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Food and Bioprocess Technology (2018) 11:913–925

https://doi.org/10.1007/s11947-018-2062-0

ORIGINAL PAPER

Separation of Sucrose and Reducing Sugar in Cane


Molasses by Nanofiltration
Jianquan Luo 1 & Shiwei Guo 1 & Yuanyuan Wu 1 & Yinhua Wan 1

Received: 30 August 2017 / Accepted: 15 January 2018 / Published online: 30 January 2018
# Springer Science+Business Media, LLC, part of Springer Nature 2018

Abstract
Recovery of sugars from cane molasses is a promising approach to increase the added value of molasses and reduce its
environmental pollution. In this work, for the first time, nanofiltration (NF) was used for the separation of sucrose and reducing
sugar in cane molasses by a cascade diafiltration-concentration process. The retention difference between sucrose and reducing
sugar by all the tested NF membranes was not distinct at 25 °C, while due to the thermal-induced pore size change and enhanced
solute diffusivity, the NF retention behavior changed significantly at 60 °C, and the DL membrane with a sucrose retention of
96% and a reducing sugar retention 5% was selected for the process optimization and modeling. High temperature (55–60 °C),
low permeate flux (below 15 Lm−2 h−1), and high sugar concentration resulted in a low retention of reducing sugar due to the
dominant diffusive mass transfer, which was desirable for the molasses separation by NF. Mathematical modeling could well
predict the diafiltration and concentration processes if using right sugar retention data. The deviations between prediction lines
and experimental data in the cross-flow filtration of real solution were mainly caused by the permeate flux variation rather than
membrane fouling. After diafiltration, the ratio of sucrose in total molasses sugar increased from 76.1 to 87.9%, while in the
permeate of the second concentration step, the ratio of sucrose was only 2.4%. Thus, the retentate of diafiltration could be directly
used for sucrose crystallization to avoid the accumulation of reducing sugar and salts, and the permeate of the second concen-
tration step could be concentrated by NF270 at room temperature to produce syrup drinking.

Keywords Diafiltration . Membrane filtration . Sugar recovery . Molasses purification . Modeling

Introduction M. Sharma et al. 2016) since the price of cane molasses is


lower than $150/ton, and the sugar factory can get little profit
Cane molasses, a thick and brown syrup obtained as a from the molasses sale. Moreover, the fermentation with cane
byproduct from the processing of sugarcane into sucrose, con- molasses as carbon source produces a large amount of high-
sists of fermentable carbohydrates (i.e., sucrose, glucose, fruc- strength wastewater; thus, the molasses demand in down-
tose) and some non-sugar organic materials (e.g., pigments, stream industry is decreasing (Nandy et al. 2002). Therefore,
amino acids, inorganic salts, phenolic compounds) (Baikow recovery of sugars from cane molasses is a promising ap-
2013). The quantity of cane molasses available in China is proach to increase the added value of molasses and reduce
about 4800,000 tons/year, and it is mainly used as a supple- its environmental pollution.
ment for livestock feed and as a source of carbon in fermen- Considering that pigments, inorganic salts, sucrose, and
tation processes (e.g., ethanol production) (Valli et al. 2012; reducing sugar are the main components in cane molasses,
three operations including decolorization, desalination, and
sugar fractionation are required to recover the sugars (account
* Jianquan Luo for 50% of the total weight) from the molasses. In most pat-
Jqluo@ipe.ac.cn ents, cane molasses was decolorized and desalted by chemical
* Yinhua Wan treatment (e.g., organic solvent, alkaline, acid) followed by
yhwan@ipe.ac.cn ion exchange (Riffer 1977; Nakasone et al. 1985; Ou 1985;
Clarke 1995). In addition, an integrated process including
1
State Key Laboratory of Biochemical Engineering, Institute of softening, filtration, and chromatography (i.e., ion-exclusion)
Process Engineering, University of Chinese Academy of Sciences,
Chinese Academy of Sciences, Beijing 100190, China
was successfully applied in beet molasses purification
914 Food Bioprocess Technol (2018) 11:913–925

(Lameloise and Lewandowski 1994; Kearney and Kochergin temperature and lower permeate flux are preferred thanks to
2002); however, it was not economical in cane molasses in- the more significant diffusive mass transfer. Accordingly, ef-
dustry because of its high level of suspended solids and hard- fective separation of sucrose and reducing sugar in cane mo-
ness resulting in high cost of the pretreatment (Kearney and lasses can be achieved by NF at high temperature, especially
Kochergin 2002). Recently, membrane technology combined at low permeate flux. However, most studies only focused on
with chemical treatment, activated charcoal adsorption, or ion the purification of oligosaccharides (e.g., fructo-oligosaccha-
exchange has also been reported for sugar decolorization rides, galacto-oligosaccharides) by NF (Goulas et al. 2002;
(Bernal et al. 2016; W. Li et al. 2016; Susanto et al. 2016; Kuhn et al. 2010; Pruksasri et al. 2015; Córdova et al. 2016).
Zhu et al. 2016). Regarding the sugar fractionation, Donovan The present work was undertaken to select a suitable NF
and Hlavacek (2002) patented a nanofiltration (NF) process membrane for separation of sucrose and reducing sugar (i.e.,
for the separation of sucrose and reducing sugar in cane mo- glucose and fructose) in cane molasses, investigate the effect
lasses, and stated that by using NF, reducing sugar content in of process parameters on the separation performance, and clar-
molasses could be decreased from 23 to 2%, and the ash level ify the mechanisms behind various phenomena induced by
reduced from 17 to 7%, while the sucrose content increased to temperature and permeate flux. Moreover, a diafiltration
75%, which could be fed to crystallization equipment for su- followed by multistage concentration processes was proposed,
crose recovery. In our previous study, an integrated membrane aiming at improving the NF separation efficiency to sucrose
process including a loose ultrafiltration (UF) for clarification, and reducing sugar. We also attempted to establish mathemat-
a tight UF for decolorization, and a NF for sucrose concen- ical models for diafiltration/concentration process both under
trating and glucose/fructose/salt removing was proposed for bench-scale dead-end mode and pilot-scale cross-flow mode.
sugarcane juice refining (Luo et al. 2016). These indicated that Finally, a real solution (cane molasses after partial decoloriza-
NF process was promising for sugar fractionation in cane tion by a tight UF) was treated by the cross-flow NF module to
molasses purification. However, to the best of our knowledge, validate the proposed process and models. This study not only
there has been no systematic work on the separation of sucrose elucidated the separation mechanisms for small neutral solutes
and reducing sugar in cane molasses. by NF, but also offered an alternative to recover sugars from
NF, as a membrane technology based on both charge effect cane molasses.
and size exclusion, is a powerful tool for separation of small
molecules and salts, which has attracted growing attention in
many fields such as wastewater treatment, water purification, Materials and Methods
desalination, food processing, and bio-separation (Luo and
Wan 2013; Wang et al. 2002; Altmann et al. 2016; Meyer Cane Molasses, Chemicals, and Membranes
et al. 2017). Since the molecular weight difference between
sucrose and glucose/fructose is only 162 Da, the separation of Cane molasses was provided by Yaoming Sugar Industry Co.,
sucrose and reducing sugar is challenging. Goulas et al. Ltd. (Guangdong, China), which contained ~ 80 wt.% soluble
(2002) found that using DL membrane at 20.7 bar, the sucrose solids (~ 47.4 wt.% sucrose and ~ 16.5 wt.% reducing sugar).
rejection was 99 and 97% at 25 and 60 °C, respectively, while About 1.5 kg cane molasses was diluted with 3 L deionized
fructose rejection was 77 and 53%, respectively, and the lower water, and the solution was adjusted to pH 7 by adding solid
sugar rejection at higher temperature was caused not only by sodium hydroxide. After pH adjustment, this diluted molasses
the enhanced diffusivity of solutes but also by the larger ef- was centrifuged at 5000g and 25 °C for 15 min by a refriger-
fective pore size (i.e., thinner layer of adsorbed water mole- ated centrifuge (4k-15, Sigma, Germany), which has a viscos-
cules on the pore wall at higher temperature). Kuhn et al. ity of 1.4 × 10−3 Pa s at 55–60 °C (2.9 × 10−3 Pa s at 20 °C).
(2010) reported that the rejection of glucose/fructose by six The supernatant was decolorized by 2 kDa spiral-wound UF
NF membranes was below 30% at 25 °C, while the sucrose membrane (Sepro Membranes, USA) under concentration
rejection was up to 93%. Zhao et al. (2013) showed that at mode, and the resulting permeate (i.e., light-colored molasses)
30 °C, the rejection difference between sucrose and glucose for NF diafiltration contained 123.57 g L −1 sucrose,
was decreasing with increase of permeate flux, for example, 38.85 g L−1 reducing sugar, and 50 mS cm−1 conductivity.
their rejections were 42 and 96% at 5 Lm−2 h−1, respectively, Sucrose, glucose, and fructose were of analytical grade and
but increased to 80 and 99.8% at 20 Lm−2 h−1, respectively. purchased from Xilong Scientific Co., Ltd. (Guangdong,
Bandini and Morelli (2017) recently claimed that the rejec- China). For the model solution with mixed sugars, the total
tions of dextrose and fructose reduced at higher temperature, sugar concentration was 190 g L−1, and the concentration ratio
while such reduction became smaller at higher permeate flux. of sucrose, glucose, and fructose was 140:25:25 except else-
Therefore, it could be concluded that the separation efficiency where stated. Nine commercial NF membranes were tested in
of disaccharide and monosaccharide by NF was mainly this work, and their main properties are summarized in
governed by their diffusivity difference, and higher Table 1.
Food Bioprocess Technol (2018) 11:913–925 915

Table 1 Main properties of the NF membranes examined

Membrane Manufacturer Surface material MgSO4 rejection (%)a Permeability


(L h−1 m−2 bar−1)b

NF270 Dow-Filmtec Poly(piperazinamide) 97 16.1 ± 0.3


XN45 Trisep Poly(piperazinamide) 96 7.3 ± 0.2
DK GE-osmonics Polyamide 98 8.2 ± 0.5
DL GE-osmonics Polyamide 96 8.6 ± 1.1
NT102 Microdyn-Nadir Poly(piperazinamide) 95 8.1 ± 0.3
NT103 Microdyn-Nadir Polyamide 98 9.1 ± 0.6
NF70 Development Center Poly(piperazinamide) 98 12.2 ± 0.8
NF40-I of Water Treatment Poly(piperazinamide) 95 20.7 ± 0.2
Technology, Hangzhou
NF40-II Poly(piperazinamide) 98 18.1 ± 1.4
a
MgSO4 rejection determination conditions: 2000 ppm, 4.8–7.6 bar, 25 °C
b
Pure water permeability was measured at a constant flux of 132.7 Lm−2 h−1 , 25 °C

Experimental Setup and Procedure membranes were compacted at 35 bar for 30 min. For the
membrane selection and process optimization, 26 mL model
Dead-end Filtration at Constant Flux solution was concentrated to 13 mL at 13.26 Lm−2 h−1 and
1200 rpm, and two temperature of 25 and 60 °C was
The dead-end filtration experiments were conducted in a employed except elsewhere stated. During the concentration
laboratory-constructed magnetically stirred cell at constant process, the first 1 mL permeate was discarded to eliminate the
flux mode (Fig. 1a). This device could be fitted with a mem- interference effect of the residual water in the pipeline, and the
brane disc with an effective membrane surface area of 4.52 × rest 12 mL permeate and the corresponding retentate were
10−4 m2, and the working volume of the cell was 13 mL. Feed collected for analysis. The average transmembrane pressure
solution was pre-filled into an injection column (Superloop (TMP) during the concentration process was recorded. For
50 mL, Pharmacia, Sweden) and then pumped into cell for the cascade NF processes, the operating procedure was de-
the concentration mode, while for the diafiltration mode, de- scribed as follows. Fourteen milliliters of model solution
ionized water was pumped into cell directly. More detailed was injected into the cell, and after discarding the first 1 mL
information of this setup could be found in our previous work permeate, 39 mL deionized water was pumped into the cell at
(Luo et al. 2009). A new membrane was used for each series 13.26 Lm−2 h−1, 1200 rpm, and 60 °C. The permeate was
of experiments, and each membrane disc was firstly dipped in collected every 5 mL in vials for analysis (the average TMP
50% ethanol solution for about 5 s to remove manufacturing for each sample was also recorded). The permeate from
residues from the membrane and then soaked in deionized diafiltration operation was further concentrated by NF at
water for at least 12 h prior to use. Before the water perme- 39.8 Lm−2 h−1 and 60 °C, where 130 mL model solution
ability measurement at different fluxes, all the virgin (sucrose 10.4 g L −1 , reducing sugar 14.7 g L −1 ) was

Fig. 1 Schematic diagrams of a


dead-end filtration under constant
flux mode and b cross-flow
filtration under constant pressure
mode
916 Food Bioprocess Technol (2018) 11:913–925

concentrated to 13 mL, and the permeate sample was collected For a batch filtration, the average sugar concentration in the
every 15 mL for analysis. The permeate from the first concen- retentate is calculated as follows:
tration operation was further concentrated by NF at
1
132.7 Lm−2 h−1 and 60 °C, where 130 mL model solution Cr;av ¼  ðC f þ C r Þ; ð2Þ
(sucrose 1.5 g L−1, reducing sugar 12.0 g L−1) was concen- 2
trated to 13 mL, and the permeate sample was collected every where Cf and Cr are the sugar concentrations in the feed and
15 mL. Membrane permeability was examined again after the retentate.
filtration to monitor the irreversible fouling.
Modeling for Dead-end Filtration Under Constant Flux Mode
Cross-flow Filtration at Constant Pressure (Fig. 1a)

The cross-flow filtration was performed in a pilot-scale device (a) Diafiltration process
(Fig. 1b) consisting of a 5-L feed tank with an insulating
jacket, a feed pump, a spiral-wound membrane module (effec- During the constant volume diafiltration, the loss of solute in
tive membrane area = 0.34 m 2 ), and a water bath tank the dead-end cell was equal to the mass in the permeate, that is,
equipped with a circulating pump. The feed temperature could V0 dC ¼ −C p dV; ð3Þ
be controlled by the circulating water bath. The diafiltration
was carried out at 25 bar, 55 °C, and a cross-flow velocity of where V0 and V are the cell volume and diafiltration solvent
5 L min−1, where 3 L real solution (light-colored cane volume, respectively, and V0 is the same as Vr (retentate
molasses) was diafiltrated by 9 L deionized water at constant volume).
volume diafiltration mode. Then, the first concentration oper- Substituting Eq. (1) into Eq. (3), and then integrating it at
ation was conducted at 10 bar, 55 °C, and 5 L min−1, where V = 0, C = Cf gives,
8 L permeate from the diafiltration process was concentrated  
to 0.8 L. Finally, the second concentration operation was car- V
C r ¼ C f ∙exp ðRobs −1Þ : ð4Þ
ried out at 5 bar, 55 °C, and 5 L min−1, where 6.5 L permeate V0
from the first concentration process was concentrated to
0.65 L. After each test, NF membrane module was rinsed
using hot deionized water with the same temperature as feed
(b) Concentration process
temperature. Membrane permeability was examined before
and after the filtration to monitor the irreversible fouling.
During the concentration process, the solute mass in the
cell was equal to the feed mass minus the mass in the perme-
Analytical Methods ate,
V0 dC ¼ C f dV f −C p dV p ; ð5Þ
Sucrose content was measured by Roe colorimetric method (J.
Li 2008), and reducing sugar concentration was determined where Vf and Vp are the feed and permeate volumes, respec-
by the method of Miller with dinitro salicylic acid reagent tively, Vf/V0 should be larger than 1, and Vp = Vf − 13.
(Miller 1959). Substituting Eq. (1) into Eq. (5) and then integrating it at
Vf = V0, C = Cf, following equation can be obtained:
Calculation and Modeling   
Vf
Robs ∙exp ðRobs −1Þ −1 −1
V0
The observed retention (Robs) of sucrose and reducing sugar is Cr ¼ C f  : ð6Þ
Robs −1
defined as follows:
 
Cp
Robs ¼ 1−  100; ð1Þ Modeling for Cross-flow Filtration Under Constant Pressure
C r;av
Mode (Fig. 1b)
where Cp is the sugar concentration in the permeate and Cr,av
is the average concentration in the retentate for a specific (a) Diafiltration process
operation period of time for sampling, that is, the average of
the solute concentration in the retentate at the beginning and The diafiltration process in cross-flow filtration was similar
that at the end of collecting a given volume of permeate to that in dead-end filtration, which could be modeled by Eq.
sample. (4).
Food Bioprocess Technol (2018) 11:913–925 917

(b) Concentration process but also the enlargement of the membrane pore size (Dang
et al. 2014). Many studies confirmed the increase in effective
In dead-end filtration, fresh feed was continuously pumped pore size of NF membranes at higher temperature by both
into the cell, while in cross-flow filtration, all the feed was modeling and physical characterization (R. R. Sharma and
poured into the feed tank in the beginning and then Chellam 2005; Ben Amar et al. 2007; Saidani et al. 2010;
recirculated in the system. The solute mass in the retentate is Mänttäri et al. 2002). Such thermal-induced pore size change
equal to the feed mass minus the mass in the permeate: was caused by two possible reasons: one is the thinner hydra-
tion layer on the pore wall owing to higher diffusivity of water
Cr V r ¼ C f V f −C p V p ; ð7Þ
molecules (Luo and Wan 2013); another is the structural
where Vr is the retentate volume. changes in network pores due to the thermal expansion of
Substituting Eq. (1) into Eq. (7), the following equation can polymer (Saidani et al. 2010).
be obtained: First, the separation of sucrose and reducing sugar by dif-
ferent NF membranes was evaluated at 25 °C, and as shown in
Vf Fig. 2a, except for XN45, NT102, and NF40-II, the retention
ð1 þ Robs ÞC f ∙
þ C f ð1−Robs Þ
Vr   of sucrose and reducing sugar by each NF membrane is sim-
Cr ¼ : ð8Þ
Vf Vf ilar, indicating that these NF membranes cannot be used for
1þ þ Robs ∙ 1−
Vr Vr this purpose at room temperature. For XN45 and NF40-II, the
retention of sucrose was higher than 95%, while their reducing
sugar retention was around 70 and 50%, respectively, imply-
ing that their separation efficiency was not high and econom-
Results and Discussion ical. Surprisingly, for NT102, reducing sugar had a much
higher retention than sucrose (80 vs. 50%), and this might
Effect of Membrane Type on Separation of Sucrose be related to its special pore structure or material affinity.
and Reducing Sugar Actually, Koschuh et al. also found similar results with
polyethersulphone NF membranes (R glucose > R sucrose)
As listed in Table 2 (Ribeiro et al. 2006), the molecular weight (Koschuh et al. 2005).
difference between sucrose and glucose/fructose is only When temperature became 60 °C, the sugar retention be-
162 Da, and their Stokes radius difference is around 0.1 nm; havior greatly changed for all the NF membranes as expected.
thus, it is difficult to separate them only based on size exclu- Comparing the results in Fig. 2a, b, it was found that for
sion at room temperature. Regarding the solute diffusivity, NF270 and XN45, the retention of both sucrose and reducing
when the temperature increased from 25 to 60 °C, their diffu- sugar distinctly declined at 60 °C, especially for reducing
sivity difference raised from 0.15 × 10−9 to 0.34 × 10−9 m2 s−1, sugar. This was reasonable considering the increase in the
implying that the separation of sucrose and reducing sugar by solute diffusivity and the enlargement of the membrane pore
NF could be enhanced at higher temperature. It was reported size at higher temperature (Goulas et al. 2002; Dang et al.
that with increasing temperature, solute rejection by NF would 2014). For NT103 and NF70, the retention of reducing sugar
decrease due to not only the increase in the solute diffusivity decreased as expected, while their sucrose retention

Table 2 Main properties of the sugars in cane molasses (Ribeiro et al. 2006)

Index Sucrose Glucose Fructose

Structure

Molecular weight (Da) 342 180 180


Stokes radius (nm) 0.471 0.365 0.361
Diffusivity (10-9 m2s-1) at 25 oC 0.523 0.679 0.686
Diffusivity (10-9 m2s-1) at 60 oC 1.114 1.447 1.461
918 Food Bioprocess Technol (2018) 11:913–925

Fig. 2 Retention of sucrose and a b


reducing sugar by different NF 100 100
membranes at a 25 °C and b T=25 C o
T=60oC
60 °C; TMP during separation of 80 80
sucrose and reducing sugar by
Sucrose
different NF membranes at c

Retention (%)

Retention (%)
60 60 Reducing sugar
25 °C and d 60 °C. Permeate
flux = 13.27 Lm−2 h−1
40 40
Sucrose
Reducing sugar
20 20

0 0
NF X D DL NT NT NF NF NF NF X D DL NT NT NF NF NF
27 N45 K 10 10 70 40 40 27 N45 K 10 10 70 40 40
0 2 3 -I -II 0 2 3 -I -II

c 40
d 40
o Sucrose: 70 gL-1 Sucrose: 140 gL-1
T=25 C T=60 oC
Reducing sugar: 25 gL-1 Reducing sugar: 50 gL-1
32 32

24 24
TMP (Bar)

TMP (Bar)
16 16

8 8

0 0
NF X D DL NT NT NF NF NF NF X D DL NT NT NF NF NF
27 N45 K 10 10 70 40 40 27 N45 K 10 10 70 40 40
0 2 3 -I -II 0 2 3 -I -II

unexpectedly increased to 94% at 60 °C, which was possibly Effect of Operating Parameters on Separation
caused by the positive change in polymer physical state (pore of Sucrose and Reducing Sugar
deformation) for these two membranes (Saidani et al. 2010).
This phenomenon became more obvious for NT102, where Separation of sucrose and reducing sugar by DL was conduct-
the retention of both sucrose and reducing sugar increased to ed at 45, 55, and 60 °C, respectively, and when temperature
90% at 60 °C (their retention was only 50 and 80% at 25 °C, ascended from 45 to 55 °C, the sucrose retention decreased
respectively). However, NF40-I and NF40-II could not sustain from 96 to 94%, and the reducing sugar retention declined
the high temperature, and the sugar retention greatly dropped from 42 to 14% (Fig. 3a). However, the average TMP during
at 60 °C. Regarding DK and DL with good reputations in the the filtration increased from 29 to 30 bar. Theoretically, the
applications under extreme conditions, their sucrose retention operating TMP was supposed to descend due to lower sugar
could be kept at 96% at 60 °C, while the reducing sugar retention and smaller solvent viscosity at higher temperature.
retention greatly declined to 15 and 5%, respectively, meaning Thus, such unexpected TMP increase was caused by increas-
that their slightly increased pore size was perfect for the sep- ing osmotic pressure at higher temperature (osmotic pressure
aration of sucrose and reducing sugar. Compared to the results calculation: π = nRT, T is temperature) (Luo et al. 2016).
in literature, the obtained separation factor for sucrose and When temperature increased to 60 °C, the sugar retention
reducing sugar was the highest in this study (Table 3), which did not further decline but the TMP decreased from 30 to
was attributed to the suitable NF membrane, operating tem- 27 bar, which was caused by the dominant viscosity reduction
perature, and permeate flux. Moreover, as shown in Fig. 2c, d, (Luo and Wan 2013).
the operating TMP at constant flux for different membranes is As shown in Fig. 3b, the rotating speed from 800 to
corresponding to their sugar retention, that is, larger sugar 1600 rpm in the dead-end cell has negligible effect on the
retention resulted in higher TMP, implying that the permeate sugar retention and TMP, implying that the back diffusion of
flux in this case is dominated by osmotic pressure difference these small solutes is intensive at higher temperature and the
across the membrane, and lower reducing sugar retention was concentration polarization layer is quite thin. As seen in Fig.
not only good for separation efficiency but also helpful to save 3c, when the permeate flux increases from 6.64 to
energy. Thus, the DL membrane was selected for the further 19.91 Lm−2 h−1, the TMP went up linearly, indicating that
study. these experiments were operated below Bthreshold flux^
Food Bioprocess Technol (2018) 11:913–925 919

Table 3 Comparison of sucrose/


reducing sugar separation by NF Membrane used Sucrose Reducing sugar Separation Reference
membranes with the results in (temperature) retention (%) retention (%) factor (Rsuc/Rred)
literature
DL (60 °C) 97 53 1.83 Goulas et al. (2002)
NF45 (32 °C) 95 72 1.32 Wang et al. (2002)
DL (25 °C) 92 10 9.20 Kuhn et al. (2010)
NF-3D (30 °C) 96 42 2.30 Zhao et al. (2013)
DL (60 °C) 96 5 19.2 Present study

(Luo and Wan 2013). Moreover, the effect of permeate flux reducing sugar retention enhanced obviously when the perme-
had negligible effect on the sucrose retention, while the ate flux increased from 13.27 to 19.91 Lm−2 h−1, implying that

a 40
b 40
100 100
1200 rpm 60 oC
13.27 Lm -2h-1 13.27 Lm-2h-1
80 30 80 30
Retention (%)

Retention (%)
TMP (bar)
60 60

TMP (bar)
20 20
Sucrose Sucrose
40 Reducing sugar 40 Reducing sugar
TMP
TMP
10 10
20 20

0 0 0 0
45 55 60 800 1200 1600
Temperature (oC) Rotating speed (rpm)

c 100 40 d 100 Sucrose: reducing sugar (g/g) =14:5


40

60 oC
1200 rpm 60 oC
80 80 1200 rpm
30 30
13.27 Lm-2h-1
Retention (%)
Retention (%)

TMP (bar)

60 60

TMP (bar)
Sucrose
Reducing sugar 20 Sucrose 20
TMP Reducing sugar
40 40
TMP
10 10
20 20

0 0 0 0
6.64 13.27 19.91 95 190 228
Permeate flux (Lm-2h-1) Total concentration (gL-1)

e 40
100 Sucrose: 140 gL-1
60oC
1200 rpm
80 30
13.27 Lm-2h-1
Retention (%)

60
TMP (bar)

20
Sucrose
40 Reducing sugar
TMP
10
20

0 0
14:1 14:3 14:5
Sucrose/reducing sugar (g/g)

Fig. 3 Effect of temperature (a), rotating speed (b), permeate flux (c), total sugar concentration (d), and sucrose/reducing sugar ratio (e) on the retention
of sucrose and reducing sugar as well as TMP by DL membrane
920 Food Bioprocess Technol (2018) 11:913–925

a lower permeate flux with dominant diffusive mass transfer the residual sucrose. Finally, a relatively pure reducing sugar
was preferred for separation of sucrose and reducing sugar. could be obtained in the permeate of the second concentration
step. This cascade NF process was conducted by both dead-
Effect of Sugar Concentration and Ratio end and cross-flow filtrations (using model solution and light-
on Separation of Sucrose and Reducing Sugar colored cane molasses, respectively) at 55–60 °C, and the
experimental data and modeling results were compared to
Cane molasses normally contains 50–65% sugars and cannot gain deeper understanding on this separation process.
be directly treated by NF because of its high osmotic pressure
and high viscosity. Thus, a dilution operation is required, and NF Diafiltration
the effect of total sugar concentration on the sugar retention
was investigated. As seen in Fig. 3d, with increase of sugar As shown in Fig. 5a, the sucrose concentration in the retentate
concentration from 95 to 228 g L−1, the TMP raises remark- is decreasing, which is in agreement with the prediction line
ably due to the higher osmotic pressure and larger solution (Rsucrose = 94%), while the retention of reducing sugar (30–
viscosity, while the sugar retention decreases slightly because 40%) in the prediction line is much higher than that obtained
the concentration polarization becomes more serious and the in Fig. 3a (< 10%). This was explained as follows: the sugar
concentration gradient-driven mass transfer across the mem- concentration in the retentate was decreasing during
brane is enhanced. A lower retention of reducing sugar is diafiltration, while for the results in Fig. 3a, the concentration
desirable while a higher sucrose retention is preferred. mode was used and the sugar concentration in the retentate
Therefore, a suitable dilution factor is important to achieve was increasing; since their initial feed concentrations were the
both high separation efficiency and high sucrose recovery. same, the average concentration in the retentate for the
During the NF of diluted molasses, the concentration ratio of diafiltration experiment should be much lower than that for
sucrose and reducing sugar was changing attributed to their the concentration experiment; Fig. 3d, e showed that with
different retention, and thus, the effect of concentration ratio decreasing sugar concentration, the retention of reducing sug-
on the sugar retention was examined. As seen in Fig. 3e, with ar increased significantly; thus, during the diafiltration, the
increase of reducing sugar content (sucrose concentration is prediction line with a higher reducing sugar retention of 30–
constant), both sucrose and reducing sugar retention slightly 40% could match the experimental data. Moreover, as shown
decreases because of the increasing concentration polariza- in Fig. 5b, the TMP was declining during diafiltration because
tion, indicating that the sugar concentration ratio has negligi- of less osmotic pressure resulted from sugar molecules as well
ble effect on the separation efficiency while the viscosity- as lower solution viscosity (smaller filtration resistance).
induced mass transfer determines the sugar retention (at con- While the light-colored molasses was used as feed and a
stant operating conditions). cross-flow membrane system was employed (Fig. 5c), the
sucrose concentration in the retentate followed the prediction
Separation of Sucrose and Reducing Sugar in Cane line with a sucrose retention of 94% at the beginning of
Molasses by Cascade NF Process diafiltration (V/V0 < 1.5), but when V/V0 was larger than 2,
the sucrose retention in the experiment was found to be much
In order to improve the separation efficiency and sugar recov- higher than 94%. For reducing sugar, the prediction line with a
ery, an integrated diafiltration-concentration process (cascade retention of 40% greatly deviated from the experimental data,
NF process) was proposed as illustrated in Fig. 4. First, con- even when predicting the reducing sugar concentration in the
stant volume diafiltration was carried out to remove most of retentate by a retention of 60%, a deviation still occurred as V/
reducing sugar by adding deionized water, and the permeate V0 > 2.5. Such increase in sugar retention was mainly caused
from diafiltration was further concentrated by the same NF by the augment of permeate flux during diafiltration under
membrane (DL), where the retentate rich in sucrose was constant TMP mode (see Fig. 5d), which was verified by the
recycled to the diafiltration step, and the permeate was con- results in Fig. 3c. Generally, more serious fouling formation
centrated by the second concentration step to further recover (as additional selective layer or narrowing membrane pores)

Fig. 4 Schematic diagram of


integrated diafiltration-
concentration process for the
separation of sucrose and
reducing sugar in light-colored
molasses
Food Bioprocess Technol (2018) 11:913–925 921

Fig. 5 Experimental/predicted a b
solutes concentration in the 150
Model solution
20
Model solution

Concentration in retentate (gL-1)


retentate (a) and TMP (b) during
diafiltration step using dead-end 120
15
filtration cell under constant flux
mode. Model solution: sucrose 90
Sucrose

143 g L−1, reducing sugar

TMP (bar)
Reducing sugar
Prediction: Robs=94% 10
51 g L−1, permeate flux = Prediction: Robs=30%
60
13.27 Lm−2 h−1; experimental/ Prediction: Robs=40%

predicted solutes concentration in 5


30
the retentate (c) and permeate flux
(b) during diafiltration step using
cross-flow module under constant 0
0.0 0.5 1.0 1.5 2.0 2.5 3.0
0
0.0 0.5 1.0 1.5 2.0 2.5 3.0
pressure mode. Light-colored
V/Vo V/Vo
molasses: sucrose 123.57 g L−1,
reducing sugar 38.85 g L−1,
TMP = 25 bar c 150
d 80
Light-colored molasses Light-colored molasses
Concentration in retentate (gL-1)

120

Permeate flux (Lm-2h-1)


60

90 Sucrose
Reducing sugar 40
Prediction: R obs=94%
60 Prediction: R obs=40%
Prediction: R obs=60%
20
30

0 0
0.0 0.5 1.0 1.5 2.0 2.5 3.0 3.5 0.0 0.5 1.0 1.5 2.0 2.5 3.0
V/V0 V/V0

for the real solution would increase the solute retention (Luo dominant. As shown in Fig. 6a, the prediction line well
et al. 2013); however, in this work, the permeability loss after matches the experimental data for sucrose, while for reducing
experiment was only 3.95% (Table 4), indicating that the dif- sugar, as Vf/V0 > 5, the prediction line with a retention of 70%
ferent permeate flux (13.27 vs. 15–28 Lm−2 h−1) and feed deviates from the experimental data, and the experimental
concentrations (194 vs. 171.4 g L−1) were mainly responsible retention reduces to 65% because of the increasing sugar con-
for the sugar retention variation, and membrane fouling would tent in the retentate during the concentration operation. This
not be a bottleneck for this application in industry. increment in sugar concentration not only reduced the reten-
tion of reducing sugar but also elevated the TMP (Fig. 6b).
NF Concentration When concentrating the permeate from the diafiltration of real
solution, the sugar concentration in the retentate of cross-flow
In order to improve sucrose recovery, a concentration opera- membrane module was increasing with Vf/V0 as the same as
tion under a higher permeate flux of 39.8 Lm−2 h−1 was car- those for model solution, because its average permeate flux
ried out to treat the permeate from the diafiltration step. The was similar as that in dead-end filtration (Fig. 6c, d).
sugar retention was first measured at such permeate flux, In the second concentration step, a high permeate flux was
which was 97 and 70% for sucrose and reducing sugar, re- used, and the sucrose retention raised to 98% and the reducing
spectively. This remarkable increment in reducing sugar re- sugar retention increased to 76–78%. As seen in Fig. 7a, the
tention at higher permeate flux indicated that the separation of reducing sugar concentration becomes much higher than the
sucrose and reducing sugar by NF could not be operated at sucrose concentration in the retentate, implying that a further
high permeate flux, where the diffusive mass transfer was not concentration operation is meaningless. The TMP during the

Table 4 Water permeability of DL membranes before and after filtration during different steps

Water permeability (Lm−2 h−1 bar−1) Diafiltration step 1st concentration step 2nd concentration step

Before After Before After Before After

Model solution with dead-end filtration 8.1 ± 0.4 7.4 ± 0.6 8.6 ± 0.5 8.2 ± 0.3 8.4 ± 0.3 8.2 ± 0.4
Light-colored molasses with cross-flow filtration 7.6 7.3 7.6 7.6 7.6 7.6
922 Food Bioprocess Technol (2018) 11:913–925

Fig. 6 Experimental/predicted a 100


b 20
solutes concentration in the Model solution Model solution

Concentration in retentate (gL-1)


retentate (a) and TMP (b) during Sucrose
Reducing sugar
the first concentration step using 80 Prediction: Robs=97%
15
dead-end filtration cell under Prediction: Robs=65%
constant flux mode. Model Prediction: Robs=70%

TMP(bar)
60
solution: sucrose 10.5 g L−1,
10
reducing sugar 14.6 g L−1,
permeate flux = 39.8 Lm−2 h−1;
40

experimental/predicted solutes 5
concentration in the retentate (c) 20
and permeate flux (b) during the
first concentration step using 0 0
2 4 6 8 10 0 2 4 6 8 10
cross-flow module under constant
Vf/V0 Vf/Vo
pressure mode. NF permeate of
light-colored molasses: sucrose
5.77 g L−1, reducing sugar c 60 d 80
7.90 g L−1, TMP = 10 bar Light-colored molasses Light-colored molasses
Concentration in retentate (gL-1)

Sucrose
Reducing sugar

Permeate flux (Lm-2h-1)


45 Prediction: Robs=97% 60
Prediction: Robs=65%

30 40

15 20

0 0
2 4 6 8 10 2 4 6 8 10
Vf/Vr Vf/Vr

Fig. 7 Experimental/predicted a 50
b 25
solutes concentration in the Model solution Model solution
Concentration in retentate (gL-1)

retentate (a) and TMP (b) during


the second concentration step 40 20
using dead-end filtration cell
Sucrose
under constant flux mode. Model
TMP (bar)

30 Reducing sugar 15
solution: sucrose 1.53 g L−1, Prediction: Robs=98%
reducing sugar 12.0 g L−1, Prediction: Robs=76%

permeate flux = 132.7 Lm−2 h−1;


20 Prediction: Robs=78% 10

experimental/predicted solutes
concentration in the retentate (c) 10 5
and permeate flux (b) during the
second concentration step using 0 0
2 4 6 8 10 2 4 6 8 10
cross-flow module under constant Vf/Vo
Vf/Vo
pressure mode. NF permeate of
light-colored molasses: sucrose
0.68 g L−1, reducing sugar c 25
d 80
6.34 g L−1, TMP = 5 bar Light-colored molasses Light-colored molasses
Concentration in retentate (gL-1)

20
Permeate flux (Lm-2h-1)

60

15
Sucrose
40
Reducing sugar
10 Prediction: Robs=97%
Prediction: Robs=78%
Prediction: Robs=55% 20
5

0 0
2 4 6 8 10 2 4 6 8 10
Vf/Vr Vf/Vr
Food Bioprocess Technol (2018) 11:913–925 923

Fig. 8 A proposed cascade


nanofiltration process for
separation of sucrose and
reducing sugar based on the
experimental data and
mathematical modeling

concentration process continuously ascended as expected Figure 8 shows a proposed cascade NF process for sep-
(Fig. 7b). Regarding the real solution, as shown in Fig. 7c, aration of sucrose and reducing sugar based on the exper-
the sucrose concentration in the retentate was well predicted imental data and mathematical modeling. By using three
by the model with a retention of 97%, while the prediction line times water for diafiltration of light-colored molasses, the
with a reducing sugar retention of 78% was far higher than the ratio of sucrose in total sugar increased from 76.1 to
experimental data. This was caused by a much lower permeate 87.9%, and the impurities (e.g., reducing sugar, monova-
flux in cross-flow filtration (30–40 vs. 132.7 Lm−2 h−1, see lent salts, and small pigments) could be partly removed
Fig. 7d), and its retention of reducing sugar reduced to 55%. It from the molasses. In the NF process patented by
can be concluded that the reducing sugar retention was greatly Donovan and Hlavacek (2002), under a permeate flux of
affected by the permeate flux, and the separation of sucrose 14 Lm−2 h−1 at 65 °C, the ratio of sucrose in total sugar
and reducing sugar by NF should be operated below increased from 72.1 to 96.3% when three times water was
15 Lm−2 h−1 at 55–60 °C. Moreover, as listed in Table 4, the consumed, while this ratio was 62.0% in the permeate (in
membrane permeability decline after filtrations is not signifi- the present study, it was 41.9%). This comparison indicat-
cant for both model and real solution (less than 10%), espe- ed that the NF membrane used in Donovan and Hlavacek’s
cially for cross-flow filtrations with real solution (less than work had lower rejection of both sucrose and reducing
5%), meaning that the residual pigments in light-colored mo- sugar than that in our study, and their process would obtain
lasses would not cause obvious fouling to polyamide NF higher purity of sucrose but much lower sucrose recovery.
membrane and the cross-flow operation can further reduce Then, the treated diluted molasses could be used for su-
membrane fouling. Anyway, the separation performance of crose crystallization, and the diafiltration permeate was
dead-end and cross-flow filtrations was similar under the same further concentrated by 30 times (the resulting concentrate
operating conditions, and the results obtained with model so- has similar sucrose content as the diluted molasses) and
lution as feed could be used to guide industrial process. then recycled to the diafiltration step. In the permeate of

Table 5 Estimated economic analysis for sugar recovery from cane molasses by membrane process

Cost ($/ton molasses) Cane molasses Membrane and filtration process Evaporation/crystallization
150 8 30
Income ($/ton molasses) White sugar Fructose/glucose syrup
230 45

The prices of molasses, white sugar, and syrup in Chinese domestic market are used for calculation; the membrane modules are supposed to be used for at
least 1 year, supposing that 50% of sucrose in molasses can be crystallized and 80% of fructose/glucose can be extracted as liquid
924 Food Bioprocess Technol (2018) 11:913–925

the second concentration step, the ratio of sucrose was only Youth Innovation Promotion Association (2017069) of Chinese
Academy of Sciences.
2.4%, and this stream could be concentrated by NF270 at
room temperature to produce syrup drinking. A rough cost
estimation for the separation of sucrose and reducing sugar
from cane molasses by membrane processes is shown in
Table 5. Supposing that 50% of sucrose in molasses can be
References
crystallized and 80% of fructose/glucose can be extracted
Altmann, K., Clawin-Rädecker, I., Hoffmann, W., & Lorenzen, P. C.
as liquid, this novel technology is economically feasible if
(2016). Nanofiltration enrichment of milk oligosaccharides (MOS)
the membrane modules are able to maintain their perfor- in relation to process parameters. Food and Bioprocess Technology,
mance at 60 °C for at least 1 year. 9(11), 1924–1936.
Baikow, V. E. (2013). Final molasses. In Manufacture and refining of raw
cane sugar (pp. 218–224): Elsevier.
Bandini, S., & Morelli, V. (2017). Effect of temperature, pH and compo-
Conclusion sition on nanofiltration of mono/disaccharides: experiments and
modeling assessment. Journal of Membrane Science, 533, 57–74.
This work demonstrated that a cascade nanofiltration (NF) Ben Amar, N., Saidani, H., Deratani, A., & Palmeri, J. (2007). Effect of
temperature on the transport of water and neutral solutes across
process consisting of one diafiltration and two concentra- nanofiltration membranes. Langmuir, 23(6), 2937–2952.
tion steps could accomplish the separation of sucrose and Bernal, M., Ruiz, M. O., Geanta, R. M., Benito, J. M., & Escudero, I.
reducing sugar (i.e., glucose and fructose) in cane molasses (2016). Colour removal from beet molasses by ultrafiltration with
at high temperature. All the tested NF membranes could activated charcoal. Chemical Engineering Journal, 283, 313–322.
not separate sucrose and reducing sugar at 25 °C, while Córdova, A., Astudillo, C., Giorno, L., Guerrero, C., Conidi, C., Illanes,
A., et al. (2016). Nanofiltration potential for the purification of high-
they showed totally different retention behavior at 60 °C. ly concentrated enzymatically produced oligosaccharides. Food and
NT102, NT103, NF70, NF40-I, and NF40-II were not ther- Bioproducts Processing, 98, 50–61.
mal stable at 60 °C, and the sucrose retention of NT102, Clarke, S. J. (1995), Softening and purification of molasses or syrup,
NT103, and NF70 unexpectedly increased at higher tem- US5454875 A
Dang, H. Q., Price, W. E., & Nghiem, L. D. (2014). The effects of feed
perature. The retention of both sucrose and reducing sugar
solution temperature on pore size and trace organic contaminant
for NF270 and XN45 obviously declined at 60 °C as ex- rejection by the nanofiltration membrane NF270. Separation and
pected, displaying low separation efficiency and sucrose Purification Technology, 125, 43–51.
recovery. For DK and DL, the sucrose retention was kept Donovan, M., & Hlavacek, M. (2002), Process for purification of low
above 95% at 60 °C, while the reducing sugar retention grade sugar syrups using nanofiltration, US6406546 B1.
Goulas, A. K., Kapasakalidis, P. G., Sinclair, H. R., Rastall, R. A., &
greatly declined to 15 and 5%, respectively, which was
Grandison, A. S. (2002). Purification of oligosaccharides by
suitable for this purpose. nanofiltration. Journal of Membrane Science, 209(1), 321–335.
High temperature (55–60 °C), low permeate flux (< Kearney, M., & Kochergin, V. (2002). Chromatographic applications in
15 Lm−2 h−1) and high sugar concentration resulted in a low the cane sugar industry. International Sugar Journal, 104, 194–203.
retention of reducing sugar due to the dominant diffusive mass Koschuh, W., Thang, V. H., Krasteva, S., Novalin, S., & Kulbe, K. D.
(2005). Flux and retention behaviour of nanofiltration and fine ul-
transfer, which was desirable for the molasses separation by trafiltration membranes in filtrating juice from a green biorefinery: a
NF. Diafiltration/concentration of the model solution and membrane screening. Journal of Membrane Science, 261, 121–128.
light-colored molasses by the DL membrane could be well Kuhn, R. C., Maugeri Filho, F., Silva, V., Palacio, L., Hernández, A., &
predicted by the mathematical modeling if using right sugar Prádanos, P. (2010). Mass transfer and transport during purification
retention data. The deviations between prediction lines and of fructooligosaccharides by nanofiltration. Journal of Membrane
Science, 365(1–2), 356–365.
experimental data in the cross-flow filtration of real solution Lameloise, M.-L., & Lewandowski, R. (1994). Purification of beet mo-
were mainly caused by the permeate flux variation rather than lasses by ion-exclusion chromatography: fixed-bed modelling.
membrane fouling. Moreover, the separation performance of Journal of Chromatography A, 685(1), 45–52.
the dead-end and cross-flow filtrations was similar under the Li, J. (2008). Study on sucrose separation from molasses by membrane
filtration. Master thesis: Guangxi University.
same operating conditions, and the results obtained by dead-
Li, W., Ling, G.-Q., Huang, P., Li, K., Lu, H.-Q., Hang, F.-X., et al.
end filtration with model solution could be used to guide in- (2016). Performance of ceramic microfiltration membranes for
dustrial process. treating carbonated and filtered remelt syrup in sugar refinery.
Journal of Food Engineering, 170, 41–49.
Acknowledgements The authors thank the Development Center of Water Luo, J., Ding, L., Chen, X., & Wan, Y. (2009). Desalination of soy sauce
Treatment Technology, Hangzhou, for kindly providing membrane sam- by nanofiltration. Separation and Purification Technology, 66(3),
ples used in this study. 429–437.
Luo, J., Hang, X., Zhai, W., Qi, B., Song, W., Chen, X., et al. (2016).
Funding Information The authors thank the Key Research Program of Refining sugarcane juice by an integrated membrane process: filtra-
Chinese Academy of Sciences (No. KFZD-SW-211-3) for the financial tion behavior of polymeric membrane at high temperature. Journal
supports and. This work was supported by the B100 Talents Program^ and of Membrane Science, 509, 105–115.
Food Bioprocess Technol (2018) 11:913–925 925

Luo, J., & Wan, Y. (2013). Effects of pH and salt on nanofiltration—a Riffer, R. (1977), Process for the production of a colorless sugar syrup
critical review. Journal of Membrane Science, 438, 18–28. from cane molasses, US4046590 A.
Luo, J., Zhu, Z., Ding, L., Bals, O., Wan, Y., Jaffrin, M. Y., et al. (2013). Saidani, H., Amar, N. B., Palmeri, J., & Deratani, A. (2010). Interplay
Flux behavior in clarification of chicory juice by high-shear mem- between the transport of solutes across nanofiltration membranes
brane filtration: evidence for threshold flux. Journal of Membrane and the thermal properties of the thin active layer. Langmuir,
Science, 435, 120–129. 26(4), 2574–2583.
Mänttäri, M., Pihlajamäki, A., Kaipainen, E., & Nyström, M. (2002). Sharma, M., Patel, S. N., Lata, K., Singh, U., Krishania, M., Sangwan, R.
Effect of temperature and membrane pre-treatment by pressure on S., et al. (2016). A novel approach of integrated bioprocessing of
the filtration properties of nanofiltration membranes. Desalination, cane molasses for production of prebiotic and functional
145(1), 81–86. bioproducts. Bioresource Technology, 219, 311–318.
Meyer, P., Hartinger, M., Sigler, S., & Kulozik, U. (2017). Concentration Sharma, R. R., & Chellam, S. (2005). Temperature effects on the mor-
of milk and whey by membrane technologies in alternative cascade phology of porous thin film composite nanofiltration membranes.
modes. Food and Bioprocess Technology, 10(4), 674–686. Environmental Science & Technology, 39(13), 5022–5030.
Miller, G. L. (1959). Use of dinitrosalicylic acid reagent for determination Susanto, H., Roihatin, A., & Widiasa, I. N. (2016). Production of color-
of reducing sugar. Analytical Chemistry, 31(3), 426–428. less liquid sugar by ultrafiltration coupled with ion exchange. Food
Nakasone, S., Miyagi, S., Aragaki, T., & Higa, Y. (1985). Process for and Bioproducts Processing, 98, 11–20.
clarifying and desalinating sugar cane syrup or molasses. US, Valli, V., Gómez-Caravaca, A. M., Di Nunzio, M., Danesi, F., Caboni, M.
4492601. F., & Bordoni, A. (2012). Sugar cane and sugar beet molasses,
Nandy, T., Shastry, S., & Kaul, S. N. (2002). Wastewater management in antioxidant-rich alternatives to refined sugar. Journal of
a cane molasses distillery involving bioresource recovery. Journal of Agricultural and Food Chemistry, 60(51), 12508–12515.
Environmental Management, 65(1), 25–38. Wang, X.-L., Zhang, C., & Ouyang, P. (2002). The possibility of separat-
Ou, D.-Y. (1985), Separation of sucrose from molasses, US4519845 A. ing saccharides from a NaCl solution by using nanofiltration in
Pruksasri, S., Nguyen, T.-H., Haltrich, D., & Novalin, S. (2015). diafiltration mode. Journal of Membrane Science, 204(1–2), 271–
Fractionation of a galacto-oligosaccharides solution at low and high 281.
temperature using nanofiltration. Separation and Purification Zhao, L., Zhao, H., Nguyen, P., Li, A., Jiang, L., Xia, Q., et al. (2013).
Technology, 151, 124–130. Separation performance of multi-components solution by membrane
Ribeiro, A. C. F., Ortona, O., Simões, S. M. N., Santos, C. I. A. V., technology in continual diafiltration mode. Desalination, 322, 113–
Prazeres, P. M. R. A., Valente, A. J. M., et al. (2006). Binary mutual 120.
diffusion coefficients of aqueous solutions of sucrose, lactose, glu- Zhu, Z., Mhemdi, H., Zhang, W., Ding, L., Bals, O., Jaffrin, M. Y., et al.
cose, and fructose in the temperature range from (298.15 to 328.15) (2016). Rotating disk-assisted cross-flow ultrafiltration of sugar beet
K. Journal of Chemical & Engineering Data, 51(5), 1836–1840. juice. Food and Bioprocess Technology, 9(3), 493–500.

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