food and bioproducts processing 9 7 ( 2 0 1 6 ) 88–99

Contents lists available at ScienceDirect

Food and Bioproducts Processing

journal homepage: www.elsevier.com/locate/fbp

Mass transfer modeling in osmotic dehydration:

Equilibrium characteristics and process dynamics
under variable solution concentration and
convective boundary

H. Pacheco-Angulo a , E. Herman-Lara b , M.A. García-Alvarado a ,

I.I. Ruiz-López c,∗
a Unidad de Investigación y Desarrollo en Alimentos, Departamento de Ingeniería Química y Bioquímica, Instituto
Tecnológico de Veracruz, Av. M.A. de Quevedo S/N. Col. Formando Hogar, C.P. 91860 Veracruz, Veracruz, México
b Coordinación de Posgrado e Investigación, Departamento de Ingeniería Química y Bioquímica, Instituto Tecnológico

de Tuxtepec, Av. Dr. Víctor Bravo Ahuja S/N. Col. 5 de Mayo, C.P. 68350, Tuxtepec, Oax. , México
c Facultad de Ingeniería Química, Benemérita Universidad Autónoma de Puebla, Av. San Claudio y 18 Sur. Ciudad

Universitaria, Puebla, Puebla, México

a r t i c l e i n f o a b s t r a c t

Article history: The aim of this study was to model both the dynamic and equilibrium mass transfer periods
Received 22 April 2015 for water, osmotic solute and food solids interchange between product and solution during
Received in revised form 10 an osmotic dehydration (OD) process. The OD model is able to represent situations where
November 2015 concentration of osmotic media changes during the process or where interfacial resistance
Accepted 25 November 2015 to mass transfer cannot be neglected. Water and solute are considered to move within the
Available online 8 December 2015 product by a diffusion mechanism based on Fick’s second law, while external convective
mass transfer is considered in the fluid. The state-space form of the model is analyti-
Keywords: cally solved for one-dimensional mass transfer in products with flat slab, infinite cylinders
Interfacial resistance and sphere geometries. The developed theory was applied to the analysis of equilibrium
Mass Biot number and OD dehydration curves of carrot slices obtained at 40 ◦ C in sodium chloride solutions
Mass transfer with and without stirring and different ratios between solution volume and product mass.
Osmotic dehydration Water and NaCl diffusivities were identified in the narrow ranges of 6.0–7.6 × 10−10 m2 /s
Variable solution concentration and 3.5–4.1 × 10−10 m2 /s, respectively, demonstrating the applicability of the proposed model
Equilibrium distribution under a wide range of operating conditions.
© 2015 The Institution of Chemical Engineers. Published by Elsevier B.V. All rights reserved.

1. Introduction
Osmotic dehydration is a solid–liquid contact operation
involving the immersion of food products, especially fruits
and vegetables, in hypertonic solutions such as brines or
syrups. When the food is immersed in the solution, an osmotic
pressure gradient is developed between the involved phases
originating a dynamic mass transfer period in which water
is removed from food toward the liquid media with a simul-
taneous solute gain by the product (Khan et al., 2008; Goula
and Lazarides, 2012; Herman-Lara et al., 2013; Souraki et al.,
2013, 2014). If processing is performed for a long enough
time, then both water loss and solute gain reach a stationary
state, where the driving potential for mass transfer between
food and solution becomes zero (Sablani and Rahman, 2003;
Herman-Lara et al., 2013). This operation involves several mass

∗
Corresponding author. Tel.: +52 222 2295500x7250.
E-mail addresses: irving.ruiz@correo.buap.mx, irvingisrael@hotmail.com (I.I. Ruiz-López).
http://dx.doi.org/10.1016/j.fbp.2015.11.002
0960-3085/© 2015 The Institution of Chemical Engineers. Published by Elsevier B.V. All rights reserved.
 food and bioproducts processing 9 7 ( 2 0 1 6 ) 88–99 89

Nomenclature
 dynamic viscosity (Pa s)
A surface area available for mass transfer (m2 )  dimensionless group related with product-to-
A state-space matrix osmotic media mass ratio
aw water activity density (kg/m3 )
Bi mass Biot number (dimensionless)
chemical potential (J/mol)
C concentration (g/L)  dimensionless coordinate
d maximum inner diameter of flask (m) , dimensionless concentration in product: local
D diffusion coefficient (m2 /s) and average, respectively
F Faraday constant (96485.34 C/mol)
Fo Fourier number for mass transfer (dimension- Subscripts
less) 0 at beginning of the process
g gravitational constant (9.81 m2 /s) ◦ at infinite dilution
Gr mass Grashof number (dimensionless) f denotes food solids
kc convective mass transfer coefficient (m/s) e at equilibrium
Ke equilibrium partition coefficient (kg product/kg i at the product–solution interface
osmotic media) j denotes either water or osmotic solute
L, Lc characteristic lengths for diffusion and convec- k denotes node numbering
tion, respectively (m) o denotes osmotic media
m solute molality (mol solute/kg solvent) p denotes product
m mass in product (kg) s denotes osmotic solute
M mass in osmotic media (kg) t at time t
n number of nodes w denotes water
N number of components
n+ , n− valences of cation and anion, respectively
(dimensionless) transfer mechanisms; however, diffusion of water and solute
R gas constant (8.314 J/mol K) within product are usually considered the controlling factors,
Re Reynolds number (dimensionless) usually described by Fick’s second law (Kaymak-Ertekin and
Sc Schmidt number (dimensionless) Sultanoğlu, 2000; Rastogi and Raghavarao, 2004; Goula and
Sh Sherwood number (dimensionless) Lazarides, 2012; Souraki et al., 2012; da Silva et al., 2013, 2014;
t time (s) Rodríguez et al., 2013).
T temperature (K) Depending on modeling assumptions, non-steady-state
u axial or radial coordinate (m) diffusion equation may be solved under analytical or
U food solids-to-(osmotic solute + water) mass numerical techniques (Kaymak-Ertekin and Sultanoğlu, 2000;
ratio in product (kg/kg) Porciuncula et al., 2013; Rodríguez et al., 2013); however, the
v orbital velocity (1/s) use of analytical models remains widespread due to sev-
V volume (m3 ) eral practical advantages, including easier implementation
X mass fraction of a given component in product and lower computational effort. Analytical solutions for OD
(kg/kg product) process in well-stirred systems (i.e., those with negligible
X* mass fraction in product free of food solids external resistance to mass transfer) can be classified in
(kg/kg osmotic solute + water) two main groups based on the available amount of work-
X state-space vector ing solution (Crank, 1975). Most studies consider an infinite
Y mass fraction of a given component in solution volume of osmotic media (i.e., of constant concentration;
(kg/kg solution) Rastogi and Raghavarao, 2004; Rodríguez et al., 2013; Souraki
Y* mass fraction in solution free of food solids (kg et al., 2012, 2013, 2014), experimentally achieved by using
osmotic solute + water) mass ratios between solution and product of 10 and above
x1 , x2 coded temperature and time, respectively (Herman-Lara et al., 2013). The use of lower ratios between
W food solids-to-(osmotic solute + water) mass osmotic media and product may result in an appreciable
ratio in osmotic media (kg/kg) decrease of solute concentration during product impregna-
tion, affecting water loss and solute gain rates as well as
Greek letters final dehydration and impregnation levels at equilibrium.
˛ parameter defining product geometry Therefore, special analytical solutions considering a finite vol-
ı mass ratio between osmotic media and product ume of osmotic media (i.e., of variable concentration) should
ε volume fraction occupied by osmotic media (m3 be applied in these cases (Singh et al., 2007; Bellary et al.,
solution/m3 solution + product) 2011), or alternatively, resort to a numerical solution allow-
ϕ thermodynamic factor (dimensionless) ing the use of additional assumptions such as variable mass
 dimensionless concentration in solution of involved phases (Kaymak-Ertekin and Sultanoğlu, 2000). As
± mean ionic activity coefficient of solute (dimen- a diffusion-controlled process is presumed in the aforemen-
sionless) tioned models (Crank, 1975), these may not be applicable to
◦+ , ◦− limiting (zero-concentration) ionic conduc- describe experimental conditions where convective resistance
tances of cation and anion, respectively to mass transfer may occur (for example, processes conducted
(S m2 /mol) without or with mild stirring), which may be required in prod-
ucts with fragile structures.
90 food and bioproducts processing 9 7 ( 2 0 1 6 ) 88–99

Analytical solutions considering both diffusion and con- Similarly, the mass ratio between food solids and the sum
vection at product surface have also been developed and are of osmotic solute and water in product and osmotic media are
expressed in terms of a mass Biot number (Crank, 1975), whose defined as
value may be used to identify the controlling mechanism (da
Xf Yf
Silva et al., 2013, 2014). A well-known fact in mass trans- U= and W= (4)
fer operations is that any solute will not distribute equally Xs + Xw Ys + Yw
between two or more phases due to different chemical and
Above expressions are related with regular mass fractions
physical affinities (Corzo and Bracho, 2004; Toğrul and İspir,
either of water or osmotic solute by simply algebra (for j = s, w)
2008). Consequently, an equilibrium relationship is required
to completely characterize a multiphase system. In drying, for Xj∗
example, the equilibrium water contents in product and air Xj = (5)
1+U
are related through the sorption isotherm, and a mean parti-
tion constant should be used to obtain the correct mass Biot Yj∗
definition to apply the existing analytical solutions. In order Yj = (6)
1+W
to consider a convective boundary condition in the OD model,
some studies have considered that product and solution equil- 2.2. Description of mass transfer equilibrium
ibrate at the same concentration (da Silva et al., 2013, 2014).
However, the use of models with convective boundary in OD According to equilibrium thermodynamic theory (Gibbs, 1876),
processes is close to non-existent because: (i) equilibrium data a necessary and sufficient condition for mass transfer equilib-
are scarce and should be experimentally obtained, (ii) existing rium in OD process is given by,
analytical solutions are only applicable for solutions of infinite    
volume (Crank, 1975) and (iii) physical properties necessary to
j =
j (7)
product osmotic media
evaluate convective mass transfer coefficient (such as viscos-
ity and density of solution, or diffusivity of solute in osmotic or, equivalently, in terms of water activity (Barbosa-Cánovas
media) are not readily available in comparison with other well- and Vega-Mercado, 2010)
characterized systems such water vapor–air mixtures.
The objective of this study was to develop a rigorous model (aw )product = (aw )osmotic media (8)
to describe the simultaneous water and solute interchange
between product and solution during an OD process, applica- According to Ross (1975), water activity in a multi-
ble under any ratio between product and osmotic media and component system can be developed as the product sequence
any convective mass transfer condition. To fully achieve this of water activities of each involved solute in a series of binary
purpose the following topics were covered: (i) mathematical mixtures. In this case,
description of mass equilibrium during OD, (ii) development
of a general model for unsteady state mass transfer of dif- N
aw = ˘ awi = aws awf (9)
fusing substances, (iii) evaluation of diffusion coefficients of i=1
water and solute and (iv) assessment of dominant mass trans-
fer phenomena under different experimental conditions. The Components such as proteins and carbohydrates, etc., are
model was validated using experimental OD data of carrot all lumped in Eq. (9) in the mixture of food solids. Since
slices in NaCl solutions. the effect of a given solute on water activity depression
mainly depends upon its molar fraction (Barbosa-Cánovas
and Vega-Mercado, 2010), it is clear that high-molecular
2. Theory
weight substances originally present in product such as
proteins, oligo- and polysaccharides will have a negligible
2.1. Basic definitions effect on water activity depression and thus in mass trans-
fer equilibrium. On the other hand, the impact of mono and
In order to develop an equilibrium relationship for OD process, disaccharides such as fructose, glucose and sucrose on OD
it will be considered that product (p) and osmotic (o) media are equilibrium will depend on the original amount of these sub-
made up from water (w), osmotic solute (s) and a mixture of stances in product and their lixiviated fraction, and the type
solids (f) which are naturally present in the product and may and concentration of osmotic solute. However, their effect on
leach into the osmotic solution, such as carbohydrates, fat and water activity depression may be also considered negligible
proteins. According to this assumption, under most OD processes performed with brines or syrups,
as will be later demonstrated. Therefore, if food solids do not
Xf + Xs + Xw = 1 (1) contribute to the water activity depression (awf ≈ 1) and the
osmotic solution is not in saturation, then mass transfer equi-
librium will be reached when the compositions of the binary
Yf + Ys + Yw = 1 (2)
mixtures between water and osmotic solute (i.e., excluding
food solids) in involved phases satisfy (for j = s, w)
where, X and Y represent the mass fractions of a given compo-
∗ ∗
nent in product and osmotic media, respectively. Let us define Xje = Yje = (1 + Ue ) Xje = (1 + We ) Yje (10)
the fractions of osmotic solute or water free of leaching food
solids in involved phases as (for j = s, w) From Eq. (10) it is clear that mass compositions Xje and Yje
are related by (for j = s, w)
Xj Yj
Xj∗ = and Yj∗ = (3) Yje = Ke Xje (11)
Xs + Xw Ys + Yw
 food and bioproducts processing 9 7 ( 2 0 1 6 ) 88–99 91

1 + Ue equilibrium relationship relating mass fraction of specie j in

Ke = (12)
1 + We osmotic solution with those of the other components in prod-
uct and may have multiple mathematical representations.
Two important results are derived from Eqs. (11) and (12)
under the given assumptions: 2.4. Dimensionless form of osmotic dehydration model

(i) Partition coefficient (Ke ) is the same for both water and In this study, OD model is solved in dimensionless form under
osmotic solute. the following assumptions:
(ii) Ke is always greater than unity (since Ue > We ).
(1) Product has a constant density.
Additionally, if Ke does not change with the concentration (2) Apparent diffusivities of both solute and water in product
of osmotic solution, then the following statements apply: are constants.
(3) Mass transfer occurs in one direction in products with flat
(i) Equilibrium compositions for water and osmotic solute slab, infinite circular cylindrical or spherical geometries.
distribute along a straight-line equation with zero inter- (4) Equilibrium relationship Eq. (19) is given by Eq. (11).
cept.
(ii) Mass fraction of water in osmotic media at equilibrium Thus, Eqs. (16)–(19) can be rewritten as (for j = s, w),
only depends on its corresponding fraction in product.
The same statement holds for solute. ∂ ∂2 ˛∂ j
j j
(iii) Unsteady-state equations for water and osmotic solute = + (20)
∂Foj ∂ 2  ∂
concentrations can be solved independently from each
other. dj  
= − (˛ + 1) Bij ji + j (21)
dFoj
The previous statements still apply if it is considered
that food solids are not lost during OD process (We = 0 and ∂ ji  
Ke = 1 + Ue ). By assuming a negligible net mass change between = −Bij ji + j (22)
∂
involved phases, the following steady-state mass balance can
be written (for j = s, w) where, ˛ takes value 0, 1, or 2, for infinite slabs, infinite
cylinders or spheres, respectively, while the following dimen-
mp Xj0 + Mo Yj0 = mp Xje + Mo Yje (13) sionless variables and groups were introduced

Finally, the combination of Eqs. (11) and (13) produce the fol- Xj − Xje Yj − Yje Dj t u
j = ; j = ; Foj = ; = (23)
lowing key relationships Xj0 − Xje Yj0 − Yje L2 L

Yj0 − Yje mp kc o 1 mp AL
=− =−
1
(14) Bij = Ke   ; = ; = (˛ + 1) (1 − ε) (24)
Xj0 − Xje Mo ı Djp /L p Ke Mo Vop

Xj0 + ıYj0 Here u and L represent the mass transfer direction (axial or
Xje = (15)
1 + ıKe radial) and the characteristic length for diffusion, respectively.
It can be observed that solution of dimensionless Eqs. (20)–(22)
2.3. General model for osmotic dehydration process only depends on parameters ˛, Bij and . Eq. (22) satisfies the
following limits:
The following equation system describes the mass transfer of
specie j (j = 1, . . ., n) between disperse and continuous phases ∂ ji
= −Bij ji for  → 0 (25)
in an OD process (without chemical reactions): ∂
 
∂ p Xj    ji =0 for  → 0 , Bij → ∞ (26)
= ∇ · Djp ∇ p Xj (16)
∂t
  ji = −j for Bij → ∞ (27)
d εVop o Yj  
= kc A o Yji − Yj (17)
dt Eqs. (25)–(27) represent the boundary conditions for (i)
    convective boundary with infinite surrounding media, (ii)
−Djp ∇ p Xji = kc o Yji − Yj (18) diffusion-controlled process with infinite surrounding media
and (iii) diffusion-controlled process with finite surrounding
Yji = fj (Xki ) for k = 1, . . ., n (19) media, respectively. Thus, Eqs. (20)–(22) share the analytical
solutions provided by Crank (1975) in these circumstances.
where, Vop is the combined volume of product and osmotic For simplicity but without loss of generality, the subscript j
media, kc is the convective mass transfer coefficient, A is the is hereafter dropped from equations.
surface area available for mass transfer, ε is the volume frac-
tion occupied by osmotic media, and the subscript i indicates 2.5. State-space representation of OD model and
at the product–solution interface. Eqs. (16) and (17) represent analytical solution
both the concentration change of specie j within a homoge-
neous and isotropic solid by diffusion and in osmotic solution Eq. (20) can be expressed as an equivalent system of ordinary
by convection, respectively, while Eq. (18) express the mass differential equations by using a discrete representation of
flux between product surface and bulk solution. Eq. (19) is an spatial derivatives. If central finite differences are used, then
92 food and bioproducts processing 9 7 ( 2 0 1 6 ) 88–99

the following model is obtained for 1 ≤ k ≤ N, where k repre- same advantages and limitations of the analytical ones pro-
sents a point in space vided by Crank (1975) (such as constant partition coefficient,
constant product density, etc.), with the added benefit that it
d k k+1 −2 k+ k−1 ˛ k+1 − k−1 can move between limiting cases. However, product shrinkage
= + (28)
dFo ()
2 (k − 1)  2 or variable diffusivity could be also considered in the current
model by updating matrix A during time.
Points outside of the boundary where k < 1 or k > N, i.e., k+1
for k = N (interface) and k−1 for k = 1 (center), can be estimated 3. Methods
by applying convective boundary Eq. (22) and a symmetry con-
dition (only half domain is solved). Thus, 3.1. Osmotic dehydration experiments

k+1 = k−1 − 2Bi ( k +  ) for k=N (29) The developed theory was applied to the analysis of OD data
sets using carrot as the food model system. All experiments
k−1 = k+1 for k = 1 (30) were conducted in NaCl solutions at a temperature of 40 ◦ C.
Fresh carrots, approximately 10 cm-long and 2.7 cm-diameter,
Eqs. (21) and (28)–(30) can be combined to form the state- were locally purchased (Puebla, Pue., México) and processed
space representation the same day. Carrots were washed, dried with a cloth and
then mechanically cut into circular 0.3 cm-thick slices with-
dX out removing the peel. On average, 4 slices were obtained
= AX (31)
dFo from the central part of each root while remaining portions
were reserved for the initial water/dry solids analysis. Carrot
where the state-vector X ∈ RN+1 is defined as
slices were OD-processed in separated dilution bottles placed
  in a controlled-temperature water bath (±0.1 ◦ C), which were
XT = 1 2 ... N  (32)
allowed to equilibrate before introducing samples. Samples
were osmodehydrated in separated bottles to eliminate varia-
and the non-zero elements of state-space matrix A ∈
tions in the solution-to-product ratio and avoid the mixing of
R(N+1)×(N+1) are
solution (in free convection experiments) that are introduced
a (1, 1) = − 2
; a (1, 2) = 2 by sampling removal when all samples are processed in a sin-
()2 ()2
(33)
gle recipient.

2
⎫ The following variables were recorded from these exper-
a (i, i) = − ⎬ iments at the beginning and during OD process: water
()2
for 1 < i < N (34) fraction in product (Xw ), volumetric NaCl concentration
a (i, i ± 1) =
2(i−1)±˛ ⎭
2(i−1)() 2 (g/L) in osmotic media (Cs ), product mass (mp ) and solution
mass (Mo ). Water fraction in product was determined by
a (N, N − 1) = 2
; a (N, N) = −
[2(N−1)+˛]Bi+2(N−1) oven-drying the samples until constant weight was attained
(35)
()2 (N−1)()2
(when mass change was less than 0.001 g over and 8-h
period). On the other hand, NaCl concentration in osmotic
−[2(N−1)+˛]Bi
a (N, N + 1) = (36) media was determined with a sodium ion meter (HI 931101,
(N−1)()2
Hanna Instruments, Woonsocket, RI, USA). Corresponding
a (N + 1, N) = − (˛ + 1) Bi; a (N + 1, N + 1) = − (˛ + 1) Bi (37) NaCl fractions in osmotic media (Ys ) were calculated from
the volumetric solution concentration (Cs ) and its density
Eq. (31) is an homogeneous linear time-invariant system of ( o ). Several experiments were completed in order to fulfill
ordinary differential equations, which accepts the well-known different objectives as follows. A brief description of all
solution (Ogata, 2010) experiments is given in Table 1.

X (t) = eAFo X (0) (38) 3.2. Estimation of equilibrium relationship

Mean concentration of water and osmotic solute in prod- The first set of OD experiments was conducted to character-
uct can be estimated by applying a spatial-averaging of local ize the effect of brine concentration on the mass equilibrium
values (Whitaker, 1977) relationship between product and osmotic media by identify-
ing parameter Ke . Carrot slices were processed without stirring
1 1 under several brine concentrations (20, 40, 60, 80, 100, 120, 140,
˛
= dVp / dVp =  d/  ˛ d (39) 160, 180 and 200 g/L NaCl solution) with a fixed ratio between
Vp Vp 0 0
solution volume and product mass (Vo /mp ) of 4:1. In these
An explicit solution to Eq. (39) was developed in this study experiments, carrot slices were immersed in brines for a total
from the trapezoidal rule, giving the expression of 24 h. This time was considered long enough for reaching
mass equilibrium in the product within the proposed solu-

 tions according to previous similar studies with other plant
(˛ + 1)  
N−1
˛ ˛ ˛
= 0 1 +2 [(k − 1) ] k + [(N − 1) ] N materials (Herman-Lara et al., 2013). Mass balances for water,
2
k=2 osmotic solute and food solids allowed the straightforward
(40) estimation of Xse , Ywe , Ue , We and Ke by assuming Xs0 = 0 (prod-
uct initially has a negligible amount of osmotic solute) and
The state-space solution in Eq. (38) corresponds to a con- Yf0 = 0 (osmotic solution does not have food solids at the begin-
stant state-matrix A. In this case, the given solution shares the ning of the OD process).
 food and bioproducts processing 9 7 ( 2 0 1 6 ) 88–99 93

Table 1 – Summary of all experiment sets.

Experiment set Purpose Experimental conditionsa

Stirring (rpm) Cs (g/L) Vo /mp (L/kg)

1 Evaluate equilibrium coefficients 0 20–200 4:1

2 Estimate diffusion coefficients 190 100 20:1
3 Appraise external resistance to mass transfer 0 100 4:1
4 Appraise external resistance to mass transfer 0 100 20:1
5 Appraise external resistance to mass transfer 0 150 20:1

a
All experiments were conducted at 40 ◦ C.

3.3. Estimation of effective water and solute
diffusivities in carrot slices
Carrot slices were processed with a single brine concentration
(100 g/L NaCl solution) in separated dilution bottles (50 mm of
inner diameter) with a fixed Vo /mp ratio of 20:1. Bottles were
then placed in a thermal bath with orbital stirring (190 rpm).
The Vo /mp ratio was selected to avoid a significant dilution
of osmotic solution, while the high stirring speed was used
to allow for a negligible external resistance to mass trans-
fer (Herman-Lara et al., 2013). Samples were withdrawn from
the solution at predefined immersion times (5, 10, 15, 20, 25,
30, 40, 50, 60, 80, 100, 120, 150, 180, 210 and 250 min), gently
blotted dry with a paper towel to remove adhering osmotic
solution. Product and osmotic solution were analyzed for their
water/total solids content and NaCl as previously described.
Experimental OD curves (Xs vs t, Xw vs t) were fitted to OD
model formed by Eqs. (38) and (40) in order to estimate Ds
and Dw , where carrot samples were considered to be slabs
(˛ = 0) due to their dimensions. Parameter  was calculated
from experimental variables Ke , Vo , mp0 and Cs0 as well as
corresponding physical property o , estimated by solving Eq.
(A6). Equilibrium compositions were estimated with Eq. (15).
Osmotic solute fraction in product (Xs0 ) and food solids frac-
tion in solution (Yf0 ) were assumed to be negligible in the
same way as during the estimation of equilibrium relation-
ship. In this case, two scenarios were considered; OD model
was solved with (i) Bis = Biw = 1000 in order to consider a
diffusion-controlled process and (ii) Bis and Biw were simul-
taneously estimated with Ds and Dw .
3.4. Appraisal of external resistance to mass transfer
under no stirring conditions
Carrot slices were processed without stirring under the fol-
lowing conditions: (i) 100 g/L NaCl solution with a Vo /mp ratio
of 20:1, (ii) 100 g/L NaCl solution with a Vo /mp ratio of 4:1 and
(iii) 150 g/L NaCl solution with a Vo /mp of 20:1 (experiment sets
3–5 in Table 1). Remaining experimental details are the same
as above. Experimental OD curves were fitted to the proposed
model in order to estimate Bis and Biw using the values for Ds
and Dw determined as detailed in Section 3.3. Moreover, these
data were also used to evaluate Ds and Dw , where Bis and Biw
were determined in advance with the aid of empirical mass
transfer correlations.
3.5. Estimation of mass Biot number from empirical
relationships
The value of external mass transfer coefficient kc can be cal-
culated from empirical correlations for the Sherwood number
(Sh). For natural convection, these expressions are given in
terms of mass Grashof (Gr) and Schmidt (Sc) numbers. How-
ever, under forced convection conditions, the mass Grashof
(Gr) is replaced by Reynolds (Re) number. These dimension-
less groups are given below (Geankoplis, 1993; Büchs et al.,
2000):
L3c sw g sw vd2 sw sw Lc kc
Gr = , Re = , Sc = , Sh =
2sw sw sw Dsw Dsw
(41)
The Reynolds number (Re) definition in Eq. (41) is a special
form given by Büchs et al. (2000) for rotary shaking systems.
The following correlations have been recommended for mass
transfer around flat surfaces under natural (Geankoplis, 1993)
and forced convection (Basmadjian, 2004), respectively
Sh = 0.54(GrSc)1/4 (42)
Sh = 0.66Re1/2 Sc1/3 (43)
Convective mass transfer coefficients were calculated
under studied experimental conditions and further used to
estimate a theoretical Bi number according to the definition
given in Eq. (24) and properties summarized in Appendix A.
3.6. Data analysis
Nonlinear regression (based on ordinary least squares) was
used to estimate Ds , Dw , Bis and Biw according to the described
experiments (Table 1). Diffusion coefficients Ds and Dw were
individually fitted to experimental solute or water fraction
evolution curves from experiment set 2 by assuming a negligi-
ble external resistance to mass transfer (Bis and Biw were set to
1000) or a convective boundary (Bis and Biw were also fitted dur-
ing regression procedure). External resistance to mass transfer
in experiments conducted without stirring was appraised by
simultaneously fitting Bis to experimental solute and water
fraction evolution curves from experiment sets 3–5, where
corresponding value for water transport was calculated as
Biw = Ds Bis /Dw with Ds and Dw values obtained from exper-
iment set 2. In addition, Ds and Dw were also estimated by
fitting experiment sets 3–5 with mass Biot numbers calcu-
lated with empirical mass transfer relationships. A summary
of all properties used in unsteady-state model solution is pre-
sented in Table 2. The fitness quality of the identified model
was quantified by the generalized determination coefficient
(R2 ) and statistical significance of parameter estimates was
evaluated through their 95% confidence intervals (95% CI).
Nonlinear regression procedures as well as statistical analysis
were performed using Matlab Statistics Toolbox 7.3 (Math-
Works Inc., Natick, MA, USA).
94 food and bioproducts processing 9 7 ( 2 0 1 6 ) 88–99
Table 2 – Summary of variables used during solution of unsteady-state OD modela .
Experiment set Xw0 (g/g)b Cs0 (g/L)b
2 0.903 100.0
3 0.904 100.3
4 0.904 100.3
5 0.909 150.2
a
In all experiment sets: Xs0 = 0, Yf0 = 0, Ke = 1.08, ˛ = 0, N = 50, Xse and Xwe were calculated with Eq. (15).
b
Value determined during experiments.
c
Calculated by solving Eq. (A6).
d
Calculated from Cs0 .
e
Calculated with Eq. (24).
4. Results and discussion
4.1. Equilibrium and distribution data
Eq. (15) provides a simple way to estimate final dehydration or
impregnation levels in product based on experimental condi-
tions and equilibrium characteristics of product and osmotic
solute. This equation reduces to that previously reported by
Beristain et al. (1990) if Ke = 1, i.e., by considering that osmotic
media and product equilibrate at the same composition. How-
ever, in some cases the model proposed by Beristain et al.
(1990) has failed to provide a satisfactory prediction of experi-
mental mass equilibrium values (Parjoko et al., 1996). A quick
inspection of Eq. (15) reveals that overestimation of Xje will
occur for increasing values of the difference Ke − 1, a fact that
was previously observed by Parjoko et al. (1996) and is now
explained by the lack of a proper equilibrium term in the
model reported by Beristain et al. (1990).
Equilibrium data for water, NaCl and leached food solids
are summarized in Table 3. According to these data, Ke values
did not exhibit a significant change with osmotic media con-
centration (p < 0.05) (Fig. 1). Thus, Ke can be simply estimated
as the slope of the Yje vs Xje plot simultaneously consider-
ing data for both NaCl and water, as shown in Fig. 2. An
excellent agreement was found between experimental and
predicted results (R2 = 0.998). Appreciable deviations of this
linear behavior have been reported by other authors for NaCl
Fig. 1 – Effect of NaCl fraction in osmotic media on
equilibrium partition coefficient for osmodehydrated carrot
at 40 ◦ C. Experimental data were calculated with Eq. (12). Ke
in continuous line is the slope of the plot Yje vs Xje (for
j = s, w).
o (g/L)c Ys0 (g/g)d e Bij (j = s, w)
1058.1 0.094 0.0436 Estimated from experimental data
or set to 1000
1058.2 0.094 0.2181 Estimated from experimental data
1058.2 0.094 0.0436 or calculated with Eqs. (41)–(43)
1089.5 0.137 0.0424 and (A1)–(A6)
concentrations of about 0.15 g NaCl/g solution and above (del
Valle and Nickerson, 1967; Corzo and Bracho, 2004). It is readily
observable that these water and solute data distribute along a
straight-line with approximately the same slope in both cases,
confirming the fact that a single Ke value is able to describe the
mass equilibrium of these species according to the theoreti-
cal analysis. In this case, Ke was identified as 1.083 with 95%
CI ranging from 1.075 to 1.092, i.e., the distribution constant
is significantly higher than unity, which was an anticipated
result from the developed theory (Section 2.2).
It was considered that OD process reaches equilibrium
when Xe∗ = Ye∗ , as stated in Eq. (10). A necessary condition to
validate this assumption is that food solids do not contribute
to water activity depression. On average, carrots slices lost
about the 33.6 ± 13.3% of their initial solids content. Sucrose,
glucose and fructose account for about the 53% of the dry
matter content of carrot (Soujala, 2000; Nyman et al., 2005),
the rest being both soluble and insoluble fiber, proteins and
fat. According to Nyman et al. (2005), sucrose, glucose and
fructose represent the 3.8%, 1.25% and 1.14% of the fresh
weight of carrot, respectively. By assuming that all lixiviated
solids are sucrose, glucose and fructose in their initial pro-
portions, estimated differences in water activity calculated
with Ross equation and Raoult’s law are less than 0.1% than
that obtained by neglecting these components. A compara-
ble result was obtained in product where differences in water
activity with and without considering sucrose, glucose and
fructose in the calculations were lower than 0.5%. Overall, pre-
dicted differences in water activity between both phases at
Fig. 2 – Distribution data for NaCl and water during osmotic
dehydration of carrot at 40 ◦ C.
 food and bioproducts processing 9 7 ( 2 0 1 6 ) 88–99 95

Table 3 – Equilibrium dehydration and impregnation levels of osmotic dehydration of carrot slicesa .
Cs0 (g/L) Ue × 102 (g/g) We × 103 (g/g) Xse × 101 (g/g) Yse × 101 (g/g) Xwe × 101 (g/g) Ywe × 101 (g/g) Ke (g/g)

20 9.7 ± 0.8 3.9 ± 1.0 0.05 ± 0.01 0.17 ± 0.00 9.07 ± 0.07 9.79 ± 0.01 1.09 ± 0.01
40 7.9 ± 0.6 7.6 ± 0.3 0.32 ± 0.04 0.29 ± 0.01 8.95 ± 0.04 9.64 ± 0.01 1.07 ± 0.01
60 7.5 ± 0.0 8.5 ± 0.7 0.52 ± 0.04 0.41 ± 0.01 8.79 ± 0.04 9.51 ± 0.01 1.07 ± 0.00
80 6.5 ± 0.9 10.2 ± 1.6 0.76 ± 0.05 0.52 ± 0.01 8.62 ± 0.03 9.38 ± 0.01 1.06 ± 0.01
100 7.6 ± 0.7 9.2 ± 2.4 0.88 ± 0.12 0.68 ± 0.03 8.41 ± 0.09 9.22 ± 0.01 1.07 ± 0.01
120 7.8 ± 0.8 8.9 ± 3.0 0.98 ± 0.13 0.84 ± 0.03 8.30 ± 0.11 9.07 ± 0.03 1.07 ± 0.01
140 7.7 ± 3.1 7.0 ± 3.0 1.05 ± 0.09 1.00 ± 0.02 8.24 ± 0.19 8.93 ± 0.01 1.07 ± 0.03
160 4.8 ± 1.6 11.6 ± 0.8 1.40 ± 0.07 1.11 ± 0.01 8.14 ± 0.18 8.78 ± 0.01 1.04 ± 0.02
180 6.8 ± 2.4 7.7 ± 1.6 1.41 ± 0.08 1.25 ± 0.02 7.95 ± 0.14 8.67 ± 0.00 1.06 ± 0.03
200 9.6 ± 0.8 3.2 ± 0.4 1.34 ± 0.11 1.43 ± 0.11 7.78 ± 0.13 8.54 ± 0.03 1.09 ± 0.01
psdb 1.5 1.8 0.08 0.04 0.12 0.01 0.02

Temperature = 40 ◦ C, Vo /mp = 4 L/kg, slice diameter = 2.7 cm, slice thickness = 0.3 cm.
a
Data expressed as means ± standard deviation of three independent experiments.
b
Pooled standard deviation.

equilibrium were in the order of the 1.34%. These results give
support to the theoretical analysis presented in Section 2.2.
Several authors have used partition constants, such as that
defined by Eq. (11), albeit in their reciprocal form ( K1e =
to describe OD equilibrium (del Valle and Nickerson, 1967;
Parjoko et al., 1996). These values were transformed when
necessary to allow a direct comparison with our results. For
example, del Valle and Nickerson (1967) obtained distribution
constants for NaCl in swordfish muscle ranging from 1.09 to
1.43 (5–37 ◦ C, 0.01–0.31 g/g NaCl solution). Sarang and Sastry
(2007) reported distribution coefficients for NaCl from 1.04 to
1.09 during OD of Chinese water chesnut (25–80 ◦ C, 50–100 g/L
NaCl solution). A similar study was conducted by Corzo and
Bracho (2004), reporting separated distribution coefficients for
water (from 1.60 to 2.00) and NaCl (from 1.28 to 1.89) during
osmotic dehydration of sardine sheets (32–38 ◦ C, 0.15–0.27 g/g
NaCl solution). Corzo and Bracho (2004) considered that
mpe = mp0 − (mw0 − mwe ) + (mse − ms0 )
ignoring the lixiviation of food solids and, according to Eq.
(5), leading to the underestimation of Xse and Xwe and to the
overestimation of Kse and Kwe . Our research group proposed a
method to estimate Kse from total solids gain data by estimat-
ing Xse as (Herman-Lara et al., 2013)
these cases, deviations from the theoretical behavior may be
due to an increased mass transfer resistance caused by higher
syrup viscosities and solute deposition on product surface,
Xje
Yje ),
which may lead to a pseudo-equilibrium state.
4.2. Dehydration and impregnation curves
Fig. 3 shows the evolution of solute and water fractions
during OD of carrot slices under forced convection and the
ratio between solution volume and product mass (experiment
set 2, Table 1). These data were used to evaluate diffusion
coefficients assuming both a negligible external resistance to
mass transfer (Bis and Biw were set to 1000) or a convective
boundary (Bis and Biw were also fitted during regression pro-
cedure). By assuming a diffusion-controlled process, water
and NaCl diffusivities were estimated as 6.0 × 10−10 m2 /s
and 4.1 × 10−10 m2 /s, respectively (Table 4), allowing a good
reproduction of experimental dehydration and impregnation
(44) curves (R2 > 0.96, Fig. 3). These diffusion coefficients remained
mostly unaffected (values changed between 4% and 6% of
their original value) when Bis and Biw were also estimated
with data from the same experiment achieving a similar
fitness quality (R2 = 0.97) with overlapping model curves.
However, while estimated Biot numbers were consistent with
a diffusion-controlled process (Bis = 74.4 and Bis = 50.7), their
95% CI indicated a non-significant parameter estimation.

Xse = 1 − Xf 0 − Xwe (45)

This procedure, while neglecting leaching of food solids

as well, leads to an overestimation of Xse and the underes-
timation of Kse . This fact may explain some distribution for
NaCl and water during OD of radish (40 ◦ C, 0.05–0.25 g/g NaCl
solution) with values as low as 0.66 and 0.88, respectively
(Herman-Lara et al., 2013).
Several studies have also investigated the distribution
coefficients of diffusing substances during OD process in sugar
solutions (Parjoko et al., 1996; Rahman et al., 2001; Sablani
et al., 2002; Toğrul and İspir, 2008; Ruiz-López et al., 2011b).
However, in all cases osmotic solute has been grouped with
solids originally present in foods. Thus, a direct comparison
with the results obtained in this work is not attainable. On the
other hand, distribution coefficients for water have shown a
different trend to that expected in this study, with Kwe values Fig. 3 – Experimental and fitted evolution of water and
very often lower than unity, especially at high syrup concen- sodium chloride mass fractions in product during osmotic
trations, indicating that water cannot be eliminated even if dehydration of carrot slices using a 10% NaCl solution at
osmotic media provides the driving force for mass transfer. In 40 ◦ C with stirring (190 rpm) and a high Vo /mp ratio (20:1).
96 food and bioproducts processing 9 7 ( 2 0 1 6 ) 88–99

Table 4 – Estimated diffusion coefficients and mass Biot numbers during OD of carrot slices.
Cs0 (g/L) Stirring (rpm) Vo /mp (L/kg) Parameters Valuea 95% CIb R2 Predicted Bic

100 190 20:1 Dw (m2 /s)d 6.0 5.4/6.6 0.966 Biw = 87.9
Ds (m2 /s)d 4.1 3.8/4.5 0.976 Bis = 126.7
Dw (m2 /s) 6.3 4.5/8.2 0.972e
Ds (m2 /s) 4.3 3.4/5.3
−
Bis 74.4 266.2/414.9
(Biw ) 50.7
−
100 0 4:1 Bis 26.4 0.9/53.7 0.862e,f Bis = 21.3
(Biw ) 18.3 Biw = 14.8
Dw (m2 /s)d 7.6 5.3/10.0 0.787
Ds d 3.5 3.3/3.9 0.991
−
100 0 20:1 Bis 89.0 113.4/291.4 0.932e,f Bis = 27.0
(Biw ) 61.7 Biw = 18.8
Dw (m2 /s)d 7.0 5.5/8.4 0.891
Ds (m2 /s)d 3.7 3.6/3.9 0.991
−
150 0 20:1 Bis 4148 4.1E6/4.2E6 0.925e,f Bis = 28.3
(Biw ) 2877 Biw = 19.7
Dw (m2 /s)d 6.1 4.9/7.2 0.878
Ds (m2 /s)d 3.6 3.3/3.9 0.975

a
Diffusivity values × 1010 .
b
Bold numbers indicate non-significant parameter estimates at the given confidence level.
c
Estimated from empirical correlations.
d
Diffusivity values estimated by considering a negligible external resistance to mass transfer (Bis = Biw = 1000).
e
Parameters estimated by simultaneously fitting Xs and Xw curves during nonlinear regression with Biw = Ds Bis /Dw .
f
Dw and Ds values were obtained from experiment set 2.

Empirical correlations allowed the estimation of Biot number
for water and NaCl transport under these experimental
conditions as 87.9 and 126.7, respectively. In both cases,
these values indicate a strictly diffusion-controlled process,
which is reached for practical purposes when mass Biot
number is higher than 30 or 40 in analytical solutions for
invariable properties of continuous phase (Córdova et al.,
1996; Yanniotis, 2008; Ruiz-López et al., 2011a). Under such
conditions, theoretical model curves overlap no matter the
mass Biot value used to generate them. In this case, as long
as Bi > 30 (process is diffusion-controlled) water and solute
diffusivities will be estimated free of convective mass transfer
effects, but any Bi value will produce a good fit of experimental
data, explaining the lack of significance of this parameter.
OD experiments conducted without stirring were pre-
sumed to show an important resistance to mass transfer
outside product (Figs. 4 and 5). In this case, minimum Bi num-
bers for water and solute transfer were identified as 18.30
and 26.38 (Table 4), respectively. These values, obtained with
the lowest Vo /mp ratio (4:1) (experiment set 3, Table 1), are
near the limit of a diffusion-controlled process. On the other
hand, the analysis of remaining experimental data produced
mass Biot numbers estimations well in the zone of a diffusion-
controlled process (Biw > 61, Bis > 88). However, under natural
convection conditions, all regression procedures produced
non-significant estimations of Bi numbers (p = 0.05). The Bi
values estimated with empirical correlations allow gaining
a better insight into the mass transfer phenomena and the
lack of significance of regression parameters. Under natural
convection conditions Bi values are in the ranges of 14.8–19.7
and 21.3–28.3 for water and NaCl transfer, respectively. Again,
these values are near the limit of a diffusion-controlled

Fig. 4 – Effect of solution concentration on dehydration Fig. 5 – Effect of solution mass-to-product volume ratio on
(j = w) and impregnation (j = s) curves of carrot slices (40 ◦ C, dehydration (j = w) and impregnation (j = s) curves of carrot
no stirring and Vo /mp = 20 : 1 L/kg). slices (40 ◦ C, no stirring and 10% NaCl).
 food and bioproducts processing 9 7 ( 2 0 1 6 ) 88–99
Fig. 6 – Effect of mass Biot number on dehydration (j = w)
and impregnation (j = s) curves of carrot slices (40 ◦ C, 10%
NaCl and a Vo /mp ratio of 20:1). Arrows indicate the
direction in which Bi is increased. Numbers refer to the Bi
values used in model solution.
process where a change in Bi value will not alter the model
behavior in an important way. This fact jointly with experi-
mental data dispersion did not allow a reliable identification
of Bi. In fact, the rate at which mass transfer occurs under
natural convection conditions is practically the same to that
observed under forced convection conditions, causing exper-
imental data to overlap, as shown in Fig. 6. Moreover, this
figure also exhibits the minimal separation between simulated
OD curves obtained under different Bi values ranging from
10 to 1000, which is well between the observed experimental
dispersion. In this way, diffusion coefficients could be also esti-
mated from experiments conducted without stirring as shown
in Table 4. This time, water diffusivities were estimated in
the range of 6.1–7.6 × 10−10 m2 /s, while corresponding values
for NaCl are between 3.5 × 10−10 and 3.7 × 10−10 m2 /s. In this
case, the 95% CI for these values overlap with those previously
calculated under forced convection conditions.
Figs. 4 and 5 allow observing the effect of solution con-
centration and solution-to-product ratio on impregnation and
dehydration curves. From Eq. (15) it is clear that the use of
a higher solute concentration (Ys0 ) will led to an increase
of water loss and solute gain at equilibrium. On the other
hand, decreasing Vo /mp (and thus Mo /mp ) will led to a reduc-
tion of water loss and solute gain at equilibrium. Moreover,
as Mo /mp → ∞, Xje → Yj0 /Ke and when Mo /mp → 0, Xje → Xj0 .
All these cases can be predicted with current equilibrium and
unsteady-state models. A notable feature of proposed model
is that, in addition to describing water and solute fractions
in the product, it also allows the prediction of osmotic media
concentration evolution, which may change in a significant
way especially in experiments conducted with a low Vo /mp
ratio. For example, by lowering the Vo /mp ratio from 20:1 to
4:1, the final dilution of osmotic media increases from 4% to
18% (Fig. 7).
Estimated diffusivities for water were smaller than the cor-
responding NaCl values, which may be very likely due to its
lower molecular weight as reported elsewhere (Panagiotou
et al., 1999). Diffusivity values are comparable to those
obtained during OD of other foodstuffs. For example, water
and NaCl diffusivities during OD of potato (25–55 ◦ C, 0.10–0.18 g
solute/g solution) have been estimated in the ranges of
8.7–12.3 × 10−10 and 8.2–12.2 × 10−10 m2 /s, respectively (Khin
97
Fig. 7 – Effect of Vo /mp ratio on dilution of osmotic media.
et al., 2006). Comparable results were obtained during OD
of cherry tomato (25 ◦ C, 0.10 and 0.25 g solute/g solution)
with water and NaCl diffusivities values in the ranges of
1.2–1.8 × 10−9 and 0.2–0.5 × 10−9 m2 /s (Azoubel and Murr,
2004). Sarang and Sastry (2007) reported NaCl diffusivities in
the range of 7.5–18.5 × 10−10 during OD of Chinese water ches-
nut (25–80 ◦ C, 50–100 g/L NaCl solution).
There are few reports regarding the estimation of Bi number
during OD of foods. Selected studies include that of da Silva
et al. (2013), who performed the OD of coco parallelepipeds
(6 mm × 10 mm × 31 mm) in sucrose solutions under forced
convection conditions (magnetic stirring at 60 Hz, 35 ◦ Bx, 40 ◦ C)
and reported fitted values as Biw = 7.75 and Bis = 5.00. In a later
work, da Silva et al. (2014) studied the OD of pineapple cubes
(side length of 15 mm) in sucrose solutions without stirring
(40 and 70 ◦ Bx, 30 ◦ C) estimating Bi values in the ranges of
1.5–2.3 and 0.62–0.95 for water and solute transport, respec-
tively. Unlike current study, Bi values for solute transfer were
smaller than those estimated for water; however, it should be
highlighted that da Silva et al. (2013, 2014) analyzed solute
transfer as total solids and did not report a statistical analy-
sis of estimated parameters to allow a further comparison of
observed differences with values obtained in this study.
5. Conclusions
Proposed models allowed the satisfactory description of both
dynamic and equilibrium mass transfer periods for water,
osmotic solute and food solids interchange between prod-
uct and solution during an osmotic dehydration (OD) process.
The mathematical description of OD equilibrium helped to
explain differences between previous studies, describing the
necessary adjustments to eliminate them and providing well-
founded bases for further investigations. A better insight of
mass transfer phenomena occurring during OD of carrot slices
in NaCl solutions was gained, where convection was almost
negligible even in non-stirred osmotic media. Further stud-
ies are required to evaluate governing mechanism for mass
transfer in other systems.
Acknowledgments
The authors wish to thank the Consejo Nacional de Cien-
cia y Tecnología (CONACYT) for providing financial support
through project 130011. Hermelinda Pacheco Angulo acknowl-
edges her doctoral scholarship from CONACYT. Miguel Ángel
98 food and bioproducts processing 9 7 ( 2 0 1 6 ) 88–99
García Alvarado acknowledges his sabbatical financial support
from CONACYT.
Appendix A. Properties used in empirical
prediction of mass Biot numbers
Diffusion coefficient for NaCl–water mixture. Poling et al. (2001)
proposed the following equation to describe the effect of
solute concentration on mutual diffusion coefficients in elec-
trolyte solutions of a single salt:
w
Dsw = D◦sw ϕ (A1)
sw
where, the diffusion coefficient at infinite solution (D◦sw ) and
thermodynamic factor (ϕ) are given by (Poling et al., 2001)
RT 1/n+ + 1/n−
D◦sw = (A2)
F2 1/◦+ + 1/◦−
∂ ln ± m ∂±
ϕ =1+m =1+ (A3)
∂m ± ∂m
with + = 5.01 × 10−3 and − = 7.63 × 10−3 S/m2 mol for Na+
cation (n+ = 1) and Cl− anion (n− = 1), respectively (Pitzer et al.,
1984).
Mean ionic activity coefficient ( ± ) of solute. Tabulated data
(100 kPa) in the ranges of 0.1–6 molal NaCl and 0–100 ◦ C pro-
vided by Pitzer et al. (1984) were fitted in this study with
predictions within the ±4% of the original data (R2 = 0.9895):
± = 0.7358 + 0.2170x2 − 0.0591x12 − 0.0472x12 x2 − 0.0303x1 x22
+ 0.0098x13 − 0.0972x23 + 0.1393x24 (A4)
where, x1 = [T (◦ C) − 50] /50 and x2 = (m − 3.05) /2.95.
Dynamic viscosity of solvent (w ) and solution (sw ). Tabulated
data (100 kPa) in the ranges of 0–6 molal NaCl and 20–100 ◦ C
provided by Kestin et al. (1981) were fitted in this study with
predictions within the ±3% of the original data (R2 = 1.0000):
sw × 103 = 0.6487 − 0.3626x1 + 0.2179x2 − 0.1289x1 x2
+ 0.1745x12 + 0.0466x22 + 0.0782x12 x2 − 0.0499x1 x22
− 0.1094x13 + 0.0092x23 − 0.0367x13 x2
+ 0.0300x12 x22 + 0.0491x14 (A5)
where, x1 = [T (◦ C) − 60] /40 and x2 = (m − 3) /3. Eq. (A5)
becomes w when x2 = −1.
Density of solvent ( w ) and solution ( sw ). Tabulated data
(100 kPa) in the ranges of 0–6 molal NaCl and 0–100 ◦ C pro-
vided by Pitzer et al. (1984) and Geankoplis (1993) were fitted
in this study with predictions within the ±3% of the original
data (R2 = 1.0000):
sw = 1093.4898 − 26.8911x1 + 94.6352x2 − 2.5050x1 x2
− 3.8475x12 − 8.9248x22 + 3.2483x12 x2 + 1.3048x1 x22
+ 0.7381x13 + 1.4752x23 − 0.9954x13 x2 − 0.5638x1 x23
− 1.3408x12 x22 − 0.3065x14 − 0.3796x24 (A6)
where, x1 = [T (◦ C) − 50] /50 and x2 = (m − 3) /3. Eq. (A6)
becomes w when x2 = −1.
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