Challenges in Manufacturing of Hemp Fiber-Reinforced Organo Sheets With A Recycled PLA Matrix

polymers
Article
Challenges in Manufacturing of Hemp Fiber-Reinforced
Organo Sheets with a Recycled PLA Matrix
Maximilian Salmins * , Florian Gortner * and Peter Mitschang *
Leibniz-Institut für Verbundwerkstoffe GmbH, Erwin-Schroedinger-Strasse 58, 67663 Kaiserslautern, Germany

* Correspondence: maximilian.salmins@ivw.uni-kl.de (M.S.); florian.gortner@ivw.uni-kl.de (F.G.);
peter.mitschang@ivw.uni-kl.de (P.M.)
Abstract: This study investigates the influence of a hot press process on the properties of hemp
fiber-reinforced organo sheets. Plain-woven fabric made from hemp staple fiber yarns is used as
textile reinforcement, together with a recycled poly-lactic acid (PLA) matrix. Process pressure and
temperature are considered with three factor levels for each parameter. The parameter influence
is examined based on the B-factor model, which considers the temperature-dependent viscosity of
the polymer, as well as the process pressure for the calculation of a dimensionless value. Increasing
these parameters theoretically promotes improvements in impregnation. This study found that
the considered recycled polymer only allows a narrow corridor to achieve adequate impregnation
quality alongside optimal bending properties. Temperatures below 170 ◦ C impede impregnation
due to the high melt viscosity, while temperature increases to 185 ◦ C show the first signs of thermal
degradation, with reduced bending modulus and strength. A comparison with hemp fiber-reinforced
virgin polypropylene, manufactured with identical process parameters, showed that this reduction
can be mainly attributed to polymer degradation rather than reduction in fiber properties. The
process pressure should be at least 1.5 MPa to allow for sufficient compaction of the textile stack, thus
reducing theoretical pore volume content to a minimum.
Keywords: natural fiber reinforced thermoplastic polymers; organo sheet; recycled PLA; hemp fiber;
B-factor model
Citation: Salmins, M.; Gortner, F.;

Mitschang, P. Challenges in
Manufacturing of Hemp Fiber- 1. Introduction
Reinforced Organo Sheets with a
Global challenges such as the scarcity of fossil resources demand increasing efforts to
Recycled PLA Matrix. Polymers 2023,
substitute these materials. The substitution can be achieved by using bio-based materials
15, 4357. https://doi.org/10.3390/
or by recycling instead of using virgin materials [1–3]. The use of bio-based materials can
polym15224357
also lead to reduced energy consumption, compared to conventional materials, e.g., glass
Academic Editor: Carlo Santulli fiber-reinforced polymer composites [4–6]. Natural fiber-reinforced polymer composites
are attractive materials for use in automotive applications—for which up to 37% of total
Received: 29 September 2023
Revised: 17 October 2023
biocomposites in Europe are produced [7]. Hemp fibers are bast fibers and are among
Accepted: 30 October 2023
the most commonly used natural fibers for composite applications [4,7–10]. They can
Published: 8 November 2023 be cultivated in Europe, which further enables sustainable manufacturing with limited
transport distance, compared to natural fibers cultivated in southeast Asia [11,12]. Bast
fibers have a particular structure, as depicted in Figure 1. Hemp plants cultivated in Europe
reach heights of about 2 m with stem diameters between 3.5 and 8.4 cm. Hemp plants
Copyright: © 2023 by the authors. cultivated in China can grow to heights between 4 m and 7 m [8]. The stem consists of
Licensee MDPI, Basel, Switzerland. the outermost layer, the epidermis, which surrounds several fiber bundles. Those can be
This article is an open access article up to 3 m long but are cut down to a length of 1 m before processing. The fiber bundles
distributed under the terms and
are composed of elementary fibers—often between two and twenty, but sometimes up to
conditions of the Creative Commons
forty elementary fibers—which are held together by pectin. The length of the elementary
Attribution (CC BY) license (https://
fibers can be up to 100 mm, with the most common range being reported between 10 mm
creativecommons.org/licenses/by/
and 40 mm [13]. Typical fiber diameters vary between 15 µm and 50 µm. The center of the
4.0/).
Polymers 2023, 15, 4357. https://doi.org/10.3390/polym15224357 https://www.mdpi.com/journal/polymers

Polymers 2023, 15, x FOR PEER REVIEW 2 of 23
Polymers 2023, 15, 4357 2 of 22
and 40 mm [13]. Typical fiber diameters vary between 15 µm and 50 µm. The center of the
stem can be described as a woody core followed by the innermost part, the lumen, which
stem can be described as a woody core followed by the innermost part, the lumen, which is
is hollow. This hollow lumen can also be found inside elementary fibers [8].
hollow. This hollow lumen can also be found inside elementary fibers [8].
Fiber bundle Elementary fiber

Ø 50 µ m Ø 15-50 µ m
Length: 1-3 m Length: 10-40 mm
Epidermis
Woody core
Hemp stem
Ø 3.5-8.4 mm
Lumen
Figure
Figure1.1.Schematic
Schematicrepresentation
representationofofthe
thebast
bastfiber
fiberstructure,
structure,after
after[8,13].
[8,13].
The
Thefinal
finalmorphology,
morphology,the thedegree
degreeof offiber
fiberseparation
separationand andthethefiber
fiberproperties
propertiesdepend depend
on a multitude of conditions during cultivation and
on a multitude of conditions during cultivation and retting [10,13–15]. retting [10,13–15]. TheTheextraction
extraction of
primary
of primary or elementary
or elementary fibersfibers
fromfrom the plant stem begins
the plant with the
stem begins retting
with process,process,
the retting in which in
the
whichsurrounding tissue is tissue
the surrounding dissolved by bacteria
is dissolved by and fungiand
bacteria [14,16].
fungiField retting
[14,16]. is the
Field mostis
retting
common
the mostprocess.
commonPlant stemsPlant
process. remain stems onremain
the field onfor
theseveral
field for weeks andweeks
several plant and tissueplantis
dissolved by microbiological
tissue is dissolved organisms. organisms.
by microbiological This process Thishas toprocess
be monitored
has to to beprevent
monitored over-to
retting
prevent and decreasesand
overretting in mechanical
decreases inproperties
mechanical [14,15]. However,
properties [14,15].some fibers can
However, some still be
fibers
collected
can still prematurely, which in turnwhich
be collected prematurely, leads into turn
incompletely
leads to separated
incompletely fiberseparated
bundles. The fiber
chemical
bundles. composition
The chemical and the resulting
composition andfiber
theproperties reported
resulting fiber in the reported
properties literature in may the
literature
vary widely mayduevary widely
to these dueuncontrollable
often to these often influences.
uncontrollable Theinfluences.
fiber bundles Theare
fiber bundles
separated
are separated
from wooden frompartswooden parts by breaking
by mechanical mechanical andbreaking and scutching
scutching processes processes
after the afterrettingthe
retting [1,8,11,12,14,17].
[1,8,11,12,14,17].
Duvaletetal.
Duval al.[13]
[13]studied
studiedthe thetensile
tensileproperties
propertiesofofhemphempfibers
fiberstotocompare
comparethe theimpact
impact
of the sampling area within the stem—either the top, middle or bottom. They foundfound
of the sampling area within the stem—either the top, middle or bottom. They lim-
limited
ited variations
variations in mechanical
in mechanical properties
properties between
between the sampling
the sampling areas.areas.
This is This is mainly
mainly due
todue
theto the standard
standard deviation,
deviation, whichwhichdid notdid notsignificant
allow allow significant statistical
statistical differentiation.
differentiation. How-
However,
ever, they described
they described that taken
that fiber fiber taken
from thefrom the middle
middle of theof the showed
stem stem showed the highest
the highest ten-
tensile strengths. They also report that hemp fiber diameter
sile strengths. They also report that hemp fiber diameter may influence the Young’s mod- may influence the Young’s
modulus—with
ulus—with a hyperbolic
a hyperbolic decrease
decrease withwithan an increasing
increasing diameter—while
diameter—while thethestrength
strengthatat
break showed a higher
break showed a higher scatter [13].scatter [13].
Lietetal.
Li al.[18]
[18]investigated
investigatedmechanical
mechanicalproperties
propertiesbased
basedon onnano-indentation
nano-indentationand andde- de-
scribedsimilar
scribed similarfindings,
findings,even eventhough
thoughthey theytootoowere
werenotnotable
abletotofind
findstatistical
statisticalsignificance.
significance.
Placet et al. [19] used a modelling approach to describe the diameter dependence ofofthe
Placet et al. [19] used a modelling approach to describe the diameter dependence the
Young’s modulus in hemp fibers, in comparison to experimentally
Young’s modulus in hemp fibers, in comparison to experimentally determined values. The determined values. The
resultsfor
results forultimate
ultimatetensile
tensilestrength
strengthshow showaahyperbolic
hyperbolicdependence
dependencewith withregard
regardtotothe thefiber
fiber
diameter near the rupture zone. It has also been indicated that
diameter near the rupture zone. It has also been indicated that clamping distance can haveclamping distance can have
ananeffect
effectononultimate
ultimatetensile
tensilestrength
strength[10]. [10].
The fibers consist of four macromolecules; namely, cellulose, hemicellulose, lignin and
The fibers consist of four macromolecules; namely, cellulose, hemicellulose, lignin
pectin. Cellulose functions as the fiber backbone and is thermally stable, withstanding
and pectin. Cellulose functions as the fiber backbone and is thermally stable, withstanding
temperatures of up to 350 ◦ C before degradation. Hemicellulose acts as a support material
temperatures of up to 350 °C before degradation. Hemicellulose acts as a support material
within cell walls. Lignin is a complex molecule that binds cells, fibers and vessels within
within cell walls. Lignin is a complex molecule that binds cells, fibers and vessels within
plants. Both hemicellulose and lignin are reported to show the first signs of thermal degra-
dation at temperatures greater than 200 ◦ C, which overall limits the use of thermoplastic
Polymers 2023, 15, 4357 3 of 22
polymers for the manufacturing of composites to those with melt temperatures below this
threshold [8].
Polyethylene (PE) [20], polypropylene (PP) [21–29] and poly-lactic acid (PLA) [30–32]
are, therefore, among the most commonly used thermoplastic polymers [33]. Composites
with a random fiber orientation made in injection molding processes [4,20–22,30,31] or
based on non woven fiber mats [4,8,23,24,34] are the biggest share. However, some authors
reported approaches for composites with increased mechanical potential due to unidirec-
tional reinforcement [4,27,32,35]. It has been indicated that the mechanical performance of
natural fiber-reinforced composites might be limited, due to poor fiber–matrix adhesion,
which could be overcome by fiber treatment or matrix functionalization [36–38]. PLA is
one of the most promising bio-based polymers and has the highest volume of industrial
applications [5,7,39,40]. Its comparatively low melting temperature enables the production
of natural fiber reinforced composites without compromising the fiber properties [41].
While natural fiber components can withstand temperatures up to 200 ◦ C [8], thermal
degradation in PLA is a complex process [42], with some literature indicating a limited
thermal stability for temperatures above 190 ◦ C [43]. This degradation is related to the
thermal instability of ester groups within the PLA [44], which is further enhanced by
moisture, oxygen or mechanical loads [45]. The presence of oxygen may lead to an earlier
onset of degradation at 150 ◦ C, compared to 270 ◦ C in vacuum [44]. This behavior may
be disadvantageous when the processing of polymers with melt temperatures at these
temperatures is considered. Processing PLA at temperatures of 200 ◦ C in air may lead to
thermal oxidation with degradation, due to random chain scission [46–48].
Continuous reinforcement with natural fibers is possible, when the fibers of a defined
length are spun into a staple fiber yarn. Most often, a low fraction of synthetic fibers is
used to stabilize the yarn and allow sufficient tensile strengths for weaving processes.
These yarns can be used for textile production—i.e., woven or non-crimp fabrics—as a
semi-finished product for composite production [9].
Woven fabrics can be used for the production of continuously fiber-reinforced compos-
ites, so-called organo sheets. Fiber bundles within the textiles have to be impregnated with
the matrix polymer during organo sheet manufacturing. The impregnation of dry fiber
textiles with a thermoplastic matrix is a complex process that is influenced by a variety of
factors. Figure 2 shows a schematic of the impregnation of a dry textile with a thermoplastic
polymer matrix. Both the polymer and the textile are separate, with defined thicknesses
Xf(t<0) , before the process starts. Then, pressure is applied, through which the textile layers
are compacted to a defined thickness Xf(t=0) . The stack is heated to temperatures above
the melting temperature of the polymer, which in turn allows the impregnation of the
porous textile stack and the displacement of air. The polymer is distributed homogeneously
across the textile surface, which facilitates impregnation only through the stack thickness.
Displacement of the trapped air allows a hydrostatic equilibrium to be established. This
facilitates relaxation of the textile, and its thickness increases again [49–51].
t<0 t≈0 t < timp t > timp t = tfinal
XI p
Poly- XI XI p
mer
p X p
Xf(t<0) XI I_final = Xf(n)
Xf(n)
Xf(t=0) Xf(n)
Fibers Ximp
Ximp Ximp
Figure
Figure2.
2.Schematic
Schematicof
ofimpregnation
impregnationprocess,
process, based
based on
on [51]
[51] after
after [49,50].
[49,50].
Initial state Macro-impregnation Micro-impregnation

Polymer
Polymers 2023, 15, 4357 t<0 t≈0 t < timp t > timp t = tfinal 4 of 22
XI p
The process
Poly- of XI impregnationX can be divided
p into two distinct phases—macro- and
I
micro-impregnation.
mer A schematic for material and pore distribution in these phases is
shown
Xf(t<0) in Figure 3. The molten polymer impregnates
p X
the macro-pores p
around the fiber
XI I_final = Xf(n)
bundles during macro-impregnation, Xf(n) whereas the polymer fills the micro-pores within a
Xf(t=0) Xf(n)these processes are influenced by the
fiber bundle during micro-impregnation. Both of
Fibers
local permeability. Values of permeability
Ximp for inter-bundle impregnation—around the
fiber bundles—are significantly higher than theXimp values measured Ximp for intra-bundle—in
between fiber bundles and around individual fibers. High values of permeability facilitate
impregnation [52]. of impregnation process, based on [51] after [49,50].
Figure 2. Schematic
Initial state Macro-impregnation Micro-impregnation

Polymer
Polymer
Fiber bundles Macro-pores Micro-pores
Figure 3. Schematic
Figure3. Schematic of
of macro-
macro-and
andmicro-impregnation,
micro-impregnation,after
after[51].
[51].
The
The B-factor
B-factor model,
model, developed
developed by by Mayer
Mayer [53]
[53] and
and refined
refined by
by Christmann
Christmann [51],
[51], has
has
been proposed as a means to compare the impregnation performance of processes
been proposed as a means to compare the impregnation performance of processes with with
different parameter combinations. The B-factor model was originally developed in order to
different parameter combinations. The B-factor model was originally developed in order
allow the transfer of the optimum impregnation parameters determined in a laboratory test
to allow the transfer of the optimum impregnation parameters determined in a laboratory
to a series production line. The B-factor, as a dimensionless constant, summarizes process
test to a series production line. The B-factor, as a dimensionless constant, summarizes pro-
parameters such as pressure p and time t, as well as the temperature dependent viscosity
cess parameters such as pressure p and time t, as well as the temperature dependent vis-
η(T(t)) [54]. The first part of the B-factor is the b-integral, described in Equation (1):
cosity η(T(t)) [54]. The first part of the B-factor is the b-integral, described in Equation (1):
t a 𝑡𝑎 1 1
Z
b =𝑏 = ∫𝑡0 𝜂(𝑇(𝑡))dt,𝑑𝑡, (1)
(1)
t0 η ( T ( t ))
This integral
This integral cancan alternatively
alternatively be be calculated
calculated asas the
the sum
sum of of the
the individual
individual reciprocal
reciprocal
viscositiesat
viscosities attime
timeintervals
intervalsof ofdiscrete
discretetemperatures,
temperatures,as asininEquation
Equation(2): (2):
1
𝑏 = ∑𝑛𝑘=0 (𝑡𝑘 ×
1𝜂(𝑇𝑘)),

(2)
n
b = ∑ k =0 t k × , (2)
η ( Tk )
The particular temperature spectrum, in which this value of b-integral is calculated,
startsThe
with the point
particular in time at which
temperature spectrum,the melt temperature
in which this value Tmofisb-integral
exceeded.isUsually,
calculated, the
end point
starts withfor thethe calculation
point in timeofatb is reached
which the once
meltthe temperature
temperature Tmdrops below theUsually,
is exceeded. crystal-
lization
the temperature
end point for the Tcalculation
c [55]. The temperature-dependent
of b is reached once the viscosity
temperature in this timeframe
drops below the can
be approximated
crystallization based onTan
temperature c Arrhenius
[55]. The equation, incorporating
temperature-dependent the
viscosity viscosity
in this η (T
timeframe
0 0) at a
particular
can temperature,
be approximated the on
based activation energyequation,
an Arrhenius Ea, the gas constant R and
incorporating the the reciprocal
viscosity η 0 (Ttem-
0 ) at
aperature
particular temperature,
difference, (3): energy Ea , the gas constant R and the reciprocal
the activation
as in Equation
temperature difference, as in Equation (3): 𝐸𝑎 1 1
𝜂0 (𝑇) = 𝜂0 (𝑇0 ) × exp
[ 𝑅 × (𝑇 − 𝑇 )] (3)
Ea 1 10
η0 ( T ) = η0 ( T0 ) × exp × − (3)
The B-factor is then calculated by multiplying R this T b-integral
T0 with the process pres-
sure p, as described in Equation (4):
The B-factor is then calculated by multiplying this b-integral with the process pressure
p, as described in Equation (4): 𝐵 = 𝑝 × 𝑏 = 𝑝 × ∫𝑡𝑎 1 𝑑𝑡,
𝑡 0 𝜂(𝑇(𝑡)) (4)
Z ta
1
B = p×b = p× dt, (4)
t0 η ( T (t))
Polymers 2023, 15, 4357 5 of 22
Previous works reported in the literature mainly focused on the production of natural
fiber-reinforced composite parts with a random fiber orientation. However, the possibility
to manufacture staple fiber yarns from natural fibers allows for continuous reinforcement,
based on woven and non-crimp fabrics. The applicability of the B-factor model to assess
Polymers 2023, 15, x FOR PEER REVIEW
impregnation performance has mainly been researched with glass fiber textiles and petrol- 5 of 23
based polymers. It should be investigated whether this model is also applicable for the
manufacturing of composites with bio-based components—natural fibers or bio-based
polymers, or a combination
Previous of both.
works reported in theTherefore,
literaturethis study
mainly focusses
focused ononthethe manufacturing
production of
of natu-
natural fiber-reinforced organo sheets with a fabric reinforcement and a recycled poly-lactic
ral fiber-reinforced composite parts with a random fiber orientation. However, the possi-
acid matrix
bility polymer, asstaple
to manufacture well asfiber
the assessment
yarns from of the manufacturing
natural fibers allows process based onrein-
for continuous the
B-factor model.
forcement, based on woven and non-crimp fabrics. The applicability of the B-factor model
to assess impregnation performance has mainly been researched with glass fiber textiles
2. Materials and Methods
and petrol-based polymers. It should be investigated whether this model is also applicable
2.1. Materials
for the manufacturing of composites with bio-based components—natural fibers or bio-
Plain wovenorfabrics with a surface 2 , made from hemp fibers,
based polymers, a combination of both.weight of 465
Therefore, thisg/m
study focusses on the manufac-
were
turingused for manufacturing
of natural fiber-reinforcedhemp–rPLA organo
organo sheets sheets.
with a fabricThe hemp fabric,and
reinforcement with a count
a recycled
of 4.9 threads per cm in both warp and weft direction, was made
poly-lactic acid matrix polymer, as well as the assessment of the manufacturing process by Gerster TechTex, a
division of Gustav Gerster
based on the B-factor model. GmbH & Co. KG (located in Biberach an der Riß, Germany),
with 400 tex hemp staple fiber yarns produced by Wagenfelder Spinnereien GmbH (located
in
2. Wagenfeld,
Materials and Germany),
Methodsbased on a design developed within the “Durobast” project
(www.durobast.de (accessed on 29 September 2023)). A recycled PLA powder from Looplife
2.1. Materials
Polymers was used as the matrix polymer. Borealis Bj100hp polypropylene was used for
Plain woven
manufacturing fabrics
NF–PP with sheets,
organo a surface
in weight
order toofidentify
465 g/mpossible
2, made from hemp fibers, were
thermal degradation of
used
the for manufacturing
natural fibers. Selected hemp–rPLA organo sheets.
polymer properties Theinhemp
are given Tablefabric,
1. Thewith a count
materials, asof 4.9
well
threads
as per cmfor
a schematic in the
bothstacking
warp and wefttextile
of the direction, was madeare
and polymer, byshown
GersterinTechTex,
Figure 4.a The
division
red
of Gustav
arrows Gerster
describe theGmbH & Co.
direction KG (located
in which the moltenin Biberach
polymeran der Riß,
flows Germany),
for fiber with 400
impregnation.
tex hemp staple fiber yarns produced by Wagenfelder Spinnereien GmbH (located in
Wagenfeld,
Table 1. PolymerGermany),
properties based on PLA
of recycled a design
and PP.developed within the “Durobast” project
(www.durobast.de (accessed on 29 September 2023)). A recycled PLA powder from
Looplife Polymers was used as the matrixGlass polymer. Borealis MeltBj100hpBending
polypropylene
Bending was
Polymer Density Transition
used for manufacturing NF–PP organoTemperature sheets, in order to identify possible
Temperature Modulusthermal deg-
Strength
radation of the natural fibers. Selected polymer properties are given in Table 1. The mate-
1.26
rials,
rPLAas(Looplife
well as polymers)
a schematic for the3stacking59 of◦the
C textile and ◦C
152.8polymer, areGPa
3.44 shown98 in MPa
Figure
g/cm
4. The red arrows
PP (Borealis bj100hp)describe the direction
0.9 g/cm 3 in which
◦
<0 C * the molten ◦
165 C polymer flows
1.25 GPa for 35 MPaim-
fiber
pregnation.
* Glass transition temperature of polypropylene bj100hp was not detected in DSC between 0 C and 200 ◦ C.
◦
Hemp rPLA Textile and polymer

plain weave powder stack setup
Warp direction
Hemp
rPLA Impreg-
Hemp nation
rPLA direction
50 mm 50 mm
Hemp
Figure4.4.Dry
Figure Drytextile
textile(left),
(left),recycled
recycledPLA
PLApowder
powder(middle)
(middle)and
andstack
stacksetup
setup(right).
(right).
2.2. Organo Sheet Manufacturing
Table 1. Polymer properties of recycled PLA and PP.
Organo sheets were manufactured on a laboratory hot press in a modular cylindrical
tool. The tool consists of an outer steelGlass
ring and two cylindrical steel stamps with a diameter
Melt Bending Bending
Polymer
of 100 mm, and eachDensity
stamp has aTransition
thickness of 15 mm. Figure 5 shows the laboratory hot
Temperature Modulus Strength
press with the modular cylindrical press tool on the left, as well as the setup for temperature
Temperature
rPLA (Looplife
1.26 g/cm3 59 °C 152.8 °C 3.44 GPa 98 MPa
polymers)
PP (Borealis
0.9 g/cm3 <0 °C * 165 °C 1.25 GPa 35 MPa
bj100hp)
* Glass transition temperature of polypropylene bj100hp was not detected in DSC between 0 °C and
200 °C.
lighted, before cutting individual pieces on a hydraulic punching unit. The warp direction
in each textile layer was aligned within the tool. The hydrophilic behavior and the signif-
icant moisture absorption ability of natural fibers are well reported [8,56]. The textile lay-
ers and the polymer were therefore dried in a convection oven at 80 °C for a duration of 3
h, to reduce the moisture content and minimize its influence, after which a weight balance
Polymers 2023, 15, 4357 was achieved. The average moisture absorption determined for the natural fibers by this 6 of 22
drying process was 5%. The pre-dried textiles, together with the polymer powder, were
weighed before insertion into the press tool. The organo sheet was again weighed after
themeasurement
process to account
inside for
thepolymer squeeze-out.
textile stack Organo sheet
on the right—each thickness
without was ring.
the outer measured at
The stack
four points across the surface, for calculating the theoretical fiber volume
of textile and polymer was put in between the tool stamps. The stack consisted of three content.
The layers
textile laboratory
and hot
9.3 gpress was designed
of polymer and was at Leibniz-Institut
prepared to achieve für Verbundwerkstoffe and of
a theoretical thickness
consists
1.9 mmof:and a theoretical fiber volume content of 49%. The polymer was put on top of the
• bottom and middle layers—in
an electromechanical cylinderthisfor
manner,
applyingtheforces
polymer has20tokN
up to penetrate
in tandemthewith
outera layers
mem- to
reach the surface. This setup allowed
brane load cell as a means of force control,for instant evaluation of impregnation quality after
• thetwo
manufacturing process.
fixed tool halves The warp
for active direction tool
heating—each within
halfthe textile
with layers was
six cartridge highlighted,
heaters with
before cutting
a total outputindividual
of 2.4 kW,pieces on awith
together hydraulic
sheathpunching unit. The
thermocouples warp direction
for temperature in each
control,
textile layer
as well wasactive
as an aligned within
cooling unitthe tool.
with The hydrophilic
a water–air mixture.behavior and the significant
moisture absorption ability of natural fibers are well reported [8,56]. The textile layers and
The hot press is controlled by a LabView-based program and is set up for inline re-
the polymer were therefore dried in a convection oven at 80 ◦ C for a duration of 3 h, to
cording of process data at 1 Hz, including:
reduce the moisture content and minimize its influence, after which a weight balance was
• achieved.
temperatures at different
The average locations
moisture within
absorption the setup (sheath
determined thermocouple
for the natural fibers bywithin the
this drying
tool with cartridge heater for temperature control and thermocouples
process was 5%. The pre-dried textiles, together with the polymer powder, were weighed for independ-
ent recording;
before accuracy
insertion into ± 1 K),
the press tool. The organo sheet was again weighed after the process
• to account
effectivefor
forces (membrane
polymer squeeze-out.load cell; accuracy
Organo sheet± thickness
1 N), and was measured at four points
• across
the stack thickness
the surface, for (high accuracy
calculating the glass scale; fiber
theoretical accuracy
volume± 1 µm).
content.
Active cooling unit Tool with

with water-air mixture cartridge heater and
sheath thermocouple
Thermocouple
Tool
halves
Press tool for organo 50 mm Textile stack

50 mm sheet manufacturing
(a) (b)
Figure
Figure5. (a) Laboratory
5. (a) hothot
Laboratory press with
press press
with tool;
press (b)(b)
tool; setup forfor
setup temperature measurement
temperature inside
measurement thethe
inside
fiber stack.
fiber stack.
The laboratory hot press was designed at Leibniz-Institut für Verbundwerkstoffe and
consists of:
• an electromechanical cylinder for applying forces up to 20 kN in tandem with a
membrane load cell as a means of force control,
• two fixed tool halves for active heating—each tool half with six cartridge heaters with
a total output of 2.4 kW, together with sheath thermocouples for temperature control,
as well as an active cooling unit with a water–air mixture.
The hot press is controlled by a LabView-based program and is set up for inline
recording of process data at 1 Hz, including:
• temperatures at different locations within the setup (sheath thermocouple within the
tool with cartridge heater for temperature control and thermocouples for independent
recording; accuracy ± 1 K),
• effective forces (membrane load cell; accuracy ± 1 N), and
• the stack thickness (high accuracy glass scale; accuracy ± 1 µm).
The main test series to identify parameter influences was set up to manufacture hemp–
rPLA organo sheets with a target fiber volume content (FVC) of 49%. An overview of the
The main test series to identify parameter influences was set up to manufacture
hemp–rPLA organo sheets with a target fiber volume content (FVC) of 49%. An overview
Polymers 2023, 15, 4357 7 of 22
of the process parameters is presented in Table 2. This test series aimed to identify the
optimal process parameters for hemp–rPLA organo sheet manufacturing. An additional
test series, with a reduced target FVC of 37%, was conducted with the optimal parameter
process parameters
combination, to compareis presented
the effectinofTable
FVC2. on
This test series aimed
mechanical to identify
properties. A set the optimal
of reference
process parameters for hemp–rPLA organo sheet manufacturing. An
organo sheets with a PP matrix (Borealis bj100hp) was manufactured with a comparable additional test series,
with a reduced target FVC of 37%, was conducted with the optimal parameter combination,
FVC, to investigate the effect of process temperature on bending properties and to identify
to compare the effect of FVC on mechanical properties. A set of reference organo sheets with
possible thermal degradation within the hemp fibers. Five organo sheets were manufac-
a PP matrix (Borealis bj100hp) was manufactured with a comparable FVC, to investigate
tured per parameter combination for an adequate statistical basis. The overall timespan of
the effect of process temperature on bending properties and to identify possible thermal
1280 s for the hot
degradation press
within the process was Five
hemp fibers. identical for
organo eachwere
sheets parameter combination.
manufactured Process
per parameter
pressure was applied throughout the whole process. The preset variothermal
combination for an adequate statistical basis. The overall timespan of 1280 s for the temperature
profile was divided
hot press process into
was the following
identical phases:
for each 300 s were
parameter preset forProcess
combination. heating, followed
pressure was by
600applied
s of hold time andthe
throughout the finalprocess.
whole coolingThe time of 380
preset s. The effective
variothermal temperature
temperature profile curve
was
shows a considerable
divided deviation
into the following during300
phases: heating
s werewhen compared
preset to the
for heating, preset ramp,
followed by 600which
s of
is why
holdthe specific
time and theprocess data have
final cooling to be
time of considered
380 s. The for the evaluation
effective temperature of process impact
curve shows
anda considerable
impregnationdeviation duringThe
performance. heating
delaywhen compared
between to and
preset the preset ramp,
effective which is
temperature
whyhas
curve thebeen
specific process by
illustrated data havearrows
green to be considered
in Figure 6.forThe
the specific
evaluation of process
thermal impactof
expansion
theand
toolimpregnation
stamps were performance.
recorded for each The parameter
delay between preset and
combination. effective temperature
Measurements of the ef-
curve
fective has been illustrated
temperature inside thebytool
green
werearrows in Figure
conducted 6. The
without thespecific thermal
outer ring, expansion
to allow for the
of the tool stamps were recorded for each parameter combination. Measurements of the
placement of thermocouples. A comparison of preset temperature and pressure ramps for
effective temperature inside the tool were conducted without the outer ring, to allow for
organo sheet manufacturing is shown in Figure 6.
the placement of thermocouples. A comparison of preset temperature and pressure ramps
for organo sheet manufacturing is shown in Figure 6.
Table 2. Process parameter for manufacturing of hemp fiber-reinforced organo sheets.
Table 2. Process parameter for manufacturing of hemp fiber-reinforced organo sheets.

Fiber Volume
Material Temperature Pressure
Material Temperature Pressure
Content
Fiber Volume Content
170 °C 0.5 MPa
170 ◦ C 0.5 MPa
Hemp–rPLA
Hemp–rPLA 185 ◦185
C °C 1.5 MPa 1.5 MPa 37–50 vol.-%
37–50 vol.-%
◦C
200 200 °C 2.5 MPa 2.5 MPa
◦
170 170C °C
185 ◦185
C °C
Hemp–PP
Hemp–PP 1.5 MPa 1.5 MPa 43–48 vol.-%
43–48 vol.-%
200 ◦ C
200 °C
215 ◦ C
215 °C
Heating Hold time Cooling

Preset ramp Delay
200
1.5
Temperature in °C
Pressure in MPa
150
Tm_PLA 1
100
0.5
50 300 s 600 s 380 s
Measured temperature Temperature ramp Pressure ramp
0 0
0 300 600 900 1200
Time in seconds
Figure 6. Comparison of temperature ramp and effective temperature alongside pressure ramp.
Figure 6. Comparison of temperature ramp and effective temperature alongside pressure ramp.
2.3. Interpretation of Process Data for B-Factor Calculation
Figure 7 shows an exemplary set of process data for effective pressure and stack
thickness, together with the temperature curves. This correlation allows the identification
of characteristic moments during organo sheet manufacturing which in turn allow dividing
the impregnation process into four sections (I–IV). The first section (I) can be described as
impregnation starts with the temperature surpassing the polymer melt temperature. The
onset of macro-impregnation can be identified by a distinct drop in process pressure, be-
fore a plateau is reached with progresses in micro-impregnation. Macro-impregnation is
followed by micro-impregnation, with a distinct plateau in stack thickness. Minimal de-
Polymers 2023, 15, 4357 creases during this phase can be mainly attributed to polymer squeeze-out through8 the of 22
gap between the tool stamps and the outer ring. The final section (IV) shows decreases in
stack thickness, due to solidification during cooling of the setup.
the stack being
Calculation of fully compacted
the B-factor at moderate
is based on thetemperatures. The following section viscosity
reciprocal temperature-specific (II) begins
with thebegins
and usually temperature exceeding
at the melt the glass
temperature of transition
the polymer.temperature,
This pointallowing the polymer
can be identified by
powder to shift within the stack and providing conditions for progressive
the distinct drop in process pressure for temperatures higher than Tm and was identified compaction
andmanufacturing
for each nesting. The third section
process (III) consists
to calculate of the to
individual impregnation
values processes.
for the B-factor. The Macro-
range
impregnation starts with the temperature surpassing the polymer melt
for calculation usually extends over the time during which the polymer is molten and temperature. The
onset of macro-impregnation can be identified by a distinct drop in process pressure,
until the point when organo sheet is cooled below the recrystallization temperature. The
before a plateau is reached with progresses in micro-impregnation. Macro-impregnation
considered rPLA does not show a distinct recrystallization behavior during cooling. The
is followed by micro-impregnation, with a distinct plateau in stack thickness. Minimal
rangedecreases
for B-factor calculation within this study is defined as starting with the onset of
during this phase can be mainly attributed to polymer squeeze-out through the
macro-impregnation,
gap between the tooluntil the point
stamps and atthewhich
outer the
ring.temperature drops(IV)
The final section below thedecreases
shows melt tem- in
perature. This range is highlighted in Figure 7.
stack thickness, due to solidification during cooling of the setup.
XI p
XI p
XI
p
XI_final = Xf(n) p
Xf(n)
Xf(t=0) Xf(n) Stack thickness
Temperature
Ximp
Pressure
Ximp Ximp
Stack thickness in mm
Tool temperature in °C
1.7 5 150
Pressure in MPa
Molten polymer
Macro-
4 impregnation 120
1.6 Micro-
3 impregnation 90
2 60
1.5
1 Calculation of b-integral 30
I II III IV
1.4 0 0
0 300 600 900 1200
Time in sec
Figure 7. Correlation of process data with impregnation phases, with schematics based on [51]
Figure 7. Correlation
after [49,50]. of process data with impregnation phases, with schematics based on [51]
after [49,50]
Calculation of the B-factor is based on the reciprocal temperature-specific viscosity
and usually begins
2.4. Consideration at theOrgano
of Physical melt temperature of the polymer. This point can be identified by
Sheet Properties
the distinct drop in process pressure for temperatures higher than Tm and was identified
The physical organo sheet properties are calculated based on the measurements of
for each manufacturing process to calculate individual values for the B-factor. The range
weighing the stack before and the organo sheet after the process as well as thickness meas-
for calculation usually extends over the time during which the polymer is molten and
urements at four points across the organo sheet surface, as depicted in Figure 8a. The
until the point when organo sheet is cooled below the recrystallization temperature. The
measurements
consideredforrPLAthese
doesvalues allowed
not show for the
a distinct calculation ofbehavior
recrystallization theoretical fiber
during and pore
cooling. The
volume contents.
range Fiber
for B-factor calculation within this𝑣𝑓study
volume content, , wasiscalculated
defined as using
startingEquation (5), based
with the onset on
of macro-
the textile stack weight determined before the process—each stack of three textile
impregnation, until the point at which the temperature drops below the melt temperature. stacks
This range is highlighted in Figure 7.
2.4. Consideration of Physical Organo Sheet Properties

The physical organo sheet properties are calculated based on the measurements of
weighing the stack before and the organo sheet after the process as well as thickness
measurements at four points across the organo sheet surface, as depicted in Figure 8a.
The measurements for these values allowed for the calculation of theoretical fiber and
pore volume contents. Fiber volume content, v f , was calculated using Equation (5), based
on the textile stack weight determined before the process—each stack of three textile
stacks has been weighed individually—with a density of 1.45 g/cm3 for hemp fibers. It
was assumed that the fibers were completely dry—following the drying process in the
convection oven—and that the reduction in the organo sheet weight can be attributed to
Polymers 2023, 15, 4357 has been weighed individually—with a density of 1.45 g/cm3 for hemp fibers. It was as-
9 of 22
sumed that the fibers were completely dry—following the drying process in the convec-
tion oven—and that the reduction in the organo sheet weight can be attributed to polymer
squeeze-out. The resulting
polymer squeeze-out. Thevolume
resultingwas thenwas
volume divided by the area
then divided of area
by the the press
of the tool
presswith
tool a
diameter
with a of 100 mm
diameter ofto arrive
100 mm toat aarrive
theoretical thickness.
at a theoretical Three textile
thickness. Threelayers
textilewith anwith
layers average
an
of 10.5 g would
average thus
of 10.5 have thus
g would a theoretical thicknessthickness
have a theoretical of 0.92 mm:
of 0.92 mm:
Warp direction
t1
Bending 3
Bending 1
Bending 2
t4 t2
50 mm t3 50 mm
(a) (b)
Figure 8. (a)
Figure 8. Points forfor
(a) Points organo sheet
organo thickness
sheet thicknessmeasurements
measurements and (b) position
and (b) positionofofthree
threepoint
pointbending
bending
specimens within the organo sheet.
specimens within the organo sheet.
1 mtextile
vf = 1 × 𝑚𝑡𝑒𝑥𝑡𝑖𝑙𝑒 (5)
𝑣𝑓 = organo sheet × hemp × Atool
t ρ (5)
𝑡𝑜𝑟𝑔𝑎𝑛𝑜 𝑠ℎ𝑒𝑒𝑡 𝜌ℎ𝑒𝑚𝑝 × 𝐴𝑡𝑜𝑜𝑙
Matrix volume content vm was calculated in a similar manner, with (6) based on the
Matrix
total volume
weight of thecontent 𝑣𝑚 wasstack,
textile polymer calculated in adensity
with the similarof
manner, 3 for
with
1.26 g/cm (6)the
based on the
recycled
PLA
total basedofonthe
weight thetextile
data sheet provided
polymer bywith
stack, the supplier:
the density of 1.26 g/cm3 for the recycled
PLA based on the data sheet provided by the supplier:
m polymer
1
vm = × (6)
t 1 ρ 𝑚× Atool
𝑝𝑜𝑙𝑦𝑚𝑒𝑟
𝑣𝑚 = organo sheet ×PLA (6)
𝑡𝑜𝑟𝑔𝑎𝑛𝑜 𝑠ℎ𝑒𝑒𝑡 𝜌𝑃𝐿𝐴 × 𝐴𝑡𝑜𝑜𝑙
The pore volume content can finally be calculated with Equation (7) as the residual
The pore volume content can finally be calculated with Equation (7) as the residual
volume:
volume: v p = 1 − v f − vm (7)
𝑣 =1−𝑣 −𝑣
𝑝 Based on𝑓Three𝑚Point Bending Tests (7)
2.5. Evaluation of Organo Sheet Properties
Three point bending tests, following DIN EN ISO 14125 [57], were used to investigate
the effect
2.5. Evaluation ofofprocess
Organoparameters during
Sheet Properties organo
Based sheetPoint
on Three manufacturing.
Bending TestsSpecimens had a
width of 15 mm and a length, lpart , 20 times its height, tpart . The support length L was set to
Three point bending tests, following DIN EN ISO 14125 [57], were mm used to investigate
16 times the specimen thickness tpart . The testing speed was set to 5 min . Every test series
theproduced
effect of five
process
replicate organo sheets, with three specimens taken from Specimens
parameters during organo sheet manufacturing. each—a totalhadof a
width of 15 mm per
15 specimens andparameter
a length, combination—for
lpart, 20 times its height,
bendingtpart . The
tests. support length
Specimens were cut L from
was settheto
Polymers 2023, 15, x FOR PEER REVIEW 𝑚𝑚 10 of 23
16 times the specimen thickness t . The testing speed was set
organo sheets with their length parallel to the warp direction, as depicted to 5 . Every test series
𝑚𝑖𝑛 in Figure 8b. A
part
schematic
produced fiveforreplicate
the test setup forsheets,
organo three pointwithbending tests is shown
three specimens takenin from
Figureeach—a
9. total of
15 specimens per parameter combination—for bending tests. Specimens were cut from
the organo sheets with theirF length parallel to the warp direction, as depicted in Figure
8b. A schematic for the test setup for three point bending tests is shown in Figure 9.
tpart
L
lpart
Figure9.9.Setup
Figure Setupfor
forthree
threepoint
pointbending
bendingtests
tests[57].
[57].
3. Results
3.1. Polymer Properties
The specific polymer properties summarized in Table 1 were determined by using
Polymers 2023, 15, 4357 10 of 22
3. Results
3.1. Polymer Properties
The specific polymer properties summarized in Table 1 were determined by using
differential scanning calorimetry with a nitrogen atmosphere. The polymer was put into
the chamber and heated to 210 ◦ C (depicted in red), was then cooled down to 0 ◦ C during
the second cycle (depicted in black), before being heated once again to 210 ◦ C (depicted
in blue). Each step was conducted with a heating or cooling rate of 10 K/min. The
heat flux curves for these steps allow different conclusions. The polymer shows limited
crystallization behavior—the area above the reference line—during the first heating step,
until the temperature is approximately 142 ◦ C. The polymer can therefore be assumed
to initially be in a crystalline state. The following temperature range is dominated by
the resolution of crystalline structure—the area below the reference line—due to melting,
with a peak at the location of the melt temperature at 154 ◦ C. The curve arrives at a
plateau once the polymer is molten completely, for temperatures higher than 167 ◦ C.
Temperatures for processing this polymer should preferably be higher than this threshold.
Further heating to 210 ◦ C shows no significant change in heat flux. The polymer behavior
during cooling, below the glass transition temperature, was investigated during the second
process step. The curve shows linear behavior between the maximum of 210 ◦ C and the
onset of glass transition at 62 ◦ C. This leads to the conclusion that the polymer remains
completely amorphous and does not crystallize during cooling down. The final process
step was reheating the polymer to 210 ◦ C. The first characteristic feature was the glass
transition temperature, at temperatures virtually identical, at 59 ◦ C, to the other two
process steps. The second characteristic feature is the pronounced crystallization behavior,
starting at approximately 100 ◦ C. This area above the reference line is far more distinct
during this second cycle than during the first heating cycle. The levels of the necessary
energy for the formation and dissolution of the crystalline structure—striped areas below
the curve—nearly cancel each other out, whereas the first heating cycle showed a larger
negative value that can be attributed to the dissolution of the initial structure. The discussed
value is described as “standardized” in Figure 10. The absence of crystallization during the
cooling process can be attributed to the typically lower rate of crystallization of PLA when
compared to other thermoplastics [42]. This might be a problem for the process evaluation
based on the B-factor approach, since the recrystallization temperature constitutes the
second temperature boundary. The reader is advised to compare this behavior to Figure A1,
in which the DSC curve of a polypropylene bj100hp with distinct recrystallization behavior
during cooling is depicted.
A comparison of the viscosities measured and predicted for the considered PLA is
shown in Figure 11. The temperature-dependent values of viscosity can be calculated based
on an Arrhenius equation; see Equation (8). In this equation, η0 ( T0 ) is the selected viscosity
at the reference temperature T0 , Ea is the activation energy, R is the universal gas and T is a
given temperature within the range of interest:

Ea 1 1
η [ T (t)] = η0 ( T0 ) × exp × − (8)
R T T0
Adequate agreement can be achieved, with the presented values for the parameters
with T0 and η0 being taken from the data set and Ea being determined empirically.
Polymers
3, 15, x FOR 2023, 15, 4357
PEER REVIEW 11 of 23 11 of 22
Figure 10. DSC curve recorded during differential scanning calorimetry.
A comparison of the viscosities measured and predicted for the considered PL

shown in Figure 11. The temperature-dependent values of viscosity can be calcula
based on an Arrhenius equation; see Equation (8). In this equation, 𝜂0 (𝑇0 ) is the selec
viscosity at the reference temperature T0, 𝐸𝑎 is the activation energy, R is the unive
gas and T is a given temperature within the range of interest:
𝐸𝑎 1 1
𝜂[𝑇(𝑡)] = 𝜂0 (𝑇0 ) × 𝑒𝑥𝑝 [ × ( − )]
𝑅 𝑇 𝑇0
Adequate agreement can be achieved, with the presented values for the parame
Figure 10. DSC curve recorded during differential scanning calorimetry.
Figure 10. DSC curve recorded during differential scanning calorimetry.
A comparison of250 the viscosities measured and predicted130 for the considered PLA is
Viscosity η in Pa∙s
Arrhenius equation
shown in Figure 11. The temperature-dependent values of viscosity canT0be
(Ea = 130 kJ/mol; calculated
= 169 °C; η0 = 290 Pa∙s)
200 Eta* 𝜂 (𝑇 ) is the selected
Measured viscosity
based on an Arrhenius equation; see Equation (8). In this equation,
150 temperature T0, 𝐸 is the activation energy, R is the universal
viscosity at the reference
gas and T is a given temperature
100 within the range of interest:
50 𝐸 1 1
𝜂 𝑇(𝑡) = 𝜂 (𝑇 ) × 𝑒𝑥𝑝 × − (8)
𝑅 𝑇 𝑇
0
Adequate agreement can be achieved,
165 170 with
175 the presented
180 values
185 for190
the parameters
195 200
Temperature in °C
Figure 11. Comparison of measured and predicted viscosity for the considered rPLA based on an
Figure 11. Comparison of measured and predicted viscosity for the considered rPLA based o
Arrhenius equation.
250 Arrhenius equation.
Viscosity η in Pa∙s
130
Arrhenius equation
3.2. Interpretation of Process Data and
(Ea = 130 kJ/mol; B-Factor
T0 = 169 Calculation
°C; η0 = 290 Pa∙s)
200 3.2. Eta*
Measured viscosity
Interpretation of Process Data and B-Factor Calculation
The process data for organo sheet manufacturing show characteristic behavior based
150 The process Figure
on parameter combinations. data for12organo
showssheet manufacturing
a comparison of theshow
changecharacteristic behavior ba
in stack thick-
on parameter
nesses, as a result combinations.
of different Figure 12
process pressures forshows a comparison
a maximum processoftemperature
the change ofin stack th
100
170 ◦ C. Curves
nesses,
for as a result
stack of different
thickness changeprocess pressures
are displayed asfor
thea average
maximum andprocess temperatur
standard
50 170 five
deviation of the °C. Curves
individual for manufacturing
stack thicknessprocesses.
change are Thedisplayed
effect of as
thethe average
process and standard
pressure
is most pronounced
viation of between
the five0.5 MPa andmanufacturing
individual 1.5 MPa, with processes.
a significant Thedifference in thick-
effect of the process press
0
ness. The manifestation
is most pronouncedof this effect
between might0.5be MPadueandto friction
1.5 MPa,inside
with the yarn anddifference
a significant fabric in th
165 170 175 180ness. when
that is overcome 185manifestation
The pressure 190is increased 195effect
of this beyond 200
0.5be
might MPa.
due Compaction and nesting
to friction inside the yarn and fa
of the yarns and is
that
Temperature fibersinwithin
overcome°C when the textile
pressure structure mightbeyond
is increased be the reason
0.5 MPa. forCompaction
an effect this
and nestin
pronounced. The difference between 1.5 MPa and 2.5 MPa is marginal and can only be
identified in the early Sections (I and II) before the onset of macro-impregnation. This may
Figure 11. Comparison
be dueof measured
to the stackand predicted
being almostviscosity for the considered
fully compacted rPLA remaining
and a limitted based on ancompactibility,
Arrhenius equation.
due to the nesting of the yarns of the textile and polymer stack, for pressures increasing
beyond 1.5 MPa. The different stack thicknesses lead, in turn, to differences in heat conduc-
3.2. Interpretation tion
of Process
throughData
theand B-Factor
stack and a Calculation
delay in the onset of macro-impregnation. The determined
The process data
onsetforof organo sheet manufacturing
macro-impregnation based onshow characteristic
this data behavior
is highlighted basedlines for each
as vertical
pressure. The
on parameter combinations. onset 12
Figure of macro-impregnation
shows a comparisonhas of been colorcoded
the change to show
in stack the influence of
thick-
process pressure.
nesses, as a result of different process pressures for a maximum process temperature of
170 °C. Curves for stack thickness change are displayed as the average and standard de-
viation of the five individual manufacturing processes. The effect of the process pressure
is most pronounced between 0.5 MPa and 1.5 MPa, with a significant difference in thick-
ness. The manifestation of this effect might be due to friction inside the yarn and fabric
that is overcome when pressure is increased beyond 0.5 MPa. Compaction and nesting of
due to the stack being almost fully compacted and a limitted remaining compactibility,
due to the nesting of the yarns of the textile and polymer stack, for pressures increasing
beyond 1.5 MPa. The different stack thicknesses lead, in turn, to differences in heat con-
duction through the stack and a delay in the onset of macro-impregnation. The deter-
mined onset of macro-impregnation based on this data is highlighted as vertical lines for
Polymers 2023, 15, 4357 12 of 22
each pressure. The onset of macro-impregnation has been colorcoded to show the influ-
ence of process pressure.
170 °C; 0.5 MPa 170 °C; 1.5 MPa 170 °C; 2.5 MPa Temperature
10 Onset of macro-impregnation 200
Stack thickness in mm
Temperature in °C
Tm
8 160
6 120
4 80
2 40
I II III IV
0 0
0 200 400 600 800 1000 1200
Time in sec
Figure 12. Comparison of stack thicknesses for processes with a maximum temperature of 170 ◦ C
and different of stack thicknesses for processes with a maximum temperature of 170 °C
process pressures.
and different process pressures.
The most distinct impact that can be identified is that increasing process pressure
led toThe
anmost distinct
earlier onset impact that can be identified
of macro-impregnation; see is that increasing
Figure process
13a. This may pressure led
be attributed to
to
theanpressure-dependent
earlier onset of macro-impregnation;
stack height. Air within see Figure 13a. This
the stack mayheat
reduces be attributed
conduction to and
the
thus delays the onsetstack
pressure-dependent of macro-impregnation.
height. Air within the An increasing
stack reducespressure also led to
heat conduction smaller
and thus
standard
delays thedeviations. This delay caused different
onset of macro-impregnation. temperatures
An increasing pressure within the to
also led stack at thestand-
smaller onset
of macro-impregnation;
ard deviations. This delay seecaused
Figuredifferent
13b. Thetemperatures
temperature within within the
the stack
stack converges
at the onset with
of
the melt temperaturesee
macro-impregnation; determined
Figure 13b. within DSC measurements,
The temperature within theas indicated
stack by the
converges green
with the
line. temperature
melt The differences in temperatures
determined within atDSCthemeasurements,
onset of macro-impregnation
as indicated by can,
theon the other
green line.
hand,
The be attributed
differences to different heat
in temperatures rates
at the for different
onset target temperatures
of macro-impregnation can,of onthe
theprocess.
other
A delay
hand, be in the onset
attributed to of macro-impregnation
different means that
heat rates for different targetdifferent timespans—between
temperatures of the process.
550 and 750 s—are available for the considered process, which
A delay in the onset of macro-impregnation means that different timespans—between has a significant impact550 on
the overall
and 750 s—are impregnation;
available for seethe
Figure 13c. The
considered individual
process, which temperature curves,impact
has a significant as wellonas the
the
differentimpregnation;
overall timespans, cansee beFigure
compared 13c.byThecalculating
individual thetemperature
B-factor for each parameter
curves, as well setting;
as the
see Figure
different 13d. Thecan
timespans, B-factors for these
be compared byprocesses
calculating vary
the over a range
B-factor of values
for each between
parameter set-
three and twenty that also show some overlap between different process
ting; see Figure 13d. The B-factors for these processes vary over a range of values between temperatures and
pressures. The values calculated for the processes of 170 ◦ C, with a pressure of 2.5 MPa,
three and twenty that also show some overlap between different process temperatures
and 185 ◦ C, with
and pressures. The a pressure of 1.5 MPa,
values calculated for are
thecomparable
processes ofwith 170 12.2 and 13.4,
°C, with respectively,
a pressure of 2.5
and have overlapping standard deviations. The B-factor values for 185 ◦ C with 2.5 MPa
MPa, and◦ 185 °C, with a pressure of 1.5 MPa, are comparable with 12.2 and 13.4, respec-
and 200
tively, andChavewithoverlapping
1.5 MPa allow for a similar
standard comparison
deviations. with 19.3
The B-factor andfor
values 19.8,
185respectively.
°C with 2.5
An overview
MPa and 200 °C of corresponding
with 1.5 MPa allow data for
forthese figures
a similar is given inwith
comparison Table 3. and 19.8, respec-
19.3
tively. An overview of corresponding data for these figures is given in Table 3.
Table 3. Comparison of characteristic values determined for different parameter settings.
Table 3. Comparison of characteristic values determined for different parameter settings.
Timespan for
Onset of MI Temp. at
Temperature Pressure Impregnation
Timespan for in B-Factor
in Seconds Onset
Onset of MI in Temp. at Seconds
Temperature Pressure Impregnation in B-Factor
170 ◦ C 0.5 MPa 506Seconds
± 46 168 ±Onset
4 ◦C 550 ± 46 3.1 ± 0.3
Seconds
170 ◦ C 1.5 MPa 439 ± 12 158 ± 2 ◦ C 614 ± 12 8 ± 0.3
170
170 ◦°C
C 0.5MPa
2.5 MPa 415506
± 15± 46 155168
± 3 ±◦ C4 °C 550±± 15
638 46 3.1
12.2±±0.3
1.1
185 ◦ C 0.5 MPa 440 ± 6 172 ± 1 ◦ C 652 ± 6 5.4 ± 0.1
185 ◦ C 1.5 MPa 399 ± 10 162 ± 3 ◦ C 691 ± 10 13.4 ± 0.7
185 ◦ C 2.5 MPa 375 ± 7 154 ± 2 ◦ C 715 ± 7 19.3 ± 0.9
200 ◦ C 1.5 MPa 374 ± 15 165 ± 5 ◦ C 747 ± 15 19.8 ± 2.3
170 °C 1.5 MPa 439 ± 12 158 ± 2 °C 614 ± 12 8 ± 0.3
170 °C 2.5 MPa 415 ± 15 155 ± 3 °C 638 ± 15 12.2 ± 1.1
185 °C 0.5 MPa 440 ± 6 172 ± 1 °C 652 ± 6 5.4 ± 0.1
185 °C 1.5 MPa 399 ± 10 162 ± 3 °C 691 ± 10 13.4 ± 0.7
Polymers 2023, 15, 4357 185 °C 2.5 MPa 375 ± 7 154 ± 2 °C 715 ± 7 19.3 ± 0.9
13 of 22
200 °C 1.5 MPa 374 ± 15 165 ± 5 °C 747 ± 15 19.8 ± 2.3
170 °C 170 °C
Temp. at onset of MI in °C
185 °C 175 185 °C
550 200 °C
Onset of MI in sec
200 °C
170
500
165
450
160
400 Tm
155
350 150
300 145
0 0.5 1.5 2.5 0 0.5 1.5 2.5
Pressure in MPa Pressure in MPa
(a) (b)
170 °C
Timespan for impregn. in sec
750 20 185 °C
700 200 °C
15
B-factor
650
10
600
170 °C
550 185 °C 5
200 °C
500 0
0 0.5 1.5 2.5 0 0.5 1 1.5 2 2.5
(c) (d)
Figure 13. 13.
Figure Influence of process
Influence pressure
of process on the
pressure (a) (a)
on the timespan until
timespan thethe
until onset of macro-impregnation
onset of macro-impregnation
(MI); (b) stack temperature at the onset of macro-impregnation; (c) timespan
(MI); (b) stack temperature at the onset of macro-impregnation; (c) timespan forfor impregnation andand
impregnation
(d) (d)
B-factor for each parameter combination.
B-factor for each parameter combination.
3.3.3.3.
Examination of Physical
Examination Organo
of Physical Sheet
Organo Properties
Sheet Properties
TheThe
chosen
chosen stack setup
stack setupallows for for
allows instant investigation
instant investigationof the apparent
of the apparentimpregnation
impregnation
quality,
quality, after
after thethe demolding
demolding of organo
of organo sheets.
sheets. Molten
Molten polymer
polymer hashas to penetrate
to penetrate the the stacks’
stacks’
outer
outer layers
layers for proper
for proper impregnation,
impregnation, facilitating
facilitating the ruling
the ruling out ofout of unsuitable
unsuitable processprocess
pa-
parameters
rameters for thefor the process
given given process time. 14
time. Figure Figure
shows 14ashows a comparison
comparison of organo ofsheets,
organoman- sheets,
manufactured
ufactured with different
with different parameterparameter combinations,
combinations, onetest
one per per series,
test series, together
together withwith their
their
respective
respective B-factors.
B-factors. This
This comparisonclearly
comparison clearlyindicates
indicates that
that certain parameter
parametercombinations
combina-
areare
tions unsuitable
unsuitablefor fororgano
organosheetsheet manufacturing
manufacturing with with the
theconsidered
consideredprocess
processtime.
time. ForFor
example, ◦ C and 185 ◦ C
example, thethe low-pressure
low-pressure processes
processes withwith maximum
maximum temperatures
temperatures of 170
of 170 °C and 185 °C
show
show drydry spots
spots of considerable
of considerable sizesize along
along thethe
edgeedge of the
of the organo
organo sheet.
sheet. However,
However, while
while
the majority of the surface seems to be impregnated sufficiently, some dry areas can still be
the majority of the surface seems to be impregnated sufficiently, some dry areas can still
identified, for
for170
170°C◦ C and 1.5 MPa, along the edges. The evaluation of the surface quality
be identified, and 1.5 MPa, along the edges. The evaluation of the surface quality
might
might be be
an an adequate
adequate tooltool
forfor initial
initial assessment,
assessment, albeit
albeit a rather
a rather limited
limited one.
one. TheThe figure
figure
therefore
therefore hashas to considered
to be be considered in tandem
in tandem with
with Figure
Figure 15,15, which
which shows
shows an an overview
overview of the
of the
physical properties of the organo sheets that were determined after the manufacturing
process. Figure 15a compares the influence of the different process parameters on the
organo sheet thickness. The comparison to the target thickness—1.9 mm for a theoretical
fiber volume content of 49%—should allow a first assessment of the organo sheets’ porosity.
However, the resulting organo sheet weight has to be considered as well, to account for a
reduced polymer volume content due to the squeeze-out of the molten polymer through
physical properties of the organo sheets that were determined after the manufacturing
process. Figure 15a compares the influence of the different process parameters on the or-
gano sheet thickness. The comparison to the target thickness—1.9 mm for a theoretical
fiber volume content of 49%—should allow a first assessment of the organo sheets’ poros-
Polymers 2023, 15, 4357 14 of 22
ity. However, the resulting organo sheet weight has to be considered as well, to account
for a reduced polymer volume content due to the squeeze-out of the molten polymer
through the tool gap. Weighing the stack before and the organo sheet after the manufac-
the tool
turing gap. enabled
process Weighing the stack before
consideration of thisand theasorgano
effect, depicted sheet after the
in Figure 15b.manufacturing
The squeeze-
process
out enabled
increased withconsideration
both increasing of process
this effect, as depicted
pressure in Figure 15b.
and temperature. The squeeze-out
However, the effect
ofincreased
increasing with both increasing
temperatures process
was more pressure and
pronounced, duetemperature.
to reductionsHowever, theThis
in viscosity. effectre-of
increasing temperatures was more pronounced, due to reductions
sulted in a polymer loss of 28% for the combination of 200 °C and 1.5 MPa. This polymer in viscosity. This resulted
in a polymer loss of 28% for the combination of 200 ◦ C and 1.5 MPa. This polymer loss
loss has an influence on the theoretical thickness of the organo sheet. A second comparison
ofhas
theanthicknesses
influence on the theoretical
measured thickness
for different of the organo
parameter sheet. A
combinations andsecond
their comparison
theoretical
of the thicknesses
counterparts is givenmeasured
in Figurefor different
15c. parameter
The measured combinations
thicknesses are, inandmosttheir theoretical
cases, greater
counterparts
than is given
the theoretical in Figure 15c.
thicknesses, The measured
indicating that the thicknesses
excess volume are,isintaken
most upcases, greater
by pores.
The best agreement with minimal pores was determined to be the combination of 185 The
than the theoretical thicknesses, indicating that the excess volume is taken up by pores. °C
best2.5agreement with ◦ C and
and MPa, with an minimal
average poreporesvolume
was determined
content (PVC)to be ofthe0.16%.
combination
However, of 185
the corre-
2.5 MPa, with
sponding an average
standard deviation poreofvolume
4.39% content
shows some(PVC)limitations
of 0.16%. However, the corresponding
of this approach, overlap-
standard deviation of 4.39% shows some limitations of this
ping into negative volumes. It is furthermore unlikely that natural fiber-reinforced approach, overlapping into
com-
negative volumes. It is furthermore unlikely that natural fiber-reinforced
posites made with thermoplastic polymers can be manufactured without pores. The fiber composites made
with thermoplastic
structure has a hollow polymers
lumen,can and beitmanufactured without
is highly unlikely thatpores. The fiber
the highly structure
viscous has a
polymer
hollow lumen, and it is highly unlikely that the highly viscous polymer
melt completely fills up this volume. However, the theoretical fiber and pore volume con- melt completely
fillscan
tent up be this volume.for
calculated However, the theoretical
each parameter fiber to
combination, and poreavolume
enable contentofcan
further means com- be
calculated for each parameter combination, to enable a further means of comparison. The
parison. The determined values are depicted in Figure 15d. The figure clearly shows de-
determined values are depicted in Figure 15d. The figure clearly shows decreasing PVC
creasing PVC with an increasing pressure. The resulting FVC varies within the range be-
with an increasing pressure. The resulting FVC varies within the range between 37 and
tween 37 and 51 vol. %. The effective FVC and PVC have to be considered when compar-
51 vol. %. The effective FVC and PVC have to be considered when comparing mechanical
ing mechanical properties in the following chapter. Parameter combinations with low
properties in the following chapter. Parameter combinations with low pressures result in
pressures result in lower FVC near 37 vol. %, with a rather high PVC of 25 vol. %. Increas-
lower FVC near 37 vol. %, with a rather high PVC of 25 vol. %. Increasing both the pressure
ing both the pressure and the temperature facilitates a reduction in PVC, to an average of
and the temperature facilitates a reduction in PVC, to an average of 6 vol. % at 1.5 MPa
6 vol. % at 1.5 MPa and 2 vol. % at 2.5 MPa, across all temperatures. A comprehensive
and 2 vol. % at 2.5 MPa, across all temperatures. A comprehensive overview of the data
overview of the data depicted in Figure 15 is given in Table A1.
depicted in Figure 15 is given in Table A1.
Figure 14. Comparison of apparent impregnation qualities with their B-factor.

Polymers 2023, 15, 4357 15 of 22

Figure 14. Comparison of apparent impregnation qualities with their B-factor.
170 °C 170 °C
Polymer loss in weight-%

2.5 185 °C 185 °C
Thickness in mm
200 °C 30% 200 °C
Pores
20%
2
10%
Target
thickness Squeeze out
1.5 0%
0 0.5 1.5 2.5 0 0.5 1.5 2.5
(a) (b)
170 °C FVC 185 °C FVC 200 °C FVC
measured theoretical
Fiber and pore volume content

170 °C PVC 185 °C PVC 200 °C PVC
2.75
170 °C 185 °C 200 °C 50% F
Thickness in mm
2.5 V
40% C
2.25
30%
2
20% P
V
1.75 10% C
1.5 0%
0.5 1.5 2.5 0.5 1.5 2.5 1.5 0 0.5 1.5 2.5
Pressure in MPa
Pressure in MPa
(c) (d)
Figure 15. (a)
Figure 15.Measured organo
(a) Measured sheet
organo thickness
sheet in comparison
thickness with
in comparison target
with targetthickness;
thickness;(b)
(b)polymer
polymer loss
loss due to squeeze-out through the tool gap; (c) comparison of measured and theoretical
due to squeeze-out through the tool gap; (c) comparison of measured and theoretical organo organosheet
sheet thickness based on its weight; (d) theoretical fiber and pore volume content based on organo
thickness based on its weight; (d) theoretical fiber and pore volume content based on organo sheet
sheet weight and thickness.
weight and thickness.
3.4. Bending Properties

3.4. Bending Properties
Bending
Bendingmoduli
moduli andandstrengths
strengths of of
the
themanufactured
manufacturedorgano organo sheets, together with
sheets, together withtheir
theirfiber
fibervolume
volumecontent,
content, areare presented
presented in Figure
in Figure 16. 16.
As As discussed
discussed earlier,
earlier, the process
the process pressure
pressure in particular
in particular has ahas a distinct
distinct effecteffect
on theonfiber
the fiber
volumevolume
contentcontent
of theoforgano
the organo sheets,
sheets, resulting
resulting
in two in groups
two groups of values.
of values. TheThe organo
organo sheets
sheets manufactured
manufactured with
with a apressure
pressureofof0.5
0.5MPa
MPadisplayed
displayedlow lowbending
bendingmoduli,
moduli,with withvalues
valuesbarely
barelycompeting
competingwith withthetheunreinforced
unreinforcedrPLA.
rPLA. Specimens
Specimens forfor bending
bending tests
tests were were
cutcut
from from
the the
areaarea in organo
in the the organosheetsheet
wherewhere the
the polymer
polymer penetrated
penetrated the top thelayers—predominantly
top layers—predominantly dry areas
dry areas werewere not tested.
not tested. The values
The values increase
when
increase pressure
when increases
pressure to 1.5toMPa
increases and and
1.5 MPa 2.5 MPa, especially
2.5 MPa, withwith
especially process temperatures
process temper- of
170of◦ C.
atures 170For
°C.temperatures
For temperatures of 185of ◦ C, this effect is only comparable for pressures of 1.5 MPa,
185 °C, this effect is only comparable for pressures
of 1.5albeit
MPa,less so than
albeit less for 170 ◦ for
so than C. A170 further
°C. Aincrease
further to 2.5 MPa
increase toled
2.5toMPa
a reduction
led to a in the bending
reduction
in themodulus
bendingtomodulus
the leveltoofthethelevel
unreinforced rPLA. The rPLA.
of the unreinforced effect of
Theprocess temperature
effect of process tem-can be
identified
perature can bewhen comparing
identified when the organo the
comparing sheets manufactured
organo at 1.5 MPa at
sheets manufactured highlighted
1.5 Mpa in
light yellow. Even though ◦ C is the lowest considered process temperature, it resulted
170though
highlighted in light yellow. Even 170 °C is the lowest considered process temper-
ature,initthe highestinvalues
resulted for this
the highest specific
values pressure
for this level
specific for bending
pressure moduli,
level for andmoduli,
bending the highest
bending strength with 51 ±
and the highest overall bending strength with 51 ± 4 MPa. However, the overlap in stand- for
overall 4 MPa. However, the overlap in standard deviations
170 ◦ C withfor
ard deviations 1.5170
MPa °Cand
with2.51.5MPa
MPaprevent
and 2.5the determination
MPa prevent the of significant differences.
determination of signifi- The
reduction in both bending modulus and strength with an increasing
cant differences. The reduction in both bending modulus and strength with an increasing temperature might
be related to the oxidization and degradation of the matrix polymer in air [44,46–48]. This
leads to drastically reduced bending moduli, at 2.1 GPa—60% of the raw material—and
Polymers 2023, 15, 4357 16 of 22

temperature might be related to the oxidization and degradation of the matrix polymer in
air [44,46–48]. This leads to drastically reduced bending moduli, at 2.1 GPa—60% of the
raw material—and bending strengths as low as 20 MPa. Even though bending moduli
bending
showed strengths
a moderate as low as 20effect
reinforcement MPa.withEven thoughvalues
elevated bendingthatmoduli showed
were 30% a moderate
higher than
reinforcement
the raw material, iteffect
was with elevatedto
not possible values thatawere
achieve 30% highereffect
reinforcement than the
whenrawconsidering
material, it was
not possible
bending to achieve
strengths. Similar aeffects
reinforcement
have been effect when in
reported considering bending
the literature and strengths.
may be con-Similar
effects have been reported in the literature
nected to limited fiber–matrix adhesion [36–38]. and may be connected to limited fiber–matrix
adhesion [36–38].
σB-max_rPLA = 100 MPa
Bending modulus EB in GPa
Bending strength σB-max in MPa

1.5 MPa
1.5 MPa
5 T↑ 50 2.5 MPa
4 EB_rPLA 40
T↑
3 2.5 MPa 30 0.5 MPa
0.5 MPa T↑ T↑
2 20
1 10
170 °C 185 °C 200 °C 170 °C 185 °C 200 °C
0 0
35% 40% 45% 50% 35% 40% 45% 50%
Fiber volume content Fiber volume content
(a) (b)
Figure 16. (a)
Figure 16.Bending moduli
(a) Bending and and
moduli (b) bending strengths,
(b) bending compared
strengths, to to
compared effective fiber
effective volume
fiber volumecon-
content.
tent.
It was discussed earlier that especially low pressures lead to high pore volume content
It was
and, discussed
thus, earlier
a reduced that especially
mechanical low pressures
performance. lead toset
An additional high poreorgano
of five volume con- was
sheets
tent and, thus, a reduced
manufactured, with mechanical
presumablyperformance. An additional
the optimal process set ofof
conditions five
170 ◦ C and
organo sheets
1.5 MPa,
was tomanufactured, with presumably
identify the effect of pore volume the optimal
content.process conditions
Additional polymerof 170was°Cadded
and 1.5 to the
MPa,stack—17
to identify the effect of pore volume content. Additional polymer was
g instead of the initial 9.3 g—to produce an organo sheet with a fiber volume added to the
stack—17
contentg instead
of 37%. ofThetheevaluation
initial 9.3 of
g—to
stackproduce
thickness anandorgano sheetsqueeze-out
polymer with a fiber showed
volume that
the of
content pore
37%.volume content could
The evaluation be reduced
of stack thicknesstoand5%.polymer
Both bending modulus
squeeze-out and strength
showed that
increased,
the pore volume compared to thebe
content could values determined
reduced to 5%. Bothin the first test
bending series. and
modulus A B-factor
strengthvalue
of 8.7 ±
increased, 0.3 was determined
compared to the valuesfor the corresponding
determined in the firstprocess. The A
test series. corresponding
B-factor valueB-factor
of
values for the process pressure and temperatures of 0.5 MPa and 170 ◦ C, and 185 ◦ C, were
8.7 ± 0.3 was determined for the corresponding process. The corresponding B-factor values
for the
Polymers 2023, 15, x FOR PEER REVIEW
± 0.3 and
3.1process 5.4 ± 0.1,
pressure and respectively.
temperaturesThis comparison
of 0.5 MPa and 170 is depicted in Figure
°C, and 185 °C, were 17.3.1
The± colored
17 0.3
of 23
arrows alongside the horizontal dashed lines illustrate the increase
and 5.4 ± 0.1, respectively. This comparison is depicted in Figure 17. The colored arrows in bending modulus
and strength
alongside that wasdashed
the horizontal achieved by application
lines illustrate the of the optimized
increase processmodulus
in bending design. and
strength that was achieved by application of the optimized process design.
BendingModulus
Bending modulus BendingStrength
Bending strength Pore volume content
Pore volume content in %
5 50
4 40
3 30
2 20
Reduction in
pore volume content
1 10
0 0
170
170 °C
°C - 0.5
0.5 MPa
MPa 185
185 °C
°C - 0.5
0.5 MPa
MPa 170
170 °C
°C - 1.5
1.5 MPa
MPa
Figure 17. Effect of pore volume content on bending properties for a FVC of 37%.
The comparison of bending properties with the corresponding B-factor is presented

in Figure 18. The effect of increasing B-factor on the bending moduli results in a parabolic
course, with the zenith at a value of 12. A similar course can be described when bending
strength is considered. The peak is slightly earlier, at a B-factor value of 10. The effect of
temperature is distinct when comparing bending strengths at similar B-factors. This fur-
B
0 0
170
170 °C
°C - 0.5
0.5 MPa
MPa 185
185 °C
°C - 0.5
0.5 MPa
MPa 170
170 °C
°C - 1.5
1.5 MPa
MPa
Polymers 2023, 15, 4357 17 of 22
The comparison of bending properties with the corresponding B-factor is presented

in Figure 18. The effect of increasing B-factor on the bending moduli results in a parabolic
The the
course, with comparison
zenith atofabending
value ofproperties with course
12. A similar the corresponding B-factorwhen
can be described is presented
bending in
Figure 18. The effect of increasing B-factor on the bending moduli results in a parabolic
strength is considered. The peak is slightly earlier, at a B-factor value of 10. The effect of
course, with the zenith at a value of 12. A similar course can be described when bending
temperature is distinct when comparing bending strengths at similar B-factors. This fur-
strength is considered. The peak is slightly earlier, at a B-factor value of 10. The effect
ther highlights the necessity of considering the specific polymer behavior, even though
of temperature is distinct when comparing bending strengths at similar B-factors. This
the impregnation performance expressed by the B-factor might be of equal value. It might
further highlights the necessity of considering the specific polymer behavior, even though
therefore be preferential
the impregnation to increaseexpressed
performance impregnation performance
by the through
B-factor might be ofincreases in theIt
equal value.
impregnation time, for
might therefore bio-based polymers
be preferential with
to increase thermal sensitivity.
impregnation Thethrough
performance effect ofincreases
increas-
ing temperature
in the impregnation time, for bio-based polymers with thermal sensitivity. The effectB-
(T↑) is highlighted in Figure 18b) for bending strengths with equal of
factors values. temperature (T↑) is highlighted in Figure 18b) for bending strengths with equal
increasing
B-factors values.

5 50 T↑
4 40
3 30 T↑
2 20
1 10
170 °C 185 °C 200 °C 170 °C 185 °C 200 °C
0 0
0 5 10 15 20 0 5 10 15 20
B-factor B-factor
(a) (b)
Figure 18. (a)
Figure 18.Bending modulus
(a) Bending andand
modulus (b) (b)
bending strengths
bending compared
strengths totoB-factors
compared B-factorsfor
foreach
eachprocess.
process.
The The presented

presented datadata show
show thatthe
that themechanical
mechanical performance
performanceofofthe manufactured
the manufactured organo
or-
ganosheets
sheetsdecreases
decreaseswith increasing
with temperatures.
increasing However,
temperatures. However,the data
thedo notdo
data allow
notthe definite
allow the
attribution
definite of this
attribution behavior
of this to degradation
behavior of the
to degradation of fiber or the
the fiber or matrix, sincesince
the matrix, both both
PLA
and hemp fibers may experience thermal degradation during the process.
PLA and hemp fibers may experience thermal degradation during the process. Therefore, Therefore, an
additional test series focused on manufacturing hemp fiber-reinforced organo sheets with a
an additional test series focused on manufacturing hemp fiber-reinforced organo sheets
polypropylene matrix. The press processes were identical to those for hemp–rPLA organo
with a polypropylene matrix. The press processes were identical to those for hemp–rPLA
sheets, with temperatures of 170 ◦ C, 185 ◦ C and 200 ◦ C at a pressure of 1.5 MPa. An
organo sheets, with temperatures of 170 °C, 185 °C and 200 °C at a pressure of 1.5 MPa.
additional temperature level, at 215 ◦ C, was added to investigate the effect of further
An additional
increasing temperature level, at 215on°C,
the process temperature was added
thermal to investigateIt the
fiber degradation. can effect of further
be assumed that
the PP matrix does not experience thermal degradation within the considered temperature
range, which allows us to draw conclusions regarding the degradation of fiber components.
Figure 19 shows the temperature influence on bending moduli and strength for hemp–rPLA
and hemp–PP organo sheets. As discussed earlier, hemp–rPLA organo sheets show a
distinct reduction in bending properties with increasing temperatures. This behavior was
not determined for hemp–PP organo sheets, which should allow the conclusion that the
decrease in hemp–rPLA properties can be predominantly attributed to thermal degradation
in matrix properties, rather than the damaging of natural fibers. An indicator for the
occurring thermal fiber damage might be recognizable by the comparison of hemp–PP
organo sheets manufactured at 200 ◦ C and 215 ◦ C. The average values for bending modulus
and strength are slightly lower for 215 ◦ C compared to 200 ◦ C. Even though this effect can
not be described as significant, due to an overlap in standard deviation, it might hint at a
performance reduction due to degradation of lignin and pectin within the hemp fiber.
mal degradation in matrix properties, rather than the damaging of natural fibers. An in-
dicator for the occurring thermal fiber damage might be recognizable by the comparison
of hemp–PP organo sheets manufactured at 200 °C and 215 °C. The average values for
bending modulus and strength are slightly lower for 215 °C compared to 200 °C. Even
though this effect can not be described as significant, due to an overlap in standard devi-
Polymers 2023, 15, 4357 ation, it might hint at a performance reduction due to degradation of lignin and pectin 18 of 22
within the hemp fiber.
Hemp-PLA
Hemp-PLA Hemp-PP Hemp-PLA
Hemp-PLA Hemp-PP
Hemp-PP

5 60
50
4
40
3
30
2
20
1 10
0 0
170 °C 185 °C 200 °C 215 °C 170 °C 185 °C 200 °C 215 °C
(a) (b)
Figure of temperature
19. Comparison influence
of temperature in hemp–rPLA
influence and hemp–PP
in hemp–rPLA organo sheets
and hemp–PP organoon (a) on
sheets
bending modulus and (b) bending strength.
(a) bending modulus and (b) bending strength.
3.5. Consideration
3.5. Consideration of Natural
of Natural FiberFiber Morphology
Morphology
As discussed
As discussed in theinintroduction
the Section 1,section,
the morphology
the morphologyand properties of natural
and properties fibers may
of natural
fiberswidely vary. This
may widely might
vary. Thisbemight
due tobe different
due to factors,
different such as their
factors, positions
such as theirwithin the plant
positions
stem—with decreasing diameter towards the top end—and
within the plant stem—with decreasing diameter towards the top end—and climatic in- climatic influences during
plant growth and retting—especially considering the separation
fluences during plant growth and retting—especially considering the separation of tech- of technical fiber bundles.
nicalFigure 20 showsFigure
fiber bundles. an excerpt of a microsection,
20 shows an excerpt of taken from a hemp–rPLA
a microsection, taken from organo sheet. The
a hemp–
rPLAmicrosection
organo sheet. wasTheprepared
microsectionon specimens
was prepared after on
three point bending
specimens tests.point
after three Different
bend-areas
within
ing tests. the microsection
Different areas within are the
highlighted
microsectionto differentiate
are highlightedbetween fibers oriented
to differentiate in parallel
between
fibers oriented in parallel (green) and perpendicular (blue) to the picture plane, areas of and
(green) and perpendicular (blue) to the picture plane, areas of pure polymer (yellow)
purethe polyester
polymer twine
(yellow) andused
the to stabilizetwine
polyester the stable
used to fiber yarn the
stabilize (purple). This yarn
stable fiber twine(pur-shows a
constant diameter in each fiber of approximately 20 microns
ple). This twine shows a constant diameter in each fiber of approximately 20 microns and and can therefore be used
can therefore be used as a reference scale for comparison. Natural fibers oriented perpen-plane
as a reference scale for comparison. Natural fibers oriented perpendicular to the
(blue)
dicular show
to the a high
plane variance
(blue) show in bothvariance
a high fiber diameters
in both andfibershape. The figure
diameters also has
and shape. Thesome
areas of interest outlined in white circles. These areas will be
figure also has some areas of interest outlined in white circles. These areas will be used toused to discuss challenges
with
discuss regard towith
challenges natural
regardfibers as a continuous
to natural fibers as areinforcement structure. Area
continuous reinforcement I focusses
structure.
Area I focusses on clusters of fibers with moderate diameters ranging between 45 and 70 The
on clusters of fibers with moderate diameters ranging between 45 and 70 microns.
highlighted
microns. fibers show
The highlighted some
fibers showseparation lines, although
some separation it is not possible
lines, although it is not to distinguish
possible to if
distinguish if these are separate fibers or single fibers with cracks due to damaging. Hempwith
these are separate fibers or single fibers with cracks due to damaging. Hemp fibers
smaller diameters and distinct separation are also visible in the direct vicinity. Area II
highlights two large clusters of fibers with a quasi-concentric arrangement. This could be a
technical fiber bundle that is not separated completely, resulting in an elliptical cluster with
a diameter between 180 and 200 microns for the inner and between 230 and 250 microns for
the outer circle. Area III highlights a smaller cluster of elementary fibers with a diameter
between 100 and 120 microns. Area IV highlights fibers with large diameters, similar to
area I; however, the area is dominated by large fiber diameters rather than a mixture of
large and small diameters. Finally, area V highlights an incompletely separated fiber bundle
that resulted in an elongated ellipsis with an aspect ratio of six: one between the major and
minor axes. These high variances might hinder exploitation of the full potential of natural
fibers for structural applications.
250 microns for the outer circle. Area III highlights a smaller cluster of elementary fibers
with a diameter between 100 and 120 microns. Area IV highlights fibers with large diam-
eters, similar to area I; however, the area is dominated by large fiber diameters rather than
a mixture of large and small diameters. Finally, area V highlights an incompletely sepa-
rated fiber bundle that resulted in an elongated ellipsis with an aspect ratio of six: one
Polymers 2023, 15, 4357 19 of 22
between the major and minor axes. These high variances might hinder exploitation of the
full potential of natural fibers for structural applications.
Figure20.
Figure 20.Microsection
Microsectionof
ofhemp–rPLA
hemp–rPLAorgano
organosheet.
sheet.
4.4.Discussion
Discussion
The
The production
production of of organo
organosheets
sheetsasasa semi-finished
a semi-finished product
product is aiscomplex
a complex process
process with
with many influences. Process optimization is even more challenging
many influences. Process optimization is even more challenging when conventional pet- when conventional
petrol-based polymers
rol-based polymers andand synthetic
synthetic fibers
fibers areare substituted
substituted withwith recycled
recycled andand bio-based
bio-based ma-
materials, like hemp fibers or recycled PLA. Investigating the melt
terials, like hemp fibers or recycled PLA. Investigating the melt behavior of recycled behavior of recycled
PLA
PLA in DSC showed ◦
in DSC showed thatthat maximum
maximum process
process temperatures
temperatures should
should at least
at least be be
setset
to to 170
170 °C Cto
to facilitate
facilitate thethe total
total dissolution
dissolution of crystalline
of crystalline structures.
structures. However,
However, meltmelt viscosity
viscosity at tem-
at this this
temperature
perature is quiteis quite
high,high,
at 290at Pa∙s.
290 Pa
The·s.usual
The approach
usual approach to reduce
to reduce melt viscosity
melt viscosity in thermo-in
thermoplastic polymers
plastic polymers is to increaseis to increase the temperature. This results in a drastic
the temperature. This results in a drastic viscosity reduction viscosity
reduction Pa·°C ◦ C and to 32 Pa·s at 200 ◦ C. This reduction in viscosity facilitates
to 95 Pa∙stoat95185 s atand
185 to 32 Pa∙s at 200 °C. This reduction in viscosity facilitates fiber
fiber impregnation,
impregnation, but also
but also leadsleads
to antoincreasing
an increasing polymer
polymer squeeze-out,
squeeze-out, of to
of up up30%to 30% of
of the
the initial polymer weight, through the tool gap. The presented results also show a distinct
initial polymer weight, through the tool gap. The presented results also show a distinct
correlation between an increasing temperature and a decreasing performance in bending
correlation between an increasing temperature and a decreasing performance in bending
tests. A comparison of different matrix polymers showed that the reduced performance can
tests. A comparison of different matrix polymers showed that the reduced performance
be attributed to the thermal degradation of the recycled PLA, rather than the degradation
can be attributed to the thermal degradation of the recycled PLA, rather than the degra-
of fiber components. It might be advantageous to increase impregnation performance
dation of fiber components. It might be advantageous to increase impregnation perfor-
based on the B-factor value by extending hold time at the maximum process temperature
mance based on the B-factor value by extending hold time at the maximum process tem-
of 170 ◦ C. This may allow for a higher degree of micro-impregnation and reduce the pore
perature of 170 °C. This may allow for a higher degree of micro-impregnation and reduce
volume content below the average of 5%. The investigation of bending properties showed
the pore volume content below the average of 5%. The investigation of bending properties
further limitations with regard to the exploitation of the properties of natural fibers as
showed further limitations with regard to the exploitation of the properties of natural fi-
a reinforcement structure. While it was possible to achieve a reinforcement effect for a
bers as a reinforcement structure. While it was possible to achieve a reinforcement effect
bending moduli of 39% compared to the raw polymer, it was not possible to increase the
for a bending
bending strength moduli
beyondof 39% compared
a level of 50% of to the
the raw
raw material.
polymer,This
it was not possible
limitation withtoregard
increase
to
natural fiber reinforcement of PLA is in accordance with the available literature and might
be overcome by treatment of the fibers, to allow for a better fiber–matrix adhesion. The
variance in fiber separation and diameter have to be considered, together with performance
limitations such as the variance in mechanical properties due to environmental influences,
as well as limited fiber–matrix adhesion. In particular, differences in diameter might limit
the performance, for example, when smaller fibers tear at a lower force or fiber–matrix
adhesion fails for large surface fibers.
and might be overcome by treatment of the fibers, to allow for a better fiber–matrix adhe-
sion. The variance in fiber separation and diameter have to be considered, together with
performance limitations such as the variance in mechanical properties due to environmen-
tal influences, as well as limited fiber–matrix adhesion. In particular, differences in diam-
eter might limit the performance, for example, when smaller fibers tear at a lower force or
Polymers 2023, 15, 4357 fiber–matrix adhesion fails for large surface fibers. 20 of 22
Author Contributions: Conceptualization, M.S.; data curation, M.S.; formal analysis, M.S.; funding
acquisition, F.G.; investigation, M.S.; methodology, M.S.; project administration, P.M.; resources,
Author Contributions: Conceptualization, M.S.; data curation, M.S.; formal analysis, M.S.; funding
M.S.; supervision, F.G.; validation, M.S.; writing—original draft, M.S.; writing—review and editing,
acquisition, F.G.; investigation, M.S.; methodology, M.S.; project administration, P.M.; resources, M.S.;
F.G. and P.M. All authors have read and agreed to the published version of the manuscript.
supervision, F.G.; validation, M.S.; writing—original draft, M.S.; writing—review and editing, F.G.
Funding:
and The
P.M. All projecthave
authors Durobast is funded
read and agreedbyto the published
Federal Ministry
versionofofFood and Agriculture on the
the manuscript.
basis of a decision by the German Bundestag (funding reference: 2220NR090C).
Funding: The project Durobast is funded by the Federal Ministry of Food and Agriculture on the
DataofAvailability
basis a decision byStatement:
the GermanTheBundestag
data presented in this
(funding study are
reference: available on request from the
2220NR090C).
corresponding author.
Data Availability Statement: The data presented in this study are available on request from the
Conflicts of Interest:
corresponding author.All authors were employed by Leibniz-Institute für Verbundwerkstoffe GmbH
in Kaiserslautern, Germany and declare that the research was conducted in the absence of any com-
Conflicts
mercial oroffinancial All authors were
Interest:relationships employed
that could by Leibniz-Institute
be construed für
as a potential Verbundwerkstoffe
conflict of interest. GmbH
in Kaiserslautern, Germany and declare that the research was conducted in the absence of any
commercial
Appendixor A financial relationships that could be construed as a potential conflict of interest.
Appendix A
Integral 781.96 mJ
Integral 769.99 mJ Standardized 95.36 J/g
Standardized 93.9 J/g Peak 120.82 °C
Peak 120.92 °C
Crystallization
during cooling step
Heating
Heating
Cooling Cooling
Dissolution of
crystalline structure
during melting Integral -768.38 mJ
Integral -669.68 mJ Standardized -93.7 J/g
Standardized -81.67 J/g Peak 162.3 °C
Peak 166.42 °C
FigureA1.
Figure A1.DSC
DSC curve
curve for
for polypropylene
polypropylene Borealis
Borealis bj100hp
bj100hp with
with distinct
distinct recrystallization
recrystallizationbehavior
behavior
during cooling, modified based on [51].
during cooling, modified based on [51].
Table A1. Raw data supplementing Figure 15.
Table A1. Raw data supplementing Figure 15.
Measured Thick- Theoretical Thick- Polymer Weight Pore Volume Fiber Volume
Temp. Pressure
Measured Theoretical
Temp. Pressure ness ness
Polymer Weight Loss Loss
Pore Content
Volume Content Content
Fiber Volume Content
Thickness Thickness
in mm in %
in mm in %
170 °C 0.5 MPa 2.46 ± 0.06 1.85 ± 0.02 2.3 ± 0.2 24.8 ± 1.3 37.2 ± 0.9
◦C
170170 0.5 MPa 2.46 ± 0.06 1.85 ± 0.02 2.3 ± 0.2 24.8 ± 1.3 37.2 ±±0.90.9
°C 1.5 MPa 2.01 ± 0.03 1.86 ± 0.01 2.4 ± 0.4 7.4 ± 1.5 46
170 ◦ C 1.5 MPa 2.01 ± 0.03 1.86 ± 0.01 2.4 ± 0.4 7.4 ± 1.5 46 ± 0.9
170 ◦ C 2.5 MPa 1.93 ± 0.03 1.85 ± 0.03 4.7 ± 1.6 4.2 ± 1.2 47.9 ± 0.7
185 ◦ C 0.5 MPa 2.45 ± 0.04 1.84 ± 0.01 2.9 ± 2.6 24.6 ± 1.2 37.4 ± 0.5
185 ◦ C 1.5 MPa 1.98 ± 0.06 1.85 ± 0.03 6.2 ± 2.7 6.6 ± 2.8 46.6 ± 0.9
185 ◦ C 2.5 MPa 1.82 ± 0.03 1.82 ± 0.06 16.5 ± 7.5 0.16 ± 4.4 50.6 ± 1
200 ◦ C 1.5 MPa 1.91 ± 0.05 1.83 ± 0.03 28 ± 5.5 3.5 ± 2.4 47.6 ± 1.3
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Leibniz-Institut für Verbundwerkstoffe GmbH, Erwin-Schroedinger-Strasse 58, 67663 Kaiserslautern, Germany

Citation: Salmins, M.; Gortner, F.;

Polymers 2023, 15, 4357. https://doi.org/10.3390/polym15224357 https://www.mdpi.com/journal/polymers

Polymers 2023, 15, 4357 2 of 22

Fiber bundle Elementary fiber

t<0 t≈0 t < timp t > timp t = tfinal

Initial state Macro-impregnation Micro-impregnation

Initial state Macro-impregnation Micro-impregnation

Hemp rPLA Textile and polymer

Active cooling unit Tool with

Press tool for organo 50 mm Textile stack

Table 2. Process parameter for manufacturing of hemp fiber-reinforced organo sheets.

Heating Hold time Cooling

2.4. Consideration of Physical Organo Sheet Properties

Figure 10. DSC curve recorded during differential scanning calorimetry.

A comparison of the viscosities measured and predicted for the considered PL

Figure 14. Comparison of apparent impregnation qualities with their B-factor.

Polymers 2023, 15, 4357 15 of 22

Polymer loss in weight-%

Fiber and pore volume content

3.4. Bending Properties

Polymers 2023, 15, 4357 16 of 22

Bending strength σB-max in MPa

Pore volume content in %

The comparison of bending properties with the corresponding B-factor is presented

The comparison of bending properties with the corresponding B-factor is presented

Bending strength σB-max in MPa

The The presented

Bending strength σB-max in MPa

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