Role of inter-fibre bonds and their influence on sheet scale behaviour of paper fibre networks

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Role of inter-fibre bonds and their influence on sheet scale
behaviour of paper fibre networks?
P. Samantraya,b,c, R.H.J. Peerlingsa, T.J. Massartb, O. Rokoˇsa,
, M.G.D. Geersa
aMechanics of Materials, Department of Mechanical Engineering, Eindhoven University of Technology,
P.O. Box 513, 5600 MB Eindhoven, The Netherlands
bBuilding, Architecture and Town Planning, Universit´e Libre de Bruxelles, 50 Avenue F.D. Roosevelt, CP
194/2, B–1050 Brussels, Belgium
cMaterials innovation institute (M2i), P.O. Box 5008, 2600 GA Delft, The Netherlands
Abstract
In fibrous paper materials, an exposure to a variation in moisture content causes changes in
the geometrical and mechanical properties. Such changes are strongly affected by the inter-
fibre bonds, which are responsible for the transfer of the hygro-mechanical response from
one fibre to its neighbours in the network, resulting in sheet-scale deformation. Most models
developed in literature assume perfect bonding between fibres. In the 3D reality, there is some
flexibility in the bond region, even for the perfectly bonded fibres, because of the possibility
of deformation gradients through the fibre thickness. In earlier 2D idealizations, perfectly
bonded fibres were assumed, implying full kinematic constraint through the entire thickness
of the sheet. The purpose of the present study is to assess the effect of this assumption.
Using a homogenization approach, a random network of fibres is generated with different
coverages and modelled using finite elements. In order to understand the role of bonding
between fibres on the hygro-expansive behaviour of a network, a bond model is developed.
In this model, the fibres are modelled using 2D regular bulk finite elements and the bonds
are represented by interfacial elements of finite stiffness, which are introduced between each
pair of fibres bonded in the network. These embedded interfacial elements form a connection
between two respective fibres, allowing relative displacements between their mid-planes. The
hygro-elastic response of networks obtained with this bond model is investigated by varying
the bond stiffness and the network coverage under the application of mechanical loading and
changes in moisture content. Furthermore, the bond model is used to analyse the influence
of inter-fibre bonds on the anisotropic response of the paper fibre network.
Keywords: Fibrous network, hygro-expansion, inter-fibre bond, interfacial elements,
coverage, homogenization
?The post-print version of this article is published in Int. J. Solids Struct.,10.1016/j.ijsolstr.2022.111990
Corresponding author.
Email addresses: priyam.samantray@gmail.com (P. Samantray), R.H.J.Peerlings@tue.nl
(R.H.J. Peerlings), Thierry.J.Massart@ulb.be (T.J. Massart), O.Rokos@tue.nl (O. Rokoˇs),
M.G.D.Geers@tue.nl (M.G.D. Geers)
Preprint submitted to Int. J. Solids Struct. October 13, 2022
arXiv:2210.05736v1 [cond-mat.soft] 11 Oct 2022
1. Introduction
Fibrous materials like paper consist of natural fibres that are bonded in overlapping
regions, as shown in Fig. 1a. In paper in particular, individual fibres are hollow layered
structures made of wood pulp, which consist of a primary cell wall on the outer side and a
secondary cell wall S. The secondary cell wall further consists of an outer layer S1, middle
layer S2, and an inner layer S3, as indicated in Fig. 2a. Individual cell walls are furthermore
composed of three types of polymers (in particular cellulose, hemicellulose, and lignin),
having the ultrastructural composition shown in Fig. 2b. The distribution of the polymers
varies across the primary and secondary walls of the fibre, where the secondary wall layer
contains higher amounts of cellulose and hemicellulose as compared to the primary layer,
whereas lignin content is nearly the same among all the secondary layers, cf. (Neagu and
Gamstedt,2007).
During the manufacturing of paper, the fibres are preferentially oriented in the machine
direction, which entails anisotropy in the mechanical behaviour of the paper network (Lars-
son and W˚agberg,2008). The principal directions of the paper material are denoted as the
machine direction (MD) and cross direction (CD), as shown in the random fibre network
in Fig. 1b (Bosco et al.,2015b). Here, individual fibres are interconnected to each other
in overlapping regions, called bonds, complemented with freely standing parts in between
bonds. In a paper fibre network, the fibres in inter-fibre bonds are connected together by
hydrogen bonding and van der Waal’s forces (Henriksson et al.,2008). The anisotropic be-
haviour, originating at the scale of individual fibres, is transferred from one region in the
network to another through these inter-fibre bonds. The coefficient of transverse hygro-
expansion of individual fibres is nearly 20 times the corresponding value in the longitudinal
direction (Niskanen,1998). This is because at the fibril scale, the polymers (i.e., hemi-
cellulose, cellulose, and lignin) exhibit hygro-expansion that varies depending on multiple
factors, which in combination with the complex fibre microstructure (recall Fig. 2) results
in high anisotropy. For example, the hygro-expansion of the hemicellulose has been found
to be highest among all three polymers due to high solubility of its side groups (Hansen
and Bj¨okman,1998), whereas cellulose (in crystalline form) has negligible hygro-expansion,
as shown by several studies (Lindner,2017;Marklund and Varna,2009;Wang et al.,2014;
Cave,1978). The water uptake by cellulose decreases with an increase in crystallinity below
75% relative humidity (Mihranyan et al.,1978), although the wood fibre has 60–70% cellu-
lose chains in crystalline form and only the rest is in water-absorbing amorphous form and
hence contributing to hygro-expansion (Alince,2002). Apart from crystallinity, the water
absorption in cellulose depends on the temperature at which the fibres are processed, on the
solvents around cellulose, the surrounding cellulose molecules, and the processing of the fi-
bres (Fahl`en and Salm`en,2003;Uetani and Yano,2011;Berthold et al.,1994). For lignin, the
moisture content varies depending on the type, i.e., 3–5% for dioxane lignin and 10–15% for
Klason and periodate lignin. Other parameters affecting hygro-expansivity of lignin include
softening temperature (Eriksson et al.,1991) and microfibril angle (Wang et al.,2014).
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(a) a micrograph of paper fibres (b) a random paper fibre network
Figure 1: (a) A micrograph of paper showing random orientation of individual fibres, and (b) an artificially
generated network of random paper fibres subjected to hygroscopic strain. The preferential directions are
the Machine Direction (MD), oriented along ~ex, and the Cross Direction (CD), oriented along ~ey.
(a) wall layer structure
of a wood fibre
(b) ultrastructural organization of cellulose
within the wood cell wall
Figure 2: (a) A schematic diagram of different cell wall layers within a wood fibre, adapted from (Br¨andstr¨om,
2002;Gilani,2006). (b) Organisation of cellulose polymers at the ultrastructural level within a wood cell
wall, adapted from (Neagu and Gamstedt,2007).
The degree of bonding between fibres and the number of fibres in the network have a
crucial influence on the hygro-mechanical response of the network. Earlier studies demon-
strated that the effective stiffness of the network is mainly dependent on the density of
the network, fibre orientations, fibre properties, and of the inter-fibre connectivity resulting
from the bonds (Mao et al.,2017;Karakc et al.,2017;Heyden,2000;Bergstr¨om,2018;
Cox,1952). It was furthermore revealed that when subjected to moisture changes, the ef-
fective hygro-expansivity of the paper network is governed mainly by the bonded regions
of the network (Bosco et al.,2015a;Samantray et al.,2021b;Uesaka,1994;Uesaka and
Qi,1994;Vainio and Paulapuro,2007;Niskanen,1998;Larsson and W˚agberg,2008;Erkkila
et al.,2015;Nordman,1958;Salm´en et al.,1987;Schulgasser and Page,1988). In another
study (Thorpe et al.,1976), the properties of the bonded fibres were computed from load-
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displacement measurements. The hygro-mechanical properties of the paper, which are highly
dependent on the inter-fibre connectivity, thus hold significance in understanding the dimen-
sional stability of paper products like packaging materials, printed papers, corrugated boxes,
tissue papers, or paper boards. Instabilities appearing as curls or waviness at the paper
sheet scale are moreover significantly dependent on bond stiffness. In this study, the main
objective is therefore to examine the effect of the bond stiffness on the sheet-scale response
of paper network, and to critically review the assumption often made in earlier works (i.e.,
full kinematic tying in the inter-fibre bonds).
Several earlier works consider bonds between the fibres to be rigid, for both 2D and 3D
configurations (Bronkhorst,2003;Mao et al.,2017;Bosco et al.,2017;Ostoja-Starzewski
and Stahl,2000;Lee and Jasiuk,2013;Stahl and Cramer,1998). A limitation of such a
bond description is its inability to describe the influence of inter-fibre connectivity on the
sheet scale deformations, as well as the extent to which certain fibre network properties (e.g.,
bond area or bonding stiffness) affect the macroscale response that can be modified in the
manufacturing process. Some other works, on the other hand, described the bonds as flexible
and not rigid, using for instance springs (Heyden,2000). The fibres were partially bonded in
regions of overlap (Koh and Oyen,2012), and were modelled based on a non-linear contact
law with bond failure (Kulachenko and Uesaka,2012), or as two-node line elements (Liu
et al.,2011). Studies by Ramasubramanian and Perkins (1988) and Perkins (1990) consider
the shear stresses and inelastic behaviour to be present in the bonds, hence assuming their
deformability. However, most of the literature that incorporates the deformation in bonds
relates only to the response of networks under mechanical loading. Analysis and modelling
of the hygro-mechanical behaviour and the anisotropic response of the network due to non-
rigid bonds are not available, which especially in 3D entail costly computations that prevent
assessing parametric variations of the bond effect. Even though for hygro-mechanics only
perfect bonding is relevant, a perfect bonding in 3D reality is not equivalent to full compat-
ibility in 2D. There is therefore a need to understand the hygro-mechanical response of the
networks due to varying bonding properties (stiffness) connecting the fibres, along with its
influence on the anisotropy of the network using a computationally efficient 2D modelling
framework.
In this contribution, such issues are addressed by describing the inter-fibre connectivity
through an appropriate 2D bond model, starting with a periodic unit cell of randomly
generated rectangular strips (Samantray et al.,2020) that represent ribbon-shaped paper
fibres. Each fibre in the unit cell network is discretized with standard triangular finite
elements. At the regions of inter-fibre bonds, additional triangular elastic interfacial elements
with a suitable stiffness, connecting two successive fibres (in the thickness direction), are
inserted in the model. These finite stiffness elements render the bonds to be no longer
rigid and the connected fibres can therefore have relative displacements through induced
elasticity. Note that, although possible, no dissipation within the interfacial layer (plasticity
nor damage) is assumed within the inserted layer, and hence modelling of degradation of the
bond is not adopted in this work. With this model, the macroscopic behaviour of the paper
network with different values of the bond stiffness can be computed when subjected to an
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external mechanical load or a uniform moisture variation. This provides clear insights in the
sheet level response using a 2D network model with moderate computational efforts only,
while incorporating key elements of the full 3D reality. The influence of the connectivity
between fibres at the bonds on the anisotropy of the paper network at the sheet scale can
furthermore be assessed.
The contents of this manuscript is organized as follows. In Section 2, the hygro-mechanical
model for the fibre and the network is described. This includes the generation of random
networks, the bond model, and the adopted numerical discretization together with consid-
ered stacking of fibres in the network. Obtained results, illustrating the influence of the bond
stiffness at the sheet level response of the network along with its anisotropy, are detailed in
Section 3. The conclusions are finally drawn in Section 4.
Throughout this contribution, the following notation is used for operations on Cartesian
tensors and for tensor products. Scalars, vectors, and tensors are denoted as a,~a, and
A. For tensor and vector operations, the following equivalent notations are used, with
Einstein’s summation convention on repeating indices: A:B=Aij Bji, where i=x, y, z,
for the global reference system, and i=l, t, z, for the fibre local reference system. The Voigt
notation employed to represent tensors and tensor operations in a matrix format uses a
and Ato denote a column matrix and a matrix of scalars; matrix multiplication then reads
A b =Aij bj.
2. Hygro-mechanical constitutive model and numerical discretization
2.1. Fibre model
Consider a 2D configuration with plane stress assumption in the z-direction (with z
normal to the paper sheet). This assumption is adopted because a fully-complex 3D model
may easily become computationally too expensive, especially for parametric studies. The
3D reality is hence simplified by considering only the mid-planes of the fibres, see Fig. 3b
where a pair of bonded fibres is depicted. Such assumption is adopted because the main
objective of this work is to seek information about the role of stiffness in the bond on the
hygro-expansion and anisotropy of the paper networks, with affordable computational costs.
Since computational efforts are limiting in full 3D simulations, the herein proposed model
is formulated in two dimensions while accounting for the key mechanisms of a full three-
dimensional reality through bond elasticity. Earlier-mentioned instabilities, such as curls or
waviness, could be incorporated within the proposed model by introducing shell elements
instead of plane stress elements. Under such assumptions, the hygroscopic strain tensor hεf
and the stress tensor in a fibre fare given by the constitutive relations
hεf=βfχ, (1)
σf=4Cf: (εfhεf),(2)
where σf,4Cf,εf, and βfare the stress tensor, the elastic stiffness tensor, the strain tensor,
and the hygroscopic expansion tensor of the fibre. The variable ∆χ=χχ0then denotes
change in the moisture content relative to the reference value χ0, where the moisture content
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摘要:

Roleofinter- brebondsandtheirinuenceonsheetscalebehaviourofpaper brenetworks?P.Samantraya,b,c,R.H.J.Peerlingsa,T.J.Massartb,O.Rokosa,,M.G.D.GeersaaMechanicsofMaterials,DepartmentofMechanicalEngineering,EindhovenUniversityofTechnology,P.O.Box513,5600MBEindhoven,TheNetherlandsbBuilding,Architecturea...

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