Water Resources and Industry 31 (2024) 100244

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Water Resources and Industry

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The effect of pretreatment and the operating temperature on

reverse osmosis in make-up water preparation
Reem Shaheen , Edit Cséfalvay *
Department of Energy Engineering, Faculty of Mechanical Engineering, Budapest University of Technology and Economics, Műegyetem Rkp. 3, 1111,
Budapest, Hungary

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

Keywords: Raw water cannot be used directly to compensate for water losses in power plants. Thus, a series
Make-up water treatment of technological steps are required to produce ultra-pure water from fresh- or seawater. This study
Pretreatment recommends using a proper pretreatment consisting of two-steps of microfiltration, ultrafiltration
Temperature effect
and nanofiltration. Desalination was carried out using two stages of reverse osmosis. The effect of
Reverse osmosis
Multiparameter evaluation
increasing feed temperature from 25 ◦ C to 48 ◦ C on the second stage of reverse osmosis was
studied and showed an exponential increase in flux and permeability, and reduced operation
time. For freshwater, no temperature effect was observed on rejection in this temperature range;
however, the highest rejection values calculated based on conductivity were observed at a 40 %
recovery at all temperatures in seawater (96.6 % and 97.6 % at 48 and 25 ◦ C, respectively). As a
result of the multiparameter evaluation using the ranking method for the second reverse osmosis
stage, 36 ◦ C is found to be the optimum temperature.

1. Introduction

The high need for ultrapure water as a feed of thermal power plants puts critical pressure on traditional pretreatment techniques;
this leads to depending on membrane pretreatment as a promising alternative [1]. Membrane-based pretreatment technology helps
reducing the fouling of reverse osmosis (RO) membrane and energy consumption, vital for operating an RO unit properly and
increasing the lifetime of RO desalination plants [2]. Theoretically, the membrane permeability rate could be enhanced by increasing
the feed’s temperature, significantly decreasing the energy consumption of the RO unit [3]. Also, the mass transfer and the membrane
separation performance are strongly influenced by the feed water temperature [4]. Membrane desalination is a process where the
water and the dissolved salts are separated by a physical method; water molecules with a size smaller than the membrane pores in the
case of nanofiltration (NF), as partial desalination, can pass through the membrane while the hydrated divalent or multivalent salts are
prevented. Dissolved salts can rarely be transported through the membrane via diffusion [5]. In desalination, membrane processes are
more effective in energy consumption compared to thermal processes resulting in low water production costs [6]. Therefore, the range
of RO membrane applications has dramatically increased in recent years; around 80 % of the total desalination plants worldwide are
RO plants, which seems a promising source of freshwater in the future [1,7].
Currently, the priority is to obtain a more effective operation of RO desalination by minimizing energy consumption and improving
the operation process; this can occur by controlling the parameters that significantly influence process efficiency [7]. The key

* Corresponding author.
E-mail address: csefalvay.edit@gpk.bme.hu (E. Cséfalvay).

https://doi.org/10.1016/j.wri.2024.100244
Received 19 July 2023; Received in revised form 17 January 2024; Accepted 17 January 2024
Available online 18 January 2024
2212-3717/© 2024 The Authors. Published by Elsevier B.V. This is an open access article under the CC BY-NC-ND license
(http://creativecommons.org/licenses/by-nc-nd/4.0/).
R. Shaheen and E. Cséfalvay Water Resources and Industry 31 (2024) 100244

performance parameters, such as permeate flow rate, recovery and salts’ rejection, are commonly used to explain RO performance and
efficiency [8]. Feed water temperature is an important parameter influencing RO membrane efficiency and facilitating effective
operation. Due to the strong influence, high feed temperatures lead to lower viscosity, higher permeate flux and membrane perme­
ability [9]. Al-Mutaz and Al-Ghunaimi studied the changes in water permeation rate theoretically through the membrane according to
changing the feedwater temperature. In conjunction with the increasing temperature, the viscosity of the solution declines, and a
higher water diffusion rate through the membrane is obtained; thus, the membrane permeability increases [10]. In addition, feed
temperature affects solute accumulation at the membrane surface, primarily increasing the pressure drop, decreasing the flow rate
throughout the process, and lowering the membrane’s lifetime [5,11]. Both salt rejection and concentration polarization decrease due
to the quick diffusion of the salt ions through the membrane and back away from the membrane surface in conjunction with the rising
feed water temperature, resulting in lower scale formation [12,13]. Numerous researchers have examined how temperature affects the
RO process’ efficiency associated with energy concerns. The key findings may be summed up as follows.
Koutsou and coworkers analyzed the specific energy consumption (SEC). They fed the RO unit with a brackish and seawater and
experienced working under an increased temperature of the feed within the range (15–40 ◦ C). The results showed that the total SEC
was significantly reduced through the applied temperature range for brackish water as the feed temperature increased. Increasing the
temperature, viscosity decreases, leading to rising values of both permeate flux and permeability; these factors positively affect
lowering energy consumption. However, for seawater, they recommended working in a lower range of feed temperature (up to 25 ◦ C)
to avoid higher osmotic pressure, which neutralizes the positive influence of the feed temperature and increases the total energy
consumption. They mentioned one negative impact of increasing the temperature within the 30–35 ◦ C range: reduced solute rejection
occurs due to the increased solute diffusivity and, thus, degradation in the membrane’s permeate quality and increased scaling po­
tential. Therefore, the membrane performance’s degradation related to high feed temperature must be considered [7]. Similar findings
show that an increase in temperature will cause a drop in net energy consumption [4,14,15]. Meanwhile, a series of laboratory ex­
periments by Jin and coworkers showed increased salt rejection along with increased temperature [4]. Altmann and coworkers studied
the increasing temperature of feed from 25 to 40 ◦ C and observed an increased conductivity of the permeate [15].
Gedam and colleagues examined the effects of operating conditions on the performance of polyamide RO membrane (thin film
composite polyamide spiral wound RO membrane) for groundwater. As the temperature increased from 18 to 40 ◦ C at fixed measuring
time, permeate fluxes rose from 1.4 to 2.3 L/(m2⋅min), which equal to 84–138 L/(m2⋅h), and the recovery increased from 22 to 36 % as
well; meanwhile, the salt rejection declined from 92 to 85 % [16]. Similar results regarding improving the membrane permeability,
along with increasing feed temperature, were achieved by Jiang and coworkers [17].
Alsarayreh et al. assessed how adding an energy recovery device might affect the energy requirement of the RO process. They
worked on a multistage multi-pass RO system (four steps-RO). So, they carried out a simulation showing the impact of changing
applied conditions of the brackish water RO process on the plant performance indicators. Increasing the feed water temperature and
pressure enhanced the recovery; they recorded an increase in recovery by 12.7 % due to the rising temperature from 25 to 30 ◦ C. They
expected a slight reduction in permeate quality in conjunction with increasing the feed temperature [6].
Goosen and coworkers evaluated the feed temperature impact on permeate flux and salinity by experimenting with several feed
flow rates and feed water with different salinity levels. They worked within the temperature range of 20 and 40 ◦ C under 35 and 45 bar
applied pressures, and the flow rate of the feed changed from 540 to 10,180 L/h. According to their results, as the feed temperature
increased from 20 to 40 ◦ C at 35 bar, the permeate flux value increased by 50 %, showing very high sensitivity of the membrane to
temperature change. Focusing on the same effect at 45 bar, the increase in flux was 42 %, so slightly lower than at lower pressure [11].
It can be criticized why the authors obtained lower flux values at 30 ◦ C compared to 20 ◦ C at both applied pressures.
The above-listed research studied feeding the raw water directly to the desalination stage without pretreatment, negatively
affecting the membrane and the permeate quality. Pretreatment prior desalination stage seems essential, especially at industrial scale.
According to our previous results from laboratory-scale experiments, pretreating the raw water using coagulation resulted in a large
amount of residuals which would need a further step, such as sedimentation using large-volume tanks at an industrial scale to remove
the residuals. We pointed out that microfiltration (MF) is considered an effective technology in the pretreatment stage for both
seawater and freshwater, producing good quality permeate (almost free of total suspended solids (TSS)), which could be a good
alternative to the coagulation-flocculation process [18,19] and can provide a proper pretreatment prior desalination. Applying the
same technological scheme for fresh water and seawater offers a good comparison since no study like this was available before.
In our current work, raw water is pretreated first via a series of membrane filtration steps, starting from two steps of MF followed by
ultrafiltration (UF) and NF. Then the pretreated water with low conductivity and free of TSS content is suitable to feed the first reverse
osmosis unit (RO-I), i.e., the first step of the desalination unit. The permeate of the first RO is then fed to the second RO under different
temperatures, studying its effect on RO-II’s permeate flux, permeability, operation time, permeate quality, and salt rejection at a fixed
recovery.

2. Material and methods

Filtration experiments for freshwater (Budapest, Hungary) and seawater (Mediterranean Sea, Isola, Slovenia) as raw water sources
were carried out using a universal bench-scale test membrane filtration apparatus in cross-flow mode (CM-CELFA AG P_28). The liquid
flowed through twisting tubes in the apparatus to provide cross-flow filtration. The device’s membrane consisted of a 75 mm diameter
circular sheet with a 28 cm2 active surface area that was positioned atop a porous sintered disk. Membranes were conditioned prior the
first use as soaking them into distilled water for one day. Cross-flow filtration involves directing the flow of liquid parallel with the
membrane surface and the permeate leaves perpendicular to the surface. As the liquid flows over the membrane, the purified water

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passes through, while the concentrate is collected on the opposite side of the membrane. Since the tank had a capacity of 500 mL, the
processed quantity for one experiment was maximized at 0.5 L. Water is circulated between the membrane surface and the tank using a
circulation pump which maintained the cross-flow filtration mode; according to the manual, the circulation pump delivery rate is 1.81
L/min at 8 bar. The appliance’s tank was sealed and pressurized by using inert gas (Nitrogen gas); hence, the pressure inside the tank is
kept constant and greater than the atmospheric. The permeate leaves the equipment at atmospheric pressure. A Thermo Scientific
SC100 A10 type thermostat was used to keep the temperature constant throughout the experiment.
The description of raw water characteristics (chloride ion concentration, TSS content and specific electric conductivity (later on
conductivity or K)) are described in Table 1. The RO-II’s feed was pretreated by a series of membranes in the pretreatment stage as
dead-end MF (MF-I), cross-flow MF (MF-II), UF, NF, and a desalination step as RO-I. All experiments in the pretreatment stage and the
first stage of desalination (i.e., RO-I) were carried out at 25 ◦ C. After these series, the second RO was installed to improve the permeate
quality to proceed towards ultra-pure water (Fig. 1); noteworthy, Fig. 1 is a scheme showing the improvement of permeate quality by
using different stages of membrane filtration, however, the retentate flows are not indicated in the figure.
Membrane characteristics and applied pressures for each filtration step are listed in Table 2. No circulation was used in the case of
the dead-end MF-I, while feed recirculation was maintained by a circulation pump in the case of MF-II, UF, NF, RO-I and RO-II, which
were used in cross-flow mode. Permeate was collected continuously, and retentate was removed at the end of the experiment.
Noteworthy that no external pressure was used for MFs; just the hydraulic pressures over the atmospheric pressure were applied (1
bar), but in the case of the other membrane filtrations, inert nitrogen gas was introduced into the equipment to adjust and maintain the
applied pressure.
During RO-II experiments, 20 experiments were carried out at five different temperatures for both pretreated water samples (fresh-
and seawater). The tested feed temperatures were 25, 30, 36, 42, and 48 ◦ C, so relevant parameters were measured, such as measuring
time and the related permeate volume until reaching 80 % recovery (which can be defined as the volume of permeate over the initial
volume of the feed). The permeates’ conductivity was measured every 10 mL. Permeate charges were then summed up at the end, and
as the final evaluation, total mass, permeate volume, and conductivity were measured. A 340I type WTW combined pH/conductivity
meter was used to measure the conductivity; the average error was less than 2 % based on measurements. The relationship between
conductivity and seawater and its diluted solutions are shown in the supplementary material. Permeate flux, permeability and salt
rejection were calculated based on the measured data.

3. Results and discussion

3.1. Pretreatment stage

Since membrane filtration is an environmentally friendly method for particle removal, a 5–13-μm particle retention membrane was
used as an initial step in order to protect the forthcoming 0.45 μm pore-size MF membrane. UF is an efficient method for removing
natural organic matter [20] and NF is suitable for partial desalination due to its capability to retain multivalent ions; we recommend
this sequence of membrane filtration steps as pretreatment technology prior to desalination in order to have a comprehensive com­
parison for both fresh- and seawater (as raw water samples). All experiments were evaluated according to the mass balance at first,
which is given in Eqs. (1a) and (1b).
∑ ∑
min = mout (1a)

mfeed + mvoidage = mpermeate + mretentate (1b)

The average error was 0.73 %, 0.49 %, and 0.50 % for MF-II, UF, and NF, respectively; which are below an acceptable value (< 2
%).
Permeate flux (Jv) is the volumetric flow rate (dV/dt [L/h]) of permeate per unit effective area (A [m2] of the membrane. Flux was
calculated according to Eq. (2),
[ ]
1 dV L
JV = ⋅ , expressed in , (2)
A dt (m2 ⋅ h)
Dead-end particle filtration (MF-I) aims to significantly reduce raw water’s TSS content and protect the 0.45 μm pore-sized MF-II
membrane used in cross-flow mode. The filtration process was extremely quick; the average fluxes tend to be 6000 L/(m2⋅h) and 5500
L/(m2⋅h) in the case of freshwater (FW) and seawater (SW), respectively (Fig. 2).
The 0.45 μm pore-sized MF-II membrane could work efficiently, providing a quick filtration and an almost constant high flux of
about 4800 L/(m2⋅h) in case of FW. Similarly, to FW results, MF-II of SW could result in a stable flux but lower than obtained for FW
due to the composition of the SW. A flux comparison of MF-II can be seen in Fig. 3.

Table 1
Parameters of the raw water samples that used in the experiments [18,19].
Sample C −
Cl [mg/L] TSS [mg/L] K Water intake area

Freshwater 35.9 ± 1.3 58.0 ± 1.7 431.0 μS/cm Danube water, Műegyetem rkp. Budapest, Hungary (10th October 2022)
Seawater 19,534.0 ± 0.4 10.8 ± 1.0 52.6 mS/cm Isola, Slovenia (21st July 2021)

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Fig. 1. Scheme of the series of batch experiments conducted in laboratory-scale.

Table 2
Membranes’ characteristics and applied pressure differences in each filtration step.
Membrane Mode Purchased from Type Polymer Pressure drops [bar] Effective Area [cm2]

MF-I dead-end VWR International Ltd. No.413 Filter Paper, Qualitative 1.0 38.5
MF-II cross-flow VWR International Ltd. Supor@-450 Hydrophilic polyether sulfone 1.0 28.0
UF cross-flow Sterlitech Company JW Polyamide-TFC 10 28.0
NF cross-flow Sterlitech Company DL Polyamide-TFC 20 28.0
RO-I, RO-II cross-flow Sterlitech Company AG Polyamide-TFC 35 28.0

Fig. 2. Flux values versus recovery of the first step of microfiltration (MF-I) for freshwater and seawater experiments conducted at 1 bar.

As we proceed to finer filtration membranes, higher pressure must be applied to maintain the driving force of filtration, while lower
fluxes are achievable in further technological steps. Although UF showed a decline in the first 40 % of the recovery for both water
samples, average fluxes tended to be constant until the end of the experiment, see Fig. 4. NF showed a relatively stable flux rate of 150
L/(m2⋅h) and 80 L/(m2⋅h) for FW and SW, respectively throughout the experiment indicating the proper selection of treatment steps.
Since both TSS and conductivity are informative parameters and their measurements are industrially viable, they can be used to
monitor the stage of the processes easily on site. Total organic carbon (TOC) and ion content are scientifically important, but these
parameters can be measured ex-situ, meaning samples must be taken to the laboratory to be analyzed. Therefore, TSS and conductivity
were identified as the followed parameters. As it can be seen in Table 3, 75 % of the TSS can be filtered by a 5–13 μm particle-retention
MF membrane (MF-I) in the case of FW. Considering the original TSS values of raw SW and MF-I filtrates, the difference is not as
significant as observed for FW. A further decrease in TSS content could be obtained by the cross-flow MF (MF-II) in case of both water
samples. Using the UF membrane, TSS could be further decreased below ten mg/L in the case of FW. Additionally, this low value was

Fig. 3. Flux values versus recovery of the second step of microfiltration (MF-II) for freshwater and seawater experiments conducted at 1 bar.

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Fig. 4. Flux values versus recovery of the ultra- and nanofiltration steps conducted at 10 bar and 20 bar, respectively during the pretreatment stage
for fresh- and seawater experiments.

Table 3
Permeate characteristics TSS and K during the pretreatment stage using a series of membrane filtration technologies.
Freshwater Seawater

TSS [mg/L] K [μS/cm] TSS [mg/L] K [mS/cm]

Raw water 58.0 ± 1.7 431.0 10.8 ± 1.0 52.6

MF-I 14.0 ± 1.8 397.0 10.2 ± 1.1 52.1

MF-II 12.0 ± 2.3 381.0 <10 51.0
UF <10 373.0 <10 48.7
NF <10 123.0 <10 39.3

reached for SW after using MF-II. The recoveries are 100 %, 90 %, and 90 % for MF-I, MF-II, and UF, respectively. Thus, MFs/UF system
has a total recovery of 81 % which means that 81 % of the feed volume was obtained as a treated water.
In further steps, conductivity values of permeates were measured and provided better information on the quality of the water and
the enhancement of the treatment methods. These values were continuously decreasing; however, a significant decrease could be
observed for the NF steps (a reduction of 71.5 % and 25.3 % for the FW and SW, respectively). The NF permeate still represents a very
high conductivity value (39.3 mS/cm) due to the high NaCl content of SW, which can partially pass through the NF membrane
(Table 3).

3.2. First step of desalination

RO-I was used as a first step of desalination of NF permeate for both FW and SW and resulted in a permeate with an average
conductivity of 22 μS/cm and 11.70 mS/cm for FW and SW, respectively. Despite the three orders of magnitude difference in con­
ductivity in water samples, RO-I fluxes were comparable. They showed an average flux of 120 and 40 L/(m2⋅h) for FW and SW,
respectively (Fig. 5).
Mass balance was calculated for the two steps of RO and the average error was 0.38 %, and 0.46 % for RO-I and RO-II, respectively.
The low conductivity values make the permeate appropriate for further treatment with a second-step RO. RO-II experiments were
carried out to enhance the ion removal to proceed ultra-pure water; 25 ◦ C was selected as initial operating temperature of desalination.
In order to emphasize the role of NF, permeates of all stages were analyzed: cation and anion compositions after each membrane
filtration stage were measured and shown in Tables 4 and 5, respectively.
Since UF does not have a real effect on ion composition, anion and cation concentrations were very similar to the raw water (RW)
values of both samples (SW and FW). Inserting NF as a final step of pretreatment shows a benefit on the slightly reduced monovalent

Fig. 5. Permeate flux values versus recovery of first step of desalination (RO-I) for fresh- and seawater experiments conducted at 35 bar applied
pressure at 25 ◦ C.

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Table 4
Cation concentrations and standard deviations (mg/L) in the permeate of each membrane filtration stage carried out at 25 ◦ C of SW and FW samples.
sample Na+ ±Na+ K+ ±K+ Mg2+ ±Mg2+ Ca2+ ±Ca2+

SW RW 10986.00 268.33 402.00 29.56 1219.00 60.33 654.00 52.74

UF 9867.00 241.01 404.00 29.71 1359.00 67.26 506.00 40.81
NF 8877.00 216.83 415.00 30.51 568.00 28.11 205.00 16.53
RO-I 1884.50 31.40 77.75 5.55 103.25 4.77 57.50 4.52
RO-II 80.25 2.13 0.00 0.00 2.70 0.12 2.09 0.16

FW RW 17.55 0.33 3.08 0.22 14.83 0.67 45.58 3.57

UF 14.85 0.38 2.33 0.17 11.72 0.53 42.29 3.31
NF 11.43 0.14 1.79 0.13 3.05 0.14 14.40 1.13
RO-I 1.13 0.05 0.30 0.02 0.51 0.02 2.54 0.20
RO-II 0.16 0.01 0.00 0.00 0.17 0.01 0.96 0.07

Table 5
Anion concentrations and standard deviations (mg/L) in the permeate of each membrane filtration stage carried out at 25 ◦ C of SW and FW samples.
sample Cl− ±Cl− NO3- ±NO3- SO2-
4 ±SO2-
4

SW RW 19362.00 619.95 0.00 0.00 2420.00 77.49

UF 18110.00 579.86 0.00 0.00 2202.00 70.51
NF 14822.00 474.58 0.00 0.00 332.00 10.63
RO-I 3058.50 81.28 0.00 0.00 100.50 2.67
RO-II 119.12 2.99 0.00 0.00 0.70 0.02

FW RW 18.31 0.46 2.84 0.07 26.47 0.67

UF 18.08 0.46 2.70 0.07 21.81 0.55
NF 14.59 0.37 2.36 0.06 1.95 0.05
RO-I 1.17 0.03 0.03 0.00 0.82 0.02
RO-II 0.33 0.01 0.00 0.00 0.25 0.01

and significantly reduced divalent ion concentrations. The average ion concentrations given in Tables 4 and 5, are related to RW
concentration of each ion providing a rejection value (R). Rejection is calculated according to the following equation:
( )
Cp
R= 1− ⋅ 100% (3)
Cf

where cp is the permeate concentration, cf is the feed concentration provided in the same measurement unit, such as [mg/L].
Noteworthy, the standard deviation of raw SW initial potassium (K+) concentration must be considered in case of calculating the
rejection value. The effects of all filtration steps on ion rejections are illustrated in Fig. 6 and Fig. 7. As it can be seen in the figures, UF
does not have a significant role in ion rejection, but a small rejection can be observed; which could be explained due to ions attached to
organics that filtered by UF, lowered the concentration of ions in the UF permeate, thus resulting in a slight rejection value.
The role of NF is remarkable for both water samples: divalent ions, such as magnesium, calcium and sulphate: 53.4 %, 68.7 %, 86.3
% for SW (Fig. 6) and 79.4 %, 68.4 % and 92.6 % for FW (Fig. 7), respectively. Meanwhile partial rejection of monovalent ions is
noticeable by NF; the rejection values of sodium, potassium, and chloride are 19.2 %, 11.1 % and 23.5 % for SW, respectively. No
nitrate could be detected in SW, but it was measurable in FW with a rejection of 16.6 %. Due to the lower initial sodium and chloride
content of FW, these rejection values showed higher % than observed in SW (Fig. 7).
RO-I show a significant rejection of ions: it is over 82 % for sodium, potassium and chloride and over 91 % magnesium, calcium and

Fig. 6. Total rejection of ions after each step of membrane filtration related to the initial concentration for SW experiment.

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Fig. 7. Total rejection of ions after each step of membrane filtration related to the initial concentration for FW experiment.

sulphate in case of SW (Fig. 6), meanwhile the rejection obtained for RO-II meet the theoretical value (over 99 % for all ions). Besides,
RO-I and RO-II showed rejection for all ions exceeding 90 % in case of FW (Fig. 7).
Higher feed temperatures or higher pressures shall be applied to enhance the RO-II flux. Therefore, the effect of higher feed
temperatures on RO-II feed water is studied and illustrated in the following sections.

3.3. Effect of temperature on the second stage of desalination

Flux values were calculated at every two percent recovery. Still, due to the starting of batch experiments (uncertainty is high in the
beginning), the first four values were ignored from the figures. The quality of the feed mainly influences the recovery of RO. The
contaminants are inorganic salts which raise the osmotic pressure (π) and can cause membrane fouling if reaching the saturation point
which shall be avoided. To obtain a visible graph, flux values at every 10 % recovery in the range of 10–80 % are shown in Figs. 8 and 9.
The permeate flux increased along with increasing feed temperature from 25 to 48 ◦ C and showed the same trend; in case of FW
(Fig. 8), the highest flux was obtained at the highest temperature (48 ◦ C), as expected and it was more than doubled considering the
flux observed at 25 ◦ C as a basis.
The effect of temperature on flux was similar for pretreated SW as FW ones, but the difference was lower; flux increased by 38 %
during the feed temperature increase from 25 to 48 ◦ C, see Fig. 9. The highest flux was observed at the highest temperature, as expected
and it is in agreement with the values observed by Al-Mutaz and Al-Ghunaim [10]. Goosen and coworkers tested the NaCl model
solution, having a concentration similar to SW, and obtained 42 L/(m2⋅h) at 30 ◦ C at 35 bar [11]. In our case, the application of the
proper pretreatment stage, including NF, can lower the NaCl content in the feed of RO-II; thus, it can increase the flux at the same
temperature and applied pressure at an 80 % recovery, a flux of 72 L/(m2⋅h) was observed.
The average fluxes were calculated and considered as the typical flux of a given temperature; they showed an exponential
dependence on feed temperature at a constant applied pressure (35 bar). Considering the FW flux measured at 25 ◦ C as a basis, a
temperature increase up to 48 ◦ C resulted in a 119.22 % increase in the permeate flux (Fig. 9).
The exponential relationship is more visible when depicting the natural logarithm of flux at an 80 % recovery (ln Jv, 80 %) versus
inverse temperature (1/T), resulting in a linear correlation, as seen in Fig. 10 and Eq. (4).

ln Jv = − 33.268⋅ 1/T + 5.9148 (4)

where T is the temperature in Celsius in the range of 25 and 48 ◦ C.

Similar to the findings obtained for pretreated FW, the exponential dependence of average flux on feed temperature is also relevant
in the case of SW. As the feed temperature increased from 25 to 48 ◦ C, the average flux increased by 38.48 %, far below the 119.22 %

Fig. 8. Averages fluxes versus recovery during the second step of Reverse Osmosis for Freshwater experiment at 35 bar applied pressure at different
temperatures.
STDEV = ±3.53, ±4.09, ±7.63, ±7.57, ±7.29 at 25, 30, 36, 42, and 48 ◦ C, respectively.

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Fig. 9. Averages fluxes versus recovery during the second step of Reverse Osmosis for Seawater experiment at 35 bar applied pressure at different
temperatures.
STDEV = ± 9.17, ±7.12, ±8.23, ±14., and ±15.87 at 25, 30, 36, 42, and 48 ◦ C, respectively.

Fig. 10. The natural logarithm of fluxes of second step of Reverse Osmosis at 80 % recovery versus reversed temperature for pretreated freshwater.

observed for FW. The linear relationship for SW is shown in Fig. 11 and Eq. (5).

ln Jv = − 13.145⋅ 1/T +4.7267 (5)

where T is the temperature in Celsius in the range of 25 and 48 C. ◦

Considering the positive effect of feed temperature on flux, it can be stated that less time was required to reach the same recovery at
higher temperatures. Using a test membrane with an effective area of 28 cm2, 48 min were sufficient to get an 80 % recovery at 48 ◦ C,
and it took 1.5 h when operating at 25 ◦ C. As the feed temperature rose from 25 to 48 ◦ C, the process time was reduced almost to half
(decreases by 46 %) to achieve an 80 % recovery in pretreated FW (see Fig. 12).
A similar effect could be observed in the case of pretreated SW; however, due to the higher ion content of the feed, the impact of
temperature is not as significant as observed for FW (Fig. 13). By increasing the temperature from 25 to 48 ◦ C, the time required to
achieve 80 % recovery was decreased by 24.5 %.

3.4. Effect of feed temperature on the permeability

Permeability (A, see Eq. (6)) is a parameter that can be derived from flux by dividing it by the transmembrane pressure (TMP, Eq
(7)).
JV
A= (6)
TMP

Fig. 11. The natural logarithm of fluxes of second step of Reverse Osmosis at 80 % recovery versus reversed temperature for pretreated seawater.

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Fig. 12. Recovery versus treatment time of second step of Reverse Osmosis for pretreated freshwater at 35 bar applied pressure and a membrane
surface of 28 cm2.

Fig. 13. Recovery versus treatment time of second step of Reverse Osmosis for pretreated seawater at 35 bar applied pressure and a membrane
surface of 28 cm2.

TMP = Δp − Δπ; (7)

Δπ = πR − πP at 80% recovery (8)

( − ln xw ) ⋅ Ru ⋅ T
πR = (9a)
Vw(T)

in the
(9b)
case of dilute solutions : πR = cR ⋅ Ru ⋅ T,

πP = cp ⋅ Ru ⋅ T (10)

Where Δp is the applied pressure [Pa], Δp is the osmotic pressure difference [Pa], πR is the osmotic pressure at the retentate side [Pa], πP
is the osmotic pressure at permeate side [Pa], xw is the molar ratio of water in the retentate [− ], Ru is the universal gas constant (8.314
J/(K⋅mol), T is the temperature [K], Vw(T) is the molar volume of water at the given temperature [m3/mol] in the range of 25 and 48 ◦ C,
cR is the total ion concentration of the retentate [mol/m3], and cp is the total ion concentration of the permeate [mol/m3].
Eqs. (9b) and (10) are called van’t Hoff equation which is valid only for dilute solutions. Considering the chemical potential as the
original driving force of RO, Eq (9a) is recommended use, which can be used in all concentration ranges, not only for dilute solutions.
In the case of FW, the retentate is also a remarkably diluted solution, and its concentration represents an osmotic pressure lower
than 0.01 bar (i.e., 1 kPa), which can be ignored in the transmembrane pressure calculation; thus, the applied pressure was used further
as TMP in the permeability values. As flux depends on the temperature exponentially, permeability also shows an exponential rela­
tionship versus temperature. To better visualize this, the natural logarithm of permeability is plotted versus the inverse temperature
(1/T) to derive a linear correlation. Similarly to flux values, permeability is higher at higher temperatures, as expected (Fig. 14).
In the case of pretreated SW, the retentate exhibits a highly concentrated solution, which surely cannot be treated as a dilute
solution during TMP calculation; therefore, in osmotic pressure calculation of the retentate, both Eqs. (9a) and (9b) were considered
and compared (see Table 6). Differences between π R values derived from Eqs. (9a) and (9b) were higher than 0.01 bar, which means
that the original equation Eq. (9a) leads to more accurate osmotic pressure differences, so it is preferable to be used in TMP calculation
(Eq. (7)). Permeates are dilute solutions in all cases at all temperatures, thus, van’t Hoff equation Eq. (9b) can be used in all πP
calculations.
Permeability values are 2.61, 2.78, 3.02, 3.38, and 3.65 (L/(m2⋅h⋅bar)] at feed temperatures of 25, 30, 36, 42, and 48 ◦ C,
respectively, indicating an exponential relationship which can be clarified in linearization using the natural logarithm of permeability
values versus inverse temperature (see Fig. 15).
In terms of conductivity, no temperature dependence was observed in the case of pre-treated FW because all values were under the

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R. Shaheen and E. Cséfalvay Water Resources and Industry 31 (2024) 100244

Fig. 14. The natural logarithm of the permeability of second step of Reverse Osmosis versus inverse temperature for pretreated freshwater.

Table 6
Transmembrane pressures calculated for pretreated seawater in case of second step of Reverse Osmosis.
T [◦ C] 25 30 36 42 48

TMP [bar] 26.00 25.75 25.62 25.05 25.04

TMP [kPa] 2600 2575 2562 2505 2504

detection limit of our conductivity meter (two μS/cm).

Regarding the quality of the RO-II permeate in SW experiments, a significant decrease in permeate conductivity could be observed
as proceeding with the experiments and reaching a 40 % recovery. After this point, further concentration of ions on the feed side
increased the probability of ion transport through the membrane, thus increasing the conductivity of the permeate. In batch experi­
ment and cross-flow filtration mode, 40 % recovery seems to be an optimal choice for better permeate quality (see Fig. 16). It is
assumed that in continuous mode, the parabolic-shaped minimum curve would not be as remarkable as in batch mode. The lowest
conductivity was the observed at 25 ◦ C and showed an increasing tendency by temperature increased up to 48 ◦ C (see Fig. 16.).
To avoid scaling [7] it was recommended not to use higher temperatures than 25 ◦ C for raw SW. In our case, with proper pre­
treatment technology and first-step desalination (RO-I) of SW, no scaling was observed even at 48 ◦ C in RO-II’s retentate and on the
membrane surface. Higher permeate conductivity was observed at elevated feed temperatures; still, the difference between permeate
quality was not significant (288, 309, 343, 370, and 395 μS/cm at 40 % recovery at 25, 30, 36, 42, and 48 ◦ C, respectively), see Fig. 16.
Therefore, it worth analyzing the overall energy consumption of pumps, heat exchangers, and the slightly reduced permeate quality
against the significantly reduced process time, which is a subject of our other current work.
Since RO systems are used to remove dissolved salts, salt (ion) rejection is a direct way to monitor performance. Rejection refers to
the amounts of contaminants removed from the feed water and can be calculated as given in Eq. (3) by using permeate’s and feed’s ion
concentrations. Since conductivity gives information about overall ion concentration and showing a linear correlation (see Supple­
mentary Material Table 1), Eq. (3) was modified as follows. Rejection values are calculated based on the measured conductivity; see
Eq. (11).
( )
Κp
R= 1− ⋅ 100% (11)
Κf

where Kp is the permeate conductivity [μS/cm], Kf is the feed conductivity [μS/cm].

Higher salt rejection refers to the better performance of the membrane. Considering the low conductivity values of the permeates in
FW experiments, the uncertainty of the measurement was high and keeping the average values measured, they are very close to the
detection limit of our conductivity meter. Hence, the derived rejection values are smaller than the theoretical one (99.47 %) providing
rejection values of around 86 %.
In the case of SW, the highest rejection values were observed at 40 % recovery at all temperatures showing an inversed curve as the

Fig. 15. The natural logarithm of the permeability of second step of Reverse Osmosis versus inverse temperature for pretreated seawater.

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R. Shaheen and E. Cséfalvay Water Resources and Industry 31 (2024) 100244

Fig. 16. The permeate conductivities of second step of Reverse Osmosis versus recovery for pre-treated seawater at 35 bar applied pressure.

conductivity. As proceeding the recovery until 80 %, conductivity values at all temperatures increased to the extent that resulted in a
decrease in the rejection values to around 97 %, see Fig. 17. Similarly, to Jin and coworkers [4], we did not obtain a significant
decrease in rejection with increasing temperature.

3.5. Total recovery calculation

When designing a technology for ultrapure water production, the most important information is how much ultrapure water can be
produced from 1 L of raw water. Noteworthy that the permeate of RO-II still requires further treatment to reach the superior con­
ductivity value of ultrapure water (0.055 μS/cm). The last stage of the technology can be electrodeionization (EDI) in the case of FW,
and an RO-III followed by EDI in the case of SW. The total recovery of pretreatment followed by two stages of desalination is calculated
taking into consideration of the recovery of each step; obtaining 50 % that seems to be a low value (Table 7). Wastewaters formed
during the process, such as the retentates of MF-II, UF, NF, RO-I and RO-II and their total salt contents are lower than the limit of 2000
mg/L [21] so they can lead to either natural water source or they can be drained into the sewage system [22,23].

3.6. Multiparameter evaluation of RO-II experiments

The multiparameter evaluation was conducted to find the optimum operating temperature of the main desalination stage, i.e., RO-
II. The permeate conductivity and operation time to reach an 80 % recovery were the parameters used in the first aspect group (named
Group 1 in Table 8), whereas the lowest value represented the best option. Based on this, a ranking was set up, starting from the best
option of operating temperature and proceeding towards the worst. In Group 2, flux, rejection calculated based on the conductivity,
and permeability were considered the aspect of the highest value being the best. Ranking from the best option proceeded towards the
worst, are shown in Table 8, where the experiments were named operating temperatures, similarly as done in Group 1. This multi­
parameter evaluation for pretreated FW and SW resulted in the same ranking for each parameter.
In terms of permeate quality: the lowest conductivity is coupled with the highest rejection; thus, 25 ◦ C is recommended to use as an
operating temperature of RO-II. Noteworthy, the 25 % difference in conductivity measured for pretreated seawater at a 40 % recovery
between 25 and 48 ◦ C, is significantly reduced when considering the rejection value, i.e., the 25 % conductivity difference is man­
ifested in less than 1 % difference in the rejection value calculated based on the conductivity values. Higher and stable flux, and
permeability were paired with short operation time; therefore, the highest temperature (48 ◦ C) is recommended. However, no in­
formation is available on membrane lifetime at a temperature close to its maximum applicable temperature (50 ◦ C).
Overviewing a possible heat loss in energy conversion systems, where this whole make-up water treatment technology would be
installed, the possibility of heat integration via utilization of the heat loss to elevate the feed temperature of RO-II shall be analyzed,
which is the subject of our other current work. By doing so, we can conclude that the optimum operating temperature will be the center
of the examined temperature range: 36 ◦ C.

Fig. 17. Rejection values calculated based on conductivity of second step of Reverse Osmosis versus recovery for pretreated seawater.

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R. Shaheen and E. Cséfalvay Water Resources and Industry 31 (2024) 100244

Table 7
Recovery of single steps and the total recovery of the proposed technology for ultra-pure water production.
Steps MF-I MF-II UF NF RO-I RO-II Total recovery %

Freshwater 100 90 90 90 85 80 50
Seawater 100 90 90 90 85 80 50

Table 8
Multiparameter evaluation and ranking of experiments related to RO II, valid for both pretreated fresh- and seawater samples.
Parameter Desired value of parameter Ranking of experiments: from Best to Worst (Operating Temperature [◦ C])

Group 1 Conductivity The lowest is the best 25 30 36 42 48

Operation time 48 42 36 30 25

Group 2 Flux The highest is the best 48 42 36 30 25

Rejectiona 25 30 36 42 48
Permeability 48 42 36 30 25
a
Rejection calculated based on the conductivity values.

4. Conclusions

The importance of pretreatment steps comes from the high need to protect the membranes in the desalination stage. We have
proven that the same technology, including the adequately selected pretreatment and desalination stages, can be used for fresh- and
seawater to produce desalted water. To produce ultra-pure water, a further step shall be installed: electrodialysis can act as a post-
refining step after RO-II in the case of freshwater. In contrast, a third step of RO followed by an electrodialysis is supposed to be
needed in the case of seawater. The pretreatment stage, represented by a series of membrane technologies (MF-I, MF-II, UF, and NF),
was used to prepare suitable feed water, avoiding membrane fouling in the desalination stage, which was carried out using two steps of
consecutive reverse osmosis (RO-I and RO-II).
This membrane series decreased TSS content to the desired value (<10 mg/L) after UF, but to protect first-stage RO, an NF stage
was further inserted, which could remove the 71.5 % of the ions in case of freshwater calculated on permeate conductivity, and 25.3 %
of ions for seawater which are suitable for feeding the RO membrane. Considering the individual ion concentrations, we can state that,
partial rejections of monovalent ions were noticeable by NF; the rejection values of sodium, potassium, and chloride are 19.2 %, 11.1 %
and 23.5 % for seawater, respectively. Due to the lower initial sodium and chloride content of freshwater, these rejection values
showed higher % than observed in seawater. UF permeate showed a TSS content of less than ten mg/L for fresh- and seawater. RO-I
showed more significant rejection of ions than NF: it was over 82 % for sodium, potassium and chloride and over 91 % magnesium,
calcium and sulphate in case of seawater, meanwhile, the rejection obtained for RO-II meet the theoretical value (over 99 % for all
ions). Besides, RO-I and RO-II showed rejection for all ions exceeding 90 % in case of freshwater. RO-I resulted in a permeate con­
ductivity of 22 μS/cm and 11.70 mS/cm for freshwater and seawater, respectively.
The effect of increasing feed water temperature showed an exponential increase in flux and permeability and reduced operation
time. Permeate flux increased along with increasing feed temperature from 25 to 48 ◦ C showing the same trend with linear correlation
for both water samples. Moreover, the effect of temperature on operation time is not as significant in seawater as in freshwater. No
temperature dependence was observed for permeate conductivity in the case of freshwater. Meanwhile, in seawater experiments,
permeate conductivity showed a parabolic-shaped minimum curve versus recovery at all temperatures; the lowest value was obtained
at 25 ◦ C and showed an increasing tendency by increasing temperature up to 48 ◦ C. For freshwater, no temperature effect was observed
on rejection; however, the highest rejection values were observed at a 40 % recovery at all temperatures in seawater.
In conclusion, the optimum temperature of 36 ◦ C will be used in heat-integration calculations. In contrast, the heat-loss of turbine
extraction is planned to be utilized to heat the feed of the desalination stages to accelerate the make-up water treatment process to
improve the efficiency of the whole energy conversion process. With the results of heat-integration work, specific energy calculations
will be provided in our next study.

CRediT authorship contribution statement

Reem Shaheen: Writing – review & editing, Writing – original draft, Visualization, Resources, Investigation, Formal analysis, Data
curation. Edit Cséfalvay: Writing – review & editing, Writing – original draft, Validation, Supervision, Project administration, Funding
acquisition, Conceptualization.

Declaration of competing interest

The authors declare the following financial interests/personal relationships which may be considered as potential competing
interests:
Edit Cséfalvay reports financial support was provided by Hungarian National Research, Development and Innovation Office-

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R. Shaheen and E. Cséfalvay Water Resources and Industry 31 (2024) 100244

NKFIH. Edit Cséfalvay reports financial support was provided by Hungarian Academy of Sciences. Edit Cséfalvay reports financial
support was provided by National Research, Development and Innovation Fund.

Data availability

Data will be made available on request.

Acknowledgements

The project was supported by the Hungarian National Research, Development and Innovation Office-NKFIH under Project Number
FK-143215. Edit Cséfalvay is grateful for the financial support the Hungarian Academy of Sciences for the scholarship for “Gyermeket
Nevelő Kutatók számára" 89, 2022/KP. Project no. TKP-6-6/PALY-2021 has been implemented with the support provided by the
Ministry of Culture and Innovation of Hungary from the National Research, Development and Innovation Fund, financed under the
TKP2021-NVA funding scheme. The research was funded by the Sustainable Development and Technologies National Program of the
Hungarian Academy of Sciences (FFT NP FTA).
The authors thank the Department of Chemical and Environmental Process Engineering at the Budapest University of Technology
and Economics for using their lab facilities to accomplish these experiments. The authors thank the help of József Csanádi and Júlia
Boros, MSc student, in the lab experiments, and Emil Csonka for the ion chromatographic analyses.

Appendix A. Supplementary data

Supplementary data to this article can be found online at https://doi.org/10.1016/j.wri.2024.100244.

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