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Review

Application of Ceramic Membranes Derived from Waste and Natural Materials for the Removal of Organic Dyes from Wastewater: A Review

by
Keotshepile A. Malebadi
1,2,
Lawrence Sawunyama
1,2,
Naledi H. Seheri
1,2 and
Damian C. Onwudiwe
1,2,*
1
Materials Science Innovation and Modelling (MaSIM) Research Focus Area, Faculty of Natural and Agricultural Sciences, North-West University, Mafikeng Campus, Private Bag X2046, Mmabatho 2735, South Africa
2
Department of Chemistry, School of Physical and Chemical Sciences, Faculty of Natural and Agricultural Sciences, North-West University, Mafikeng Campus, Private Bag X2046, Mmabatho 2735, South Africa
*
Author to whom correspondence should be addressed.
Ceramics 2025, 8(3), 80; https://doi.org/10.3390/ceramics8030080
Submission received: 29 March 2025 / Revised: 13 June 2025 / Accepted: 16 June 2025 / Published: 25 June 2025
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Abstract

The growing demand for organic dyes across industries increases their environmental impact since wastewater containing organic dyes poses serious risks to aquatic life, human beings, and the environment. The removal of organic dye residues is a challenge for traditional wastewater treatment facilities, highlighting the need for advanced treatment techniques that balance cost-effectiveness and sustainability in the face of today’s strict environmental regulations. The use of low-cost starting materials in ceramic membrane technology has recently become more popular as a feasible option because of its affordability and effectiveness, leveraging the synergy of adsorption and filtration to improve dye removal. Recent developments in ceramic membranes derived from waste and natural materials are examined in this review paper, along with their types, mechanisms, and applications in eliminating organic dyes from wastewater. The various forms of ceramic membranes derived from waste and natural materials are classified as follows: those composed solely of inexpensive starting materials, composites of inexpensive materials, hybrids of inexpensive and commercial materials, and inexpensive materials functionalized with cutting-edge materials such as carbon nanotubes and nanoparticles. These membranes have shown promising results in lab-scale research, but their large-scale use is still limited. The factors that negate the commercialization of these membranes are also critically discussed. Finally, key challenges and future research opportunities in the development of sustainable ceramic membranes for highly efficient dye removal are highlighted.

1. Introduction

The demand and use of organic dyes is rising steadily, as their role in adding color to textiles, food, rubber, pharmaceuticals, and cosmetics continues to gain prominence across different industries [1,2]. However, their widespread use comes with a significant environmental cost, as dye-laden wastewater poses serious risks to aquatic and terrestrial life [3]. Some of the widely used organic dyes, their classification, and reported toxicity effects are shown in Table 1. Studies have demonstrated that organic dyes can cause substantial pollution even at extremely low concentrations due to strong toxicity, high solubility, and high environmental stability [4,5]. The presence of organic dyes disturbs aquatic ecosystems by reducing the penetration of light and impairing photosynthetic activity [6]. Organic dye residues are hardly removed by most traditional wastewater treatment processes, which include coagulation, air flotation, sand bed filtration, and sedimentation, leading to intense color remaining in the final effluent [7,8]. These dye residues are reported to persist in aquatic environments for up to 50 years due to their high chemical stability, resistance to light and heat, low susceptibility to oxidation, and resistance to natural biological degradation processes [9,10]. Therefore, the primary focus in the research community is finding a balance between the sustainable removal of these pollutants and their continued use under strict environmental regulations.
Several advanced techniques have been employed for the removal of organic dyes from dye-laden wastewater. These include adsorption [41], biological treatment [41,42], membrane filtration [43,44], ozonation, and advanced oxidation processes (AOPs) such as ultraviolet (UV) photolysis [45], the UV/H2O2 process, the UV/O3 process, the UV/Fenton process, and photocatalysis [46], which have been widely explored. Furthermore, hybrid processes integrating multiple treatment methods have been developed to enhance efficiency and achieve comprehensive dye removal [47]. However, the success of most of these reported advanced techniques is at the laboratory scale instead of the complementary large industrial scale due to some drawbacks. For example, biological processes like bioremediation occur slowly because organic dyes are resistant to biological breakdown [4]. Adsorption and membrane processes can result in poor selectivity and slow process kinetics and can lead to the generation of secondary contamination [48]. Photocatalysis is the most promising technique since it completely mineralizes target organic dyes with no generation of secondary pollution. However, they also have drawbacks that prevent their wide utilization, including high cost because of the high energy demand and difficulty in the recovery of utilized photocatalysts, thereby creating secondary pollutants [49]. The overall high cost of setting up advanced wastewater treatment plants and the generation of secondary contaminants are the dominating drawbacks that have limited the application of most advanced wastewater treatment techniques in the removal of organic dyes. Hence, the balancing of these issues would open more avenues for industrial applications.
Ceramic membrane technology is one such method that has greatly lowered wastewater treatment costs and improved sustainability. This cutting-edge filtering technique effectively separates pollutants from water by using highly porous and chemically stable materials with pore diameters ranging from millimeters to nanometers [50,51]. The main mechanisms that control the removal of contaminants by ceramic membranes include electrostatic interactions, adsorption, and size exclusion [52]. Ceramic membranes provide a sustainable and long-lasting water purification solution because of their remarkable thermal and chemical resilience, which makes them ideal for treating both industrial and municipal wastewater [53].
Despite these advantages, the widespread application of ceramic membrane technology has been limited by the high initial production costs of ceramic membrane technology, mainly because of the high energy requirements and costly raw ingredients [54]. To address this limitation, recent research has focused on developing ceramic membranes using low-cost starting materials. These low-cost starting materials refer to naturally abundant resources (such as clay, sand kaolin, bentonite, and zeolites) [55,56] and adequately treated industrial or agricultural waste (such as coal fly ash, red mud, rice husk ash, sugarcane bagasse ash, and eggshells) [57,58,59]. These materials are generally inexpensive due to their abundance and their minimal processing before membrane fabrication [54]. Several studies, including our work [60], have demonstrated the viability of these materials in the fabrication of sustainable ceramic membranes while maintaining performance. This, thus, enhances the feasibility and adoption of ceramic membrane technology in wastewater treatment applications [61].
Therefore, this review provides a comprehensive assessment of the effectiveness attained in the degradation process of organic dye utilizing sustainable ceramic membranes fabricated from waste and natural starting material. Additionally, it critically evaluates recent developments in membrane technology, emphasizing areas that need more optimization and improvements. The major challenges hindering the commercialization of these membranes are also discussed in detail, including issues related to fabrication costs, membrane fouling, and stability. Finally, the review identifies key challenges and future research opportunities in the development of cost-effective and sustainable ceramic membranes for highly efficient dye removal.

2. Organic Dyes as Emerging Contaminants

Environmental contamination has been further exacerbated by a rapid expansion of industrial activities, especially in the textile, chemical, pharmaceutical, and agricultural industries. The extensive use of synthetic dyes in textiles, food processing, tanneries, paint, and pharmaceuticals makes them particularly concerning among the many industrial pollutants [62]. As illustrated in Figure 1, the textiles sector is the biggest source of dye pollution in the environment, followed by dyeing processes, the paper and pulp industry, the tannery, and the paint sectors [10]. The textile industry generates around 15% of industrial wastewater, with nearly 80% of dye-laden effluents being released untreated. Consequently, aquatic ecosystems are often contaminated by these dyes, and their untreated discharge has detrimental ecological effects that upset the food chain [63]. Additionally, the released textile sludge is known to be rich in organic compounds and micronutrients, thereby causing eutrophication [64,65]. Also, many synthetic dyes have mutagenic, teratogenic, and carcinogenic characteristics, exposing public health to even greater risk [66]. The environmental impact of dye-laden wastewater is particularly severe in regions like China and South African estuaries, where the problem has intensified [67]. Despite the economic importance of dyes, it is obvious that environmentally friendly wastewater treatment techniques are desperately needed to remove remaining residues.

2.1. Dye Classification

Dyes are often divided into two groups: synthetic and natural dyes (Figure 2). The natural dyes are sustainable, biodegradable, and safe for the environment because they are derived from a range of plant and animal sources, including lichens, berries, bark, leaves, roots, and fungi. In addition, they are usually generated using fewer chemical processes, which reduces pollution. As a result, they have long been used for textile and other purposes in different countries. In contrast, synthetic dyes are chemically engineered from petroleum derivatives [69], earth minerals, and chemicals, offering a wider range of colors and improved performance compared to their natural counterparts. However, as many natural dyes are now manufactured synthetically, the distinction between natural and synthetic dyes has become increasingly difficult to differentiate.
The main dyes used in the industry are divided into three groups based on their chemical structure (azo, anthraquinone, and indigoid), ionic properties (cationic, anionic, and non-ionic), and mode of application (acid, base, and reactive) [70]. Different dye groups and their industrial uses are displayed in Figure 3. Direct dyes, acid dyes, and reactive dyes are the three subtypes of anionic dyes, which are negatively charged [71,72]. Acid dyes are water-soluble and carry functional groups like sulphonic and carboxylic acids (SO3H and COOH). These acid dyes are often used in the textile, pharmaceutical, and paper industries due to their vibrant colors and high solubility. These dyes are also suitable for materials such as wool, silk, and nylon. Reactive dyes form a covalent bond with amine or sulfhydryl groups in textile fibers, making them highly durable and resistant to washing. This high wet fastness, along with their intense color and wide range of hues, has led to reactive dyes becoming the most widely used type in textile dyeing. Direct dyes are easy to apply to a range of materials, such as leather and paper, because they are applied straight from an aqueous solution and have a strong affinity for cellulosic fibers like cotton and rayon [73,74]. Due to their solubility and chemical characteristics, several additional anionic dyes, such as reactive black 5, methyl blue, methyl orange, and alizarin red S, are widely utilized in research, especially in investigations of adsorption and photodegradation processes. Cationic dyes have a positive charge and are also known as basic dyes. These dyes are typically synthetic and act as bases. When dissolved in water, they form colored cationic salts that can readily react with the anionic sites on the surfaces of substrates such as fibers, leading to vibrant and intense hues [75,76]. These dyes are particularly useful in the textile industry, especially for acrylic fibers, due to their ability to bond quickly and firmly, creating bright and lasting colors. One of the most widely used cationic dyes, methylene blue (MB), is well known for its many industrial uses and adaptability [77]. Other well-known cationic dyes are malachite green and rhodamine B.

2.2. Chemistry and Toxicity of Selected Synthetic Dyes

Synthetic organic dyes tend to stay in the environment after being released since they are not biodegradable and cannot be eliminated by conventional water treatment methods. Due to their exceptional stability against light, temperature, water, detergents, and soaps, they are also ecologically persistent [78]. Aquatic ecosystems may be negatively impacted by the highly colored effluent released by textile and other dye-using industries [79]. The effects of some selected synthetic dyes are discussed in this section.

2.2.1. Congo Red

Congo Red (CR) is an anionic, benzidine-based dye widely employed in industries such as textiles, printing, rubber, cosmetics, leather, and biomedical laboratories due to its strong affinity for cellulose fibers and diagnostic properties. Chemically known as 1-Naphthalenesulfonic acid, 3,3′-(4,4′-biphenylene bis(azo) bis 4-amino) disodium salt, it is a highly water-soluble diazo dye that exists as brownish-red crystals and is stable in air, with a solubility of 1 g/30 mL in water [80]. Despite its industrial value, CR is highly toxic and poses significant health and environmental risks, as it can metabolize into benzidine, a known human carcinogen, and cause allergic dermatitis, skin and eye irritation, gastrointestinal issues, and respiratory problems [80,81]. The widespread and often uncontrolled discharge of these toxic dyes [82] into water sources, without proper treatment, contributes to significant environmental contamination [83,84]. Consequently, there is an urgent need to develop efficient treatment methods to degrade CR and reduce its harmful impact.

2.2.2. Malachite Green

Malachite green (MG) is a water-soluble basic dye classified as a diamino derivative within the triphenylmethane dye family [85,86]. It commonly appears as a green crystalline powder, named for its resemblance to the mineral malachite. Chemically, it is referred to as a chloride salt with the formula C23H25ClN2 or [C6H5C(C6H4N(CH3)2)2]Cl [87]; although it is often referred to by its colored cationic form due to its intense coloration and environmental persistence. MG has been applied in the textile industry and certain food products [88] since 1933 and in aquaculture to prevent and treat protozoal and fungal infections in fish eggs, fingerlings, and adult fish for its strong antifungal and antiprotozoal properties. It is also applied in the textile industry and certain food products [86]. Despite its effectiveness, MG has raised serious health concerns due to its accumulation in the internal organs of treated fish, leading to harmful internal effects. These adverse impacts extend to humans that consume such fish, as MG has been shown to compromise the immune and reproductive systems. As a result, MG is considered genotoxic and carcinogenic, posing a serious threat to living organisms [86,89], and its removal from aquatic environments is crucial to protect human health, ecosystems, and aquatic life.

2.2.3. Methyl Orange

Methyl orange (MO), also known as dimethylaminozobenzenesulfonate (C14H14N3NaO3S), is an organic sulfosalt azo dye [90] widely recognized for its high color ability and bright orange hue when dissolved in water. However, its excessive use poses significant environmental and health hazards [91], as the dye contains aromatic rings and -N=N- groups, which are highly toxic, carcinogenic, and teratogenic [92,93]. These compounds present risks to both the environment and living organisms.

2.2.4. Methylene Blue

The high demand for synthetic dyes, including methylene blue, continues to rise across industries such as silk, paper, cotton, and wool dyeing, as well as in cosmetics, food, and pharmaceuticals [94]. Methylene blue (MB), a cationic thiazine dye with a heterocyclic aromatic structure [78], has the chemical formula C16H18N3SCl and a molecular weight of 319.85 g/mol. MB is highly soluble in water and remains stable at room temperature. Classified as a phenothiazine compound, its International Union of Pure and Applied Chemistry (IUPAC) name is [3,7-bis(dimethylamino) phenothiazine chloride tetramethylthionine chloride], and it carries the color index (CI) 52,015 [95,96]. MB appears as dark green crystalline solids or a fine crystalline powder with a metallic bronze-like sheen [81]. MB is non-biodegradable and carcinogenic due to its stable aromatic ring structure. When released untreated, MB-contaminated wastewater poses serious health risks, including vomiting, increased heart rate, respiratory disorders, and skin and tissue damage [97]. It also affects microalgae species, leading to growth inhibition and protein depletion [79]. While MB is used medically as a monoamine oxidase inhibitor (MAOI) for certain conditions, excessive doses can cause serotonin toxicity. Improper contact with MB or direct skin contact with improperly handled or untreated MB-loaded water can cause redness, itching, and skin necrosis, leading to tissue and organ damage [81,98]. Due to its persistence, conventional treatment methods are often ineffective, making photocatalytic degradation a promising approach for removing MB from wastewater.

2.2.5. Rhodamine

Rhodamine B (RhoB), a fluorescent xanthene dye with the chemical formula C28H31ClN2O3 [99], is an affordable and highly water-soluble dye commonly used as a tracer in water studies, a colorant in textiles and food, and a biomarker in oral rabies vaccines [100]. Despite its widespread use, RhoB is banned in food due to its carcinogenic and developmental toxicity to both humans and animals. However, it continues to be illegally used as a food additive because of its low cost and high dyeing efficiency. When absorbed into the body, RhoB is metabolized by cytochrome P450, producing free radicals that disrupt superoxidase dismutase (SOD) activity, leading to oxidative stress, cell death, and damage to the brainstem [101]. Additionally, RhoB poses significant health risks, including respiratory issues, skin irritation, and eye discomfort, making its removal from water sources crucial [99].
In light of the highlighted health issues associated with these dyes, the pollution of the environment by dyes needs to be addressed for the sustainable management of water resources and to avoid further contamination. The environment and human health rely on effective mitigation efforts, particularly those that employ advanced wastewater treatment methods and the development of environmentally friendly alternatives. Membrane filtration technology has recently attracted much interest due to its enormous potential to remove these dyes and improve water quality and ecosystem health.

3. Ceramic Membrane Technology Overview

Membrane technology has gained widespread use in wastewater treatment due to its minimal chemical usage, environmental benefits, and effectiveness. It is currently more in demand in the water and wastewater industry because of advancements, which include improved module design and reduced costs [53,101,102]. Membrane technology has advantages over traditional treatment techniques, including reduced chemical sludge generation, a smaller carbon footprint, improved removal efficiency, and lower thermal energy use [103]. Membranes rely on a driving force for separation, acting as selective barriers that allow water molecules to flow through while retaining impurities [53,103].
As shown in Figure 4, membranes are categorized according to their shape, separation processes, and structural and material composition. Membranes can have either an anisotropic (asymmetric) or isotropic (symmetric) structure. The pore size and structure of isotropic membranes are constant throughout their thickness. They can be dense (nonporous), which restricts their ability to separate, or microporous, which permits large penetration fluxes and is frequently employed in microfiltration. Isotropic membranes have a uniform structure and consistent pore size throughout their thickness. They may be microporous, allowing high permeation fluxes and commonly used in microfiltration, or dense (nonporous), which limits their separation performance. Anisotropic membranes, on the other hand, have several layers and usually consist of a larger, highly permeable substrate that supports a thin selective layer. This structural asymmetry improves filtration effectiveness and is especially useful for reverse osmosis (RO) procedures. Furthermore, membranes can be categorized as dense (stiff) or porous. Porous ceramic membranes are a common choice for support materials and water treatment. The lattice arrangement of different components in these membranes usually indicates their asymmetrical structure.
Material composition, which roughly divides membranes into polymeric (organic) and ceramic (inorganic) types, is the most widely recognized and employed criterion of all membrane classifications. Synthetic organic polymer-based materials such as cellulose acetate, polyethersulfone, polyimide, and polysulfone make up polymeric membranes, which are semi-permeable filtering materials [104,105,106]. They are extremely desirable for pressure-driven separation processes, including MF, UF, NF, and reverse osmosis (RO), especially on a commercial scale, due to their adjustable pore sizes, superior selectivity, flexibility, and affordability [107]. However, despite these benefits, their low thermal and chemical stability and vulnerability to degradation under harsh operating conditions, such as prolonged operation, aggressive chemicals, or extreme temperatures, can seriously impair their performance, especially in wastewater treatment [108]. Inorganic ceramic membranes have drawn more interest as a dependable and long-lasting solution to these drawbacks. High-temperature sintering of inorganic materials, including silicon carbide, titanium, zirconia oxide, and alumina, produces these ceramic membranes [109,110]. Their increased environmental friendliness, scalability, and improved chemical and thermal stability under harsh operating conditions further expand their suitability for wastewater treatment operations [111]. However, because of the expensive cost of raw materials, intricate multi-step manufacturing methods, and the high sintering temperatures up to 1500 °C needed during production, the use of ceramic membranes is still mostly restricted to laboratory-scale settings [112,113,114]. Ceramic membranes are about four times more expensive than polymeric membranes, which cost about 25% of that amount per square meter [114,115]. Therefore, reducing production costs makes ceramic membranes more economically feasible for broad use, especially by addressing problems with sintering parameters, process complexity, and material selection [116]. As shown in Figure 5, recent research has focused on the use of inexpensive starting materials that are obtained from readily available and inexpensive sources.
The application of waste and natural material-derived ceramic membranes in removing contaminants from wastewater has generated a lot of interest. Among the various configurations of these membranes are capillary membranes, disc membranes, monolithic membranes, and flat sheet membranes. Numerous factors influence the selection of a particular design, such as feed characteristics, separation efficiency, scalability, and application requirements. The composition of the low-cost starting materials used in the fabrication process has a significant impact on the structural characteristics and performance of the resultant ceramic membranes. These membranes can be divided into four primary groups based on the makeup of their materials. The first category consists of membranes made entirely of low-cost raw materials. For instance, Huang et al. [118] used only coal fly ash to fabricate a cost-effective tubular ceramic membrane. Additives were also incorporated to increase pore formation and binding capacity. The second category consists of composites made from a composite of inexpensive materials. In our previous study [60], natural sand and coal fly ash were used to fabricate a flat, inexpensive ceramic membrane, proving that employing naturally occurring materials to fabricate membranes is feasible. In a similar study, Saxena et al. [119] fabricated an innovative circular ceramic membrane module by combining coal fly ash with fuller’s earth clay, using the uniaxial compaction technique to produce a value-added material. The membrane was subsequently sintered at a low temperature, which significantly contributed to lower fabrication costs. The third category comprises hybrids that combine inexpensive and commercial materials to enhance membrane properties. Muhamad et al. [120] used silicon carbide as a commercial starting material, combined with fly ash from the chipboard and palm oil waste industries, kaolin, and sand, to create inexpensive ceramic membranes. While being cost-effective, this method enables enhanced structural integrity and filtration efficiency. The final category includes membranes made from inexpensive materials that are further functionalized with advanced materials such as carbon nanotubes and nanoparticles. We have previously [49] fabricated a ceramic membrane using coal fly ash and natural sand and functionalized it using TiO2-ZnO nanoparticles to enhance its properties. This modification improved the membrane’s photocatalytic properties and boosted its effectiveness for wastewater treatment applications. In another study, sustainable ceramic membranes fabricated from silica-rich ceramic sludge and alumina-rich roller kiln waste were functionalized with multi-walled carbon nanotubes (MWCNTs). The functionalized membranes exhibited high humic acid removal efficiency, which was primarily attributed to a reduction in membrane pore size and enhanced surface properties resulting from the incorporation of MWCNTs [121].
Table 2 illustrates the economic feasibility of ceramic membranes fabricated from waste and naturally derived starting materials such as fly ash, clays, and rice husk ash, with production costs as low as USD 3.4/m2 and up to USD 250/m2. For instance, fly ash-based membranes are priced at USD 250/m2 [122], while phengite clay-based membranes cost USD 3.5/m2 [123]. In contrast, Table 3 summarizes the cost of ceramic membranes manufactured using commercial-grade starting materials, such as Al2O3, ZrO2, SiC, TiO2, and high-purity SiO2, with reported fabrication costs ranging from USD 100/m2 to as high as USD 3000/m2. The high production cost is primarily due to the high price of starting materials, purity requirements, and high sintering energy needed (often above 1200 °C). The reported total production costs include both the capital expenditures (CAPEX) and operational expenditures (OPEX). The production cost comparisons clearly show that ceramic membranes fabricated from waste and natural materials offer substantial economic advantages. Furthermore, the use of waste-derived starting materials aligns with circular economy principles and contributes to environmental sustainability by diverting industrial and agricultural residues from landfills [124,125]. They also have a longer lifespan and are more resistant to heat and chemical degradation, which lowers OPEX. These benefits make ceramic membranes fabricated from waste and natural materials attractive for large-scale water treatment applications, especially in resource-strained settings [123]. Although ceramic membranes require regular cleaning and replacement, their costs are significantly less than those of polymeric or ozonation systems [126,127].

4. Application of Ceramic Membranes Derived from Waste and Natural Materials in the Removal of Dye Removal from Wastewater

Waste and natural material-derived ceramic membranes have been used extensively in recent years to remove organic dyes from wastewater, as shown in Table 4. Their wide use stems from their affordability, as they can be fabricated using inexpensive and readily available raw materials such as clay, sand, and waste materials like coal fly ash and animal bones [104]. They also require low sintering energy during the fabrication stage, which reduces production costs. They are also widely used because of their long lifespan and mechanical and chemical stability. Ceramic membranes remove contaminants via a pressure-driven process that makes use of separation techniques like size exclusion, adsorption, and electrostatic repulsion [127,140]. Ceramic membranes’ porosity, surface roughness, and functional groups present are among their physical and chemical characteristics that affect the adsorption of organic dyes onto their surface. The two main mechanisms involved in the adsorption process are chemical and physical adsorption. Physical adsorption is controlled by van der Waals forces and electrostatic interactions and is usually reversible. While chemical adsorption involves stronger interactions, such as hydrogen bonds and coordination with inorganic oxides (like AlO3, SiO2, or FeO3) on the ceramic membrane surface [141,142,143]. For example, Rakcho et al. [144] successfully fabricated a ceramic membrane from purified clay. The fabricated membrane exhibited exceptional rejection of methyl orange and rhodamine B. Adsorption was the primary technique proposed for the removal of these organic dyes. The adsorption process was facilitated by hydrogen bonding and n–π interactions, as shown in Figure 6a.
Building on this work, Achiou et al. [134] also showed that utilizing geomaterials like clay, perlite, and industrial waste minimizes sintering temperatures to as low as 1000 °C, resulting in a reduction of fabrication costs to USD 9.91/m2, while still achieving a high-performance rate of 97.82% turbidity removal in textile wastewater treatment. The removal mechanisms in these systems vary depending on membrane composition. While Rakcho’s clay membranes primarily relied on adsorption, other studies like Saja et al. [56] demonstrated that ceramic membranes fabricated from bentonite clay could effectively remove direct red 80 and rhodamine B through the combination of the sieving mechanism and electrostatic interactions. Furthermore, another breakthrough in membrane fabrication indicated that the use of cold sintering techniques, which allow densification at temperatures below 300 °C, drastically cuts energy while retaining high filtration efficiency, including 99% pathogen removal [145].
Table 4. Selected studies on the performance of ceramic membranes derived from waste and natural materials on the removal of organic dyes.
Table 4. Selected studies on the performance of ceramic membranes derived from waste and natural materials on the removal of organic dyes.
Membrane TypeOrganic Dye RemovedCountry of Study/ScaleProcess ParametersEfficiencyRef.
Chocobofe clay-based ceramic membraneMethylene blue dyeBrazil/Bench scaleInitial dye concentration: 50 mg/L,
Pressure: 2 bar,
Temperature: 25 °C,
Porosity: 53%,
Average pore size: 0.48 µm		100% dye rejection;
Good performance after 15 reuse cycles		[129]
Cordierite and an abundant clay-based ceramic membraneMethylene blue dyeMorocco/Bench scalePorosity: 18.65–29.63%99.8% dye filtration efficiency[130]
Purified clay-based ceramic membraneMethyl orange (MO), Rhodamine B (RhB)Morocco/Bench scaleAverage pore size: 5.4 nm
Pressure: 4 bar,
Dye concentration: 50 ppm,
Water permeability: 26 L/h·m2·bar		Rejection rates: 84.5% (MO), 85.7% (RhB)[144]
Clay-based ceramic membraneMethylene blue dyeEgypt/Lab scaleSynthetic dye wastewater (100 ppm)42% dye rejection[146]
COOH-carbon nanotube-functionalized clay-based ceramic membraneAcid fuchsin dyePore size: 0.076 µm,
Dye concentration: 100 ppm		95% rejection
Sugar scum and fly ash-based ceramic membraneMethylene blue dyeMorocco/Lab scalePore size: 0–4.5 μm,
Pressure: 1 bar,
Filtration time: 2 h,
Water permeability: 2356.68 L/h·m2·bar		99.9% retention[147]
Natural clay-based ceramic membraneAcid Yellow 49, Basic Violet 16, Disperse Red 167Iran/Lab scalePorosity: 27%,
Pore size: 3.3 µm,
Pressure: 0.1 bar,
Dye concentration: 50 ppm,
Water permeability: 2491.4 L/m2·h·bar		98% retention (anionic dyes), 93% retention (non-ionic dyes)[148]
Bentonite-based ceramic membraneDirect Red 80, Rhodamine BMorocco/Lab scalePore size: 13 nm,
Pressure: 4 bar,
Dye concentration: 50 ppm,
Water permeability: 30 L/h·m2·bar		97% rejection (Direct Red 80), 80.1% rejection (Rhodamine B)[56]
Clay-based ceramic membraneCongo Red dyeMorocco/Lab scaleAverage pore size: 1.21–1.76 µm99% dye removal[149]
Zeolite-clay-based ceramic membraneIndigo Blue dyeTunisia/Lab scalePore size: 0.75 µm,
Pressure: 1.0 bar,
Permeability: 371 L/h·m2·bar		95% dye removal[150]
Potter’s clay-based ceramic membraneMethylene blue, Congo RedIndia/Lab scalePorosity: 52.51%,
Average pore size: 0.49 µm		High removal efficiency and reusability[133]
Purified natural clay-based ceramic membraneDirect Red 80Morocco/Lab scalePressure: 3 bar,
Pore size: 75–90 nm,
Permeability: 14.7–16.4 L/h·m2·bar,
Dye concentration: 50 ppm		97–99% dye removal[151]
TiO2 functionalized low cost clay/alumina based ceramic membrane Alizarin Red dyeTunisia/Lab scalePressure of 5 bars,
pH = 9,
Permeability of 117 L h−1 m−2 bar−1.
Dye concentration of 150 ppm		99% dye removal[152]
The active surface layer can be functionalized to change the surface characteristics of the ceramic membranes, such as porosity, surface charge, surface area, and mechanical strength. The efficiency of the ceramic membranes fabricated from waste and readily available materials can be practically increased by using nanosized starting materials. This technique improves the adsorption properties of the final ceramic membrane while also reducing the pore sizes of the membranes. The preferred membranes for dye removal are ultrafiltration (UF), nanofiltration (NF), and reverse osmosis (RO). The pore diameters of these membranes usually range from more than 50 nm for UF, 2 to 50 nm for NF, and less than 2 nm for RO [104]. The selection of the optimal pore size and membrane type depends on various factors, including dye type, membrane composition, and the required separation efficiency. These factors collectively influence the porosity needed for effective dye removal. For example, Saad et al. [153] used environmentally friendly glauconite clay to fabricate a cost-effective adsorbent. The glauconite clay was ball-milled to the nano-scale before adsorption to increase surface area and uniformity. The resulting adsorbent demonstrated exceptional efficacy in removing methylene blue from synthetic effluent. In another study, Hamad et al. [146] evaluated the effectiveness of both pristine and functionalized ceramic membranes in the removal of organic dyes. The findings showed that pristine clay-based ceramic membranes had a lower rejection effectiveness for acid fuchsin dye (AF) (42%), while COOH-functionalized carbon nanotube clay-based ceramic membranes achieved 95%. The functionalization of the clay-based ceramic membranes also enhanced their antifouling properties.
To achieve a balance between cost and efficiency, low-cost raw materials for ceramic membrane production can be combined with commercial starting materials. For instance, Boutaleb et al. [130] produced cost-effective ceramic membranes at a production cost of USD 14/m2 utilizing cordierite and an abundance of clay that was sintered at 900 °C. The resulting membranes removed methylene blue dye with a remarkable filtration efficiency of 99.8%. A hybrid composed of various low-cost starting materials can be utilized to develop an effective and affordable ceramic membrane for dye wastewater treatment. Each material contains inorganic components that react to form strong interactions, enhancing the membrane’s chemical and mechanical stability [147].
Additionally, Diachenko et al. [154] and Roy Barman et al. [155] demonstrated how 3D printing technologies, such as vat photopolymerization and power bed fusion, enable the fabrication of complex, high-precision ceramic membranes. These methods outperform conventional fabrication methods in design flexibility and scalability for wastewater treatment and gas separation. These findings align with the work of Hoskins et al. [156], who emphasized the importance of hybrid ceramic materials and pore structure optimization to enhance durability, permeability, and selectivity under harsh conditions. Together, these studies underscore the potential of additive manufacturing, such as extrusion-based and photopolymerization techniques, to streamline production while addressing fouling resistance and industrial feasibility.
One of the major challenges associated with the use of ceramic membranes fabricated from waste and readily available materials is their inability to completely degrade organic dyes. As a solution to this shortcoming, researchers have explored the functionalization of these membranes with materials such as nanoparticles that are capable of effectively degrading pollutants [157,158]. For instance, Oun et al. [152] fabricated a ceramic membrane using kaolin clay. The membrane was then functionalized with TiO2 nanoparticles through the slip casting method. The modified ceramic membrane demonstrated an impressive alizarin red dye removal efficiency of 99% through ultrafiltration. In another study, Kim et al. [159] fabricated a membrane using fly ash, TiO2, and polyurethane. The membrane demonstrated effective removal of methylene blue, which was attributed to the adsorptive properties of fly ash and polyurethane, as well as the photocatalytic activity of TiO2. Studies have shown that ceramic membranes fabricated from waste and readily available materials can be effectively integrated with other treatment techniques to enhance the removal efficiency of organic dyes from wastewater. These membranes can be utilized as either a pre-treatment or post-treatment method, improving overall dye removal performance or ensuring better water quality.
Real-world validation of these technologies has been demonstrated in projects such as the LIFE REMEMBrANE initiative, which showcased ceramic membranes for desalination and wastewater reuse. Fouling-resistance designs, such as cake filtration mechanisms and oxide-electrolyte composites (e.g., Al2O3-LLZO), further extend membrane lifespans in demanding applications like textile wastewater treatment [145,160]. Research indicates that affordable ceramic membranes can be successfully combined with other treatment methods. The integration of scalable 3D printing, hybrid materials, and photocatalytic functionalization offers a promising route for widespread application, significantly boosting the removal efficiency of organic dyes from wastewater. These membranes are applicable as either pre-treatment or post-treatment solutions, enhancing overall dye removal effectiveness and contributing to a sustainable future for global water management.
Ceramics 08 00080 g006
Figure 6. Mechanism for the removal of organic dyes by ceramic membranes (a) The interactions between membrane surface and dyes (MO and RhB) [144], (b) Different types of interaction between membrane and pollutants [161].
Figure 6. Mechanism for the removal of organic dyes by ceramic membranes (a) The interactions between membrane surface and dyes (MO and RhB) [144], (b) Different types of interaction between membrane and pollutants [161].
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Factors That Affect the Removal Efficiency of Organic Dyes by Waste and Natural Material Derived Ceramic Membranes

The removal efficiency of these ceramic membranes in the elimination of organic dyes depends on the membrane’s properties and operating conditions. Initial dye concentration, operating pressure, contact time, and pH of feed solution are examples of operational conditions. Membrane properties include surface hydrophilicity/hydrophobicity, surface charge, surface texture, and pore size. These factors influence crucial performance mechanisms or processes in ceramic membrane-based dye removal. Selectivity, fouling, size exclusion, permeate flow, mass transfer resistance, and dye adsorption are the main areas affected [50,162]. The size exclusion capability of a membrane is determined by its pore size. Ceramic membranes with smaller pore sizes are anticipated to have higher removal efficiencies since organic dyes usually have particle sizes between 0.5 and 2.0 microns [163]. The majority of research on the use of inexpensive ceramic membranes to remove organic dyes has demonstrated that the separation process works in combination with adsorption and charge-based rejection mechanisms rather than merely depending on size exclusion. For example, methylene blue and Congo Red, whose particle sizes are smaller than the membrane pores, were successfully removed by a cheap ceramic membrane made from easily accessible pottery clay. The membrane’s average pore size was 0.49 μm. The reported results imply that the observed removal effectiveness was primarily due to adsorption and microfiltration rather than size exclusion alone [133]. The effectiveness of organic dye removal by inexpensive ceramic membranes is also greatly influenced by contact time. Extended contact between the membrane and the dye improves adsorption and separation, but only until equilibrium is reached. This is because there are a lot of empty surface sites available in the early phases of the process. The effectiveness of elimination decreases with further filtration after this equilibrium point [164]. The surface charge of membranes, as measured by the zeta potential, affects the electrostatic interactions between the membrane and dye molecules. These interactions are important for charged dyes because they directly affect the adsorption process. The charge compatibility between the dye molecules and the membrane surface determines the type of interaction. Negatively charged dyes are best removed by a positively charged membrane surface, while positively charged dyes exhibit higher affinity towards membranes with a negatively charged surface. In a study by Cheng et al. [165], the negatively charged organic dye Titan Yellow was successfully removed using a ceramic membrane made of diatomaceous earth modified with electropositive nano-YO3. The membrane had a high removal effectiveness of 99.6% through electrostatic adsorption. Furthermore, the membrane retained a positively charged surface over a broad pH range (3–8), indicating its potential for real-world uses.

5. Future Perspectives

Future research should focus on developing sustainable ceramic membranes that can efficiently target a variety of wastewater contaminants outside of organic dyes, making this technology more feasible for large-scale industrial applications. These membranes’ porosity and surface characteristics can be changed to meet wider uses. For instance, electropositive ceramic membranes have demonstrated the capacity to retain dye molecules and multivalent cations [166], indicating their potential for the removal of several contaminants. However, membrane fouling severely limits the use of inexpensive ceramic membranes in organic dye removal by lowering lifespan and affecting performance.
Furthermore, using inexpensive ceramic membranes alone to remove organic dyes is insufficient for full contaminant mineralization and may result in the production of secondary organic pollutants. Additionally, recovering and regenerating worn ceramic membranes frequently necessitates thorough cleaning procedures, which further reduce their long-term effectiveness. Future studies should focus on hybrid treatment approaches that combine inexpensive ceramic membranes with complementary technologies to overcome these issues. For instance, coagulation and photocatalysis combined with ceramic membranes may improve treatment effectiveness overall. In these systems, photocatalysis acts as the main or post-treatment technique to guarantee complete contaminant degradation, whereas ceramic membranes and coagulants can be used as pretreatment steps. These hybrid techniques have the potential to increase membrane longevity, decrease fouling, and improve contaminant removal, making inexpensive ceramic membranes a more practical option for treating wastewater on a wide scale.

6. Conclusions

In this review, recent advances in sustainable waste and natural material-derived ceramic membranes for organic dye removal were examined. The study primarily focused on the different types of cost-effective ceramic membranes and their mechanisms for removing organic dyes. The study revealed that there are four main types of these waste- and natural material-derived ceramic membranes: entirely low-cost materials, composites of low-cost materials, hybrids of low-cost materials and commercial materials, and low-cost materials functionalized with other materials. The efficiency of these membranes in removing organic dyes from wastewater is also examined in the review. The results show that these ceramic membranes have attracted a lot of attention because of their improved efficiency and inexpensive manufacturing costs. However, their use is still restricted to the laboratory scale. Therefore, to develop their industrial deployment and maximize their potential, more studies in this interesting area are necessary.

Author Contributions

Conceptualization, D.C.O.; methodology, K.A.M.; software, L.S.; investigation, K.A.M. and L.S.; resources, D.C.O.; writing—original draft preparation, K.A.M. and L.S.; writing—review and editing, D.C.O. and N.H.S.; supervision, D.C.O. and N.H.S.; project administration, D.C.O.; funding acquisition, N.H.S. and D.C.O. All authors have read and agreed to the published version of the manuscript.

Funding

This research was funded by the North-West University and the Nano Environment (NanoEnv) Incubation Program (NW-1G03101), NWU, South Africa.

Institutional Review Board Statement

Not applicable.

Data Availability Statement

No new data were created or analyzed in this study.

Acknowledgments

The financial support of the North-West University and the Nano Environment (NanoEnv) Incubation Program, NWU, South Africa, is greatly acknowledged.

Conflicts of Interest

The authors declare no conflicts of interest.

Abbreviations

The following abbreviations are used in this manuscript:
SOSafranin O
MGMalachite green
ROReverse osmosis
CRCongo Red (CR)
RhBRhodamine B (RhB)
BGBrilliant green (BG)
EBTEriochrome black T (EBT)
MVMethyl violet (MV)
MBMethylene blue (MB)
MOMethyl orange (MO)

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Figure 1. Industries are responsible for releasing dye wastewater into the environment and their percentage contribution [68].
Figure 1. Industries are responsible for releasing dye wastewater into the environment and their percentage contribution [68].
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Figure 2. Dye classification flowchart.
Figure 2. Dye classification flowchart.
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Figure 3. Various categories of dyes and their industrial applications.
Figure 3. Various categories of dyes and their industrial applications.
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Figure 4. Classification of membranes.
Figure 4. Classification of membranes.
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Figure 5. Low-cost material sources for ceramic membrane fabrication [117].
Figure 5. Low-cost material sources for ceramic membrane fabrication [117].
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Table 1. Widely used organic dyes, their classification, and reported toxicity effects.
Table 1. Widely used organic dyes, their classification, and reported toxicity effects.
Organic Dyes Classification Adverse Impacts of the DyeRef
Congo Red (CR)Anionic azo dyeExhibit carcinogenic and mutagenic properties.
Toxicity to animals and humans. 		[11,12,13]
Rhodamine B (RhB)Cationic xanthene dyeExhibit carcinogenic and mutagenic properties.
Causes cancer in humans.		[11,14]
Brilliant green (BG)Triphenylmethane dyeHighly toxic to aquatic organisms.
Causes skin and eye irritation.
Potentially carcinogenic.		[15,16,17]
Eriochrome black T (EBT)Anionic azo dyeCauses undesirable anomalies such as astigmatism and skin allergies.
Causes high pH, chemical oxygen demand, suspended solids, and salinity.
Affects the re-oxygenation ability of water bodies. Forms carcinogenic byproducts (naphthoquinones) upon degradation.
Affects the photosynthetic abilities of phytoplanktons and aquatic plants.		[18,19,20]
Safranin O (SO)A phenazine dyeToxicity to aquatic organisms
Causes serious eye damage		[21,22]
Methylene blue (MB) thiazine cationic and basic synthetic dyesInduce fatal serotonin toxicity in humans.
A threat to fauna in aquatic ecosystems.
It causes cancer in humans.		[23,24]
Methyl orange (MO) Anionic azo dyeCauses skin irritation
Causes allergic dermatitis		[4,25,26]
Methyl violet (MV) Cationic triphenylmethane dye classIt can cause toxicity in living organisms.
Possible mutagenic effects.		[27,28]
Sunset Yellow dyeSynthetic azo dyeCauses allergic reactions,
It can cause behavioral changes in children and has possible genotoxicity.		[29,30]
Yellow dye 5 (Tartrazine)Synthetic azo dyeAssociated with hyperactivity in children.
It can cause skin rashes and asthma.
Potential carcinogenic effects.		[31,32]
Malachite greenTriphenylmethane dyeHighly toxic to aquatic life.
Carcinogenic and mutagenic.
It can cause organ damage, particularly in the liver and kidneys.		[33,34]
Eosin YXanthene dyeIt can cause skin and eye irritation.
Possible toxic effects on aquatic organisms.		[35,36,37]
Indigo Carmine (Indigo Blue)Water-soluble indigoid dyePossible adverse effects like hypertension and skin irritation.
Highly toxic to humans and can cause tumors.
When in contact with the skin, it irritates and causes permanent injury to the cornea and conjunctiva when in contact with the eyes.
It can cause gastrointestinal irritation with nausea, vomiting, and diarrhea.
It displays carcinogenic properties, which can cause acute toxicity of organs related to reproduction, development, and the neurological system. 		[38,39,40]
Table 2. Cost analysis of various ceramic membranes fabricated from waste and natural starting materials.
Table 2. Cost analysis of various ceramic membranes fabricated from waste and natural starting materials.
Raw Materials for MembranesCost of Raw Materials (USD/Kg)Total Cost of Membrane Production (USD/m2)Ref.
Flay ash, quartz, calcium carbonate-250[128]
Chocobofe clay, kaolin, magnesite concentrate, and starch27.80233.55[129]
Phengite clay, distilled water0.3133.398[123]
Abundant clay0.0912.75[130]
Fuller’s earth clay4599.03[131]
Clay (~70% clay) 7[132]
Potter’s clay1.08342.46[133]
Peridotite, perlite2.969.91[134]
Fly ash-based low-cost tubular ceramic membrane0.43250[127]
Table 3. Cost analysis of various ceramic membranes fabricated from commercial starting materials.
Table 3. Cost analysis of various ceramic membranes fabricated from commercial starting materials.
Commercial Starting Materials for Ceramic MembranesCost of Raw Materials (USD/Kg)Total Cost of Membrane Production (USD/m2)Ref.
Alumina α-Al2O3 760[135,136]
Zirconia ZrO2 500–3000[117]
Silicon carbide SiC 100–1000[137]
Silicon carbide SiC 200[138]
Commercial mullite20–30150–200[139]
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Malebadi, K.A.; Sawunyama, L.; Seheri, N.H.; Onwudiwe, D.C. Application of Ceramic Membranes Derived from Waste and Natural Materials for the Removal of Organic Dyes from Wastewater: A Review. Ceramics 2025, 8, 80. https://doi.org/10.3390/ceramics8030080

AMA Style

Malebadi KA, Sawunyama L, Seheri NH, Onwudiwe DC. Application of Ceramic Membranes Derived from Waste and Natural Materials for the Removal of Organic Dyes from Wastewater: A Review. Ceramics. 2025; 8(3):80. https://doi.org/10.3390/ceramics8030080

Chicago/Turabian Style

Malebadi, Keotshepile A., Lawrence Sawunyama, Naledi H. Seheri, and Damian C. Onwudiwe. 2025. "Application of Ceramic Membranes Derived from Waste and Natural Materials for the Removal of Organic Dyes from Wastewater: A Review" Ceramics 8, no. 3: 80. https://doi.org/10.3390/ceramics8030080

APA Style

Malebadi, K. A., Sawunyama, L., Seheri, N. H., & Onwudiwe, D. C. (2025). Application of Ceramic Membranes Derived from Waste and Natural Materials for the Removal of Organic Dyes from Wastewater: A Review. Ceramics, 8(3), 80. https://doi.org/10.3390/ceramics8030080

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