LWT - Food Science and Technology 151 (2021) 112181

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LWT
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Enhancement of fish sauce quality by application of nanofiltration

Quoc Dat Lai a, b, *, Hoang Dung Nguyen a, b
a
Department of Food Technology, Faculty of Chemical Engineering, Ho Chi Minh City University of Technology (HCMUT), 268 Ly Thuong Kiet Street District 10, Ho Chi
Minh City, Viet Nam
b
Vietnam National University Ho Chi Minh City, Linh Trung Ward, Thu Duc District, Ho Chi Minh City, Viet Nam

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

Keywords: This paper focused on application of nanofiltration (NF) for improving fish sauce quality by enhancement of
Fish sauce content of nitrogen compounds. Three kinds of NF membranes, including NF99, Desal DK and NTR7250, were
Nanofiltration investigated into separation capacity of total nitrogen (TN), amino nitrogen (AN) and NaCl from fish sauce. The
Amino nitrogen
influence of pretreatment of fish sauce by ultrafiltration (UF) on fish sauce quality was also investigated. Desal
Total nitrogen
Fouling mechanism
DK membrane exhibited the good performance for NF of fish sauce. UF pretreatment improved the rejections,
except NaCl, and permeate flux. The NF of UF pretreated fish sauce with Desal DK membrane was also carried out
at 40 bar of operating pressure. At 3.21 of concentration factor (CF), comparing to raw fish sauce, content of TN
and AN increased by 2.21 and 2.11 times, respectively; whereas, content of NaCl increased approximately 5%.
Results indicate that NF is a potential method for improvement of fish sauce quality. Hermia’s model was applied
to interpret the fouling phenomenon occurring in NF of UF pretreated fish sauce. The results showed that the best
fit to experimental data corresponds to cake layer formation model. The excellent fitting between the experi­
mental and calculating data for enhancement of fish sauce by NF was observed.

1. Introduction
Fish sauce is a traditional and staple ingredient in East and Southeast
Asia. It is a liquid extracted from fermentation of sea fish and salt. Fish
sauce is rich in flavour – active compounds which contributing to the
strong characteristic odor and taste of fish sauce (Park et al., 2002;
Yimdee & Wang, 2016; Zang et al., 2020). It has been also known as a
source of amino acids for human health (Najafian & Babji, 2019). As
CODEX STAN 302–2011, minimum content of TN and ratio of nitrogen
in amino form (determined by formal titration) to TN are 10 g/L and
40%, respectively. Quality of fish sauce is graded by being basic on TN
content: the higher content of total nitrogen determines the higher grade
of fish sauce.
In Southeast Asia, anchovy (Stolephorus indicus) is the main spice of
fish used for fish sauce production. It is mixed with sea salt, then fer­
mented in 6–12 months (Du et al., 2019; Thai Industrial Standards
Institute, 1983). When the fermentation is completed, fish sauce is
drained from the mixture and ripened in few months prior to packaging.
TN content in the first extract is in range of 30–40 g/L, depending on the
ratio of fish to salt (Lopetcharat et al., 2001). In order to enhance the
recovery of protein, after completion of first drainage, the residue is
added salt, fermented and drained again (Zhao et al., 2016). Normally,
TN content in second extract is in range of 10–20 g/L due to low protein
content in the residue. Fish sauce from second drainage is graded as
low-quality product due to low content of TN and AN. Recently, vacuum
evaporation has been applied for enhancement of quality of this product.
However, the high temperature results in the degradation of amino acids
and nitrogen volatile compounds, leading to decrease in sensory quality
of product. Moreover, high content of salt in fish sauce leads to the low
concentration factor and crystallization of sodium chloride in evapora­
tion. On the other words, evaporation is not adequate to improve the
quality of low grade fish sauce which drained from residue of first fish
sauce drainage.
Recently, membrane processes have been widely applied in food
industry for clarification, concentration and purification (Baker, 2012).
The main advantage of membrane separation is energy saving, conse­
quently, obtaining higher economic benefits than that of conventional
processes (Nath, 2017). For fish sauce, ultrafiltration (UF) has been
applied for recovery of antioxidant peptide (Najafian & Babji, 2019).
Electrodialysis has been applied for desalination of fish sauce (Ratana­
sanya et al., 2018). However, there is no report on application of
membrane separation for concentration to improve the quality of fish

* Corresponding author. Vietnam National University Ho Chi Minh City, Linh Trung Ward, Thu Duc District, Ho Chi Minh City, Viet Nam.
E-mail address: lqdat@hcmut.edu.vn (Q.D. Lai).

https://doi.org/10.1016/j.lwt.2021.112181
Received 16 January 2021; Received in revised form 7 June 2021; Accepted 19 July 2021
Available online 20 July 2021
0023-6438/© 2021 Elsevier Ltd. All rights reserved.
Q.D. Lai and H.D. Nguyen LWT 151 (2021) 112181

sauce.
NF is a membrane process with pore size being between UF and
reverse osmosis. Driving force of NF is the difference of effective pres­
sure between both sides of membranes. Mechanisms of mass transport
through NF membranes are convection, diffusion and electro-migration
(Schaefer et al., 2019). Thus, it could apply for separation of electrically
and non-electrically charged components. Recently, NF has been applied
for concentration, simultaneously rejection of salt, such as: skim milk
concentration (Khatkar et al., 2019) and whey (Léniz-Pizarro, Liu, Col­
burn, Escobar, & Bhattacharyya, 2021). Regarding amino acids, Wu
et al. (2020) applied NF for separation of amino acids in concentrated
solution. Luo et al. (2012) applied NF for desalination of soy sauce. NF
was also applied for controlling color of Japanese soy sauce (Miyagi
et al., 2013).
This research focused on the application of NF for upgrading quality
of low grade fish sauce. The screening of membranes for NF of fish sauce
was carried out. Effects of operating pressure and pretreatment by UF on Fig. 1. Scheme of plate and frame crossflow LabstakM20 system (1: feed tank,
the fish sauce quality was investigated. In addition, NF of fish sauce with 2: pump, 3: pressure gauge, 4: membranes, 5: permeate tank, 6: flowmeter).
plate and frame crossflow system for evaluation of feasibility was also
carried out. This study also analyzed the fouling mechanisms in NF 2.4. NF of fish sauce
process of fish sauce using Hermia’s model.
Screening NF membranes: This experiment was carried out by using
2. Materials and methods Labstak M20 system. Three kinds of membranes in Table 1 were inves­
tigated into the separation capacity of TN, AN and NaCl in fish sauce.
2.1. Materials Operating pressure was in range of 25–50 bar. Crossflow rate was 750 L/
h. In this experiment, permeate and retentate of NF were totally circu­
Low grade fish sauce was purchased in local companies in Phu Quoc, lated into feed tank to keep the feed unchange in chemical compositions
Vietnam. It is the second extract fish sauce, drained from fermentation of (total recirculation mode). The samples were collected when difference
residue of first extract anchovy (Stolephorus indicus) fish sauce. The TN in permeate flux in 30 min was lower than 5%.
and NaCl contents were approximately 13.4 and 205.0 g/L, respectively. The rejection (Ri ) (%) was calculated using the following formula:
All chemicals were supplied by Sigma Aldrich (USA) with analytical ( )
Cp,i
grade. Ri = 1 – 100 (1)
Cf ,i
Membranes: Membranes used in this research are showed in Table 1.
Prior to use, all membranes were flushed with water and stored in 500
Where, Cp and Cf are the concentrations of component i in the permeate
ppm NaHSO3 solution.
and the feed, respectively (g/L).
NF of fish sauce: This experiment was carried out with retentate
2.2. Membrane apparatus recycle mode by using Labstak M20 system. Crossflow rate was 750 L/h.
NF membranes and operating pressure were chosen from the screening
The membrane apparatus used in this research was plate and frame of NF membranes.
crossflow Labstak M20 system, which was manufactured by Alfa Laval Vo
(Denmark) (Fig. 1). The system is equipped Hydra Cell pump (Wanner CF = (2)
Vf
Engineering Inc., USA) and 7 couples of NF membranes with 0.252 m2 of
total active area Cf ,i Vf
Yi = (3)
Cfo,i Vfo

2.3. UF pretreatment of fish sauce Where: Cf : Concentration in feed (g/L), Cfo : Initial concentration in feed
(g/L), Vf : Volume of feed (L), Vfo : Initial volume of feed (L), CF: Con­
UF of fish sauce was conducted by Labstak M20 system with GR40PP centration factor (− ), Y: Yield of recovery (%), i: components.
membrane. Operating pressure was 5 bar. Crossflow rate was 750 L/h. Cleaning procedure: After each run of NF, crossflow membrane system
The UF was stopped when volume reduction rate was 100 L/h and was cleaned as the following procedure: Firstly, flushing with clean
permeate was brought to NF. water with approximately 5 times of the system hold up volume. Then,
recirculating clean water in 30 min at 5 bar of applied pressure and 750
Table 1 L/min of feed flow rate and following by recirculate NaOH solution
Characteristics of membranes. (pH10) in 30 min without applied pressure and 750 L/min of feed flow
No. Membranes Manufacturers Materials Pure water MgSO4 rate. Finally, flushing with clean water at 5 bar of applied pressure until
permeability Rejection pH of permeate and retentate was 6.0–7.0.
(L.m− 2.h− 1. (%)
bar− 1)
2.5. Analysis methods
1 GR40PP Alfa Laval Polysulfone – 100 kDaa
2 NF-99 Alfa Laval Composite 7.00 99b
3 Desal-DK DSS Polyamide 2.67 98c Sodium chloride (NaCl): NaCl content was analyzed as AOAC Offi­
4 NTR7250 Nitto Denko Polyvinyl – – cial Method 937.09 (Volumetric Method) (Assoc. Official Analytical
Alcohol Chemists, 2019).
a
Molecular weight cut off (MWCO). Total nitrogen (TN): TN content was analyzed as AOAC Official
b
Measured on 2000 mg/L MgSO4, 6.9 bar, 25 ◦ C. Method 940.25 (Kjeldahl method) (Assoc. Official Analytical Chemists,
c
Measured on 1000 mg/L MgSO4, 9 bar, 25 ◦ C. 2019).

2
Q.D. Lai and H.D. Nguyen LWT 151 (2021) 112181

Amino nitrogen (AN): AN content was determined as the following Table 2

equations (Thai Industrial Standards Institute, 1983): Flux expressions of Hermia model.
Fouling mechanism n value Derivative equation
CAN = CFN − CAM (4)
Complete pore blocking 2 ln(J− 1 ) = ln(J0 − 1)
+ kt
Where: CAN , CFN and CAM are the contents (g/L) of AN, formaldehyde Standard pore blocking 1.5 J − 0.5
= J0 − 0.5
+ kt
nitrogen and ammonia nitrogen, respectively. Intermediate pore blocking 1 J− 1
= J0 − 1
+ kt
Formaldehyde nitrogen: Formaldehyde nitrogen content was Cake formation 0 − 2 − 2
J = J0 + kt
analyzed by the titrimetric method (Thai Industrial Standards Institute,
1983). One mL of sample was diluted with 9 mL of water. Diluted
samples were titrated with 0.1N NaOH solution to pH 7.0. Then, adding unified equation. Where, J and J0 (L/m2.h) are the permeate flux at t (h)
10 mL of formaldehyde solution (pH 9.0, 38 %v/v) to the mixture. of operating time and initial time, respectively. The model to determine
Titration with 0.1 N NaOH solution was carried out to pH 9.0. Formal­ the fouling mechanism in the NF of fish sauce was built by linear
dehyde nitrogen content was determined as the following equation: regression analysis and the best fit of model to the experimental data
CFN = 0.1 × 14 × VNaOH (5) was selected based on the correlation coefficient (R2) value.
The variation of feed volume (VF, L) during the ultrafiltration is
Where: VNaOH is the volume (mL) of 0.1 N NaOH solution for titration of expressed as the following equation:
mixture from pH 7.0 to pH 9.0. dVF
Ammonia nitrogen: Ammonia nitrogen was analyzed by method in = − AJv (8)
dt
(Thai Industrial Standards Institute, 1983). Samples were diluted 10
folds with water. Then, 50 mL of diluted sample was poured into the Where, A: the membrane area (m2), Jv: permeate flux (L/m2.h).
Kjeldahl flask containing 100 mL of distilled water and 3 g of MgO. The The following equation describes the relationship between individ­
mixture was distilled by superheated steam to release volatile nitrogen ual solute variation in feed and permeate flows based on the mass bal­
compounds into 50 mL of 4%w/w boric acid containing methyl ance:
red-bromocresol green. Finally, distillate was titrated until obtaining the ( )
end-point with 0.05 M H2SO4 solution. Ammonia nitrogen content was d VF CF,i
= − AJv Cp,i (9)
determined as the following equation: dt
Substitute equation (1) to equation (9), equation (10) is obtained as
CAM = 5.6 × 0.05 × VH2 SO4 (6)
follows:
( )
Where, VH2 SO4 is the volume (mL) of 0.05 M H2SO4 solution. d VF CF,i
= − AJv CF,i (1 − Ri ) (10)
dt
2.6. Fouling analysis and mathematical model Rejection of other components was estimated as the mean of the
observed rejections obtained from experimental data because they did
The mechanisms of fouling in NF of fish sauce was analyzed based on not change so much. A, VF and CF o,i were determined from experimental
Hermia’ equation (Hermia, 1982): data. Using the fourth order Runger – Kutta method, solve the set of
( )n equations (from equation (8) to equation (10)). Matlab software (version
d2 t dt R2017b) was used to analysis the algorithm of mathematical model
=k (7)
solution (Doan & Lai, 2021).
dV 2 dV

Where, V is volume (L) of accumulative permeate at t (h) of operating

3. Results and discussion
time. k is constant of model. The values of n have been established for
different fouling mechanisms.
3.1. Screening of NF membranes
Equation (7) developed four empirical models (see Fig. 2) that
describe fouling behaviors. Table 2 summarizes the four models in a
3.1.1. Permeate flux
Permeate flux of three kinds of NF membranes is shown in Fig. 3.

Fig. 3. Permeate flux of NF membranes under different operating pressure (▴:

Fig. 2. Schematic representation of fouling mechanisms: (a) complete blocking; NF99, ●: NTR7250, ■: Desal-DK; solid-filled: non-pretreated fish sauce, non-
(b) intermediate blocking; (c) standard blocking and (d) cake layer formation. filled: UF-pretreated fish sauce).

3
Q.D. Lai and H.D. Nguyen
Result indicates that permeate flux linearly increased with increase in
operating pressure. It implies that, the concentration polarization was
eliminated by turbulence of fluid at 750 L/h of cross-flow flowrate (Asefi
et al., 2019). The result shows that, with the same operating pressure,
Desal DK exhibited the highest permeate flux; whereas, NF99 membrane
showed the lowest permeate flux. It means that total resistant in NF of
fish sauce with NF99 membrane was higher than one with Desal-DK;
although data in Table 1 exhibit that pure water permeability of NF99
was higher than one of Desal DK. It means that, membrane resistant of
Desal-DK membrane was higher than that of NF99. This phenomenon
can be explained by the fact that the high concentration of NaCl in fish
sauce results in high electrical charge of pore (Bawornruttanaboonya
et al., 2015; Jundeea et al., 2012; Wang et al., 2018). It leads to the
swollen of active layer which is caused by repulsive force between
electrically charged groups. The swollen results in decrease in resistant
of membrane to permeate flux (Izak et al., 2007; Kitazawa et al., 2018).
Desal-DK is made from polyamide which possesses more electrically
charged groups than two others. Thus, its active layer could be swollen
more than that of NFT99, made from composite, and NTR7250 made
from polyvinyl alcohol.
Result in Fig. 3 also indicates that pretreatment of fish sauce by UF
improved the permeate flux of three kinds of membranes. With the UF
pretreatment, macromolecule in fish sauce, such as protein, was
removed. Thus, the gel layer formation on membrane surface was
limited, consequently, resistant to permeate flux reduced. The formation
of gel layer on membrane surface by protein was observed and analyzed
by Sioutopoulos et al. (2019).
3.1.2. Rejection of TN and AN
Rejection of TN by three kinds of membranes in NF of fish sauce is
showed in Fig. 4. Result indicates that rejection of TN was significantly
influenced by kinds of NF membranes and pretreatment of fish sauce by
UF. In case of non-pretreated fish sauce by UF, at the same operating
pressure, NF99 exhibited the highest rejection of TN; whereas, the
lowest rejection was obtained with Desal DK. At 40 bar of operating
pressure, rejection of TN in un-pretreated fish sauce by NF99, NTR7250
and Desal DK were 62.48, 53.70 and 42.17%, respectively. Pretreatment
of fish sauce by UF resulted in increasing rejection of TN in fish sauce by
NF99 and Desal DK, but insignificantly influence on one by NTR7250.
The rejections of TN in NF of UF pretreated fish sauce by NF99 and Desal
DK membranes were insignificantly different and higher than one by
NTR7250. At 40 bar of operation pressure, rejection of TN in UF pre­
treated fish sauce by NF99, NTR7250 and Desal DK were 67.59, 55.58
and 62.48%, respectively.
Rejection of AN in NF of fish sauce by three kinds of membranes is
Fig. 4. Rejection of TN by different kinds of NF membranes. (■: Desal DK, ▴:
NF99, ●: NTR7250; continuous line: UF pretreated fish sauce, dashed line: non-
pretreated fish sauce).
4
LWT 151 (2021) 112181
showed in Fig. 5. In case of non-pretreated fish sauce, rejection of AN
was lower than that of TN. For example, at 40 bar of operation pressure,
rejection of AN in non-pretreated fish sauce by NF99, NTR7250 and
Desal DK were 53.74, 37.25 and 30.34%, respectively. However, rejec­
tion of AN and TN in UF pretreated fish sauce were approximate to each
other. At 40 bar of operation pressure, rejection of AN in UF pretreated
fish sauce by NF99, NTR7250 and Desal DK were 59.69, 47.05 and
56.84%, respectively. Rejection of AN in NF of UF pretreated fish sauce
was higher than one of non-pretreated fish sauce. It implies that the
pretreatment of fish sauce by UF resulted in an increase in rejection of
AN. This result is good accordance with the one obtained by using NF for
desalination of soy sauce (Luo & Wan, 2013). Rejection of AN in desa­
lination of soy sauce diluted 2 folds with deionized water by NF270 and
Desal DK were 59.47 and 67.52% at 24 bar of operating pressure.
However, Kovacs and Samhaber (2009) reported that, in nanofiltration
of amino acid solutions in concentration range of 0.001–2.0 M by Desal
DK membrane, rejections of glycine and glutamine at pH 7 were
approximately in range of 20–25 and 40–45%, respectively.
Results in Figs. 4 and 5 indicate that operating pressure significantly
influenced rejections of TN and AN. Rejections of TN and AN were
lowest at 35 bar of operating pressure. In NF, transport of weakly
electrically charged solutes, like peptides or amino acids, through NF
membrane is contributed by three mechanisms: diffusion, convection
and electro-migration (Schaefer et al., 2019). At low permeate flux,
electro-migration is predominant and determines rejection.
Electro-migration is enhanced by operating pressure, consequently,
leads to decrease in rejection. On the contrary, at high permeate flux,
convection is predominant. Increase in permeate flux restricts the con­
vection, thus, increase rejection of solutes. This is also reason for in­
crease in rejections of TN and AN when pretreating fish sauce by UF,
which led to an increase in permeate flux (Fig. 3).
3.1.3. Rejection of NaCl
Rejection of NaCl in NF of fish sauce is showed in Fig. 6. Increase in
operation pressure results in a decrease in rejection of NaCl. Rejection of
NaCl by NF membranes has been reported by many authors (Cao et al.,
2020; Peng et al., 2019). However, it has not been carried out at high
concentration of NaCl like fish sauce.
Result in Fig. 6 indicates that, pretreatment by UF led to decrease in
rejection of NaCl. Increase in operating pressure also caused decrease in
rejection of NaCl. In NF, with NaCl, a strongly electrical electrolyte,
electro-migration is significantly predominant (Szymczyk et al., 2003).
Increase in permeate flux causes increase in electromigration of elec­
trolyte through NF membrane, leading to reduce rejection of NaCl. Thus,
result in Fig. 6 can be explained by increase in permeate flux which is
Fig. 5. Rejection of AN by different kinds of NF membranes. (■: Desal DK, ▴:
NF99, ●: NTR7250; continuous line: UF pretreated fish sauce, dashed line: non-
pretreated fish sauce).
Q.D. Lai and H.D. Nguyen
Fig. 6. Rejection of NaCl by different kinds of NF membranes. (■: Desal DK, ▴:
NF99, ●: NTR7250; continuous line: UF pretreated fish sauce, dashed line:
unpretreated fish sauce).
resulted by UF pretreatment and increase in operating pressure (Fig. 3).
Desal DK membrane exhibited the good performance for NF of fish
sauce due to high permeate flux, high rejection of nitrogen compounds
and low rejection of NaCl, compared to NF99 and NTR7250.
3.2. NF of fish sauce
NF of UF pretreated fish sauce was carried out with Desal DK
membrane at 40 bar of operating pressure. Permeate flux in NF of UF
pretreated fish sauce by Desal DK membrane is showed in Fig. 7.
Permeate flux significantly reduced with time of operation. At initial
time, permeate flux was 14.15 L.m− 2.h− 1. At the time obtaining 3.21 of
CF, permeate flux was 4.97, L.m− 2.h− 1, approximately 2.85 time lower
than that at initial time. From Darcy’s equation (Baker, 2012), flux
decline in NF was caused by increase in resistant to permeate and dif­
ference of osmotic pressure between retentate and permeate sides. The
change in difference in osmosis pressure between retentate and
permeate sides was insignificant due to very low rejection of NaCl,
which determines osmosis pressure in fish sauce. Hence, flux decline in
NF of fish sauce can be explained by fouling resulting in increase in
fouling resistant, consequently in total resistant to permeate flux.
In order to model the permeate flux and estimate the maximum
theoretical CF value, a mathematical derived from combination between
film theory and osmosis pressure model was applied. This model is
expressed as the following equation:
(α)
Jv = kln (11)
CF
Where, Jv : permeate flux (L.m− 2.s− 1), k: Constant representing for mass
transfer coefficient in boundary layer on membrane surface (L.m− 2.s− 1),
Fig. 7. Permeate flux in NF of UF-pretreated fish sauce by Desal DK membrane
at 40 bar of operating pressure.
5
LWT 151 (2021) 112181
CF: concentration factor, α: Maximum concentration factor obtained by
NF.
Nabetani et al. (2012) successfully applied this model for modeling
permeate flux in purification of anserine and carnosine from chicken
extract by NF. Pan et al. (2013) also applied it for estimation of theo­
retical content of solid content in NF of coffee extract for concentration.
With the application of linear regression, estimated values of k (L/m2.s)
and α from equation (11) were 7.49 and 5.86.
The analysis of Hermia’s fouling model is stated in Table 3. The re­
sults show the fitting of the experimental results to the cake layer for­
mation model during the NF of fish sauce. This mechanism occurs when
large content of soluble solids found in fish sauce are unable to enter the
membrane pores. It can explained by the formation of boundary layer,
which caused to form of cake layer on membrane surface. Ibrar et al.
(2019) stated that the ion strength and sodium chlorine insignificantly
influence on fouling of NF membranes. Thus, in this case, fouling was
caused by adsorption of nitrogen compounds on surface and wall of
pores. Ariono et al. (2018) found cake filtration to be the dominant
fouling mechanism during the filtration palm kernel oil by using Her­
mia’s model. Lamdande et al. (2020) also found gel layer formation
having the main role in flux decline during the crossflow ultrafiltration
of crude extract of yerba mate.
Contents of TN, AN and NaCl in retentate in NF of UF pretreated fish
sauce by Desal DK membrane at 40 bar of operating pressure are shown
in Fig. 8. Result indicates that, contents of TN, AN and NaCl in retentate
against CF was linear. It means that change in rejections of these con­
stituents was insignificant in NF of fish sauce with Desal-DK membrane.
At 3.21 of CF, content of TN and AN were 28.81 and 12.98 (g/L), means
that they increased 2.21 and 2.11 folds compared to in feed, respec­
tively. And, the ratio of TN to AN was in range of 0.45–0.46 in NF of fish
sauce and insignificantly changed in NF. Whereas, content of NaCl at
3.21 of CF was 215.76 g/L, increasing 5% compared to in feed. These
figures indicate that quality of fish sauce was improved without the
significant increase in salt content which can causes the cardiovascular
disease. This is the advantage of this method over the enhancement of
nitrogen compounds content by evaporation. Furthermore, due to
insignificant augment in NaCl content, it does not lead to precipitation
of salt in storage of products, which occurs with evaporation.
Contents of TN, AN and NaCl in accumulative permeate in NF of UF-
pretreated of fish sauce by Desal DK membrane at 40 bar of operating
pressure are shown in Fig. 9. Due to the very low rejection of NaCl,
content of NaCl in accumulative permeate insignificantly changed and
was approximately 200 g/L at 3.21 of CF. Contents of TN and AN at 3.21
of CF were 6.43 and 3.07 g/L, respectively.
Recovery yields of TN, AN and sodium chloride are depicted in
Fig. 10. The recovery yields of TN and AN were approximate to each
other due to the insignificant difference in their rejection by Desal-DK
membrane. At 3.21 of CF, recovery yields of TN and AN were 66.98
and 65.64%, respectively. It means that there is amount of TN and AN in
permeate side. Nevertheless, their contents in permeate size was low
(Fig. 9). The permeate can be utilized for supply in fermentation in fish
sauce production to recover nitrogen and salt resources, simultaneously,
reduce the waste of production.
Based on equation (11), theoretically estimated values of contents
and recovery yields of TN, AN and NaCl in retentate is shown in Table 4.
The maximum contents of TN and AN can be reach 47.97 and 21.54 g/L,
Table 3
Hermia fouling model and fitting accuracy in terms of R.2.
Mechanism Modeling of flux R2 value
Complete pore blocking ln(J − 1
) = − 4.0571 + 0.1515t 0.7465
Standard pore blocking J− 0.5
= 0.1318 + 0.0117t 0.8236
Intermediate blocking J− 1
= 0.0173 + 0.0037t 0.888
Cake layer formation J− 2
= 0.0003 + 0.0002t 0.9633
Q.D. Lai and H.D. Nguyen LWT 151 (2021) 112181

Fig. 8. Concentrations in retentate in NF of UF-pretreated fish sauce by Desal
DK membrane at 40 bar (©: Total nitrogen, □: Amino nitrogen, △: NaCl).
approximately 3.5 times higher than that in raw fish sauce. These figures
are even higher than that in 1st grade of fish sauce (CODEX STAN
302–2011). Thus, NF is a promising method for enhancement of fish
sauce quality.
The concentration of retentate (feed) in NF of UF-treated fish sauce
by Desal DK membrane at 40 bar based on the flux decline model by
Hermia and the proposed mathematical model (Equation (7) to equation
(10)) which shown in Fig. 11. The results indicate that the model has a
good agreement between experimental data with each other. In case of
NaCl, in mathematical model, concentrations over time was higher than
those of experimental data. In the first stage, they were asymptotic and
fitted. In order to reach 49.17 g/L of TN, it need to operate NF process of
UF-treated fish sauce in 9.21 h. The content of AN and NaCl in feed were
22.36 and 233.44 g/L, respectively. The results can be used to predict
the time operation and the concentration of compounds for a target
content of amino compounds at the end of the NF operation.
4. Conclusions

Application of NF for improvement of fish sauce quality was inves­

Fig. 9. Concentrations in accumulative permeate in NF of UF-treated fish sauce
by Desal DK membrane at 40 bar (©: Total nitrogen, □: Amino nitrogen,
△: NaCl).
tigated. Desal DK membrane showed the high permeate flux and re­
jections of TN and AN; low rejection of NaCl. Thus, Desal DK membrane
is suitable for NF of fish sauce for improvement of quality. UF pre­
treatment of fish sauce enhanced the permeate flux and rejections of TN
and AN. The NF of fish sauce at 40 bar of operating pressure with UF-
pretreatment with Desal DK membrane was conducted. Result showed
that, at 3.21 of CF, contents of TN and AN increased 2.21 and 2.11 times,
with being 66.98 and 65.64% of recovery yields, respectively. Maximum
theoretical value of CF was estimated as 5.68. It is feasible to apply NF
with UF-pretreatment for improving fish sauce quality.
Fouling mechanisms were evaluated by Hermia’s model and cake
layer formation was inferred to be the most significant mechanism. A
mathematical model was applied to predict the concentration in feed of
nitrogen compounds and NaCl in NF of UF-treated fish sauce by Desal
DK membrane at 40 bar. A good agreement between the predicted and
experimental values was achieved, showing that this model may be
applied as a tool to the scaling up of processes for the enhancement of
fish sauce quality with high nitrogen compounds.

Data availability statement

Data available on request from the authors.

Fig. 10. Recovery yields in NF of UF-pretreated fish sauce by Desal DK mem­

brane at 40 bar (©: Total nitrogen, □: Amino nitrogen, △: NaCl).

Table 4
Contents and recovery yields of TN, AN and NaCl in retentate of NF of UF-
pretreated fish sauce by Desal DK membrane at maximum theoretical value of
CF.
Constituent Content in retentate (g/L) Recovery yield (%)

TN 47.97 61.09
AN 21.54 59.19
NaCl 229.27 19.08

Fig. 11. Relationship between experimental and calculated values of concen­

trations in feed as a function of operation time.

6
Q.D. Lai and H.D. Nguyen
CRediT authorship contribution statement
Quoc Dat Lai: Conceptualization, Data curation, Formal analysis,
Methodology, Writing – original draft. Hoang Dung Nguyen: Funding
acquisition, Investigation, Supervision, Writing – review & editing.
Declaration of competing interest
All the authors declare that they have no conflict of interest.
Acknowledgments
We acknowledge the support of time and facilities from Ho Chi Minh
City University of Technology (HCMUT), VNU-HCM for this study.
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