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Review Article
2025
:18;
782025
doi:
10.25259/AJC_78_2025

Removal effect of recycled solid wastes and clay minerals on graphene oxide from water

, , , , , ,
aDepartment of Architecture and Engineering, Yancheng Polytechnic College, Yancheng 224005, China
bSchool of Transportation Engineering, Nanjing Tech University, Nanjing 211816, China.
cSchool of Civil Engineering, Shaoxing University, Shaoxing 312000, China.

*Corresponding author: E-mail address: wellswang@usx.edu.cn (W. Wang)

Received: , Accepted: ,
© 2025 Arabian Journal of Chemistry - Published by Scientific Scholar
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This is an open-access article distributed under the terms of the Creative Commons Attribution-Non Commercial-Share Alike 4.0 License, which allows others to remix, transform, and build upon the work non-commercially, as long as the author is credited and the new creations are licensed under the identical terms.

Abstract

Graphene oxide (GO), a hydrophilic nanomaterial with a high surface area, offers broad utility in aqueous systems, but poses critical environmental risks due to its stability, persistence, and resistance to degradation. To combat GO-related water pollution, this study reviews the efficacy of clay minerals (e.g., illite, sepiolite) and solid wastes (e.g., basalt powder, iron tailings) as sustainable, low-cost adsorbents. Key findings reveal that these materials exhibit strong adsorption capacities for GO, driven by van der Waals forces, electrostatic interactions, and hydrogen bonding. Illite and sepiolite significantly reduce GO concentrations, whereas basalt powder outperforms other solid wastes in adsorption efficiency. Composite adsorbents, which combine clay with carbon-based materials or metal oxides, can improve the removal rate of GO and introduce catalytic degradation capabilities to break down adsorbed GO, thereby addressing long-term environmental persistence issues. There are still challenges in optimizing adsorption conditions, deepening mechanism understanding, and designing environmentally friendly GO derivatives. Combining pollution source control with advanced adsorption-catalytic mixing systems can reduce the risk of GO contamination. Overall, clay minerals and solid waste show great potential as scalable, renewable GO removal solutions. By further optimizing their properties and combining them with sustainable technologies, these materials can effectively protect aquatic ecosystems while advancing innovation in green water treatment.

Keywords

Adsorption
Clay minerals
Graphene oxide
Recycled solid wastes
Water treatment methods

1. Introduction

Graphene oxide (GO), as an oxidized derivative of graphene, introduces numerous oxygen-containing functional groups (such as hydroxyl (-OH), carboxyl (-COOH), and epoxy (-C-O-C-)) on its surface. These functional groups impart significant hydrophilicity and high water solubility of GO, allowing it to remain stably dispersed in water over a wide concentration range [1-3]. Such functional groups not only confer GO with high surface reactivity and a large specific surface area but also enhance its stability in aqueous solutions and polar solvents. Due to its unique physical and chemical properties, GO has demonstrated broad application prospects in many fields, such as environmental technology, high-temperature materials, water treatment, and building materials [4-6]. However, as the scale of GO production and application continues to expand, its environmental release problems are becoming increasingly serious. Although GO is used as an adsorbent in some applications, throughout the life cycle of raw material acquisition, transportation, preparation, use, disposal, demolition, recycling, and reuse, GO can enter natural water bodies and potentially affect nearby groundwater or surface water environments. Additionally, after entering aquatic systems, GO may interact with inorganic ions and natural organic matter, thereby posing threats to aquatic organisms and human health and destabilizing the ecosystem [7,8].

GO may exist as a contaminant in industrial wastewater during composite material manufacturing, coating construction, and wastewater treatment. Among them, for the sewage treatment industry, the content of GO in industrial wastewater is generally 1-100 mg/L [9,10]. High content of GO is not conducive to water health; it also has certain biological toxicity. Current research has extensively evaluated the biological toxicity of GO. Zhao et al. [11] found that GO damaged freshwater algae membranes through the shielding effect and oxidative stress mechanism, thereby triggering toxic response. Guo et al. [12] demonstrated that the accumulation of GO significantly affected Drosophila’s weight and lifespan. Souza et al. [13] reported that GO caused serious damage to the gills and liver tissue of zebrafish, significantly altering its liver cell morphology and structure. Yang et al. [14] also noted that after 10 μg/mL GO treatment, the incubation and survival rates of zebrafish embryos were significantly reduced, and the malformation rate was as high as 11.11%. Mohamed et al. [15] documented the effect of GO on DNA mobility, causing DNA damage and exhibiting obvious genotoxicity. El-Yamany et al. [16] pointed out that injecting GO nanosheets into mice induced chromosomal aberrations and DNA fragmentation in lung cells. Chen et al. [17] noted that GO would denude and necrotize mucosal epithelial cells of the mouse digestive system, which may lead to malnutrition of maternal and offspring mice. Peng et al. [18] pointed out that GO is cytotoxic to human skin and can have different interactions with different cells. Based on the above research findings, GO toxicity is significantly positively correlated with its concentration. Deposition or direct contact with sharp nanosheets can cause damage and stress reactions in bacterial cell membranes. Therefore, addressing the environmental toxicity of GO is crucial to prevent its potential harm to the environment.

Although the toxicity problem of GO requires urgent solution, its excellent physical and chemical properties, particularly its large specific surface area and abundant oxygen-containing functional groups, make it a promising material for various applications. A typical example is the application of GO in cement-based materials. The oxygen-containing groups on its surface can interact with cement and water molecules, providing numerous adsorption sites, significantly enhancing the hydration rate and crack resistance of cement [19-21]. Research also indicates that incorporating GO into cement-based materials improves the bonding strength of cement, thereby enhancing its compressive strength.

In water pollution control, the adsorption method has become one of the most commonly used technologies due to its low cost, ease of operation, and high efficiency in removing pollutants. The effectiveness of the adsorption method largely depends on the selection of suitable adsorbent. Therefore, finding suitable adsorbents has become the key to optimizing the treatment effect [22-24]. In recent years, clay minerals and solid wastes have gradually become a focus of research due to their rich mineral composition, high specific surface area, good dispersion, and reproducibility. In particular, illite and sepiolite, two clay minerals, are widely used in wastewater treatment due to their excellent adsorption properties and low cost. Illite, as a potassium-rich clay mineral, not only exhibits a high melting point and specific surface area but also demonstrates strong adsorption capacity [25]. Sepiolite, known for its natural fibrous mineral structure, can effectively treat wastewater containing heavy metal ions due to its superior adsorption properties. Besides clay minerals, solid wastes such as fly ash have been extensively studied as an adsorbent and shown significant effects in removing heavy metals, organic matter, and dyes from water [26,27]. The utilization of solid wastes not only reduces treatment costs but also aligns with the goals of resource recovery and sustainable development, making it a research hotspot in promoting the concept of “treating waste with waste”.

In summary, although GO has excellent performance, it affects the balance of the aquatic system, causing adverse effects on the aquatic environment and aquatic organisms, which will eventually enter the ecological cycle and bring harm to human health. As adsorbents, GO, clay minerals and solid waste exhibit characteristics such as strong adsorption capacity, low cost, and strong regeneration ability and have the potential of large-scale water treatment. More research now focuses on the adsorption of GO to other toxic and harmful substances, and less considers the environmental impact of GO itself. Therefore, based on the above, in order to seek an effective, environmentally friendly and sustainable adsorption method for GO, this study takes clay minerals and solid waste as the object, aiming at systematically evaluating the removal effect of different clay minerals and solid waste on GO in water, exploring its adsorption mechanism and influencing factors, and providing theoretical support for the environmental management of GO. The main contents of the research include characterization of GO, analysis of macroscopic adsorption effects, adsorption kinetics, isotherm and thermodynamic analysis, comparative analysis of microscopic mechanisms, and discussion of future research directions.

2. Characterization of GO

GO exhibits strong hydrophilicity, which is closely related to the abundant polar functional groups on its surface, enabling it to disperse well in aqueous solution. Additionally, the enhanced surface chemical reactivity of GO allows it to interact with various chemicals, expanding its application potential in catalysis, sensors, and composite materials [28,29]. Its high dispersibility and negative charge enable it to efficiently adsorb a variety of pollutants, especially heavy metal ions and organic dyes, during water treatment. However, the dispersibility of GO may also lead to its persistence and potential toxicity in the environment [30]. Therefore, it is of great scientific significance to study its removal methods and environmental impact. To gain a deeper understanding of the structure and properties of GO, researchers have employed various characterization methods, including scanning electron microscopy (SEM), atomic force microscopy (AFM), transmission electron microscopy (TEM), X-ray diffraction (XRD), Fourier transform infrared spectroscopy, and Raman spectroscopy (FT-IR). Specific relevant results have been illustrated in Figure 1.

Microstructure characterization of GO: (a) AFM diagram of GO [29], (b) SEM diagrams of GO wrinkle and curling [29], (c) FTIR diagram of GO [29], (d) TEM diagrams of GO folding and stacking [29], (e) Raman spectra of GO [29].
Figure 1.
Microstructure characterization of GO: (a) AFM diagram of GO [29], (b) SEM diagrams of GO wrinkle and curling [29], (c) FTIR diagram of GO [29], (d) TEM diagrams of GO folding and stacking [29], (e) Raman spectra of GO [29].

Figure 1(a) is an AFM diagram of GO. Studies have shown that exfoliated GO typically exhibits a uniform thickness of approximately 1nm. Due to the introduction of oxidized functional groups, the surface of GO often displays significant roughness, particularly in samples with a high degree of oxidation. The AFM diagram clearly illustrates the irregular surface undulations [31]. The SEM diagram (Figure 1b) further reveals that GO has a sheet-like structure and may exhibit slight agglomeration on the surface. Its layered characteristics and large specific surface area indicate that GO possesses strong dispersion in water [32]. The FT-IR diagram (Figure 1c) provides critical information for qualitative analysis of the functional groups on the surface of GO. Specifically, the absorption peak at 1735 cm-1 corresponds to the stretching vibration of C–O in the carboxyl group (-COOH); the absorption peak near 1624 cm-1 is attributed to the C–C stretching and C-OH bending vibrations caused by the SP2 carbon atoms on the GO plane; the absorption band at 1122 cm-1 represents the stretching vibration of C–O [32]. In addition, the TEM diagram (Figure 1d) offers a high-resolution structural view of GO, revealing its flake-like features and local bending or folding phenomena caused by the presence of oxidized groups [33]. Raman spectra are an important tool for analyzing the surface defects and number of layers of GO (Figure 1e). The Raman spectra of GO typically contains D, G, and 2D peaks, where the D peak represents the structural defects caused by oxidized groups, and the G peak relates to the orderly arrangement of carbon atoms [34]. Otta and Ferrari et al. [35] pointed out that the Raman spectra of GO may exhibit multiple characteristic peaks, such as 2D and 2D’ characteristic peaks, as well as combination peaks such as D+D’, which further revealed the surface defects and structural characteristics of GO. Anusuya et al. [36] studied the defects of GO and reduced GO (rGO) through first-order Raman scattering and found that point defects (0D) and line defects (1D) were crucial to the performance of the material. Research by Yang et al. [37] showed that the Raman signal intensity of GO increased with the increase of the number of layers (1-4 layers), while rGO showed the opposite trend, indicating the influence of π-π stacking effect on the Raman signal intensity.

3. Macroscopic Adsorption Effect Analysis

3.1. Removal effect of clay minerals on GO

The high stability of GO in water and its rich surface functional groups can easily negatively impact aquatic ecosystems, especially when released on a large scale or retained in the water environment, posing a serious threat to the growth, reproduction, and ecological balance of aquatic organisms. Therefore, removing GO from water has become an urgent scientific and technological challenge. Effective removal of GO from water not only helps prevent environmental pollution but also provides opportunities for the recycling of GO, which holds significant environmental protection and resource reuse value.

The adsorption method is a widely used separation and purification technology in environmental protection, wastewater treatment, air purification, and other fields. It has become an ideal choice for removing pollutants from water due to its advantages of high efficiency, low cost, and simple operation. Clay minerals have been extensively studied as effective adsorbents for removing GO from water due to their excellent physical and chemical properties, particularly their large specific surface area, strong adsorption capacity, and high ion exchange capacity. The adsorption performance of clay minerals on GO is influenced by many factors, including mineral type, surface functional groups, solution pH, temperature, and ionic strength. Figure 2 outlines the current experimental steps for removing GO using clay minerals, aiding in understanding the adsorption mechanism and effectiveness of clay minerals on GO removal under different experimental conditions. As shown in Figure 2, the GO operation process for clay mineral removal mainly includes 5 steps: material pretreatment, GO solution configuration, pH adjustment, adsorption reaction, and data measurement. The specific methods and points of attention during the experiment are as follows: (1) In the material pretreatment stage, GO should be ultrasonically treated for 30 mins to ensure the stable dispersion of GO, and the clay minerals should be screened through a 0.074 mm mesh screen to ensure uniform particle size. (2) GO solution configuration, that is, mix the pre-treated GO with deionized water and configure it into 50 mL GO solution. (3) pH adjustment: the pH value of the GO solution is determined by a pH meter, and the adjustment of the acid-base degree is mainly through the mixing of NaOH and HCl solutions. (4) Adsorption reaction: the mixture of clay minerals and GO aqueous solution is shaken on the shaking table at a speed of 240 rpm for 3 h, after shaking, the sample bottle is removed and left in the incubator for 24 hrs to promote adsorption. (5) In the data measurement stage, 1 mL of the superserum is taken with a pipette gun and diluted to 25 mL by adding deionized water, and the absorbance at the corresponding wavelength was measured by UV-visible spectroscopy.

Main operation process for removing GO using clay minerals [33].
Figure 2.
Main operation process for removing GO using clay minerals [33].

Table 1 summarizes the adsorption performance of different clay minerals on GO under various conditions. Li et al. [32] investigated the adsorption behaviour of illite on GO at different pH values, and found that at an initial GO concentration of 80 mg/L, a temperature of 303K, pH=3, and an illite mass of 150mg, the adsorption rate of GO by illite reached up to 93.80%, indicating optimal adsorption performance. Studies have demonstrated that in acidic environments, electrostatic attraction between the surface negative charge of illite and the cationic groups on the surface of GO promotes GO adsorption. In addition, Al2O3 and K2O components in illite partially dissolve at low pH conditions, forming Al3+ and K+, which further enhances the adsorption capacity of GO. The pH value and surface properties of solid particles significantly influence GO aggregation and deposition in aqueous solutions. Li et al. [38] examined the adsorption performance of red sandstone on GO. At 303K, pH=4, and a red sandstone mass of 40 mg, the adsorption rate of GO by red sandstone was 89.08%. The research revealed that CaCO3 in red sandstone reacted with H+ under acidic conditions to produce Ca2+, promoting GO adsorption through coordination with oxygen-containing functional groups on the GO surface. However, higher acidity can inhibit adsorption because of excessive acidic ions interfering with the adsorption process.

Under acidic conditions, sepiolite (SEP) also exhibits high GO adsorption capacity. Li et al. [39] reported that at 303K and pH=3, the adsorption rate of GO by sepiolite reached 94.80%, demonstrating effective removal. Studies have shown that under acidic conditions, the dissolution of cations in SEP (such as Mg2+ and Ca2+) weakens interlayer binding forces, leading to lattice structure disruption and increased porosity, thereby enhancing specific surface area and improving GO adsorption. Conversely, under high pH conditions, the carboxyl groups on the surface of GO may be protonated, which inhibits electrostatic interactions with cations, resulting in a decrease in adsorption performance. Huang et al. [40] studied the role of attapulgite in GO removal. At pH=3, the removal rate of GO by attapulgite was 92.83%. MgO and CaO in attapulgite partially dissolved in acidic environments, releasing Mg2+ and Ca2+ [41]. These cations compressed or penetrated the double layer, directly adsorbed oxygen-containing functional groups on the surface of GO, and effectively removed GO [42,43]. Lv et al. [44] investigated the adsorption performance of GO by calcareous sand and found that its adsorption performance was closely related to pH. When pH<6, electrostatic repulsion occurred between GO and calcareous sand, thereby weakening adsorption. As pH decreased, the negative charge generated on the surface of GO decreased, and the adsorption between GO and calcareous sand increased. The amount of GO adsorbed by calcareous sand first increased and then decreased with pH changes, increasing with the increase of initial GO concentrations. Adsorption primarily occurred through chemical adsorption and hydrogen bonding or hydroxyl interactions with oxygen-containing functional groups on the surface of GO. Jiang et al. [45] found that basalt powder (BSP) exhibited excellent GO adsorption performance. Under 303K and pH=3, the maximum GO adsorption by BSP is 112 mg/g, with an adsorption rate of 99%. Ca2+ ions in basalt powder electrostatically attracted oxygen-containing functional groups on the surface of GO, thus forming adsorption salts and enhancing GO adsorption capacity.

Table 1. Comparison of optimal adsorption effect factors of clay minerals.
Adsorbent Temperature (K) pH Adsorbent mass (mg) GO initial concentration (mg/L) Removal rate (%) Equilibrium time (min) Reference
Illite 303 3 150 80 93.80 2160 [32]
Red sandstone 4 40 80 89.08 1440 [38]
Sepiolite 3 30 100 94.80 2160 [39]
Attapulgite 3 40 100 92.83 2160 [43]
Basalt powder 3 70 80 99.00 1440 [45]

In summary, clay minerals are widely used in water pollution control because of their large specific surface area and high ion exchange capacity. Different types of clay minerals can effectively adsorb GO in water, and the adsorption properties of illite and sepiolite are particularly outstanding. In adsorption, the surface functional groups of clay minerals and dissolved metal cations, such as Al3+, Mg2+, and Ca2+, play a key role in the removal of GO. In addition, the adsorption of GO by clay minerals is significantly affected by pH value. In an acidic environment, these metal oxides are partially dissolved, and the released cations can undergo electrostatic interaction or complexation with oxygen-containing functional groups (such as carboxyl groups and hydroxyl groups) on the surface of GO, thus promoting the sedimentation and removal of GO. However, at higher pH conditions (pH>6), the carboxyl group on the GO surface is deprotonated, resulting in increased electrostatic repulsion, which inhibits adsorption. Future research should explore optimizing adsorption performance by adjusting experimental conditions like pH value and temperature, etc., so as to provide effective solutions for GO removal in water treatment.

3.2 Removal effect of solid wastes on GO

Solid wastes have attracted extensive attention in recent years as a potential adsorption material, particularly for GO removal in water treatment [46]. The adsorption performance of solid wastes is influenced by various factors such as pH, temperature, types of adsorbent and initial GO concentration. This section summarizes researches on the adsorption of GO by different solid wastes, with specific data presented in Table 2.

Li et al. [47] investigated the adsorption effect of carbide slag on GO. Under conditions of pH=11, a carbide slag mass of 5 mg, an initial GO concentration of 80 mg/L, and temperature of 303K, the removal rate of GO by carbide slag reached a maximum value of 97.04%. This high efficiency was mainly attributed to the reaction between the carboxyl groups on the surface of GO and hydroxyl groups on the surface of carbide slag. In an alkaline environment (pH=11), hydroxide ions reacted with metal ions (such as Al2O3, Fe(OH)3) in carbide slag to form insoluble metal hydroxides, thereby enhancing the adsorption effect. Zhou et al. [48] examined the adsorption performance of iron tailings on GO. At a temperature of 303.15K, an iron tailings mass of 50 mg, an initial GO concentration of 60 mg/L, and pH=7, the adsorption rate of GO by iron tailings was 89.92%. The main mechanism involved electrostatic adsorption between surface anionic groups (such as carboxyl and hydroxyl groups) and metal cations on the surface of iron tailings particles. In addition, metal ions in iron tailings may interact with GO through the formation of complexes, thus further enhancing its adsorption capacity. However, the study also noted that the adsorption equilibrium time of iron tailings was relatively long, reaching 1680 mins, which may limit its adsorption efficiency in practical applications. Jiang et al. [42] studied the application of fly ash for GO removal. At pH=6, a temperature of 303K, a FA mass of 5 mg, and an initial GO concentration of 60mg/L, the maximum removal rate of GO by FA was 93.00%. Studies indicated that at low pH levels, oxygen-containing functional groups in GO were easily protonated, thus reducing the hydrophilicity of GO and promoting its aggregation to form flocs. In this process, Al3+ and Ca2+ ions in FA played an important role, which further promoted GO removal through electrostatic adsorption and complexation [49]. Jiang et al. [50] explored the adsorption effect of gypsum on GO. Under conditions of pH=8.0, a gypsum mass of 60 mg, an initial GO concentration of 80 mg/L, and a temperature of 303K, the maximum removal rate of GO by gypsum reached 93.30%. Gypsum provided OH− ions in an alkaline environment, promoted the ionization of CaSO4 to form Ca2+, and then reacted with OH− to form Ca(OH)2. Ca(OH)2 further reacted with CO2 in the air to form CaCO3. Both Ca(OH)2 and CaCO3 had strong adsorption capacities, which could significantly improve the removal effect of gypsum on GO. The adsorption mechanism of gypsum mainly relied on the chemical adsorption between surface metal ions (Ca2+) and oxygen-containing functional groups in GO. Li et al. [33] studied the removal performance of GO by waste glass (WG) in an acidic environment. Under conditions of pH=3, a waste glass mass of 40 mg, an initial GO concentration of 80 mg/L, and a temperature of 313K, the adsorption rate of GO by waste glass reached 95.50%. In acidic conditions, GO exhibited self-aggregation characteristics, promoting its aggregation and deposition. Waste glass contained high levels of Al2O3, CaO, and MgO, which were partially dissolved under acidic conditions and released cations such as Al3+, Ca2+, and Mg2+. These cations promoted the condensation and aggregation of GO in aqueous solution [25] and enhanced the electrostatic attraction between waste glass and GO [27].

Table 2. Comparison of optimal adsorption effect factors of solid wastes.
Adsorbent Temperature (K) pH Adsorbent mass (mg) GO initial concentration (mg/L) Removal rate (%) Equilibrium time (min) Reference
Calcium carbide slag 303 11 5 80 97.04 60 [47]
Iron tailings 303.15 7 50 60 89.92 1680 [48]
Fly ash 303 6 5 60 93.00 720 [42]
Waste gypsum 303 8 60 80 93.30 360 [50]
Waste glass powder 313 3 60 80 95.50 750 [33]

Based on the researches summarized above, the optimal conditions for GO adsorption by solid wastes are compared, as shown in Table 2. The table shows that the adsorption effect of solid waste adsorbing GO is also affected by pH value. Among them, calcium carbide slag has the best effect in alkaline environment (pH=11), waste glass powder has a higher adsorption efficiency in acidic environment (pH=3), and the pH value corresponding to the best adsorption rate of other materials is in the range of 6∼8. The mechanism of GO adsorption by solid waste mainly involves the electrostatic adsorption and complexation of metal cations with the carboxyl and hydroxyl groups on the surface of GO. In addition, different materials have obvious differences in the adsorption time of GO, the highest removal rate of iron tailings can reach 90%, but its equilibrium time reaches 1680 mins. Future studies can further improve the adsorption capacity of industrial solid waste in the water treatment process from the perspective of optimizing experimental conditions (such as pH value, temperature).

4. Comparative Analysis of Adsorption Kinetics, Isotherm and Thermodynamics

4.1 Clay mineral application

Adsorption kinetics, isotherm and thermodynamic analysis are crucial methods for evaluating the adsorption performance of solid wastes on GO. Researches by various scholars have demonstrated that the adsorption behavior of solid wastes on GO exhibits significant temperature, pH and time dependence, with both physical and chemical effects influencing the adsorption process.

Figures 3 and 4 present the adsorption isotherms and thermodynamics of GO adsorbed by different clay minerals, respectively. Table 3 provides a comparative analysis of the adsorption kinetics, isotherms and thermodynamics of GO by solid wastes and clay minerals. Li et al. [32] found that the adsorption of GO by illite conformed to Langmuir isotherm model, indicating monolayer adsorption with uniform adsorption sites. Thermodynamic analysis revealed that the adsorption process was endothermic, with increasing temperature promoting the reaction. Adsorption kinetic analysis showed a sharp increase in the adsorption rate within the initial 1000 mins, followed by a gradual slowdown until equilibrium was reached at 2160 mins. The pseudo-second-order kinetic model fitting results suggested that the adsorption process of GO by illite was primarily chemical adsorption, which was spontaneous with high thermodynamic stability. Li et al. [38] observed that the adsorption of GO by red sandstone conformed to Langmuir isotherm model, indicating monolayer adsorption with increased capacity at higher temperatures. Kinetic studies indicated that the adsorption process of GO by red sandstone conformed to the quasi-second-order kinetic equation, implying that the adsorption reaction was dominated by chemical action. The adsorption equilibrium was reached after 2800 mins, further proving the slow nature of the process. Li et al. [39] reported that the adsorption process of GO by sepiolite conformed to the quasi-second-order kinetic model, and the adsorption process was mainly controlled by chemical action. Rapid adsorption occurred within the first 100 mins, reaching equilibrium after 2160 mins. Intragranular diffusion and liquid film diffusion were identified as the main factors influencing the adsorption rate. Isotherm analysis showed that the adsorption of GO by sepiolite was consistent with Langmuir and Temkin models, indicating that the adsorption of GO was dominated by monolayer adsorption accompanied by endothermic reaction. Thermodynamic analysis results further confirmed that the adsorption of GO by sepiolite was a spontaneous endothermic process, with an entropy increase reflecting the high efficiency of the adsorption reaction. Li et al. [43] found through adsorption kinetic experiments that the adsorption process of GO by attapulgite conformed to the quasi-second-order kinetic model, indicating the coexistence of physical adsorption and chemical adsorption. Isotherm studies showed that the adsorption of GO by attapulgite conformed to Langmuir model, indicating monolayer adsorption. Thermodynamic calculation revealed that the adsorption of GO by attapulgite was an endothermic reaction, with increasing temperature enhancing the adsorption process. Jiang et al. [45] demonstrated that the adsorption process of GO by BSP best fitted Langmuir model, indicating monolayer adsorption. Thermodynamic analysis showed that the adsorption of GO by BSP was a spontaneous endothermic reaction, with adsorption capacity increasing with temperature. Kinetic experimental results indicated that the adsorption process of GO by BSP was consistent with the pseudo-first-order kinetic model, with rapid adsorption occurring within 500 mins and equilibrium reached after 1440 mins. Desorption experiments revealed that BSP exhibited good reversibility in alkaline environments (pH=10), achieving a desorption rate of 86%, highlighting its promising engineering applications.

Adsorption isotherms of GO adsorption by different clay minerals: (a) Attapulgite [43], (b) Sepiolite [39], (c) Red sandstone [38], (d) Basalt powder [45], (e) Illite [32].
Figure 3.
Adsorption isotherms of GO adsorption by different clay minerals: (a) Attapulgite [43], (b) Sepiolite [39], (c) Red sandstone [38], (d) Basalt powder [45], (e) Illite [32].
Adsorption thermodynamics of GO adsorption by different clay minerals: (a) Attapulgite [43], (b) Sepiolite [39], (c) Red sandstone [38], (d) Basalt powder [45], (e) Illite [32].
Figure 4.
Adsorption thermodynamics of GO adsorption by different clay minerals: (a) Attapulgite [43], (b) Sepiolite [39], (c) Red sandstone [38], (d) Basalt powder [45], (e) Illite [32].
Table 3. Comparative analysis of adsorption kinetics, isotherm and thermodynamics of GO by solid wastes and clay minerals.
Adsorbent pH Adsorbent mass (mg) GO concentration (mg/L) Removal rate (%) Isotherm Kinetic model References
Attapulgite 3 40 100 92.83

Langmuir

Freundlich

Pseudo-First-Order

Pseudo-Second-Order

 [43]
Sepiolite 3 30 100 94.80

Langmuir

Freundlic

Temkin

Pseudo-First-Order

Pseudo-Second-Order Elovich

Intraparticle-diffusion

Boyd-Ruthven-Ho

 [39]
Red sandstone 4 40 80 89.08

Langmuir

Freundlich

Pseudo-First-Order

Pseudo-Second-Order

 [38]
Basalt powder 3 70 80 99.00

Langmuir

Freundlich

Langmuir

Freundlich

 [45]
Illite 3 150 80 93.80

Langmuir

Freundlich

Pseudo-First-Order

Pseudo-Second-Order

 [32]
Calcareous sand 6 70 100 91.50

Langmuir

Freundlich

 - [44]
Calcium carbide slag 11 5 80 97.04

Langmuir

Freundlic

Temkin

Pseudo-First-Order

Pseudo-Second-Order Elovich

Intraparticle-diffusion

Boyd-Ruthven-Ho

 [47]
Iron tailings 7 50 60 89.92

Langmuir

Freundlic

Temkin

Pseudo-First-Order

Pseudo-Second-Order

Weber–Morris

 [48]
Fly ash 6 5 60 93.00

Langmuir

Freundlich

 - [42]
Waste gypsum 8 60 80 93.30

Langmuir

Freundlich

 - [50]

The results show that the adsorption of GO by clay minerals usually conforms to the Langmuir isothermal adsorption model, and the adsorption process is mainly monolayer adsorption. In addition, the adsorption process of GO by clay minerals is usually spontaneous endothermic and conforms to the quasi-second-order kinetic model, indicating that chemisorption plays a leading role in this process. However, the types of clay minerals also affect the adsorption characteristics of GO. For example, BSP conforms to the quasi-first-order kinetic model, and the adsorption process of sepiolite conforms to the Langmuir and Temkin isothermal models, indicating that GO is mainly adsorbed in a single layer on the surface of sepiolite, accompanied by certain adsorption energy changes, and the process is influenced by both chemical and electrostatic effects.

4.2 Solid wastes application

Studying the kinetics, thermodynamics and isotherm characteristics of GO removal by solid wastes not only provides a theoretical basis for improving water pollution control efficiency, but also offers a feasible technical pathway for waste resource utilization, environmental protection and sustainable development, which holds significant academic value and application prospects.

Figure 5 presents the thermodynamic analysis diagram of GO adsorption by various solid wastes. Lv et al. [44] demonstrated that the adsorption of GO by calcareous sand was mainly monolayer adsorption, with no significant lateral interactions or steric hindrance effects during the adsorption process. The binding of GO to calcareous sand surface was mainly driven by physical forces, and all adsorption sites exhibited equal affinity. Thermodynamic analysis indicated that the adsorption of GO by calcareous sand was a spontaneous endothermic reaction, with the adsorption efficiency significantly increasing as temperature rises. Li et al. [47] investigated calcium carbide slag and found that its adsorption process conformed to Langmuir isotherm model, indicating monolayer homogeneous adsorption. The adsorption kinetics was consistent with the pseudo-second-order kinetic model, with rapid adsorption occurring within 10 mins and equilibrium reached within 1 hour. Increasing temperature promoted the adsorption reaction, indicating that the adsorption process was endothermic, thereby enhancing the removal capacity of GO by carbide slag. Zhou et al. [48] reported that the adsorption of GO by iron tailings conformed to Langmuir model, representing monolayer adsorption. However, increasing temperature inhibited the adsorption reaction, suggesting that the adsorption process was exothermic. The adsorption kinetics conformed to the pseudo-first-order kinetic model, characterized by two stages: surface adsorption and intra-particle diffusion. Weber-Morris model fitting revealed that particle diffusion was the key factor influencing the adsorption rate in the initial stage. According to the study of Jiang et al. [42], the adsorption of GO by fly ash followed Langmuir isotherm model, with monolayer adsorption increasing as temperature rises. Thermodynamic analysis confirmed that the adsorption of GO by fly ash was a spontaneous exothermic reaction, favoring lower temperatures for optimal adsorption. This process demonstrated that fly ash could effectively remove GO from water through a simple and rapid chemical reaction. Jiang et al. [50] found that the adsorption of GO by gypsum conformed to Langmuir and Freundlich models. Thermodynamic analysis revealed that the adsorption of GO by gypsum was a spontaneous exothermic process, with the adsorption effect weakening as the temperature increased. Thermo-gravimetric analysis experimental results indicated that the entanglement between gypsum and GO enhanced the adsorption effect. The adsorption mechanism involved both physical adsorption and chemical interactions, resulting in the best adsorption effect at an optimal temperature. Li et al. [33] found that the Freundlich model better described the adsorption isotherm of GO by waste glass. The adsorption process exhibited exothermic behaviour as temperature rises. Kinetic experiments showed that the adsorption of GO by waste glass conformed to the pseudo-second-order kinetic model, with rapid adsorption in the first 50 mins, followed by a gradual slowdown until reaching equilibrium after 12.5 hrs. Internal diffusion was not the rate-limiting step. Additionally, after 5 cycles, the adsorption rate remained at 78.1%, indicating high reusability and stability of waste glass.

Adsorption thermodynamics of GO adsorption by different solid wastes: (a) Calcium carbide slag [47], (b) Iron tailings [48], (c) Waste gypsum [50], (d) Fly ash [42], (e) Waste glass powder [33].
Figure 5.
Adsorption thermodynamics of GO adsorption by different solid wastes: (a) Calcium carbide slag [47], (b) Iron tailings [48], (c) Waste gypsum [50], (d) Fly ash [42], (e) Waste glass powder [33].

The above results show that, similar to clay minerals, the adsorption of GO by solid waste typically conforms to the Langmuir isothermal adsorption model, and monolayer adsorption plays a leading role in this process. However, some solid wastes exhibit obvious exothermic characteristics during the process of removing GO (such as iron tailings, fly ash, and gypsum), which means that for these materials, lower temperatures are more conducive to improving the efficiency of their adsorption of GO. Additionally, the adsorption behavior of iron tailings differs from that of calcium carbide slag. The adsorption process of iron tailings is not a quasi-second-order kinetic model but conforms to the characteristics of the quasi-first-order kinetic model, exhibiting the two-stage characteristics of surface adsorption and internal diffusion of particles.

5. Microscopic Mechanism Analysis

5.1. Physical adsorption mechanism

In the study of GO adsorption by solid wastes and clay minerals in water, analyzing the microscopic mechanisms provides deeper insights. A comparative analysis of the microscopic mechanisms of GO adsorption by different solid wastes and clay minerals is presented in Figure 6.

Microscopic mechanism of GO adsorption by different solid wastes and clay minerals: (a) GO/Illite [32], (b) GO/Red sandstone [38], (c) GO/Sepiolite [39], (d) GO/Attapulgite [43], (e) GO/Waste glass powder [33], (f) GO/Basalt powder [45].
Figure 6.
Microscopic mechanism of GO adsorption by different solid wastes and clay minerals: (a) GO/Illite [32], (b) GO/Red sandstone [38], (c) GO/Sepiolite [39], (d) GO/Attapulgite [43], (e) GO/Waste glass powder [33], (f) GO/Basalt powder [45].

Figure 6(a) illustrates GO adhering to the illite surface, showing the interaction between illite and GO. Figure 6(b) displays the SEM morphology of GO/red sandstone after adsorption, clearly showing film-like GO attached to the surface of red sandstone particles. Figure 6(c) depicts the image of SEP/GO, where fiber structures are visibly attached to the tulle surface, indicating GO accumulation on SEP. Figure 6(d) shows the image of attapulgite after GO adsorption, revealing tulle-like GO attached to the acicular attapulgite surface. Figure 6(e) demonstrates significant GO adsorption on the surface of waste glass, with obvious cluster accumulation, strongly suggesting waste glass’s substantial adsorption effect on GO. Figure 6(f) demonstrates a significant accumulation of GO within basalt powder, indicating its robust adsorption capacity on GO.

Surface adsorption is the primary mechanism responsible for GO adsorption by various solid wastes and clay minerals [13,12]. It mainly includes the van der Waals force, charge interaction, and hydrogen bond. The Van der Waals force is a type of non-specific weak interaction force resulting from the instantaneous dipole induction effect between molecules [51]. In the adsorption process, GO’s layered structure and the surface of the adsorbent (such as the layered silicate of illite, the porous amorphous SiO2 of WG) through physical contact to produce van der Waals force, prompting GO to adhere to the surface of the adsorbent, this physical adsorption plays a leading role in the initial stage, especially at high concentrations of GO or low temperature conditions more significant [52,24]. Clay minerals such as illite, sepiolite, and attapulgite possess abundant hydroxyl groups and negative charges on their surfaces, which can interact with the oxidized groups of GO through electrostatic attraction. Under high pH conditions, both the surface of GO and most clay minerals exhibit negative charges, thereby enhancing the electrostatic interaction between them [32]. Moreover, the oxygen-containing functional groups of GO (such as -COOH, epoxy) will form a hydrogen bond network with the hydroxyl (-OH), silica (Si-O), or metal oxides (such as Al-O, Fe-O) on the surface of the adsorbent, further strengthening the adsorption process. Hydrogen bonding mainly occurs in the later stages of adsorption (such as the equilibrium stage), especially at near-neutral pH conditions [53]. Li et al. [32] found that the adsorption mechanism of GO by illite mainly involved electrostatic interactions and hydrogen bonding. Specifically, electrostatic attraction occurred between the negatively charged surfaces of GO and illite, while hydroxyl groups on the GO surface formed hydrogen bonds with water molecules on the illite surface, significantly enhancing the adsorption effect of GO. As illustrated in Figure 7, the AFM test results of GO and illite/GO composites further verify this adsorption mechanism. Research also indicates that the interaction between illite surface functional groups and GO surface oxidation groups is a critical pathway for GO adsorption. Figure 8 shows the macroscopic reaction effect of GO aqueous solution after adding illite.

Atomic Force Microscope (AFM) test: (a) GO, (b) GO/lite [32].
Figure 7.
Atomic Force Microscope (AFM) test: (a) GO, (b) GO/lite [32].
Changes of solution before and after adsorption [32].
Figure 8.
Changes of solution before and after adsorption [32].

Studies have shown that the adsorption of GO by clay minerals (such as illite, sepiolite) and solid wastes (such as fly ash) is primarily accomplished through Van der Waals force, surface electrostatic interaction, and hydrogen bonding. Van der Waals forces play a dominant role in the initial stage of adsorption. The carboxyl group on the surface of GO is easy to protonate at a higher acidic level, resulting in strong hydrogen bonding with the surface of clay minerals. In addition, the electrification of the adsorbent surface will affect the ability of clay minerals and solid waste to adsorb GO, such as the electronegativity of illite will enhance its electrostatic adsorption with GO.

5.2 Chemical adsorption mechanism

Chemical adsorption represents another important mechanism for GO adsorption by various minerals. Chemical adsorption typically involves electron transfer or the formation of chemical bonds, resulting in the formation of stable chemical bonds between the adsorbed substance and the adsorbent [7,54]. To further analyze which chemical bonds in GO are involved in the adsorption process, the changes in functional groups and the migration and disappearance of chemical bonds in GO can be analyzed using FT-IR. For instance, Li et al. [38] found in Figure 9 that after red sandstone adsorbed GO, the C=O peak (at 1734 cm-1) disappeared, which may be due to the combination of Ca2+ in red sandstone with O-C=O bond in GO, resulting in GO solidification, indicating that GO had ionic reaction or coordination reaction on the surface of red sandstone [55,56]. Additionally, some solid wastes, such as iron tailings and BSP, contain metal ions like iron and aluminum, whose surfaces can coordinate with GO, further promoting the adsorption process.

FT-IR analysis of GO, Red sandstone, and GO/Red Sandstone [38].
Figure 9.
FT-IR analysis of GO, Red sandstone, and GO/Red Sandstone [38].

Jiang et al. [45] found that the adsorption of GO by BSP conformed to the pseudo-first-order kinetic model and was a spontaneous endothermic process, indicating that electron transfer and chemical reactions may occur during adsorption, resulting in strong chemical adsorption. In contrast to chemical adsorption, physical adsorption typically fixes GO molecules on the solid surface through weaker interaction forces (such as van der Waals forces, hydrogen bonds, and electrostatic forces). Physical adsorption does not involve significant electron transfer or chemical bond formation and is relatively reversible. Clay minerals like sepiolite and attapulgite often interact with GO surfaces through van der Waals forces and hydrogen bonds, forming weak physical adsorption [7]. This physical adsorption mechanism typically occurs when the GO surface is rich in oxidized groups, which can interact with the adsorbent surface through non-covalent interactions. Li et al. [39] showed that the adsorption process of GO by sepiolite was dominated by physical adsorption, in which GO interacted with the surface hydration layer of sepiolite through surface hydrogen bonds and van der Waals forces. Although the adsorption intensity was weak, this process still exhibited significant adsorption performance at low temperatures and neutral pH values. The study also revealed that the adsorption process of sepiolite not only depended on physical forces but was also influenced by surface diffusion and liquid film diffusion, highlighting the complexity of the adsorption process.

Beyond direct physical adsorption and chemical adsorption, surface modification and complexation play crucial roles in enhancing the adsorption of GO by solid wastes and clay minerals. Surface modification can significantly improve the adsorption performance by introducing new functional groups or altering surface charge density. When specific chemical substances are added to the surface of wastes or minerals, new complexes or composites can form, thereby enhancing the adsorption capacity. For instance, Lv et al. [44] pointed out that the surface of calcareous sand can be chemically modified to introduce amino or hydroxyl functional groups, thereby enhancing its adsorption capacity for GO. Thermodynamic parameter analysis revealed that GO adsorption by calcareous sand was a spontaneous endothermic process, with the modified calcareous sand exhibiting superior adsorption capacity, indicating that surface modification not only improved the adsorption efficiency but also changed the interaction mechanisms between GO and the adsorbent.

The presence of other ions and molecules in the solution can influence GO adsorption. In actual water bodies, inorganic ions (such as Ca2⁺, Na⁺, Mg2⁺, etc.) and organic matter may compete with GO for adsorption sites, thereby affecting the adsorption efficiency. Numerous studies have shown that the concentration of these ions, pH values, and temperatures have a significant impact on GO adsorption [46,45]. Zhou et al. [48] experimentally observed that iron tailings exhibited different adsorption behaviors toward GO at different pH values. Under low pH conditions, the high concentration of H⁺ ions reduces the negative charge on the GO surface, resulting in decreased adsorption efficiency. Moreover, calcium ions in the solution can complex with carboxyl and phenolic hydroxyl groups of GO, further influencing the adsorption process.

6. Development Prospect

Based on the above results, the efficient adsorption properties of clay minerals and solid waste can be further translated into practical solutions for industrial applications. First of all, the use of fly ash, iron tailings and other industrial waste as low-cost adsorbent raw materials, through simple modification (such as pickling or mechanical grinding) to improve its adsorption capacity, and combined with modular adsorption devices to adapt to different water quality conditions - such as acidic wastewater using BSP, alkaline wastewater using calcium carbide slag. At the same time, for reversible materials (such as BSP), the development of mild regeneration process to extend their cycle life, and the adsorption of the composite resources applied to the field of building materials (such as strengthening the performance of cement), to achieve the “waste to waste” circular economy goal.

However, it is worth noting that solid waste, including calcium carbide slag, and iron tailings, has certain toxicity, such as calcium carbide slag with strong alkaline and heavy metal risk. Therefore, it is necessary to evaluate the risk of heavy metal release through a leaching toxicity test and add a curing agent for stabilization before using this type of adsorption material [57]. The toxicity of fly ash, gypsum, and waste glass powder is relatively low and can be directly used in experiments after physical separation and high-temperature treatment [58]. In addition, industrial wastewater can be pretreated according to the respective properties of solid waste to reduce the possibility of secondary pollution.

With water pollution becoming increasingly severe, traditional single-material adsorption methods are facing problems such as low treatment efficiency and limited adsorption capacity. Consequently, the application of composite materials in water treatment has attracted increasing attention. Composite materials, composed of two or more distinct materials, aim to exert the synergistic effect between the components, thereby providing superior performance compared to single material [59,60]. In recent years, composite materials have demonstrated significant potential in removing GO from water and have become a research hotspot for innovative water treatment materials.

Composite materials can significantly enhance their adsorption capacity for GO by integrating different types of adsorbents. For example, combining clay minerals with carbon-based materials (such as activated carbon, graphene, etc.) can effectively increase the specific surface area of​the composite material, thus providing more adsorption sites and improving the adsorption efficiency. Additionally, the multifunctionality of composite materials is another key advantage [61]. Besides adsorption, many composites possess additional functionalities such as catalytic degradation, antibacterial, and antioxidant properties. For instance, the combination of metal oxides and clay minerals can not only enhance GO adsorption capacity but also decompose the structure of GO through catalytic degradation reactions, thereby reducing its long-term environmental impact. This dual functionality not only improves treatment efficiency but also helps mitigate secondary pollution from pollutants.

Furthermore, the natural degradability of composite materials is another outstanding advantage. Many composite materials (such as biomass materials, natural minerals, etc.) are naturally degradable, which makes their use in water treatment processes more environmentally friendly. By developing such degradable composite adsorbents, efficient removal of GO from water can be achieved while avoiding environmental burdens caused by material accumulation. These materials can degrade naturally or be broken down by environmental microorganisms after treatment, preventing secondary pollution associated with traditional adsorbents. The versatility, enhanced adsorption performance, and environmentally friendly and degradable characteristics make them have broad application prospects in future water treatment technologies. As research into composite materials advances, they are expected to play an increasingly important role in GO removal and provide effective solutions for water environment protection.

7. Conclusions

GO, as a novel nanomaterial characterized by significant hydrophilicity and a large specific surface area, exhibits extensive application potential in aqueous environments. However, due to its high dispersion, chemical stability, and difficulty in degradation, GO-induced water pollution has emerged as an urgent global environmental challenge that requires immediate attention. To address this issue, clay minerals and solid waste have been explored as effective adsorbents for GO removal. These materials are favored for their natural renewability, low cost, non-toxicity, and environmental friendliness. This article reviews relevant literature and experimental results, evaluates the performance of different clay minerals (such as illite and sepiolite) and solid wastes (such as BSP, iron tailings) in removing GO from water, and explores their underlying adsorption mechanisms. The main research findings are summarized as follows:

  • (1)

    Clay minerals and solid waste can efficiently remove GO. Illite, sepiolite, BSP and other materials have excellent adsorption capacity for GO, and the highest removal rate is 99%. The adsorption mechanism involves charge interaction, hydrogen bonding, and complexation, and the adsorption properties are affected by pH, temperature, and other factors.

  • (2)

    The adsorption process is controlled by kinetics and thermodynamics. The GO adsorption mostly conforms to quasi-second-order kinetics and the Langmuir isothermal model and is mainly monolayer chemisorbed. The adsorption process of most materials is a spontaneous endothermic reaction, and the increase in temperature helps to improve the adsorption effect.

  • (3)

    The adsorption of GO by clay minerals and solid wastes has practical significance in industry. By converting industrial waste into highly efficient adsorbents, developing adaptive adsorption systems and recycling technologies, and combining with the resource path, the problem of GO pollution can be solved on a large scale, and green, low-carbon transformation and sustainable development in the field of water treatment can be promoted.

  • (4)

    The composite material can improve the adsorption and degradation performance. The combination of clay minerals and solid waste with carbon-based materials or metal oxides enhances adsorption capacity and imparts catalytic degradation, enabling more efficient GO removal and reducing long-term environmental impacts.

Acknowledgment

This work was supported by the National Natural Science Foundation of China (52179107, 52478364), and the Scientific Research Fund of Yancheng Polytechnic College (ygy2007).

CRediT authorship contribution statement

Jiajia Fu: Original draft writing, investigation. Wei Wang: Review and edit the draft, methodology. Yingdi Pang: Original draft writing, validation. Mengqi Xu: Conceptualization, visualization. Yani Shi: Methodology, visualization. Jinhua Ding: Investigation, validation. Na Li: Review and edit the draft, validation. All authors have read and approved the final manuscript.

Declaration of competing interest

The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

Declaration of Generative AI and AI-assisted technologies in the writing process

The authors confirm that there was no use of artificial intelligence (AI)-assisted technology for assisting in the writing or editing of the manuscript and no images were manipulated using AI.

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