Moisture transport in paperboard

Test method development

Merit Lassing
Department of Chemical Engineering, Lund University

Abstract Paperbased packaging material is used as a container for preserved food. During the retorting
process, problems sometimes occur where the paperbased material absorbs too much moisture and looses
its stability. To find a solution to this problem, the properties of the paperboard must be known at elevated
temperatures and pressure. In this work a test apparatus was developed in order to measure the moisture
transport through the paperboard at the conditions in a retort. The test data was used in a convection and
diffusion model, were the effective diffusivity for water vapor in the paperboard was estimated.
The results were compared to earlier experimental data for paperboards and the diffusivities for water vapor
in air and paper fibers. The effective diffusivity of water vapor in paperboard was found to be higher than
for paper fibers, but lower than for air. Compared to other paperboard materials, the diffusivity for the Tetra
Recart board was somewhat lower.

Introduction Preserving food by canning is a com- The relative humidity depends on the temperature
mon method to give the food long term durability and which changes pw,s and the pressure which changes
temperature resilience. Recently, new retorting tech- pw in a closed system. The partial pressure for water
niques have enabled new packaging materials, one of vapor at saturation is expressed as
them is Tetra Recart which is paperboard-based. The
3816.44
Tetra Recart packaging material consists of 65% pa- pw,s = 133.32 · e(18.3036− T +227.03 ) (2)
perboard which has been laminated with several lay-
ers of polypropylene and one layer of aluminium foil The partial pressure of water vapor, pw , is described
to make the material retortable and provide a sealed by [2]
barrier around the food. pw = yH2 O · P (3)
When sterilizing the filled paperboard box, steam
and pressurized air is mixed in the retort. The en- Moisture transport Mass transfer by diffusion oc-
vironment is moist and hot with pressure changes, curs when the total pressure is constant while the
not the most suitable for a paperboard material. It concentrations of a certain component are different.
is therefore important to know the properties of the When there is a bulk transport of a component, it is
packaging material at the conditions in the retort. described by the convective transport.
When the concentrations changes over time, a
Packaging material Paperboard consist of fibers transient analysis of the mass transfer is required.
which form flocs. Due to the properties of the fiber The general equation for mass transfer is used.
and the manufacturing process, there are three differ-
∂CA ∂CA ∂CA ∂CA
ent directions of paperboard. MD which is the ma- + vx + vy + vz = (4)
chine direction of the in-plane surface and CD which ∂t ∂x ∂y ∂z
 2
∂ 2 CA ∂ 2 CA

is the cross machine direction of the in-plane surface. ∂ CA
= DAB + + + RA
Finally there is the z-direction which is across the pa- ∂x2 ∂y 2 ∂z 2
perboard thickness.[1]
On the left hand side there is the accumulation and
the convective transport in the different directions.
The air-water system The concentration of water
On the right hand side there are the terms for diffu-
vapor in air can be expressed by relative humidity.
sive transport and chemical reactions.
pw
RH = (1)
pw,s

1
 If there is no chemical reaction and transport only
occurs in one direction the equation will be [3]
 2 
∂CA ∂CA ∂ CA
+ vx = DAB (5)
∂t ∂x ∂x2
The convective term for mass transfer through
a stagnant component where flux is caused by both
convection and diffusion is expressed by
−DAB dCA
v= (6)
Ctot − CA dx
The equation for mass transfer in one direction, with
no chemical reaction will then be [3]
 
∂CA −DAB ∂CA ∂CA
+ = (7)
∂t Ctot − CA ∂x ∂x
 2 
∂ CA
= DAB Figure 1: Test apparatus - moisture transport is
∂x2
shown by the arrows. 1. packaging material and
Method The goal was to develop a moisture trans- silicone seals, 2. RH and temperature transmitter 3.
port test apparatus which allowed diffusivity mea- pressure transmitter 4. pressure equalizer
surements in the lateral direction, for both the MD
and CD. Due to symmetry, 1/4 of the actual test apparatus
Water vapor is transported from the humid auto- geometry was drawn in the model, which consisted
clave, through the paperboard into the apparatus. The of three subdomains.
concentration of water vapor inside is measured us-
ing relative humidity, temperature and pressure trans- • The packaging material. Only the paperboard,
mitters. The volume of the apparatus is known which with a total thickness of 1.5 mm, was consid-
means the amount of transported water vapor can be ered. The thickness of polypropylene and alu-
estimated. Figure 1 shows the principle of the test minum was neglected since the diffusivities in
apparatus. The packaging material is placed horizon- these layers are much smaller than in paper-
tally on top of the apparatus in between silicone rub- board. The length of the packaging material
ber seals, and the equipment is sealed using a metal was 10mm.
lid and clamps. The only moisture transport into the
apparatus should be through the paperboard. • The thin air space between the lid and the test
The test apparatus was placed in the autoclave apparatus was assumed to have the thickness
where the retort programme held the temperature and of the packaging material and silicone seals,
pressure constant at 125◦ C and 3.8 bar for one hour. which meant a total thickness of 4 mm. The
A reference test was performed without the packag- length of this layer was 20 mm.
ing material, to see if there was any background leak- • The void space inside the test apparatus was
age of moisture. When investigating the diffusion assumed to be rectangular, with 1/4 of the test
through the packaging material, a stack of five sam- apparatus volume at 3.8 bar and 125◦ C.
ples with 10 mm diffusion length were used.
Obtained relative humidity data was recalculated The properties of the three subdomains are de-
to concentrations of water vapor. The concentrations scribed by the parameters in table 1.
were used in COMSOL Multiphysics when simulat- The diffusivity in the air, Dair , was estimated
ing the moisture transport to find a corresponding dif- to 1.1·10−5 m2 /s, using equation 3.15 in [3]. The
fusivity. In COMSOL, the 3D convection and diffu- background leakage into the test apparatus was esti-
sion model was found to be suitable, which uses the mated to 0.0023 mol/(m2 ·s) using the concentration
general equation for mass transfer.

2
Table 1: Properties of the packaging material, the
thin air layer and the void space

Subdomain Paper- Thin air Inside

parameter board layer space

Diffusion, D Dair Dair

D [m2 /s]
Convective flux
−D dc −Dair dc
-x-direction, Ctot −c dx Ctot −c dx 0
u [m/s]
−D dc −Dair dc
-y-direction, Ctot −c dy Ctot −c dy 0
v [m/s] Figure 2: Concentration change in the experiments.
-z-direction, 0 0 0
w [m/s] The background leakage also seemed to be repete-
Reaction, R 0 0 0.023 tive, since similar results were obtained on different
[mol/(m3 s)] occasions. When the leakage was taken into con-
sideration, the water vapor increase due to diffusion
through the packaging material could be measured.
Simulation was performed on each experiment.
data from the reference test. It was expressed as a re- The time span was 3340 s, the same time as the test
action parameter in the void space in the model. The apparatus had held 125◦ C at 3.8 bar pressure dur-
initial concentration inside the test apparatus was de- ing the retort tests. Simulated results can be seen in
cided by each experiment. The water vapor con- figures 3 and 4. The initial concentration of water
centration in the autoclave was assumed to be 70.4 vapor inside the test apparatus and the outer concen-
mol/m3 , which is the concentration of water vapor at tration in the autoclave was given as boundary condi-
3.8 bar and 125◦ C when RH is is 100%. The initial tions in COMSOL. The effective diffusivity in paper-
concentration of water in the packaging material was board was estimated to a value where the simulated
assumed to be the same as inside the test apparatus. end concentration was the same as the obtained end
The diffusivity was assumed to be isotropic. concentration in the experimental data.

Results The experimental concentrations of water

vapor can be seen in figure 2. The results from the
experiments were found to be similar.

Table 2: Relative humidity and concentration inside

the test apparatus at the start and end of the tests

RH [%] C [mol/m3 ]
start end start end
Test 1 28.7 54.4 20.2 38.3
Test 2 30.1 55.1 21.1 38.8
Test 3 31.1 56.9 21.9 40.1
Test 4 29.9 56.9 21.1 40.0
Test 5 32.5 57.3 22.9 40.3
Ref. test 20.5 32.9 14.5 23.2 Figure 3: The simulated concentration change inside
the void space of the test apparatus.

3
 m2 /s [5]. This value was recalculated to an estimated
value for 125◦ C and 3.8 bar, using the temperature
proportional dependence for diffusivity, ∼ T 1.5 to ∼
T 2.0 , and the inversely proportional pressure depen-
dence, 1/P. The diffusivity was then 3.0·10−6 m2 /s
which is about ten times larger than the measured
diffusivity for the Tetra Recart material.
Finally it should be noted that the COMSOL model
is simplified and could be improved. When test data
is compared to simulated concentrations, the exper-
imental data shows a non-linear increase, while the
simulated concentrations increase almost linearly.
The concentration curve should have a slightly non-
linear behavior as the difference between the out-
side and inside concentration decrease. However, the
measured concentration curve levels out before the
Figure 4: A COMSOL illustration of the concentra- concentrations are equal which could be explained
tion gradient in the simulated model. by the swelling of paper fibers. Furthermore, the
background leakage term in the model has no depen-
The diffusivity of the paperboard was estimated dence of the autoclave concentration which means it
to 4.2 · 10−7 m2 /s with a standard deviation of 2.5 · does not abate as the concentrations levels out.
10−8 m2 /s, as can be seen in table 3.
Conclusions Comparisons between the effective dif-
fusivity for the Tetra Recart paperboard and exper-
Table 3: The diffusivities of the Tetra Recart paper-
imental data for other paperboard materials showed
board, obtained by simulation.
some differences. It is however diffucult to make any
clear conclusions considering that there is no previ-
Diffusivity D [m2 /s]
ous data for diffusivities at the elevated temperature
Test 1 4.07 · 10−7
and pressures. The obtained diffusivity is however
Test 2 4.00 · 10−7
much higher than the diffusivity of water in paper-
Test 3 4.34 · 10−7
board fibers which suggests that the studied transport
Test 4 4.60 · 10−7
mechanism does not occur solely through the fibers.
Test 5 4.09 · 10−7
Further tests are needed before any clear conclu-
Average 4.2 · 10−7
sions can be made regarding the accuracy of this test
Standard deviation 2.5 · 10−8
apparatus and the paperboard properties at elevated
temperatures. Furthermore, there is need for some
improvements to the COMSOL model.
The simulated model in figure 4 shows a concen-
tration gradient in the paperboard. This agrees with Nomenclature
the moisture profile that could be seen by inspection
of the samples just after retorting. C Concentration [mol/m3 ]
Earlier studies by Foss et al estimated the diffu- DAB Diffusivity, comp. A in comp. B [m2 /s]
−14 2
sivity to 3.8·10 m /s for water in paper fibres at Ni Flux of component i [mol/m2 s]
◦
23 C and atmospheric pressure [4]. The diffusivity Ptot Total pressure [P a]
in paper fibers is therefore much lower than the ef- pw Partial pressure of water vapor [P a]
fective diffusivity through Tetra Recart paperboard. pw,s Partial pressure of water vapor at sat.[P a]
Most likely, the diffusion in the paperboard does not RA Chemical reaction of component A
follow the same mechanisms as pure fiber diffusion. RH Relative humidity [%]
Earlier experiments on TBA material at 23.7◦ C t Time [s]
and 1 atm gave an effective diffusivity of 7.17·10−6 T Temperature [◦ C]

4
 vi Convective flow term, i:th direction [m/s]
yi Mole fraction of component i

References
[1] Pappersteknik, Fellers, C., Norman B., Avd. för
pappersteknik, KTH, 1996

[2] ”Systemet luft-vatten” (literature for the course

Sep. FK.), Stenström, S., Dept. Chem. Eng.,
Lund University, 2004

[3] ”Transportprocesser” (literature for the course

Sep. FK.), Stenström, S., Dept. Chem. Eng.,
Lund University, 2004

[4] Simultaneous heat and mass transport in paper

sheets during moisture sorption from humid air,
Foss, W.R. et al, Int. J. Heat and Mass Transfer
(2003) vol 46. p.2875 − 2886

[5] Diffusion i kartong, experimentell bestämning

av diffusionskoefficienter i PaToF-projektet,
Andersson E, Dept. Chem. Eng., Lund Univer-
sity (2001)