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Microstructure Sphericity Hard Foams IMP

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Prudhvi Gogineni
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© © All Rights Reserved
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Composites: Part A 188 (2025) 108515

Contents lists available at ScienceDirect

Composites Part A
journal homepage: [Link]/locate/compositesa

Pulp fibre foams: Morphology and mechanical performance


Markus Wagner a,1 , Veronika Biegler b,1, Sebastian Wurm a , Georg Baumann a, Tiina Nypelö d,e,
Alexander Bismarck b,c , Florian Feist a,*
a
Vehicle Safety Institute, Graz University of Technology, Inffeldgasse 13/6, 8010 Graz, Austria
b
Institute of Materials Chemistry, Faculty of Chemistry, University of Vienna, Währinger Straße 42, 1090 Vienna, Austria
c
Department of Chemical Engineering, Imperial College London, South Kensington Campus, London SW7 2AZ, United Kingdom
d
Department of Chemistry and Chemical Engineering, Chalmers University of Technology, Kemigården 4, 412 58 Gothenburg, Sweden
e
Department of Bioproducts and Biosystems, Lignocellulose Chemistry, Aalto University, Puunjalostustekniikka 1, 00076 AALTO, Finland

A R T I C L E I N F O A B S T R A C T

Keywords: Cellulose (pulp) fibre foams serve as bio-based alternative to fossil-based cellular lightweight materials. The
Fibre foams mechanical properties of cellulose fibre foams are inferior compared with traditional polymer foams and
Cellulose available information is often limited to compression properties. We present a comprehensive analysis of cel­
Production
lulose fibre foams with densities ranging from 60 to 130 kg/m3, examining their compression, tensile, flexural,
Mechanical properties
Morphology
and shear properties. Key findings include a high mean zenithal fibre angle which decreases with increasing
density, as well as a high strain rate amplification (SRA) in compressive strength, which also decreases with
increasing density. With respect to formulation, the addition of carboxymethyl cellulose (CMC) enhanced fibre
dispersion, bubble homogeneity of the wet foam, and dimensional stability of the end-product.
These results provide a foundation for numerical models and advance the understanding of cellulose pulp fibre
foams, highlighting their potential for certain applications.

1. Introduction plant fibre materials [8], and cellulosic fibre foams manufactured as
potential eco-friendly alternatives [9].
The demand for lightweight materials for various structural, thermal, Pulp fibre foams have received significant interest [10–12]. The
and acoustic insulation applications is pertinent and driven by the need production of porous materials directly from cellulose pulp fibres offers
for improved energy efficiency achieved by lightweighting [1]. Light­ a cost-effective alternative to structural foams. Pulp fibres with di­
weighting is currently realised by the utilization of polymer or metal mensions of 1–3 mm in length and 15–28 µm in diameter [13],
foams either on their own or as core material in sandwich composites. depending on their origin, often serve as raw material for production of
Structural foams are attractive because of their high specific strength, microfibrillated cellulose (MFC) and cellulose nanofibrils (CNF) by
energy absorption potential, and favourable (thermal and acoustic) mechanical, chemical (HCl hydrolysis) or enzymatic disintegration [14].
insulation properties [2–4]. The environmental impact associated with Nanocellulose-based foams account for a large proportion of cellulose
these foam materials, includes significant CO2 emissions during pro­ foams [15]. However, the costly production of CNF requiring high en­
duction, raw material scarcity, and the generation of microplastics at the ergy input renders them an economically unfavourable solution to
end of their lifecycle, which prompted an increased interest in sustain­ replace low-cost polymer foams [16].
able alternatives [5,6]. While fossil-based foams offer ease of production Pulp fibre foams are commonly produced by incorporating air into
and cost-effectiveness, particularly for packaging and low-cost struc­ aqueous fibre suspensions containing suitable surfactants to stabilise the
tural applications, the pursuit for sustainable alternatives has led to the liquid froth. The fibre froth is moulded, the suspension medium drained
exploration of mycelium-based composites [7], pressed non-woven and the froth dried, resulting in pulp fibre foams with adjustable

Abbreviations: CMC, carboxymethyl cellulose; SRA, strain rate amplification; MFC, microfibrillated cellulose; CNF, cellulose nanofibrils; CTMP, chemi-thermo­
mechanical-pulp; BSKP, bleached softwood kraft pulp; SR, Schopper Riegler; SDS, sodium dodecyl sulphate; SEM, scanning electron microscopy; µCT, micro-
computed tomography; EPS, expanded polystyrene; EPP, expanded polypropylene.
* Corresponding author.
E-mail address: [Link]@[Link] (F. Feist).
1
Authors contributed equally.

[Link]
Received 5 August 2024; Received in revised form 25 September 2024; Accepted 7 October 2024
Available online 9 October 2024
1359-835X/© 2024 The Authors. Published by Elsevier Ltd. This is an open access article under the CC BY license ([Link]
M. Wagner et al. Composites Part A 188 (2025) 108515

properties depending on the additives used [10,17–20]. Additives are


± 1.2 SR. The fibre length (length weighted average, lf) was determined
used to improve the common issues of cellulose based materials, such as
using the L&W Fibre Tester Plus, ABB (Switzerland) in the wet state
their flammability [20,21], hydrophilicity [18] and poor mechanical
(Table S1). Sodium-carboxymethylcellulose (CMC, MW 250 000) and
properties of low-density foams [20,22]. Foam materials are mainly
the anionic surfactant sodium dodecyl sulphate (SDS, ≥ 99 %) were
characterised by their mechanical properties under compression, in
purchased from Sigma Aldrich and used as received.
addition to their density and morphology. The behaviour of fibrous
foams in compression has been intensively studied [11] to determine
their modulus and strength, with a view to optimizing the structure of 2.2. Manufacturing of pulp fibre foams
fibre networks. Ketoja et al. [23] described the failure mechanism of
well-bonded 3D networks (foams) of chemi-thermomechanical-pulp The pulp sheets were dispersed according to TAPPI standard T-200:
(CTMP), bleached softwood kraft pulp (BSKP) and a weakly bonded m in a valley beater (FRANK PTI, Germany). After the dispersion process
network formed by viscose and CNF. They state that under compressive in the valley beater, aqueous pulp fibre solutions were dewatered to pulp
loading, the central deformation mechanism is fibre buckling. A lower fibre content of 10 wt%. CMC (5 wt% in water) functioning as a viscosity
foam density, implying a longer segment length with fewer inter-fibre modifier and dispersing agent in the wet foam, was mixed using a
crossings, results in weaker structural response. If fibre segments are kitchen mixer equipped with a whisking head (1000 W, Kenwood, UK).
not strengthened by other fibres, the structure cannot withstand applied Before frothing, SDS (0.5 wt% with respect to the dry fibre weight) was
loads. To gain further insights into the mechanical response of bonded added. Depending on the desired density, the pulp solution was frothed
fibre networks, Bergström et al. [24] studied uniaxial compression of until the target density was reached. After frothing, the fibre froth was
non-bonded air-laid southern pine pulp fibres networks. The synergistic transferred into an open polyoxomethylene mould (310 mm (x), 310
effect of fibres bonded via elasto-plastic contacts and fibre–fibre adhe­ mm (y), and 20 mm (z). During production, gravity acts in the negative z
sion led to greater non-reversible deformations compared to networks direction.) and dried in a laboratory oven at 80 ◦ C for 8–12 h. The foam
comprising only elasto-plastic fibre contacts. Pöhler et al. [22] produced was considered dry when a moisture content below 10 wt% was
BSKP and hemp fibre networks bonded with polymeric additives (locust reached. The foam plates were stored at ~25 ◦ C at ~40 %RH prior to
bean gum and polyvinyl alcohol), CNF, and paper fines. Their primary characterisation.
objective was to enhance fibre–fibre bond strength, particularly by
increasing the inter-fibre contact areas. Polymeric components, partic­ 2.3. Foam morphology
ularly polyvinyl alcohol, were shown to provide the most significant
strength improvements. Measured compression properties deviated Scanning electron microscopy (SEM) (JCM-6000, JEOL, Germany)
from theoretical predictions made using Sampson’s unified theory for was used to investigate the foam morphology. The SEM was operated at
statistics of flocculated and random fibre networks [25]. While such an acceleration voltage of 10 kV using a secondary electron detector.
approaches based on Sampson’s theory show promise, further refine­ Prior to imaging, all samples were fixed with carbon tape to a sample
ment is necessary to enhance their accuracy and reliability. Carbox­ holder and gold-coated using a sputter coater (JEOL Fine Coater JFC-
ymethyl cellulose (CMC) is a cellulose derivate from various hard- and 1200, Germany) for 40 s at 30 mA.
softwood sources. Its thickening, stabilizing, and film-forming proper­ Micro-computed tomography (µCT) scans were performed using
ties makes it a favourable additive in the textile and paper industries an UMITOM XL (Tescan). Specimens with densities of 60 and 130 kg/m3
[26,27]. CMC is also commonly used as additive to enhance the texture were produced by cutting a cylindrical shape with a diameter of 20 mm
of gluten-free bread. Due to CMC’s physiological inertness, CMC is from a foam panel 20 mm in height. To ensure stable mounting and
regarded to be generally safe to end-users and the environment. CMC prevent image blur, specimens were securely housed in thin-walled 3D-
was reported to enhance the strength of hand sheets [28], which makes printed PLA sample holders with a tight fit. The spatial scan resolution
it a prime candidate to use as polymeric additive to improve the strength was set to 15 µm, aligning closely with the recommended 1/1000 ratio
of pulp foams [22]. for sample and voxel size [29 30]. To generate a scan of the complete
We provide a comprehensive mechanical evaluation of pulp fibre specimen, it was necessary to perform three partial scans and stitch them
foams containing a bio-based polymeric binder with a wide range of together after the acquisition process. A scan voltage of 40 kV and a
densities under various loading conditions. We report essential current of 375 µA were utilized over an acquisition time of ~70 min. No
compression, tension, bending, and shear properties along with struc­ spectral filter was employed during scanning to produce pictures with
tural characteristics, such as pore and fibre orientation, across a wide high contrast. The resulting three-dimensional datasets were analysed
range of densities. The data provided enable the suitability assessment of using the Dragonfly software, Version 2022.2 (Build 1409) for Windows
such foams for a variety of applications, with emphasis on structural (Comet Technologies Canada Inc., Montreal).
applications in mechanical and civil engineering, and the sports/leisure Pore size was assessed by manual thresholding. Isolated islands with
industry. Besides static mechanical properties we also investigate the fewer than nine voxels and one- or two-voxel thick voids were excluded
high strain rate response of pulp fibre foams, closing the gap in literature to avoid false identification of pores, resulting in a minimal pore size of
shown by Pääkkönen et al. [29] and offering novel insights crucial for 30 µm. These small free spaces between fibres represent voids rather
impact applications relevant to packaging, energy-absorbing automo­ than pores templated by air bubbles and where therefore disregarded.
tive parts, or personal safety equipment such as impact liners for hel­ The segmented data was analysed using the “PoreSpy” [31] and
mets. We provide data that will facilitate the generation of material “OpenPNM” [32] software plug-ins, both utilize the Snow algorithm
models suitable for both quasi-static evaluations and dynamic load developed by Gostick [33]. Various pore metrics were evaluated,
cases, hence enabling their future adoption. including pore volume Vp , the mean Sauter diameter d32 , the maximum
Feret diameter F, which represents the largest extent of a pore [34], and
2. Methods the sphericity Ψ. Sphericity describes the ratio of the surface area of an
ideal spherical pore, based on the measured pore volume (Vp), to the
2.1. Pulp and chemicals estimated pore surface area (Ap) from the µCT measurement (Eq. (1). A
value of Ψ equal to 1 represents a perfectly sphere-shaped pore.
Once dried bleached softwood kraft pulp sheets (BSKP) of a
( 1 )2
composition of 85 % spruce, 10 % pine, and 5 % larch were kindly 6 π 2 Vp 3

provided by Zellstoff Pöls AG (Austria). The Schopper Riegler (SR) for all Ψ= (1)
Ap
samples was determined according to TAPPI standard T 227 to be 11.3

2
M. Wagner et al. Composites Part A 188 (2025) 108515

Fibre orientation was assessed using a an in-house developed Python ∫ s

tool. This tool applies Gaussian smoothing to the three-dimensional EA = F(s) ds (4)
0
greyscale data sets. Skeletonization was then performed, using the
“skimage” python library [35] and the Hessian matrix was calculated for where F(s) is the force dependent on the displacement s. The specific
each remaining filled voxel. The local orientation of each voxel was energy absorption SEA enables comparison between different foam
derived from the eigenvalues of the corresponding Hessian matrices. A structures and is the ratio of EA of a certain structure and its mass m:
similar approach, based on the greyscale values with an subsequent
EA
evaluation of their second derivative, has already been proposed by SEA = (5)
Frangi et al. [36] It was shown that the orientation of the fibre network m
can be derived with reasonable accuracy even when the fibre diameter is Tensile tests were performed at a test speed of 20 mm/min according to
smaller than the resolution of the µCT scan [37]. standard ISO-1926 on five dog bone shaped specimens (Figure S2). Test
Relative density was assessed by dividing the envelope density ρ* specimens had a length of 150 mm (x direction), with a gauge length of
by the skeletal density ρs . The envelope density was determined by the 55 mm and a width (y direction) of 25 mm and a height (z direction) of
ratio of foam weight and volume. The skeletal density was measured 20 mm. The ends of the test specimens were coated with a highly viscous
using helium-pycnometry (Micrometics AccuPyk) to be ρs = 1449 ± 3 epoxy resin (Uhu Endfest 300) and a casting epoxy resin (Greenpoxy) to
kg/m3 and the porosity ϕ calculated by Eq. (2) [4]: ensure clamping without compressing the material in the jig. The
ρ* specimens were pre-loaded with 2 N and tests ended after a 95 % decline
ϕ = 1− (2) in force was detected. Tensile strengths and moduli were determined
ρs
from engineering stress–strain curves. To validate the modulus calcu­
Density distribution was determined utilizing segmented data to lated from the traverse displacement the strain was also recorded using a
correlate scan data and ρ* [38]. The dataset segmented by manual video-extensometer for selected samples.
thresholding, without further modifications such as island processing, Flexural tests were performed in three-point bending following
was used. Each filled voxel was assigned a weight such that the sum of standard ISO 1209–2. The setup consisted of two half-cylindrical sup­
all voxels equalled the specimen weight. The assigned voxel weights ports with a diameter of 30 mm separated by 240 mm and a half-
varied among different specimens. This variability was crucial due to the cylindrical impactor moving at 20 mm/min. Prior to testing a preload
relative scale of the greyscale data for each specimen. The highest of 2 N was applied. The test ended when the force dropped by 95 % from
brightness value was assigned to the maximum x-ray absorption, while its peak or after reaching a displacement s of 60 mm. Test specimens had
the minimum absorption was set to zero. Consequently, manual dimensions of 290 × 40 × 20 mm with the force being applied in the z
thresholding and individual voxel weight assignment were required for direction of the foam. Drying of wet foams caused the formation of a skin
each specimen. The density distribution was analysed in the x, y, and z on the open mould side, for this reason two different configurations were
directions resulting in a density distribution along each main axis. tested for each density group: one in which the skin layer is in contact
with the impactor (4 specimens/density) and one perpendicular to it (3
2.4. Mechanical properties specimens/density).
Force-displacement curves were used to calculate the energy ab­
Quasi-static mechanical tests were performed using a universal sorption capacity using Eqs. (6) and (7) [40]. The flexural modulus E
testing machine (UTM Z020, ZwickRoell). The machine was equipped was calculated as follows:
with 20 kN load cell with an accuracy class of 0.2 %. The experiments L3 F
were carried out at 20 ◦ C, about 70 %RH (Remark: Aimed RH was 65 %, E= (6)
48Is
as proposed for testing of wood-products, e.g. EN 319:1993).
Uniaxial compression tests were performed following standard ISO BH3
I= (7)
844. The testing speed was 5 mm/min, resulting in a strain rate of 12
0.0042 s− 1. At least five specimens were tested for each configuration. A
pre-force of 2 N was been applied prior to testing and the measurement where L is the span length, F the measured force, I the second moment of
ended when a force level of 15 kN was reached. Engineering stress over area, s the displacement, H the specimen height, and B the specimen
engineering strain curves were generated. Foam specimens were tested width.
in out-of-plane (force applied in foam production height direction, i.e. z Double lap shear tests were performed following standard ISO-
direction) and in-plane orientations (force applied perpendicular to the 1922. Two foam panels measuring 240 × 50 × 20 mm (x, y and z di­
height direction, i.e. in the xy-plane). The out-of-plane specimens were rection, respectively) were adhesively bonded to three parallel poplar
50 × 50 × 20 mm plates and the in-plane specimens were 20 × 20 × 20 plywood plates with 8 mm thickness and 5 ply’s each. (Figure S3). This
mm cubes (Figure S1). test configuration represents an out-of-plane shear load case. The two
The densification strain was determined using the tangential outer plates are connected to a plywood block acting as spacer. Tests
method, which was also used by Li et al. [39]. This method defines the were performed at a speed of 20 mm/min following pre-loading of 2 N.
densification strain as the intersection point of the tangents to the “stress The experiment ended when a 95 % force drop was detected. For each
plateau” region and to the densification region. specimen, the relative displacement of each support was measured using
The mean crush strength σ m , an indicator for the energy absorption Blender (version 2.79b) target tracking. From the relative displacements
capacity, was obtained as follows: of the supports, the mean engineering shear strain γ of 4 locations was
∫ calculated as follows [41]:
1 εD
σm = σ (ε) dε (3) ∑n=4 Δxk
εD 0 k=1 ( z0 )
γ= (8)
n
where εD is the densification strain and σ(ε) the stress at any given strain.
The amount of energy absorbed EA was determined by integrating the where Δx is the measured displacement and z0 the height of the spec­
area underneath the force–displacement curve: imen. The output force–time curve was used to calculate the engineering
shear stress, which was used to produce the shear stress–strain curve.
The shear modulus has also been assessed by Eq. (9) for the initial linear

3
M. Wagner et al. Composites Part A 188 (2025) 108515

region. 3. Results and discussion


F/A
G= (9) 3.1. CMC and SDS-stabilized pulp fibre froth templates: Morphology and
γ
shape retention
Tests were performed in triplicate. The low number of repetitions was
justified due to the large shear area per test and that each specimen Pulp fibre foams were prepared by frothing cellulose pulp fibres
suspended in CMC and SDS solution. SDS served as a surfactant in the
consisted of two separate foam panels.
Dynamic out-of-plane compression tests were performed using a froths and CMC as a foam stabilizer. The addition of CMC led to a narrow
bubble size distribution, and resulted in smaller bubbles throughout the
universal Split Hopkinson bar [42,43]. Besides the stress–strain signal
derived from the strain-gauges on the bar-system a high-speed camera wet froths (Fig. 1a). CMC was added to the formulation to increase the
viscosity and as fibre–fibre adhesive. In the wet froth CMC prevents
(Phantom Veo 640) was used at a frame-rate of 50 kfps to track the
deformation behaviour of the foam specimen. Cylindrical samples with a bubble coalescence and thus premature collapse of the foam structure
during drying [44]. The foam density, and thus the porosity, is
diameter and height of roughly 20 mm and densities of 60, 100 and 130
kg/m3 were used for the dynamic tests. These specimens were tested in controlled by the amount of water and incorporated air into the froth.
Fig. 1b shows optical micrographs of liquid froths: The froth solely
out-of-plane configuration at two different strain rate levels (low and
high dynamic). stabilised by SDS had an inhomogeneous texture with clotted fibres and
fewer and less well dispersed bubbles, while the froth also containing
CMC had a smooth and homogeneous texture containing many bubbles
separating the pulp fibres. SDS in conjunction with hydrophilic fibres
lead to repulsion between fibres and air bubbles [19]. The viscosifying
effect of CMC kinetically stabilised air bubbles and imparted

Fig. 1. A) schematic of pulp fibre froth preparation and morphology of wet froths and dry cellulose pulp fibre foams, b) optical micrographs showing the structure of
wet pulp fibre froths stabilised solely with SDS (top), and SDS and CMC (bottom); c) scanning electron micrographs of pulp fibre foams produced by drying SDSand
CMC stabilised froths showing the incorporation of CMC films in the 3D pulp fibre network.

4
M. Wagner et al. Composites Part A 188 (2025) 108515

dimensional stability to the wet froth, preventing drainage, bubble likely bonding fibre joints. Increasing the CMC concentrations to 26 wt%
coalescence and allowing froth moulding. The half-lives of the air resulted in the formation of lamellae between fibres in the 3D network
bubbles in the foam can be extended by the increased viscosity of the and a lower form stability, i.e. higher shrinkage (~19 % − Figure S4).
suspension caused by the addition of CMC, which provides improved The increased froth stability due to the addition of CMC eliminated the
colloidal stability. need for post-processing to adjust the pulp foam density. We simply
Froth stability during drying is critical; high viscosity provided by dispersed the desired fibre concentration in the suspension medium,
CMC supports the structure and prevents collapse. Pöhler et al. [22] which was sufficient to adjust the overall foam density. The porosity of
showed that the homogeneity of fibre foams can be tailored by poly­ the pulp fibre foams varied between 91 and 96 % (Table S5).
meric additives; PVA addition resulted in the formation of more het­
erogeneous dry 3D fibre network structures when compared to the use of
SDS alone as stabiliser. Drying of SDS-stabilised froths results in rapid 3.2. Morphological and structural analysis of pulp fibre foams via µCT
froth collapse already during drainage, resulting in the formation of
sheet-like porous pulp fibre structures, whereas SDS and CMC stabilised µCT was used to analyse the foam structure and to evaluate the fibre
froths retain their structure during drying with minimal volume and pore orientation and distribution (Fig. 2a). The density distribution
shrinkage of about 1 %. After moulding these froths can be transferred in the height direction (z) of pulp fibre foam was rather inhomogeneous
directly into an oven for drying. During drying, a densified skin layer (Fig. 2b). Local density minima were found in the region between 7 and
(Fig. 1a right) forms on the open mould side, which slows water evap­ 10 mm from the bottom, i.e. in the middle layer, for both high and low
oration from bulk froth volume. The optimal CMC concentration in dry density foams. The bottom side had the target density (within error). In
foams was determined to be 5 wt%. CMC forms films spanning fibres and trough-thickness direction the density decreased towards the middle
increasing again towards the top surface. The dense skin layer (Fig. 2b)

Fig. 2. A) µCT scans of pulp fibre foam (d = 20 mm, h = 20 mm), full view of 60 kg/m3 specimen, cross-section of 60 kg/m3 specimen,) µCT cross-section (xy-plane)
of cellulose pulp fibre foams (up). full view of 130 kg/m3 specimen, cross-section of 130 kg/m3 specimen, µCT cross-section (xy-plane) of cellulose pulp fibre foams
(below). b) comparison of density spread in z direction for a 60 kg/m3 and a 130 kg/m3 foam, c) Density distribution of a 60 kg/m3 foam in x, y and z direction.

5
M. Wagner et al. Composites Part A 188 (2025) 108515

was confirmed on the open-mould side. Upon drying a denser layer, i.e. a generally much broader (d32 from 30 µm up to about 3,000 µm) when
skin, formed at the freely exposed surfaces due to higher drying rates in compared to PU foams with similar densities containing pores in the
analogy to bread baking in which a crust forms within the first minutes range between 300–1,100 µm [52]. Larger pores are more prone to be
[45]. Faster drying of wet froths results in the formation of a permeable elongated than smaller ones; so higher density foams with larger pores
yet insulating foam layer increasing the time required for drying [46]. also exhibited a lower mean sphericity (Ψ = 0.35) as compared to foams
Consequently, the froth dries in a heterogeneous manner, from outside with a lower density (Ψ = 0.5) (Figure S7), which is in agreement with
to inside, resulting in different heating rates through the foam structure. the broader Feret diameter distribution. This is in contrast to polymer
The skin retains the shape of the froth in analogy to solidifying bread foams which exhibit pores with a higher mean sphericity of 0.7 and
doughs [45]. Water removal occurs by either permeation, diffusion above [53]. The evaluation of the pore centroid distribution mirrors the
through the liquid phase or evaporation and diffusion through the results from the µCT-density analysis (Fig. 2c), showing more pores
gaseous phase [47]. In the wet froth, fibres were dispersed in the liquid located in the middle of the specimen along the z direction, with little
foam phase and bubbles stabilised by CMC (Fig. 1b), forming films upon variance in the xy-plane (Figure S8). Fibre orientation analysis (Fig. 3)
drying. The internal pressure in the froth increased as water is removed, revealed that foams with 60 kg/m3 density exhibited over 60 % of fibres
causing the CMC-films to burst. The remnants of films can be seen in with a zenithal fibre angle θ of 80◦ to 90◦ , meaning that most fibres were
micrographs (Fig. 1c). CMC-film rupture caused pores to interconnect aligned in the xy-plane. Pulp fibre foams have a layered structure similar
leading to an open porous heterogeneous foam structure (Fig. 1a right). to paper products. Higher density foamss possessed a less severe,
Increasing the CMC content and thus the viscosity of the suspension although still very pronounced in-plane orientation, with over 50 % of
medium resulted in thicker films stable enough to withstand the built-up the fibres being oriented within 10◦ of the xy-plane. The in-plane φ angle
of pressure resulting in a partly closed pore network (Figure S5). In the distribution however was similar between foams of both densities,
latter stages of drying, water evaporation slowed down as the outer layer exhibiting an only slight preferred direction. It is assumed that this in-
become less porous. Combined with the increasing internal pressure due plane fibre orientation preference was induced by spreading the froths
to increasing temperature and water vapour volume bubbles expand in the mould.
pushing fibres apart, leading to bigger pores in the foam interior pro­ The pore orientation analysis (Figure S9) mirrored the trends shown
moting the formation of a heterogeneous foam structure. Fibre foams Fig. 3, with fibres a predominant orientation in the xy-plane. Therefore,
produced by draining prior to drying of froth stabilised by SDS alone both the fibre and pore analyses indicate a level of orthotropic distri­
exhibited a density gradient caused by fibre filtration [17,48]. bution as opposed to the transversal isotropic assumption. However,
Pulp fibre foams produced by drying frothed fibre suspensions con­ since the in-plane spread was negligible in relation to the overall scatter
taining CMC possessed a narrow density distribution in the xy-plane and the density distribution in the z direction a transversal isotropic
(Fig. 2b), thus suggesting a transversal isotropic density distribution. assumption is justified. The µCT evaluation revealed the inhomogeneity
The density variation in the z direction reduced from 36.5 % to 11.1 % of pulp fibre foams, which will affect their mechanical properties.
when increasing the foam density from 60 kg/m3 to 130 kg/m3, which is
expected to affect compression, bending and shear behaviour, resulting 3.3. Mechanical properties of pulp fibre foams
in more isotropic foams that can be compared with expanded poly­
styrene (EPS) [49]and expanded polypropylene (EPP) [50]. 3.3.1. Compression
The overall structure of pulp fibre foams is influenced by the bubble Compression is the most critical load case for porous materials.
size distribution in wet froths. The foam density depends besides the Compression stress–strain curves of cellulose foams in out-of-plane
water content on the amount of air incorporated into wet fibre froths. orientation (load applied in z direction) are shown in Fig. 4. Pulp fibre
Air bubbles are entrapped between fibres in the viscous suspension foams with a density of less than 130 kg/m3 do not exhibit a pronounced
medium. Al-Qararah et al. [51]showed that the homogeneity of the difference between the elastic and plateau regions. Instead, a single,
microstructure of foam-formed porous fibre materials of approximately almost linear elastic region was observed up to the densification strain
the same envelop density depends on the Sauter mean pore diameter εD. The absence of a defined plateau region, typically attributed to
d32 ; the larger the pore diameter the more heterogeneous the pore buckling behaviour in open and closed-cell synthetic foams [4], suggests
structure leading to decreased mechanical properties. Pore analysis of that this mechanism has limited effect for low density pulp fibre foams
our foams showed that most pores had a rather small d32 . For foams with when loaded out-of-plane. This behaviour is further supported by the
a nominal density of 60 kg/m3 most pores had a d32 of about 0.6 mm and low percentage of fibres oriented in the out-of-plane direction for low
below (Figure S6a und b). Foams with a density of 130 kg/m3 possess density foams (Fig. 3).
slightly larger pores with most exhibiting a d32 of about 0.7 mm. This Noteworthy is the significant change in the materials response when
observed trend toward larger pores in higher-density foams was attrib­ evaluated in the in-plane direction (loading applied in the xy-plane). In
uted to more defined porosity and a shift toward a slightly more closed- this orientation, the pulp fibre foams exhibited a pronounced plateau
cell structure, with clearer pores and a less random fibre distribution. As region for all densities, though at relatively low levels (Fig. 4). The clear
a result, higher-density foams contained more pronounced cell walls, distinction between the initial elastic region and the plateau region, can
which could accommodate larger pores. In contrast, lower-density be attributed to bending and buckling of numerous fibres, which were
foams exhibited a more random and loosely arranged fibre network aligned in the (xy) plane as well as to the higher density skin layer. The
resulting in smaller porosity, as voids created by the random arrange­ in-plane Young’s modulus E at equal density was over four times higher
ment of fibres, rather than gas bubbles, were also classified as pores in compared to the out-of-plane direction, in line with literature data [54].
the applied analysis. The volume-weighted distribution was similar be­ The compression results obtained are presented in Table 1.
tween the 60 kg/m3 and 130 kg/m3 foams, with a low content of small Gibson and Ashby [4] proposed approximations for the compression
pores (d32 ≤ 0.15 mm), followed by a steep increase in pore diameter modulus E* of open cell foams:
occurrence until a peak was reached. After this peak, the number of ( * )2 * ( * )2
larger pores gradually decreased, with only a few large pores (d32 ≥ 2 E* ρ E ρ
= C1 * ≈ (10)
mm) remaining. This represents a relatively broad distribution. Notably, ES ρs E S ρs
slightly different results were observed for the maximum Feret diameter,
where higher-density foams exhibited an even broader distribution. This where Es is the modulus of cellulose, C1 a factor (of order 1), ρ* the
suggested that the frothing process did not allow for homogeneous envelope density of the foam and ρs the density of cellulose. The plateau
distribution of the incorporated air, leading to slightly larger and more strength σ*pl can be approximated by:
elongated pores. The pore size distribution of pulp fibre foams was

6
M. Wagner et al. Composites Part A 188 (2025) 108515

Fig. 3. A) out-of-plane fibre orientation distribution of a 60 kg/m3 foam, b) out-of-plane fibre orientation distribution of a 130 kg/m3 foam, c) in-plane fibre
orientation distribution of a 60 kg/m3 foam, d) in-plane fibre orientation distribution of a 130 kg/m3 foam.

Fig. 4. A) mean out-of-plane stress strain curves for compression, b) mean in-plane stress strain curves for compression.

( )3/2
σ *pl ρ*
Table 1 ≈ C1 * (11)
Compression modulus E, mean crush strength σc , compression strength at 10% σ ys ρs
densification strain σ10% , densification strain εD, specific energy absorption SEA
of cellulose pulp fibre foams. where σys is the yield strength and the proportionality factor C1 can be
approximated by 0.3. However, these equations did not accurately
Specimen *
ρ [kg/ E[kPa] σc [kPa] σ10% [kPa] εD SEA [J/
m3] [-] g] describe the compression properties of pulp fibre foams. The measured
modulus and plateau strength were less than 10 % of the predicted
out-of-plane
SC 1 60 74 ± 38 170 10 ± 3 0.91 1.04 ±
values, when the softwood fibre elastic modulus is assumed to be 18 GPa
0.15 and the yield strength is assumed to be 1 GPa (Table 2) [55]. Long spans
SC 2 80 300 ± 280 28 ± 10 0.87 1.70 ± between fibre–fibre connections, low buckling resistance of individual
170 0.20 fibres or fibre–fibre debonding may contribute to the overall compres­
SC 3 100 190 ± 70 330 34 ± 15 0.86 2.00 ±
sive behaviour not aligning with predictions. The densification strains
0.39
SC 4 130 780 ± 480 82 ± 16 0.81 2.95 ±
300 0.33
in-plane Table 2
SC 5 60 620 ± 270 46 ± 8 0.95 0.94 ± Predicted modulus E*predicted, plateau strength σ*pl_predicted, and densification
170 0.28 strain εD_predicted of cellulose pulp fibre foams.
SC 6 80 1,220 ± 490 100 ± 20 0.93 1.68 ±
Density [kg/m3] E*predicted [MPa] σ*pl_predicted [MPa] εD_predicted [-]
240 0.17
SC 7 100 2,350 ± 770 180 ± 10 0.92 2.47 ± 60 28.8 2.4 0.94
260 0.31 80 51.2 3.7 0.93
SC 8 130 2,560 ± 1,010 230 ± 40 0.92 3.02 ± 100 80 5.2 0.91
480 0.33 130 135.2 7.7 0.88

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M. Wagner et al. Composites Part A 188 (2025) 108515

εD, however, are close to predicted values, with less than 10 % deviation dense skin layers, mimicking wood-like structures, and reported in-
between measured values and predicted ones: plane compression moduli up to 5.5 MPa while maintaining a density
of only 50 kg/m3. Ketola et al. [19]showed that the surfactant used to
ρ*
εD ≈ 1 − 1.4* (12) stabilise wet froths also influences the mechanical properties of pulp
ρs fibre foams. The choice of fibre and surfactant does affect fibre orien­
tation; well bonded fibres in an anisotropic 3D random fibre network
Fig. 5 displays a fitted power law for the compression modulus and σ 10%
possess the highest strength (0.015 MPa) along the loading direction
of pulp fibre foams as function of density. The exponent for the in-plane
with the highest anisotropy. A closed cell pore structure forms when
modulus function is 1.71 (±0.17), which correlates with a closed-cell
using smaller building blocks, such as CNF [58–60] or regenerated
foam structure, meaning that the modulus increases with density simi­
cellulose [61], which results in an isotropic structure able to distribute
larly to that in closed pore foams. The exponent in out-of-plane
the applied stress more evenly resulting in much improved compression
configuration is 3.16 (±0.45), which is associated with the presence of
moduli and strengths. For similar pulp fibre foams with a density of 90
an open network structure [56], indicating that the fibre orientation has
kg/m3 and 161 kg/m3 moduli of 460 kPa [62] and 1,100 kPa were re­
significant impact on the mechanical properties. Based on the in-plane
ported [9], which aligns with our findings.
exponent and the strong in-plane fibre orientation, it can be assumed
Comparing the moduli of our pulp fibre foams with conventional EPS
that fibre buckling represents the dominant deformation mechanism in
foams of similar densities highlights their inferior compression proper­
compression. This buckling behaviour might be similar to the buckling
ties. EPS foams with a density of 64 kg/m3 have a modulus of 17.3 MPa,
of struts and faces observed in closed-cell foams, suggesting a compa­
those of 80 kg/m3 have similar moduli (18.3 MPa) while increasing the
rable underlying mechanism and, therefore,e a similar exponent. How­
foam density further to 120 kg/m3 results in significantly higher
ever, the overall stiffness and strength are low due to the limited
compression moduli of 51.8 MPa [72]. In contrast, the pulp fibre foams
connectivity within the fibre foams, likely contributing to the lower than
achieved only 0.5 to 4 % of the compression moduli reported for EPS.
expected proportional factor in the equation. The expected proportional
One advantageous property of fibre foams is their high densification
factor should roughly equal Es, while the determined proportional factor
strain of 0.8 to 0.95. In comparison to EPS foams, which have a densi­
ranged between 1/10 x Es and 1/100 x Es. This explanation aligns with
fication strain of about 0.6 to 0.65, [50] pulp fibre foams can be com­
the higher exponent observed in the out-of-plane configuration, where
pressed ~30 % further before they reach densification, which offers
fewer fibres were oriented along the loading path. Consequently,
significant advantages in terms of energy absorption.
buckling is less dominant, and fibre bending and compression become
more significant, leading to a higher exponent typically associated with
3.3.2. Dynamic compression
fibrous networks. The fitted functions for in and out-of-plane moduli
The quasi-static and dynamic compression stress–strain curves of
showed a good fit with an r2 value over 0.75 while the fitted function for
pulp fibre foams with densities of 60, 100 and 130 kg/m3 are shown in
stress at 10 % strain showed even better correlation with an r2 value over
Fig. 7. A significant increase in compressive stress at any given strain
0.9. These fitted functions can be used as the basis of most numerical
was observed with increased strain rates (See Table 3). It is important to
simulation, and as opposed to discrete data points, enable easier density
note that both the high dynamic and low dynamic curves terminate at
optimization for uniaxial compression load cases.
lower strain values. This behaviour is inherent to Split Hopkinson
Fig. 6 places these resulting fitted material behaviour functions
pressure bar tests [42,43] when maintaining a constant specimen size;
within the broader context of other cellulose-based foams. The out-of-
the achievable compression strain decreases with the applied loading
plane properties agree fairly well with reported data for pulp fibre
speed.
foams, while the in-plane properties are among the highest values
Low density (60 kg/m3) pulp fibre foams display a strain rate
documented for such foams. Micro- and nanofibrillated foams signifi­
amplification factor of up to five, meaning that the strength at a given
cantly outperform pulp fibre foams.
strain and strain rate is up to five times larger than in a quasi-static
The compression properties of pulp fibre foams can be improved by
configuration. This is a significant increase of the strain-rate de­
crosslinking [57] or hydrolysing the cellulose pulp fibres [9]. However,
pendency compared to EPS foams with similar densities [73]. Increasing
crosslinking and hydrolysis of 3D networks of pulp fibres often involve
the density (130 kg/m3) of pulp fibre foams seems to result in a strain
harmful chemicals and negatively impact the biodegradability and
rate amplification comparable to EPS foams (112 kg/m3). The high
sustainability aspects. In-plane measurements have shown the influence
strain rate sensitivity for low density pulp fibre foams proves particu­
of the skin layer and fibre orientation in resisting compressive forces.
larly advantageous for energy absorption applications, such as for
Reichler et al.50 designed a lightweight structure with intentionally
packaging and personal safety equipment. Furthermore, this data

Fig. 5. A) modulus and b) stress at 10% strain fit function with respect to density, for the in-plane and out-of-plane compression cases of cellulose pulp fibre foams.

8
M. Wagner et al. Composites Part A 188 (2025) 108515

Fig. 6. A) modulus of fibre foams, b) stress at 10% strain references: pulp fibre foams[18,22,23,54,62–65]; Hydrolysed fibre foams [9]; Regenerated fibre foams
[66,67]; Nanofibrillated fibre foams [60,68]; Microfibrillated fibre foams [54,69]; Microcrystalline cellulose foams [70,71].

Fig. 7. Stress–strain curves of dynamic compression tests of a a) 60 kg/m3 foam b) 100 kg/m3 foam c) 130 kg/m3 foam and strain rate amplification comparison
between d) 60 kg/m3 cellulose foam and 61 kg/m3 EPS and e) 130 kg/m3 foam and 112 kg/m3 EPS.

enables the utilization of strain rate dependent material models within


Table 3
numerical simulations such as models based on the constitutive law by
Mean crush strength σm at 25 % strain for 20 mm thick with low (400 – 500 1/s)
Chang [74], which are essential for the adoption of materials in safety
and high dynamic (700 – 750 1/s) loading of cellulose pulp fibre foams.
and energy absorption applications. While the high strain compression
Specimen ρ* [kg/m3] Strain rate [1/s] σm [kPa] behaviour may not completely outweigh the limited compression
SH 1L 60 460 62 ± 11 properties, it substantially enhances the suitability of such foams for
SH 1H 60 742 107 ± 16 impact attenuation applications, as they become stronger with
SH 2L 100 477 155 ± 27 increasing loading rate, i.e. providing a load-rate adaptivity.
SH 2H 100 708 204 ± 45
SH 3L 130 399 225 ± 30
SH 3H 130 712 326 ± 49 3.3.3. Tension
Tensile stress–strain curves of pulp fibre foams with varying densities
are shown in Fig. 8a. The tensile strength in the xy-plane of pulp fibre
foams decreases with decreasing density; however, the tensile strength

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M. Wagner et al. Composites Part A 188 (2025) 108515

Fig. 8. A) mean tensile stress strain curves of pulp fibre foams with varying density. b) failure initiation and propagation until final failure of pulp fibre foams with a
density of 130 kg/m3.

of pulp fibre foams with a density of 60 kg/m3 decreased much more


Table 4
significantly caused by the broad density distribution within these
Peak force Fmax , displacement at peak force s, modulus of rupture MOR and
foams. The centre of the foam with a nominal density of 60 kg/m3 had a
specific energy absorption at 40 mm displacement of cellulose pulp fibre foams.
density of only ~30 kg/m3 and this was likely where the failure initiated
(Fig. 8c). Presence of fines in pulp used to produce pulp fibre foams, such Specimen ρ* [kg/ Struck Fmax [N] s[mm] MOR SEA
m3] side [kPa] [mJ/g]
as CTMP, results in improve fibre–fibre bonding, which in turn was
found to increase their tensile strength [17]. Skin layers provide a denser SB 1 60 Skin 6.57 ± 7.97 150 ± 10.73 ±
0.54 12 1.32
network and, therefore, higher network strength, which positively
SB 2 60 No Skin 5.91 ± 7.93 133 ± 3 9.02 ±
contributes to the tensile strength of pulp fibre foams. Tensile testing 0.14 1.58
along the z-axis, as performed by Ketola et al. [19], showed that the z- SB 3 80 Skin 11.19 ± 8.23 252 ± 10.06 ±
strength is mainly influenced by the fibre orientation. In foams 1.75 40 1.77
comprising a layered structure fewer fibre–fibre connections in z di­ SB 4 80 No Skin 13.37 ± 13.56 301 ± 20.54 ±
1.14 26 2.92
rection was observed. Generally, the tensile strength of the pulp fibre
SB 5 130 Skin 28.14 ± 7.34 633 ± 17.53 ±
foams is much lower than that of synthetic polymer foams, though not as 2.47 56 1.39
severely as their compression properties, with approximately 15 % of SB 6 130 No Skin 31.87 ± 11.20 717 ± 21.74 ±
the tensile strength of EPP [75] and about 10 % compared to EPS [76]. 3.31 74 8.90
Fig. 8b shows where the failure of the foams initiated. It is evident
that local separations begin to occur at low strain levels (below 0.01).
they fully fail (Fig. 9a), while EPS foams tend to fracture shortly after
These localised separations, indicated by red lines, did occur in areas of
reaching their flexural strength, similar to the behaviour observed in
the foam with minimal interconnectivity between fibres, attributed to
tension [80].
density inhomogeneities. Following the initial appearance of these
fractures, the tensile strength was reached at a strain of approximately
3.3.5. Shear
0.02 while fracture propagation continued until complete separation
Shear failure is the predominant core failure mode of foam materials
occurred up to strains of ~0.14. The failure strain of pulp fibre foams is
in sandwich panel applications, underscoring the significance of this
between that of EPS and EPP foams. For instance, EPS have lower failure
property for pulp fibre foams. Shear stress–strain curves are shown in
strains of ~0.04 to 0.05, [77,78] while EPP foams can exhibit failure
Fig. 10. Similar to the behaviour observed in tension and flexural
strains ranging from 0.08 up to ~0.2 at room temperature [75,79]. Pulp
loading cases (Table 5), pulp fibre foams reached their peak strength
fibre foams reach their peak tensile strength rather quickly until fully
relatively early, and the stress gradually decayed until full separation.
separated, whereas EPS and EPP fail shortly after reaching their tensile
Our tests were limited to out-of-plane shear properties, as this represents
strength. This tensile fracture behaviour data is crucial for numerical
the most relevant load case for sandwich panel applications. Cellulose
modelling in safety applications, as it is essential for predicting failure
fibre foams with a density of 60 kg/m3 achieve only about 14 % of the
and fracture.
shear modulus reported for lower density (30 kg/m3) EPS and merely 8
% of its shear strength τxz max [81]. For comparable EPS foam densities of
3.3.4. Flexure
75 kg/m3, the shear strength of pulp fibre foams is only 5 %. However, it
Under flexural loading (with force applied in z direction) all speci­
is worth noting that limited shear data are available for comparable
mens exhibited tensile failure on the non-struck side, but no observable
cellulose foams, even though such values are important for the design of
shear failure. The configuration in which the denser skin layer was
possible sandwich structures and when modelling complex load cases.
loaded in tension surpassed the maximum forces compared to the
samples in which the skin layer was under compression, except for the
lowest density where the maximum force Fmax (See Table 4) was rela­ 3.4. Structure-density relation to mechanical properties
tively similar (Fig. 9a). The surface difference of the non struck side is
shown in Fig. 9b and c. The observed behaviour is due to the dense skin Fig. 11 illustrates the stiffness increase in compression, tension, and
layer offering additional strength in tension while potentially buckling shear as a function of density, highlighting the sensitivity to both density
and contributing less in compression. Pulp fibre foams with 60 kg/m3 and fibre orientation under various loading conditions. Most notable
might not profit from the skin layer because of its lower density (Fig. 9a). was the strong progressive trend observed for out-of-plane compression,
Pulp fibre foams exhibit a gradually decreasing flexural force until which is explained by the increased initial density and the higher

10
M. Wagner et al. Composites Part A 188 (2025) 108515

Fig. 9. A) mean three-point-bending force–displacement curves: b) skin struck side fracture c) no skin struck side fracture.

Fig. 10. A) mean shear stress over strain curves, b) fracture process of a 130 kg/m3 shear specimen.

Table 5
Shear strength τxz max and shear modulus G of cellulose pulp fibre foams.
Specimen ρ* [kg/m3] τxzmax [kPa] G[kPa]

SS 1 60 18 ±7 820 ± 345
SS 2 80 20 ±3 949 ± 169
SS 3 100 31 ±1 1,182 ± 119
SS 4 130 41 ±7 1,991 ± 418

percentage of fibres oriented in this direction with increased density. In


contrast, the in-plane compressive stiffness shows only a slight pro­
gressive trend, resulting from the combination of increased initial den­
sity and the regressive effect of the lower percentage of fibres orientated
in this direction. The shear stiffness also displays a progressive trend
attributable to the increased percentage of fibres oriented out-of-plane
which increased with increasing density, whereas low-density foams,
with stronger in-plane orientation and layering, had less resistance to
shear. Conversely, the in-plane tensile stiffness exhibits a regressive
trend with increasing density, due to the lower percentage of fibres
oriented in the in-plane direction. Fig. 11. Stiffness increase over density for compression, tension and
shear loading.

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M. Wagner et al. Composites Part A 188 (2025) 108515

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