
CF 10% + PLA 0.20
CF-Prepreg 20% + PLA 17.02 2.69 0.24
Figure
Figure CFtesting
11. Tensile
11. Tensile 20% + machine
PLA
testing machine
withwith a sample.
a sample. 0.26
Pure-PLA 0.27
An XRD test
Table 1. Dimensions of was conducted
the prepared on test
tensile untreated, NaOH treated, and silane-acetone treated
specimens.
fillers
AntoXRD
examine the conducted
test was impact of theon treatment
untreated,on NaOHthe crystalline
treated, andstructure. The equipment
silane-acetone treated
used was a Samples
Malvern Panalytical X-ray Length mm
diffractometer. Width
The mm
clearance Thickness
between
fillers to examine the impact of the treatment on the crystalline structure. The equipment the mm
punch and
the CF-Prepreg
die is a typical10% + PLA
problem in cutting the samples that is supposed
used was a Malvern Panalytical X-ray diffractometer. The clearance between the punch to be 0.28
adjusted based on
the CF
sample 10% + PLA
thickness. Instead of using a standard cutting device, the
and the die is a typical problem in cutting the samples that is supposed to be adjusted 0.20
clearance is constant
andCF-Prepreg
based cannot
on the be changed.
sample + PLAThis would
20%thickness. Insteadaffect the asample
of 17.02
using standardedge quality,
2.69
cutting which
device, would
0.24
the impact
clearance is
the failure
constant CFof
and 20% the+samples
cannot PLA duringThis
be changed. the tensile
wouldtest [83,84].
affect As a result,
the sample the sheared
edge quality, 0.26
whichedges may
would
impact the Pure-PLA
failure of the samples during the tensile test [83,84]. As a result,0.27
the sheared
edges may be altered. Accordingly, hard surfaces emerge, altering the sample’s mechani-
calAn XRD testand
properties wasperhaps
conducted on untreated,
leading NaOH treated,
to unpredictable collapse.and silane-acetone
Stress treated
concentrations at the
fillers to examine
sample’s the impact
end frequently of thethe
impact treatment on the
mechanical crystalline
behavior structure.
of the sheets. The equipment
Polymers 2022, 14, 2194 10 of 19
be altered. Accordingly, hard surfaces emerge, altering the sample’s mechanical properties
and perhaps leading to unpredictable collapse. Stress concentrations at the sample’s end
frequently impact the mechanical behavior of the sheets.
During the blanking process, the pressure applied to the punch and die may generate
stress distributions, which can affect the geometry difference between a specific burr size
and the intersecting surface [85]. The extruded composites were cut into little bits due to
the limitations of the extruder, which creates restricted quantities of the combinations. As a
result, the sheared edges may be altered, resulting in the formation of rough surfaces that
change the mechanical characteristics of the sample and may lead to inconsistent failure.
2.1. Fourier Transform (FTIR)

The infrared test is used to evaluate the presence of the functional groups, CF and
CFRP. The chemical reaction occurred as a result of the inclusion of the filler. The Fourier
Transform Infrared Spectroscopy (FTIR) is used to confine the successful coupling between
the polypropylene matrix and the filler [82]. The FT/IR-4700 from JASCO was used for
the test.
2.2. XRD
To investigate the effect of pretreatment on the crystalline structure, XRD tests were
performed on an untreated filler, NaOH treated filler, and silane-acetone treatment bonding
agent. The Malvern Analytical X-ray diffract meter was utilized.
2.3. TGA
TGA testing is used to determine thermal deterioration and thermal stability. TGA
Q500 from TA Instruments was used for the test. The apparatus was loaded with samples
weighing 5 to 10 mg, and the temperature was increased from 40 to 800 ◦ C. TGA data may
be shown using two graphs: weight % versus temperature and derivative weight versus
temperature.
3. Results and Discussion

Two kinds of composite materials—CF/PLA and CFRP/PLA—have been produced to
investigate different properties, such as thermogravimetric analysis (TGA), X-ray diffraction
(XRD), and Fourier-transformed infrared spectroscopy (FTIR), as well as the tensile testing
machine. Basically, CFRP sheets and carbon fiber sheets (CF) were used to produce thin
layers of the composite blends mixed with PLA, and many tensile specimens were punched
from each sheet using a commercial dog-bone cutting machine. The Mitutoyo thickness
gauge (Model 547-526S) was used to determine the thickness of the thin film due to the
high resolution (0.001 mm) and accuracy (0.0002). In this study, the average readings along
the gage length of the sample were considered [86].
3.1. Mechanical Characterization

A sample of the stress–strain curves for the five composites investigated in this study
is depicted in Figure 12, where the detailed values are listed in Table 2. In general, it has
been observed that the tensile test experimentations revealed that carbon fiber enhanced
the mechanical properties of the recycled PLA. However, the CF composite at 20% demon-
strated significantly higher ultimate strength, with around 10% more than the CFRP for
the same reinforcement percentage. Still, for the 10%, the CFRP is 7% higher than the CF,
whereas the ductility for the CFRP composites possesses higher values due to the expired
impregnated epoxy in the prepreg leftover pieces [87–89]. A reduction of 18.4% in the
ultimate tensile strength of the recycled PLA concerning the commercial PLA 3D Printing
Ultimaker filament properties (UTS = 45.6 MPa) has been estimated [90].
Polymers 2022, 14, 2194 11 of 19
Figure12.
Figure 12.Stress-strain
Stress-straincurve
curvefor
forthe
therecycled
recycledPLA
PLAand
andfour
fourrecycled
recycledcomposites.
composites.
Table 2 illustrates the mechanical properties of the experimental work conducted in

Table 2. The mechanical properties of the recycled Carbon/PLA composites with standard devia-
this research associated with the standard deviations.
tion (SD).
Table 2. The mechanical properties of the recycled Carbon/PLA composites with standard deviation
Elastic Modulus Yield Strength Ultimate Strength Ductility
(SD).
Material ID GPa MPa MPa %
Value ElasticSD
Modulus Value
Yield Strength
SD Ultimate Strength
Value SD Value Ductility
SD
Material ID GPa MPa MPa %
Pure PLA 5.02 ±0.53 35.83 ±0.60 37.20 ±0.40 6.01 ±0.44
CF 10%/PLA 6.26 Value±0.36 SD 39.07 Value ±1.97 SD Value
39.90 SD
±1.60 Value
3.40 ±0.82SD
Pure PLA
CF 20%/PLA 5.91 5.02 ±0.12±0.53 45.6835.83 ±6.00 ±0.60 37.20
47.81 ±0.40
±3.90 6.01
4.16 ±±0.44
0.55
CFRP CF
10%/PLA
10%/PLA 4.19 6.26 ±0.23±0.36 39.7739.07 ±5.70 ±1.97 43.07
39.90 ±4.70
±1.60 8.80
3.40 ±±0.82
0.50
CFRP 20%/PLA
CF 20%/PLA 3.78
5.91 ±0.13±0.12 38.7345.68 ±1.21 ±6.00 43.58
47.81 ±0.70
±3.90 9.20
4.16 ±0.31
±0.55
CFRP 10%/PLA 4.19 ±0.23 39.77 ±5.70 43.07 ±4.70 8.80 ±0.50
CFRP 20%/PLA 3.78Table 2±0.13
illustrates38.73the mechanical ±1.21 properties43.58of the experimental
±0.70 9.20 conducted
work ±0.31 in
this research associated with the standard deviations.
Figure
Figure12 12shows
showsthat thatthe
thestress–strain
stress–strainproperties
propertiesofofthe therecycled
recycledPLA PLAproperties
propertiesare are
lower
lowerthan
thanthe thereinforced
reinforcedCarbonCarbonfiber/PLA
fiber/PLAcomposite
compositedue dueto tothe
thefact
factthe
thereinforcements
reinforcements
enhance
enhancethe theproperties
propertiesofofthe thepure
purerecycled
recycledPLA PLA[91,92].
[91,92].
The
Theparameter
parameterthat thatcharacterizes
characterizes materials’
materials’ resistance
resistanceto to
deformations
deformations is the modulus
is the modu-
oflus
the elasticity, i.e., stiffness, which is the extent to which an object resists
of the elasticity, i.e., stiffness, which is the extent to which an object resists deformation deformation
ininresponse
responseto to an
an applied force [93]. [93]. There
Thereare areseveral
severalwayswaystoto estimate
estimate stiffness
stiffness from
from ex-
experimental data. It can be either the slope of the stress–strain curve
perimental data. It can be either the slope of the stress–strain curve at any specified stress at any specified
stress or strain
or strain (tangent (tangent
stiffness stiffness
or tangent or tangent
modulus), modulus), or the
or the slope slope
of the of theline
straight straight line
connecting
connecting
the origin of thethe
origin of the stress–strain
stress–strain curve withcurve another with another
point on thepoint
curveon (secant
the curve (secant
stiffness or
stiffness or secant modulus). Among all the tangent moduli, moreover,
secant modulus). Among all the tangent moduli, moreover, the tangent modulus at the the tangent modulus
atorigin
the origin (initial
(initial stiffness)
stiffness) is of isparticular
of particular significance.
significance. ThisThis
value value is associated
is associated withwiththethe
be-
behavior
havior of the material for low load values, a behavior that is linear elastic for mostbrittle
of the material for low load values, a behavior that is linear elastic for most brittle
materials.
materials.Therefore,
Therefore,the thetangent
tangentmodulus
modulusatatthe theorigin
originisisequivalent
equivalentto toYoung’s
Young’smodulus
modulus
ininthe
the elastic (reversible) deformation regime. Usually, the secant modulusis,
elastic (reversible) deformation regime. Usually, the secant modulus is,instead,
instead,aa
percentage
percentageofofYoung’s
Young’smodulusmodulusand anddescribes
describesthe thestiffness
stiffnessofofaamaterial
materialininthe theinelastic
inelastic
region of the stress–strain diagram. To evaluate the tangent
region of the stress–strain diagram. To evaluate the tangent modulus at the originmodulus at the origin correctly,
cor-
itrectly,
is of fundamental importance
it is of fundamental to have reliable
importance to haveexperimental data for low
reliable experimental load
data forvalues.
low load
Figure 13 demonstrates the elastic properties of the produced composites. It is ob-
values.
served that samples produced with 10% CF have the highest elastic modulus among the
Figure 13 demonstrates the elastic properties of the produced composites. It is ob-
blends due to the impact of the fiber reinforcement, which is 33% higher than the 10%
served that samples produced with 10% CF have the highest elastic modulus among the
Polymers 2022, 14, 2194 12 of 19
blends due
blends due to to the
the impact
impact of of the
the fiber
fiber reinforcement,
reinforcement, which
which is
is 33%
33% higher
higher than
than the
the 10%
10%
CFRP.Compared
CFRP. Comparedwith withthe therecycled
recycledPLA,PLA,thetheelastic
elasticmodulus
modulusincreased
increasedbyby18%
18%at at20%
20%CF, CF,
CFRP. Compared
whereas a reduction withof the
24% recycled
to 20% PLA,
in thethe elastic
CFRP modulus
samples was increased
observed.byA 18% at 20%
similar CF,
trend
whereas
whereas a areduction
reduction ofof24%
24% toto20%
20% ininthe
theCFRP
CFRP samples
sampleswas
was observed.
observed.AAsimilar
similar trend
trend
couldalso
could alsobebe observed[94] [94]that
thatincreased
increased theYoung’s
Young’s Modulusvaluevalue upto
to a certainlevel
level
ofcould alsoofbeobserved
content observed
fibers in the [94] that increasedthe
matrix. the Young’sModulus
Modulus valueup up toa acertain
certain level
ofofcontent
contentofoffibers
fibersininthe
thematrix.
matrix.
Figure 13.
Figure13. Elastic Modulus
ElasticModulus
13.Elastic ofofthe
Modulusof blends.
theblends.
blends.
Figure the
Figure
Figure14
Figure 14 shows
14shows
showsthe the yield
theyield strengths
yieldstrengths
strengthsforfor the
forthe various
thevarious samples
varioussamples
samplesand and indicates
andindicates that
indicatesthat for
thatfor the
forthe
the
20%
20%20%CFCF with
CFwith PLA,
withPLA, the
PLA,the resulting
theresulting yield
resultingyield strength
yieldstrength is
strengthisisthe the highest,
thehighest, while
highest,while
while20%20% CFRP
20%CFRP +
CFRP+ +PLAPLA leads
PLAleadsleads
totothe
to the lowest
thelowest value
lowestvalue
valueofofofthe
the
the yield
yield
yield strength.
strength.
strength. The
The The overall
overall
overall trend
trend
trend for
forforthe
thethe(10%
(10%
(10% CFRP,
CFRP,
CFRP, 20%
20%20% CFRP,
CFRP,
CFRP,
10%
10% CF,
CF, and
and 20%
20% CF)
CF) samples
samples showed
showed aa rise
rise ininthethe yield
yield strength
strength
10% CF, and 20% CF) samples showed a rise in the yield strength due to the contribution due
due to
to the
thecontribution
contribution
ofofthe
of the carbon
thecarbon fibers
carbonfibers
fiberstototothe
the PLA
thePLA properties’
PLAproperties’ mixing.
properties’mixing. Moreover,
mixing.Moreover,
Moreover,the the yield
theyield strength
yieldstrength
strengthof ofofpure
pure
pure
recycled
recycled PLA
PLA shows
shows aa drop of 27%
27% with
with respect
respect toto the
the commercial
commercial
recycled PLA shows a drop of 27% with respect to the commercial PLA filament. In gen- PLA
PLA filament.
filament. In In gen-
general,
eral,
eral, the yield
the yield
the yield strength
strength is estimated
is estimated
strength is estimated at aa specific
at a specific
at specific strain
strain strain
rate rate
ofrate
0.2%, ofwhich
of 0.2%,is
0.2%, which
the most
which is the
is the most
standard
most
standard method,
method,method,
standard commonly commonly referred
referred referred
commonly to as proofto as
to as proof
proof stress.
stress. stress.
Figure 14.
Figure14. Yield strength
Yieldstrength
14.Yield for
strengthfor the
forthe samples.
thesamples.
samples.
Figure
Figure15
Figure 15presents
presentsthetheUltimate
UltimateStrength
Strengthofofthe theproduced
producedsamples.
samples. Ithas hasbeen
beenshown
shown
Figure 15 presents the Ultimate Strength of the produced samples. ItIt has been shown
that the
that the ultimate
the ultimate strength
ultimate strength
strength of of the
of the CF/PLA
the CF/PLA
CF/PLA bends bends increased
bends increased with
increased with
with the the increase
the increase
increase of of
of thethe
the CFCF con-
CF con-
con-
that
tents,with
tents, withananincrease
increasefrom
from7% 7%toto28%
28%forforthe
theCFRP
CFRPatat10%
10% and
and 20% 20% contents,
contents, respectively,
respectively,
tents, with an increase from 7% to 28% for the CFRP at 10% and 20% contents, respectively,
incomparison
in comparisonto tothe
therecycled
recycledPLA PLA[95].
[95].On
Onthetheother
otherhand,
hand,ititisisshown
shownthat thatthe
theCFRP/PLA
CFRP/PLA
in comparison to the recycled PLA [95]. On the other hand, it is shown that the CFRP/PLA
ultimatestrength
ultimate strengthincreased
increasedslightly
slightlyconcerning
concerningthe therecycled
recycledPLA,PLA,but butitithas
hasaalower
lowerlevel
level
ultimate strength increased slightly concerning the recycled PLA, but it has a lower level
than
than thethe CF/PLA
the CF/PLA
CF/PLA blends,blends, which
blends, which
which is is ascribed
is ascribed
ascribed to to the
to the presence
the presence
presence of of
of the the expired
the expired impregnated
expired impregnated
impregnated
than
epoxy,as
epoxy, asclarified
clarifiedbefore.
before.TheTheslight
slightincrease
increaseininthetheultimate
ultimatestrength
strengthisisestimated
estimatedtotobe be
epoxy,
from as clarified
15% to 17% before.
for the The and
10% slight
20%increase
CFRP in the ultimate
contents, strength is estimated to be
respectively.
from 15%
from 15% toto 17%
17% for
for the
the 10%
10% andand 20%
20% CFRP
CFRP contents,
contents, respectively.
respectively.
Polymers
Polymers2022,
2022,14,
14,x2194
FOR PEER REVIEW 13 13
ofof1919
Figure 15. Ultimate Tensile Strength.

Figure15.
Figure UltimateTensile
15.Ultimate TensileStrength.
Strength.
The
Thetrends
The trendsof
trends ofthe
of the ductility
the ductility
ductilityofof the
ofthe composite
thecomposite
composite blends,
blends,
blends, i.e.,
i.e., thethe
i.e., strains
strains
the recorded
recorded
strains recordedat theat the
atpoint
the
point
point of
offailure
of failure failure during
duringduring the
thetensile
the tensile testing
testing
tensile procedure,
procedure,
testing havehave
procedure, beenbeen
have graphically
graphically
been plotted
graphically plotted ininFig-
in Figure
plotted Fig- 16.
ureIt 16.
has It has
been been observed
observed that that
the the recycled
recycled PLA PLA ductility
ductility has has
a
ure 16. It has been observed that the recycled PLA ductility has a higher strain (6.01%) at a higher
higher strain
strain (6.01%)
(6.01%) at at
the
the
the failure
failure
failure point
point inin
point comparison
comparison
in comparisonwith with
withthethe commercial
commercialPLA
thecommercial PLAfilament
filament(5.2%),
filament (5.2%),with
(5.2%), withan
with anincrease
an increase
increase
of around
ofofaround
around15% 15% in ductility
15%ininductility due
ductilitydue to the
duetotothe degradation
thedegradation of
degradationofofthe the recycled
therecycled properties
recycledproperties during
propertiesduringduringthe the
the
recycling
recycling process
process [95].
[95].Moreover,
Moreover, clear
clear evidence
evidence illustrates
illustrates
recycling process [95]. Moreover, clear evidence illustrates that the CF/PLA composite that
that the
the CF/PLA
CF/PLA composite
composite
suffered
sufferedfrom
suffered fromaaaremarkable
from remarkabledrop
remarkable drop in
drop in ductility
in ranging
ductilityranging
rangingfrom from
from43% 43%
43%toto 30%
to30%
30% for
for the
the
for 10%
the 10%
10% andand
and the
the20%20% CF CF reinforcement,
reinforcement, respectively,
respectively, which
which is is attributed
attributed to
the 20% CF reinforcement, respectively, which is attributed to the impact of the carbon to
the the impact
impact of of
the the
carboncarbonfiber
fiber
fiber reinforcement.
reinforcement.
reinforcement. On the On the
the contrary,
Oncontrary, the
the CFRP/PLA
the CFRP/PLA
contrary, composites
composites
CFRP/PLA composites exhibited
exhibited aa significant
a significant
exhibited increase
significant
increase
increase in ductility from 46% to 53% for the 10% and the 20% CFRP reinforcement, re-
in in
ductility ductility
from 46% from
to 46%
53% to
for 53%
the 10%for the
and 10%
the 20%and CFRPthe 20% CFRP
reinforcement, reinforcement,
respectively. The
re-
spectively.
reason behind The reason behind
this observation this
is observation is the
the expired impregnated expired
spectively. The reason behind this observation is the expired impregnated epoxy of the impregnated
epoxy epoxy
of the leftover of the
prepreg
waste that caused
leftover degradation of the composite matrix [79].
leftoverprepreg
prepregwaste wastethat
thatcaused
causeddegradation
degradationof ofthe
thecomposite
compositematrix matrix[79].
[79].
Figure
Figure 16.16. Strain
Strain atat
thethe failure
failure point.
point.
Figure 16. Strain at the failure point.
The
The standarddeviation
standard deviation (Equation(1))
(1)) is estimated by calculating the arithmetic mean
of The
the standard
obtained deviation(Equation
values. (Equation (1))isisestimated
estimatedby bycalculating
calculatingthethearithmetic
arithmeticmean
mean
of
ofthe
theobtained
obtainedvalues.
values.
q
S = (∑ X 2 − nβ)/(n − 1) (1)
where S is the estimated standard 𝑆𝑆 deviation,𝑋

𝑋 𝑛𝛽 / 𝑛
𝑛𝛽is/the
X 1
𝑛 value
1 of a single reading, n is (1)
(1)
the
number of measurements, and β = is the set of observations’ arithmetic means.
where
where SS isis the
the estimated
estimated standard
standard deviation,
deviation, XX isis the
the value
value of
of aa single
single reading,
reading, nn isis the
the
number of
ofmeasurements,
3.2. XRD,
number FTIR, and TGA and
measurements, andββ==isisthe
Analysis theset
setof
ofobservations’
observations’arithmetic
arithmeticmeans.
means.
Figure 17 shows the XRD and FTIR results for both CFRP and CF. It is clear that the
scattering peak is at an angle of 2θ = 25.5 [96,97]. In the FTIR test, CFRP and CF exhibit
nearly identical peaks. There are several distinctive absorption peaks at about 717, 1238,
3.2. XRD, FTIR, and TGA Analysis
3.2. XRD, FTIR,
Figure and TGA
17 shows the Analysis
XRD and FTIR results for both CFRP and CF. It is clear that the
scattering
Figurepeak is at an
17 shows theangle
XRD of 2𝜃FTIR
and = 25.5results
[96,97].forInboth
the CFRP
FTIR test, CFRP
and CF. and
It is CFthat
clear exhibit
the
Polymers 2022, 14, 2194 14 of 19
nearly identical
scattering peak ispeaks.
at anThere
angle are several
of 2𝜃 = 25.5distinctive
[96,97]. Inabsorption
the FTIR test,peaks at about
CFRP and CF 717, 1238,
exhibit
1637, 3230,
nearly and 3432
identical peaks.cmThere
−1. Of these peaks, the peak at 717 cm−1 was qualified to the bending
are several distinctive absorption peaks at about 717, 1238,
vibrations
1637, 3230, of
and methylene
3432 cm (CH
−1.−Of −), and 1238 cm−1 is the peak from
2these peaks, the peak at 717 cm−1 was thequalified
C-F bands. Thebending
to the peak at
1637, 3230, and 3432 cm 1 . Of these peaks, the peak at 717 cm−1 was qualified to the
1637 cm was
vibrations −1 attributed(CH
of methylene to 2stretching
− ), and 1238 vibrations
cm of
−1 is the the
peak C =
from C groups.
the C-F The
bands. peak
− ), and 1238 cm−1 is the peak from the C-F bands.
The at 3230
peak at
bending
cm vibrations
−1 and−13432 of methylene (CH 2stretching
1637 cm was cm −1 was
attributed ascribed
to to
stretching the vibrations vibrations
of the C = of
C the OH
groups. groups.
The
−1 was attributed to stretching vibrations of the C = C groups. The peak peak at 3230
The peak at 1637 cm
cm−1 and 3432 cm−1 was ascribed to the stretching vibrations of the OH groups.
at 3230 cm and 3432 cm−1 was ascribed to the stretching vibrations of the OH groups.
− 1
Figure 17. (a) FITR spectra of CFRP and CF; (b) XRD spectra of CFRP and CF.
Figure17.
Figure (a)FITR
17.(a) FITRspectra
spectraof
ofCFRP
CFRPand
andCF;
CF;(b)
(b)XRD
XRDspectra
spectraof
ofCFRP
CFRPand
andCF.
CF.
Figure 18 shows two graphs: (a) is the TGA for CFRP, which indicates that they began
Figure 18 shows two graphs: (a) is the TGA for CFRP, which indicates that they began
to lose weight
Figure after 300
18 shows two °C, and (b)
graphs: (a)isisthe
theTGA
TGAforforCF,
CFRP,which indicates
which thatthat
indicates they began
they began to
to lose weight after 300 ◦ C, and (b) is the TGA for CF, which indicates that they began to
lose
to weight
lose weight after 300
after °C.
300 °C,Atand
the(b)
highest
is the temperature, which indicates
TGA for CF, which is 800 °C,that
thethey
sample loses
began to
lose weight after 300 ◦ C. At the highest temperature, which is 800 ◦ C, the sample loses
70% weight
lose of its weight.
after 300The°C.CFAt outcome is more
the highest stable thanwhich
temperature, the CFRP.
is 800At°C,
around 700 °C,
the sample the
loses
70% of its weight. The CF outcome is more stable than the CFRP. At around 700 ◦ C, the
weight
70% began
of its to drop
weight. The[98–105].
CF outcomeThe PLA wasstable
is more resistant
thantothe
a continuous transition
CFRP. At around 700heat
°C, due
the
weight began to drop [98–105]. The PLA was resistant to a continuous transition heat due
to lacking
weight of contaminants.
began to drop [98–105]. Furthermore,
The PLA was the addition
resistant of
to fillers has no significant
a continuous effectdue
transition heat on
to lacking of contaminants. Furthermore, the addition of fillers has no significant effect
Tm.
to The modest
lacking changes inFurthermore,
of contaminants. the curve forms the are most of
addition likely related
fillers has notosignificant
the degreeeffect
of crys-
on
on Tm. The modest changes in the curve forms are most likely related to the degree of
tallization
Tm. for each
The modest test, suggesting
changes in the curvethatforms
the composite material’s
are most likely superior
related to the heat stability
degree of crys-is
crystallization for each test, suggesting that the composite material’s superior heat stability
preserved.for each test, suggesting that the composite material’s superior heat stability is
tallization
is preserved.
preserved.
(a) (b)
(a)
Figure 18. The TGA result for (a) CFRP (b) CF.
(b)
4.
4. Conclusions
Conclusions
4. Conclusions
In
Inthis
thisresearch,
research, the
theadopted
adopted recycling
recycling method
method was
was proven
proven practically
practically to
to be
be aafeasible
feasible
process
process forresearch,
In this
for therecycling
the recycling
the of of
thethe
adopted leftover
recycling
leftover carbon
fiber fiber
method
carbon and
wasthe
and thepractically
proven
uncureduncured CFRP
to be a prepreg
CFRP prepreg feasible
material
process
that can for the recycling
be utilized of the
in various leftover carbon
nonstructural fiber andThe
end-products. theexperimental
uncured CFRP prepreg
methodology
adopted for the research included the combination of different types of carbon fiber CF
and the CFRP prepreg mixed with waste PLA, hence the conversion of the leftover prepreg
material into intermediate products such as CF-Prepreg 10% with PLA, CF-Prepreg 20%
with PLA, CF10% with PLA, CF20% with PLA, and pure PLA, followed by the production
Polymers 2022, 14, 2194 15 of 19
of various end products using these intermediate products through the hot extrusion and
compression molding processes.
The low cost of the feedstock and simple, effective, and rapid processing methods
should result in low-cost commercial end products that retain the strong performance for
which composites are known. Furthermore, the experiment provides a practical, low-cost
method through which the components made from waste prepreg can be made in aesthet-
ically good physical forms, with a smooth and unique surface finish due to the random
orientation and arrangement of the fibers. We studied the characteristics and performance
of scrap prepreg-based laminates under various starting material states and processing
circumstances and drew several conclusions that have been summarized as follows:
1. The experimental investigation revealed the negative impact of the expired impreg-
nated epoxy of the CFRP prepreg leftover scrape that may affect the mechanical
properties of the produced composite, even though the properties of the CFRP/PLA
composites in general showed better properties than the recycled PLA.
2. For the modulus of elasticity, the CF/PLA composite at 20% has higher properties
than the CFRP at 20%—specifically, the elastic modulus is 65% and 56% higher for the
CF and the CFRP, respectively, in comparison to the PLA reference value.
3. The yield strength of the 20% CF is the highest, whereas the 20% CFRP is the lowest.
4. Carbon fiber in general enhanced the ultimate strength of the carbon/PLA blends,
starting from 7% at 10% CF to 28% at 20% CF, and 15% at 10% CFRP to 17% at 20%.
5. For the ductility, the recycled PLA showed a higher level of 15% compared to the
commercial PLA filament. For the CF/PLA, the CF has an opposite impact on the
ductility: it decreased the strain at the failure from 43% to 30% for 10% and 20% CF,
respectively. In contrast, CFRP has been attributed to uplifting the strain at failure
from 46% to 53% at the 10% and the 20% CFRP, respectively.
Producing a composite for recycled PLA and the carbon leftover waste demonstrates
promising properties that could be used for various applications employing different ratios
of the mixing parameters that can be successfully carried out with the formed material
compositions. Although the economic impact of the treatment on the process has yet to be
determined, it appears that this research will serve as the starting point for future work on
the recovery of chemical compounds from CFRP polymer resins.
Author Contributions: Conceptualization, S.A.Z. and W.A.; methodology, S.A.; software, A.E.;
validation, S.A.Z., W.A. and S.A.; formal analysis, W.A.; investigation, S.A.; resources, A.E.; data
curation, S.A.; writing original draft preparation, A.E.; writing review and editing, W.A.; visualization,
S.A.; supervision, S.A.Z.; project administration, S.A.; funding acquisition, S.A. All authors have read
and agreed to the published version of the manuscript.
Funding: UAEU, Grant no. 12R140.
Conflicts of Interest: The authors have no conflict of interest.
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1 Department of Chemical & Petroleum Engineering, United Arab Emirates University,

Received: 5 May 2022

Polymers 2022, 14, 2194. https://doi.org/10.3390/polym14112194 https://www.mdpi.com/journal/polymers

Polymers 2022, 14, 2194 3 of 19

1.2.1. Recycling Techniques

Figure 3. Recycling Process from Virgin Carbon Fiber to CFRP.

Figure 5. Samples after the cutting (a) CFRP, (b) CF.

Polymers 2022, 14, x FOR PEER REVIEW 7 of 19

Figure 6. High speed grinder.

Polymers 2022, 14, x FOR PEER REVIEW 9 of 19

Table 1. Dimensions of the prepared tensile test specimens.

Samples Length mm Width mm Thickness mm

Figure 11. Tensile testing machine with a sample.

Table 1. Dimensions of the prepared tensile test specimens.

Samples Length mm Width mm Thickness mm

2.1. Fourier Transform (FTIR)

3. Results and Discussion

3.1. Mechanical Characterization

Table 2 illustrates the mechanical properties of the experimental work conducted in

Polymers 2022, 14, 2194 12 of 19

Figure 15. Ultimate Tensile Strength.

where S is the estimated standard 𝑆𝑆 deviation,𝑋

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