439
Indonesian Journal of Science & Technology 10(3) (2025) 439-450

Indonesian Journal of Science & Technology
Journal homepage: http://ejournal.upi.edu/index.php/ijost/

Antibiotic Removal from Wastewater via Ceramic
Membrane Distillation: Toward Clean Water and
Antimicrobial Resistance Mitigation Aligned with
Sustainable Development Goals (SDGs)
Saad Aljlil1, Farid Fadhillah2,*, Nawaf Bin Darwish1, Noha A. Al-Otaibi1, Sulaiman M. Alajel3, Ali Alharthi1,
Abdulrahman Alzahrani1, Abdullah Al Tamim3, Abdullah A. Alajlan3, Abdullah Akbar3, Mohammed A. Almutairi3
1

King Abdulaziz City for Science and Technology, Riyadh, Saudi Arabia
Imam Mohammad Ibn Saud Islamic University, Riyadh, Saudi Arabia
3
Saudi Food and Drug Authority (SFDA), Riyadh, Saudi Arabia
*Correspondence: E-mail: faridfad.imamu@gmail.com

2

ABSTRACT
Antibiotic residues in wastewater represent a growing
concern for environmental and public health due to their role
in promoting antimicrobial resistance. This study investigates
the use of ceramic membrane distillation for removing
amoxicillin, ciprofloxacin, and levofloxacin under various
operational conditions. Two ceramic membranes, fabricated
from red clay with nanocellulose and silica additives, were
tested at different pH levels, temperatures, and antibiotic
concentrations. Experimental results showed consistently
high rejection rates, attributed to electrostatic repulsion and
membrane-liquid interaction. Zeta potential measurements
supported the correlation between membrane surface
charge and separation performance. The study contributes
to the body of knowledge on membrane-based water
purification technologies and supports goals related to clean
water access and reduced pharmaceutical contamination, as
reflected in the United Nations Sustainable Development
Goals.
© 2025 Tim Pengembang Jurnal UPI

ARTICLE INFO
Article History:
Submitted/Received 10 Mar 2025
First Revised 12 Apr 2025
Accepted 24 Jun 2025
First Available Online 25 Jun 2025
Publication Date 01 Dec 2025

____________________
Keyword:
Antibiotics removal,
Ceramic membrane,
Membrane distillation,
Wastewater.

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1. INTRODUCTION
Antibiotics have become a cornerstone in the treatment of microbial infections across
human and veterinary medicine. Their extensive use, especially in healthcare, livestock, and
aquaculture, has led to a significant increase in global antibiotic consumption over recent
decades [1.2]. According to the World Health Organization, annual antibiotic usage has
surpassed 100,000 tons [3]. This massive consumption has resulted in the continuous
discharge of antibiotic residues into the environment via pharmaceutical manufacturing
effluents, municipal wastewater, and agricultural runoff. Such discharges contribute to
ecological disturbances, alter microbial communities, and pose toxicological risks to higher
organisms [4,5].
A major consequence of environmental antibiotic pollution is the acceleration of
antimicrobial resistance (AMR), which occurs when residual antibiotics exert selective
pressure on microbial populations, fostering the emergence of resistant strains. Several
countries, including Saudi Arabia, India, Canada, and the United Kingdom, have reported
rising incidences of antibiotic-resistant bacteria attributed to environmental exposure [6].
These resistant microorganisms, often labeled “superbugs,” compromise the effectiveness of
standard therapies and increase morbidity and mortality rates. As such, the mitigation of
antibiotic pollutants in wastewater has become a global imperative aligned with public health
priorities and environmental protection frameworks.
Numerous water treatment technologies have been developed to address pharmaceutical
contaminants. Methods such as nanofiltration [7-9], reverse osmosis [10-12], electrodialysis
[13], forward osmosis [14], and membrane distillation [14-16] have demonstrated varying
degrees of efficiency in removing antibiotic compounds from aqueous matrices [17]. Among
these, membrane distillation (MD) has gained attention due to its ability to operate at low
pressures, tolerate high salinity, and reject non-volatile solutes.
Previous studies have primarily focused on polymeric membranes in MD applications for
antibiotic removal. Although effective, these membranes face limitations in thermal stability
and long-term fouling resistance [14,15]. In contrast, ceramic membranes offer enhanced
thermal and chemical durability, yet their application in antibiotic separation remains limited.
This study introduces a novel approach by employing two types of ceramic membranes
fabricated from modified red clay with nanocellulose and silica additives, aiming to assess
their separation performance across various operational conditions. The novelty of this work
lies in its integrated evaluation of ceramic membrane distillation for multiple antibiotics under
environmentally relevant scenarios, supported by zeta potential analysis. By addressing this
gap, the study advances membrane-based water treatment strategies and aligns with
Sustainable Development Goals, particularly SDG 6 (Clean Water and Sanitation) and SDG 3
(Good Health and Well-being).
2. METHODS
2.1. Membrane Fabrication.
The ceramic membranes used in this study were created following the procedure described
elsewhere [18], with some modifications to the composition. Two types of membranes were
produced. The first membrane (M-1) was made of 91.5% red clay, 1.5% tetraethoxysilane
(TEOS) as a silica precursor (≥99%, Aldrich), a curing agent, and 5% ammonia catalyst. This
mixture was combined with 2% sodium alginate powder (LOBA Chemie Co.) in 300 mL of
distilled water to make a paste suitable for extrusion.
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The second membrane (M-2) was fabricated by combining 91.5% Saudi Arabian red clay
with 8.5% nanocellulose powder, serving as a pore-forming agent and binder. Both
membranes were shaped using a plunger-type extruder and air-dried for three days on
wooden racks covered in plastic film to ensure uniform drying.
Sintering was performed in two stages using a Nabertherm electric furnace. In the first
stage, the temperature was gradually increased from 25 °C to 500 °C at 1 °C/min to remove
organic matter. In the second stage, the membranes were sintered from 500 to 1000 °C at a
rate of 2 °C/min for three hours to achieve densification and structural stability.
2.2. Antibiotic solution preparation
Three antibiotics—amoxicillin, ciprofloxacin, and levofloxacin—were prepared in varying
concentrations by dissolving pharmaceutical-grade tablets in 1 L of distilled water. Solutions
were stirred for 30 minutes under controlled conditions to ensure complete dissolution. The
pH was measured and adjusted using HCl and NaOH to achieve pH values of 4, 6.5, 8, 10, and
12. All membrane experiments were conducted within four hours of solution preparation to
maintain antibiotic stability. The concentration ranges for each antibiotic used in the
membrane feed system are listed in Table 1. These ranges were selected to explore the
influence of feed concentration on membrane performance.
Table 1. The concentration of antibiotic solutions used to feed into the membrane vacuum
system.
Antibiotic
Amoxicillin
Ciprofloxacin
Levofloxacin

Initial concentration (mg/L)
25, 50, 75, 100
18.75, 37.5, 56.25, 75
12.5, 25, 37.5, 50

2.3. Membrane and Antibiotic Characterization
2.3.1. Zeta Potential
The electrokinetic behavior of the membranes and antibiotics was measured using a
SurPASS™ 3 analyzer (Anton Paar, Germany) in the presence of 1 mM KCl as background
electrolyte at 25 ± 1 °C. Zeta potential measurements were conducted across a range of pH
levels to evaluate surface charge properties and their implications for separation efficiency.
2.3.2. Membrane Morphology
Surface and cross-sectional morphologies of the membranes were examined using a
scanning electron microscope (SEM, JSM-7100F, JEOL, USA). Membranes were vacuum-dried
for 24 hours and sputter-coated with gold (SPI Inc., USA) prior to imaging.
2.4. Antibiotic Removal Test
Membranes M-1 and M-2 were tested in a vacuum membrane distillation (VMD) system
operating at a feed flow rate of 55 L/h and a vacuum pressure of 3.5 mbar. The influence of
feed solution temperature, pH, and antibiotic concentration on membrane performance was
investigated using selected parameters. The experimental setup is illustrated in Figures 1 and
2.

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Figure 1. Schematic diagram of the Vacuum Membrane Distillation Process.

Figure 2. Vacuum membrane distillation (VMD) experimental setup
Permeate flux (J, kg/m²·h) was calculated based on the mass of condensed water (Md),
𝑀𝑑
active membrane surface area (A), and time (t): 𝐽 = 𝐴 .𝑡.
After each cycle, membrane cleaning was performed using deionized water at 70 °C and a
vacuum of 3.5 mbar. This process was repeated until flux and conductivity returned to
baseline (~1 µS/cm).
𝐶𝑝

Antibiotic rejection (R%) was determined using 𝑅% = (1 − 𝐶𝑓 ) . 100%, where Cp and Cf
are the permeate and feed concentrations, respectively.
2.5. Liquid Chromatography–Mass Spectrometry (LC–MS/MS)
2.5.1. Chemicals and Reagents
LC–MS/MS analysis utilized methanol, acetonitrile, water, and formic acid (99%) from
Merck (Germany). Analytical standards for amoxicillin, ciprofloxacin, and levofloxacin were
obtained from Dr. Ehrenstorfer GmbH (Germany).
2.5.2. Analytical Conditions
Quantitative analysis was carried out using an Agilent 1290 LC system coupled with a 6500
QTrap MS (Sciex, USA), equipped with an ESI source. The mobile phases included water and
acetonitrile with 0.1% formic acid. The elution protocol employed a gradient mode with a
flow rate of 0.3 mL/min and a column temperature of 45 °C. Instrumental settings such as gas
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flow rates, voltage, and temperatures were configured for optimal ionization and detection,
as previously described (Al Tamim et al., 2022). Table 2 lists the key mass spectrometry
parameters for each antibiotic.
Table 2. LC–MS/MS antibiotics analysis parameters.
Analyte
Amoxicillin
Levofloxacin
Ciprofloxacin

Precursor Ion (m/z) Product Ion (m/z)
CE
DP EP CXP
366.1
349.1 / 114.1
13 / 30 46 10 10
362.1
318.1 / 261.1
25 / 37 81 10 10
332.0
288.2 / 314.1
25 / 20 60 10

3. RESULTS AND DISCUSSION
We successfully fabricated the ceramic membranes using two different recipes. The
membrane showed a typical symmetric structure, illustrating uniform porosity from the
surface to the other end, as shown in cross-sectional view in Figure 3.

(a)

(b)

(c)

(d)

Figure 3. The tubular ceramic membrane was analyzed using scanning electron microscopy
to obtain the cross-sectional view (a, b) and top view (c, d) of the membrane. Figures (a, c)
and (b, d) are membranes M1 and M2, respectively.
The resulting membrane showed zeta potential as a function of pH, as presented in Figure
4. As shown, the membrane is slightly negatively charged across the entire pH range used in
the analyses. Similarly, all proteins are negatively charged in an aqueous solution, with
amoxicillin showing the highest negative charge, while levofloxacin shows almost neutral
charge.
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Figure 4. Zeta potentials for (a) antibiotics, (b) membranes.
Different operating parameters were then studied to investigate their impact on antibiotic
removal using two ceramic membranes. These parameters were the antibiotic’s
concentration, feed solution temperature, and pH.
3.1 Effect of antibiotic concentrations
To investigate the impact of initial antibiotic concentration, the concentration was
adjusted in each experiment run while maintaining a constant feed temperature of 50 °C and
pH of 6.5. The obtained data showed that a high removal of antibiotics from water was
achieved by the ceramic membranes (M1 and M2). The removal of antibiotics, including
amoxicillin, ciprofloxacin, and levofloxacin, was highly significant, reaching a rate of up to
99.9%. Despite the use of various concentrations for each antibiotic in the water, it did not
seem to affect the removal rate (Figure 5). When comparing the membranes' performance,
the results showed insignificant differences in their removal rates of antibiotics (p < 0.05).
However, it is noticeable that the removal of amoxicillin is consistently the highest, while
that of ciprofloxacin is consistently the lowest, even at a similar initial concentration. This is
because the flux of ciprofloxacin is the highest across the membrane. To explain this behavior,
we must examine the concept of liquid entry pressure (LEP), which is the minimum pressure
required to overcome the membrane's hydrophobic forces and allow the feed liquid to
penetrate the pores. LEP is proportional to the surface tension of the liquid, i.e., a mixture of
water and the antibiotic—other studies, such as those reported by Vieira et al. [19] showed
amoxicillin/water surface tension of above 60 mN/m while Jangde et al. [20] reported
ciprofloxacin/water surface tension at a lower value of around 50 mN/m. LEP works similarly
to osmotic pressure in a typical pressure-driven membrane. Therefore, the flux of
ciprofloxacin is higher than that of amoxicillin at the same operating condition, resulting in
lower removal of ciprofloxacin.
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Figure 5. Effect of antibiotic concentration on the removal rate. (a) amoxicillin, (b)
ciprofloxacin, (c) levofloxacin.
Additionally, Figure 5 indicates that the M1 membrane achieves slightly higher removal
than the M2 membrane in all cases. It is owing to the zeta potential of M1, which is a higher
negative charge compared to that of M2, as evidenced in Figure 4. Hence, M1 exhibits a higher
repulsive force to antibiotics than M2 does.
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3.2 Feed temperature effect on the removal
Higher feed temperatures typically result in increased permeate flux due to more
significant vapor pressure differences. Thus, to study the impact of the feed solution
temperature on the antibiotic’s removal, the feed solution temperature was adjusted to 50,
60, 70, and 80°C.
The protein removal results are shown in Figure 6. The results demonstrate high antibiotic
removal across the studied temperatures for both membranes, with removal levels exceeding
98% for all antibiotics. It is also evident that as the temperature increases, the diffusivity of
all proteins passing across the membrane increases. Thus, the removal percentage decreases
as a result.
Further investigation, the Figure 6 illustrates the relationship between the increase in feed
solution temperature and the corresponding increase in flux. As mentioned earlier, this was
attributed to the rise in vapor pressure differences and permeability, which results in a higher
driving force for the water to diffuse across the membrane, due to the rising temperature
across the membranes.

Figure 6. Effect of feed solution temperature on the antibiotic’s removal. (a) M-1, (b) M-2.
3.3. Effect of feed solution pH
The influence of pH on antibiotic removal was studied by maintaining constant antibiotic
concentrations at 50, 37.5, and 25 ppm for Amoxicillin, Ciprofloxacin, and Levofloxacin,
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respectively, and a solution temperature of 50 °C. The solution pH was adjusted to 4, 6.5, 8,
10, and 12 by adding NaOH or HCl. The results of both membranes are shown in Error! R
eference source not found.. The removal of amoxicillin and levofloxacin was over 98% in all
the studied pH levels, while ciprofloxacin removal was the lowest at pH 4 and increased to
almost 98% when the solution pH was increased to 6.5. These results were consistent with
the measured zeta potential of the antibiotics and membranes. Similar results have also been
observed in previous studies [16,20].

Figure 7. Effect of feed solution pH on the antibiotic’s removal. (a) M-1, (b) M-2.
In general, antibiotics were rejected by both membranes at a rate greater than 95%. Even
when the solution temperature, pH, and antibiotic concentration were varied, only a marginal
change occurred in the removal percentage. This high rejection efficiency is achieved due to
high LEP coupled with electrostatic repulsion.
3.4. Discussion
The ceramic membranes developed in this study exhibited strong and stable rejection
performance across various environmental conditions, including different antibiotic
concentrations, feed temperatures, and pH levels. Both membranes, particularly M-1,
demonstrated effective separation mechanisms that are likely governed by a combination of
surface charge interactions and liquid entry pressure. The slight variation in rejection rates
among the three antibiotics can be explained by their molecular characteristics and
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membrane interactions, as supported by zeta potential analysis and reference literature
[19,20].
The enhanced performance of the ceramic membranes compared to polymeric
counterparts previously reported [14-16] highlights the potential of ceramic-based systems
for more robust and thermally stable operations. Additionally, the successful membrane
regeneration using deionized water supports their practical utility for long-term applications
with minimal fouling concerns. These findings confirm that ceramic membrane distillation
systems can offer consistent rejection efficiency without being significantly affected by
fluctuations in environmental or operational variables.
3.5. Relevance to Sustainable Development Goals (SDGs)
The removal of antibiotic residues from wastewater directly addresses key targets of the
United Nations SDGs. The high rejection efficiency achieved in this study supports SDG 6
(Clean Water and Sanitation) by demonstrating an effective technology for improving water
quality and treating pharmaceutical effluents. By mitigating the release of residual antibiotics
into aquatic environments, ceramic membrane distillation can help reduce ecological
contamination and preserve freshwater resources. Furthermore, limiting the environmental
circulation of antibiotics contributes to the global effort to combat AMR, which is one of the
primary concerns outlined in SDG 3 (Good Health and Well-being). By lowering the risk of
resistant strain development due to environmental exposure, the application of ceramic MD
supports both environmental protection and public health. As a result, the present study not
only contributes technically to the field of water treatment but also aligns with broader global
goals for sustainable development. This adds new information regarding SDGs as reported
elsewhere [21-26].
4. CONCLUSION
This study examined the use of ceramic membrane distillation for the removal of
antibiotics from wastewater. The membranes demonstrated consistent separation
performance under different operating conditions. The results suggest that surface charge
and membrane structure play a key role in the rejection process. This work provides a
foundation for implementing ceramic-based membrane systems in wastewater treatment
applications aimed at reducing antibiotic pollutants.
5. ACKNOWLEDGMENT
This work was supported by King Abdul Aziz City of Science and Technology (KACST), grant
number 14-WAT3032-08.
6. AUTHORS’ NOTE
The authors declare that there is no conflict of interest regarding the publication of this
article. The authors confirmed that the paper was free of plagiarism.
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