Dispersibility of graphene-family materials and their impact on the properties of cement-based materials: Application challenges and prospects
-
Hongyan Zeng
,
Shen Qu
Abstract
Graphene-family materials (GFMs), like graphene, graphene oxide, and reduced graphene oxide, have demonstrated remarkable potential in enhancing the performance of cement-based materials (CBMs). This promise is attributed to their distinctive two-dimensional nanostructure and outstanding mechanical, electrical, and thermal properties. Nevertheless, the inherent interlamellar π–π stacking and hydrogen bonding interactions severely compromise their dispersibility within cement matrix, thereby making the limit reinforcing efficacy for CBMs. Although researchers have dedicated substantial efforts for improving dispersibility, primarily through physical treatment and chemical modification, challenges in functionalization techniques and characterization methods have hampered the achievement of satisfactory dispersion in cement matrix. To address this issue, this review systematically summarized optimization strategies for improving dispersibility of GFMs, and the characterization methods for evaluating their dispersibility within the cement matrix. By examining the impact of dispersibility of GFMs on properties of CBMs, this study further delves into the underlying dispersion mechanisms and proves synthetic approach more effective when applicating GFMs into CBMs. Drawing upon these insights, the review critically examines the challenges and prospects associated with dispersing GFMs in CBMs uniformly, with a focus on interaction mechanisms, characterization technique, test standardization, and cost effectiveness.
1 Introduction
Graphene-family materials (GFMs) have garnered substantial attention owing to their remarkable mechanical, electrical, and thermal properties [1–3]. These exceptional attributes make them promising additives for enhancing the performance of various materials, including cement-based materials (CBMs) [4]. The incorporation of GFMs into CBMs holds the potential to substantially improve their mechanical strength and durability [5–7]. More importantly, this incorporation creates a conductive network within the cement matrix, enabling the CBMs to exhibit self-sensing capabilities. Specifically, GFMs can form conductive networks where mechanical deformation or crack propagation alters network connectivity and interlayer spacing, generating detectable electrical resistance fluctuations that enable structural health monitoring. Such enhancements can result in denser microstructures, extended service life, and reduced maintenance costs. Notably, one of the challenges in utilizing GFMs into CBMs is their poor dispersibility. The inherent interlamellar π–π stacking and hydrogen bonding interactions severely hinder their dispersibility, leading to agglomeration that weakens reinforcement effects for CBMs [8–10]. Consequently, the performance improvements are highly dependent on the dispersibility of graphene within the cement matrix.
To address this challenge, researchers have developed various modification strategies from both physical and chemical perspectives. Regarding chemical methods, studies have shown that the dispersibility of GFMs can be significantly enhanced through covalent or non-covalent modifications, which create an energy barrier to prevent aggregation [11,12]. For instance, covalent modifications typically involve the introduction of functional groups onto the surface of graphene, such as carboxyl, hydroxyl, or amine groups. These functional groups have the capability to establish chemical bonds with the constituents of cement, thereby augmenting the compatibility of graphene dispersed into the cement matrix [13–15]. This improved interaction has the potential to enhance mechanical properties and durability of CBMs. By contrast, non-covalent modifications employ surfactants such as sodium dodecyl sulfate, polyethylene glycol, and polyvinylpyrrolidone, or polymers like polyacrylic acid and polystyrene sulfonate to stabilize graphene dispersions [16–19]. These agents adsorb onto the graphene surface, affording electrostatic or steric repulsion that inhibits the aggregation of graphene sheets. This approach preserves the original structure and properties of graphene while substantially enhancing its dispersibility and uniformity in aqueous or organic solvent systems. Accordingly, as reported by Wang and Zhao [20], non-covalent modifications not only enhance graphene dispersion but also contribute to improved mechanical properties and durability when incorporated into CBMs. Despite these advancements, achieving desirable dispersibility remains challenging owing to the complexity of functionalization processes and the requirement for precise characterization methodologies. Fortunately, certain physical means, such as ultrasonic treatment, ball milling, and stirring, are commonly employed to complement chemical modifications and further improve graphene dispersion [21–23]. The synthetic method, integrating physical approaches, covalent modification, and non-covalent functionalization, provides promising strategies to improve the dispersibility, thereby enabling their widespread application in various fields [24].
Characterization techniques are crucial for assessing the efficacy of modification strategies and possess significant potential for uncovering the mechanisms underlying aggregation phenomena, particularly for CBMs modified by GFMs [25]. Directly characterizing GFMs’ dispersion state within the cement matrix remains challenging due to the very small nanomaterial dosage employed in CBMs. Thus, GFMs are typically dispersed in water before being mixed with cement, rendering their aqueous dispersibility a widely adopted proxy. Furthermore, a saturated Ca(OH)2 solution, which mimics the highly alkaline milieu of cement matrix micropores, is frequently utilized as the dispersant for GFMs when investigating their dispersibility within the matrix [26]. With the rapid progression of nano-characterization techniques, various methods have been employed to evaluate the dispersibility of GFMs within the cement matrix [27,28]. Microscopy techniques such as transmission electron microscopy (TEM) and scanning electron microscopy (SEM) are commonly employed to visualize morphology and the GFMs’ dispersion state [29,30]. These techniques afford high-resolution images, enabling researchers to visually characterize the distribution of GFMs throughout the cement matrix. Dynamic light scattering (DLS) is widely used to measure the particle size distribution of GFMs in water, offering valuable insights into their dispersibility [31]. Additionally, Raman spectroscopy yields critical information on the number of graphene layers and defect presence, while UV-Vis spectroscopy indicates dispersibility through shifts in absorption peak positions and intensities variations [32,33]. By integrating these complementary characterization techniques, researchers can comprehensively and systematically evaluate the dispersibility of GFMs, thereby establishing a robust scientific basis for optimizing their applications in CBMs.
Overall, incorporating GFMs into CBMs faces several key challenges, including the development of scalable dispersion methods, enhancement of dispersion stability, assurance of precise characterization, and realization of significant performance improvements. This review seeks to explore the key issues relating to the application of GFMs in CBMs. A systematic summary of various dispersion techniques and characterization methods is provided. By examining the impact of GFMs’ dispersibility on CBM properties, this review further explores the research challenges. Moreover, it highlights potential strategies and future prospects for improving the dispersibility of GFMs and their application in CBMs.
2 Dispersion techniques for GFMs within the cement matrix
While GFMs comprise a multitude of types, three primary variants (graphene, graphene oxide [GO], and reduced graphene oxide [rGO]) predominate in applications within CBMs, with their structural disparities governing distinct dispersibility characteristics. As illustrated in Figure 1, GO is synthesized via the exfoliation of graphite oxide, whereas rGO is derived from the reduction of GO [35]. Owing to the abundance of oxygen-containing functional groups on its surface, GO demonstrates excellent dispersibility in water. However, it tends to agglomerate in the cement matrix due to interactions with metal cations [36]. Consequently, GO dispersion is primarily enhanced by increasing steric hindrance and electrostatic repulsion. In contrast, graphene lacks these hydrophilic groups and exhibits strong intermolecular forces (π–π stacking), which lead to facile agglomeration in water and inferior dispersibility compared to GO [37,38]. Although rGO retains residual oxygen-containing functional groups on its surface, it displays dispersibility comparable to that of graphene [10]. To optimize the dispersibility of graphene within the cement matrix, researchers frequently employ various dispersion techniques, including physical modifications, chemical modifications, or a combination of both. Table 1 summarizes the advantages and disadvantages of these primary dispersion techniques. Understanding these distinctions is crucial for selecting and applying the most appropriate technique. The details are discussed here.
![Figure 1
Structures of graphene-family products [34].](/document/doi/10.1515/rams-2025-0147/asset/graphic/j_rams-2025-0147_fig_001.jpg)
Structures of graphene-family products [34].
Comparisons of three dispersion techniques
| Techniques | Advantages | Disadvantages |
|---|---|---|
| Physical modification |
|
|
| Chemical functionalization |
|
|
| Combined method |
|
|
2.1 Physical modification
Physical modification refers to mechanically separate agglomerated GFMs without chemical reactions [39]. This technique enhances the quality of GFMs’ dispersions by breaking down the agglomerates into individual flakes with fewer layers and smaller lateral size, thereby improving their uniformity [24]. Generally, physical modification methods include stirring [40], ball milling [41], ultrasonic treatment [42], high shear mixing [43], extrusion [44], and microwave processing [45]. However, when dispersing GFMs into CBMs, stirring, ball milling, and ultrasonic treatment are usually preferred. This is because the dispersion process typically uses either water or a saturated Ca(OH)2 solution as the solvent [26].
The stirring treatment, including friction stirring and magnetic stirring, generates shear force that effectively disperses GFMs. For instance, friction stir processing can disperse graphene well in a metal matrix, especially in an aluminum matrix [46]. The thermal conductivity of graphene/aluminum composites can be improved by over 15% compared to the aluminum matrix due to friction stir processing [39,47]. Increasing the number of stirring passes and optimizing the ratio of stirring to welding velocity can induce significant plastic strain, thereby evenly dispersing graphene and improving the strength of graphene/aluminum composites [48]. In contrast, magnetic stirring processing can produce uniform aqueous suspensions of graphene without frequent human intervention, which greatly increases productivity. Puglia et al. [49] utilized a standard benchtop magnetic stirrer to achieve record concentrations of high-quality aqueous graphene suspensions, with a 100% efficient conversion rate by optimizing systematic parameters such as pH, protein concentration, temperature, stirrer speed, and solution volume.
Unlike stirring, ball-milling applies not only shear forces to GFMs but also generates vertical impacts and collisions with brittle balls. This breaks apart GFMs and prevents their agglomeration [50]. For example, GO prepared by solid-state ball milling disperses readily in water and organic solvents. This significantly improves cement paste’s compressive strength and hydration heat without altering GO’s structure [51]. However, ball milling can damage the structural integrity of GFMs. Temperature, duration, and rotation speed are critical settings requiring careful optimization for effective dispersion [52–54]. Despite this, ball milling remains promising since the ball-milling agent can be washed away with water or solvents. Yet studies confirm mechanical dispersion alone is often inadequate. Thus, combining ball milling with chemical methods typically yields optimal results.
Compared to alternative dispersion techniques, ultrasonication is a simpler and more promising way to spread GFMs. This method effectively lowers surface energy and improves how well graphene mixes in the cement matrix [55]. It works through powerful sound waves that create bubbles and vibrations (ultrasonic cavitation and oscillations). This energy overcomes the forces holding GFMs together, keeping their dispersion stable [22]. While researchers agree that ultrasonication improves dispersibility of GFMs, different settings are used depending on factors like effectiveness, speed, and cost. For mixing graphene into cement, key factors like the amount of chemical dispersant added and the ultrasound time are adjusted. Dispersant dosage and ultrasonication time are commonly optimized to achieve effective dispersion of graphene/cement composites [56,57]. For example, studies show that 1 h of sonication with 15% dispersant creates a stable mixture containing 1% graphene, lasting 6 h [58]. Ultrasonication was found to work better than simple mechanical mixing for graphene-cement blends. However, mechanical mixing is cheaper and easier, making it more practical for large projects [59]. To determine the stability of hydrothermally produced rGO, three types of sonication were tested: bath sonication (200 W, 35 kHz), horn sonication (750 W, 20 kHz), and high-power microtip sonication (1,000 W, 20 kHz) [60]. Notably, horn sonication achieved the most stable rGO dispersion, maintaining stability for up to 2 years by providing the optimal power intensity for dispersion. In contrast, high-power microtip sonication, despite delivering greater power intensity, failed to produce a stable rGO dispersion because the energy supplied exceeded the optimal level, resulting in instability.
Physical dispersion methods, while advantageous for their simplicity and accessibility, present limitations for dispersing GFMs in CBMs. These methods may compromise the nanostructure of GFMs, leading to inhibit the improvement effect for the modified CBMs. Microscopic analysis reveals that the sonication time and/or power affected the oxygen content on exfoliated graphene, since extended ultrasonication resulted in a decrease in the oxygen content on exfoliated graphene, with a simultaneous increase in defected sp3 carbon atoms [52]. This outcome suggests that ultrasonication not only enhances the dispersibility of graphene but also induces structural defects, with more pronounced effects observed at extended sonication durations and higher power levels [52,61]. Furthermore, ultrasonic treatment commonly elevates the temperature of the dispersion. If this heated dispersion is immediately mixed with cement, it can disrupt the cement hydration process [6]. The defects generated during physical dispersion, primarily due to mechanical energy input, are largely irreversible and severely diminish graphene’s reinforcing efficacy within the matrix. In conclusion, despite their straightforward nature and equipment availability, physical dispersion methods are typically employed only as auxiliary techniques alongside other dispersion strategies to mitigate these drawbacks.
2.2 Chemical functionalization
Chemical functionalization methods for graphene comprise two primary categories: covalent and non-covalent functionalization. Covalent functionalization establishes strong, stable bonds via direct chemical reactions with carbon atoms in the graphene lattice, enhancing material properties and facilitating integration into the cement matrix. In contrast, non-covalent functionalization relies on molecular adsorption through weaker interactions, such as π–π stacking, van der Waals forces, and hydrogen bonding, preserving graphene’ intrinsic electrical, thermal, and mechanical properties. This preservation makes them suitable for applications requiring high-performance characteristics. Comprehensive reviews of graphene functionalization are available elsewhere [15]. This section specifically summarizes common functionalization strategies employed to improve dispersibility of GFMs within the cement matrix.
The covalent bonding method leverages functional groups on organic molecules to graft onto or remove surface functionalities from graphene, enhancing steric hindrance and strengthening covalent interactions with the cement matrix [11]. This process involves sp² to sp3 hybridization conversion of carbon atoms within the graphene lattice, enabling diverse functionalization. Consequently, covalent modification is frequently used to prepare graphene dispersion with fewer layers, smaller particle sizes, and uniform dispersion [62]. Table 2 summarizes the reaction mechanism and comparative advantages of common covalent functionalization methods classified by reaction type. Notably, covalent methods exhibit significant variation across GFMs. For graphene, non-covalent modifiers are generally preferred over covalent approaches since they often must be used during the exfoliation of graphite [75,76]. Although GO serves as an excellent candidate for covalent functionalization because of its high functionality, the precise identity and distribution of the oxygen-containing groups remain debated [77]. It is generally believed that GO contains epoxide, ether, aldehyde, ketone, alcohol, and carboxylic acid groups on its surface [78–80]. This variety of groups allows for different reactions and chemistries to be used to covalently functionalize graphite oxide. When modifying reduced rGO, reaction strategies resemble those for pristine graphene rather than GO, as oxygen functionalities are substantially removed. However, it is still possible to add functionality to the residual oxygen-containing groups present on the material, thereby diazonium chemistry is considered as one of the most efficient approaches for covalently functionalizing rGO [75,76].
Covalent bonding methods of graphene based on different reaction types
| Reaction type | Mechanism and advantages | Ref. |
|---|---|---|
| Radical reactions |
|
[15,63–66] |
| Cycloaddition reactions |
|
[67–71] |
| Single atom introduction |
|
[72–74] |
Compared to covalent modification, non-covalent modification offers several advantages, including the absence of hazardous chemistry, a wide range of commercially available modifiers, and the preservation of the graphene sp2 network. Consequently, non-covalent modification is well-suited for pristine graphene and graphene. Among all non-covalent modifiers, surfactants appear to be the most promising, especially for improving the dispersibility of graphene within the cement matrix. Surfactants that are usually used to improve the graphene dispersion can be divided into two categories. Table 3 compares these surfactants and details their advantages and disadvantages. No matter what kind of surfactants, non-covalent interactions will involve hydrogen bond-π, π–π, cation-π, and hydrophobic effects, with the principal interactions for dispersion being π–π, cation-π, and hydrophobic effects. It can enhance the steric hindrance between nanosheets primarily through the stacking interactions of surfactants and graphene’s π–π bonds. Additionally, some surfactants introduce a negative charge to the surface of graphene, which prevents agglomeration by increasing electrostatic repulsion, thereby improving dispersibility. Table 3 also indicates that PCs is widely accepted as the surfactant to improve the dispersibility of graphene/cement composites. However, some studies exhibit different opinions. Polycarboxylate-ether has been proved to enhance the GO dispersion, but it cannot eliminate the agglomeration, thus its effect on improving the dispersibility of graphene/cement composites is very limited [100]. Although surfactants are predominantly employed to enhance the dispersibility of GFMs in water, their effectiveness in cement matrix is compromised by the highly alkaline pore solution [93,101,102]. Under this condition, the effectiveness of surfactants in dispersion diminishes, and certain surfactants may negatively affect cement hydration or matrix properties. Consequently, further research into optimizing the dispersibility of GFMs in CBMs remains necessary.
Commonly used surfactants for dispersing GFMs within cement matrix
| Type | Surfactants | Advantages | Disadvantages |
|---|---|---|---|
| Mineral admixtures | Silica fume |
|
|
| [81–83]/ | |||
| Fly ash | |||
| [84–87]/ | |||
| Metakaolin [88–90] | |||
| Chemical admixtures | Sodium dodecylbenzene sulfonate (SDBS) |
|
|
| [31,91,92]/ | |||
| Polycarboxylate | |||
| superplasticizer (PCs) [93–98]/ | |||
| Methylcellulose [99] |
In summary, covalent functionalization represents the predominant chemical dispersion strategy for graphene, owing to its key advantages: precise controllability, enhanced stability, and seamless integration into manufacturing processes. This approach achieves effective graphene dispersion through robust covalent bonding, ensuring long-term stability and uniformity. Simultaneously, it enables precise modification of GFMs, facilitating integration into diverse manufacturing systems. However, its efficacy varies significantly with graphene type. While covalent functionalization excels with most GFMs, it falls short when dealing with pristine graphene. The need to preserve graphene’s intrinsic properties during exfoliation makes non-covalent functionalization a more appropriate choice for pristine graphene. Non-covalent methods, such as π–π stacking interactions, van der Waals forces, and hydrogen bonding, maintain the structural integrity and superior properties of graphene, making them indispensable for applications requiring high-performance materials. Each method has its advantages and limitations, and the choice between covalent and non-covalent functionalization depends on the specific requirements of the application and the type of graphene being used. Notably, functionalization often involves synergistic interactions between multiple mechanisms, necessitating further fundamental research.
2.3 Synthetical method
Synthesis method integrates physical modifications with chemical functionalization, achieving more homogeneous dispersion than either approach alone. Consequently, it represents the most widely adopted and effective strategy for enhancing dispersibility of GFMs within cement matrix. To enhance the mechanical and piezoresistive properties of cement mortar, Zhou et al. [103] dispersed graphene nanoplatelets (GNPs) using polyvinyl pyrrolidone (PVP) surfactant combined with high-speed shear and probe ultrasonication (130 W, 20 kHz). Their parameter optimization confirmed PVP’s effectiveness in stabilizing nanoplatelets, leading to 54.5 and 36.9% improvements in flexural and compressive strength, respectively. The dispersion parameters, including surfactant concentration, ultrasonication time, shear time, and rate, were carefully optimized. Papanikolaou et al. [104] dispersed multi-layer GNPs using bath sonication (40 kHz) with four superplasticizers: lignosulphonate, naphthalene-based, and two polycarboxylates. They demonstrated that sonication alone was insufficient, and polycarboxylates, which provide steric hindrance to separate nanoplatelet from cement increased compressive strength by 15% vs lignosulphonate/naphthalene-based, with optimal dispersion stability. Wang et al. [105] investigated flash graphene dispersion in cement pastes comparing: (i) polycarboxylate superplasticizer (PCs) + probe ultrasonication (400 W, 20 kHz), (ii) dry-mixing with PCs, and (iii) mechanical stirring with PCs. Their results showed that the combined PCs-ultrasonication method reduced viscosity by 42% and increased 28-day compressive strength by 22.1%, confirming its superiority for homogeneous FG dispersion and rheological control.
Beyond synthesis methods, researchers increasingly focus on the effects of oxygen content and particle size of GFMs on their dispersibility in CBMs. Using GO as an example, its particle size and oxygen content are found to be closely related to dispersibility. As Figure 2 demonstrates, small-sized GO achieves rapid and uniform dispersion in molten caprolactam after minimal sonication, while other larger GO sheets exhibit persistent aggregation even after extended sonication. This visual comparison directly confirms that reduced lateral dimensions critically enhance GO dispersibility in polymer-compatible media [106]. Furthermore, while graphene with maximal oxygen content tends to aggregate, functionalized graphene with 5% oxygen content obtained remarkable improvement on cement strength of CBMs. This optimal performance stems from balanced surface polar groups that promote effective dispersion and interaction with hydrated cement [107]. As a result, graphene polarity governs both aqueous dispersion and chemical interactions with cement matrices, a finding corroborated by studies using GO additives [108,109]. Additionally, an optimal dispersion treatment process is also necessary to uniformly disperse GO. Yan et al. [110] evaluated the impact of treatment process on the dispersibility of GO by adding superplasticizers at different ultrasonic dispersion times. The results showed that adding superplasticizers at 0 min resulted in poorer dispersibility compared to the GO solution subjected to ultrasonic treatment alone. That is because the long chains in superplasticizers molecules wrap around GO aggregates, making it difficult to fully separate them during ultrasonic process. In contrast, when the superplasticizers were added at 30 min, the original GO aggregates had already been partially separated. In this case, the distance between GO was large enough to allow the superplasticizers to penetrate the gaps among them. Consequently, superplasticizers absorbed onto the surface of GO separated them through steric hindrance, maintaining uniform dispersion in the 30 min group, as illustrated in Figure 3.
![Figure 2
Dispersibility of different sized GOs in caprolactam melt at 90°C for different sonication time [106].](/document/doi/10.1515/rams-2025-0147/asset/graphic/j_rams-2025-0147_fig_002.jpg)
Dispersibility of different sized GOs in caprolactam melt at 90°C for different sonication time [106].
![Figure 3
SP-assisted dispersion mechanism under different processes: (a) Reference; (b) 0 min; (c) 15 min; (d) 30 min [110].](/document/doi/10.1515/rams-2025-0147/asset/graphic/j_rams-2025-0147_fig_003.jpg)
SP-assisted dispersion mechanism under different processes: (a) Reference; (b) 0 min; (c) 15 min; (d) 30 min [110].
3 Characterization methods for GFMs dispersions
When graphene-family suspensions are incorporated into cement, they may exhibit distinct states, including well-dispersed, grain-adsorbed, and self-agglomerated. To characterize these states, various analytical methods have been developed with advancements in nanotechnology, including microscopy techniques and spectroscopy techniques. However, direct characterization within the cement matrix remains challenging due to the significant disparity in dosage and material size between GFMs and CBMs. Consequently, their dispersibility is frequently evaluated in surrogate environments (e.g., water or Ca(OH)2 solution, which mimics cement pore conditions) [111]. This section critically examines the application of these characterization methods and discusses their respective advantages and limitations.
3.1 Microscopy techniques
Microscopy techniques are employed to study and analyze the structure, morphology, and properties of GFMs’ dispersions at micro- and nanometer scales. Commonly used methods include SEM, TEM, and atomic force microscopy (AFM). Although all three techniques can be utilized to investigate the distribution, surface morphology, internal structure, and mechanical properties of graphene with high resolution, they each play distinct roles in characterizing dispersibility of GFMs within the cement matrix.
3.1.1 SEM
SEM is a powerful tool for characterizing the surface morphology and distribution of GFMs within the cement matrix. Its high-resolution imaging capabilities bridge microscopic features with macroscopic properties, enabling direct observation of dispersion states including well-dispersed, grain-adsorbed, and self-agglomerated configurations. SEM analysis reveals critical aspects such as dispersion homogeneity, material orientation, and interaction mechanisms with cement particles. For instance, Figure 4 demonstrates that incorporating 15% silica fume significantly reduces graphene agglomerate size from 100 to 20 μm. The images indicate silica fume particles intercalating between graphene layers, disrupting interfacial interactions and enhancing dispersion during mixing [112]. Furthermore, extensive SEM studies have elucidated dispersion mechanisms of GFMs in cement systems and their impacts on hydration kinetics and performance of CBMs [104,113,114]. Quantitative evidence confirms that optimal dispersion enhances mechanical properties: cement mortars with 0.03% graphene exhibited 28-day compressive strength increases of 17.5% (ultrasonication/surfactant) and 13.7% (mechanical stirring/surfactant), with SEM verifying graphene embedment within the matrix [59]. Such uniform dispersion, achievable with surfactants like sodium dodecyl benzene sulfonate, promotes hydration reactions and inhibits crack propagation [115].
![Figure 4
SEM images of 1-day cured graphene/cement pastes with varying silica fume content: (a) 0% silica fume and (b)–(d) 15% silica fume [112].](/document/doi/10.1515/rams-2025-0147/asset/graphic/j_rams-2025-0147_fig_004.jpg)
SEM images of 1-day cured graphene/cement pastes with varying silica fume content: (a) 0% silica fume and (b)–(d) 15% silica fume [112].
While SEM provides high-resolution images for detailed visualization of graphene-family distribution within the cement matrix, it has notable limitations. SEM primarily provides microstructural information at a highly magnified point, lacking the capability to reveal the overall dispersion across the entire GFMs-modified CBMs. Furthermore, SEM may struggle to detect GFMs due to nanoscale dimensions relative to the cement matrix phases, particularly when unevenly dispersed or incorporated in low nano dosage. Due to these limitations, SEM alone is insufficient for a comprehensive understanding of GFMs’ dispersions. To fully assess the dispersion quality, additional characterization techniques are required.
3.1.2 TEM
Like SEM, TEM can also provide high-resolution images to analyze GFMs’ dispersions and examine their distribution within the cement matrix. However, this technique works by transmitting a focused beam of high-energy electrons through an ultra-thin sample to create highly detailed images based on the interactions of the electrons with the sample’s internal structure. It excels at analyzing thickness, defects, crystal structure, and stacking order of individual graphene nanosheets, and is particularly capable of providing two-dimensional images that reveal the internal arrangement and detail atomic structure of GFMs’ dispersions. TEM analysis of dispersed graphene confirmed the successful exfoliation of graphite using sodium dodecyl sulfate, producing a mixture of monolayer and multilayer graphene sheets [116]. Figure 5 identifies monolayer graphene edges, demarcated by blue and red lines. The graphene exhibited lateral dimensions exceeding 1 μm. In contrast, TEM images of rGO revealed wrinkled, partially bent multilayer nanosheets with lateral dimensions in the micrometer range. As the application of GFMs in CBMs increases, other studies related to GFMs’ dispersions characterized by TEM techniques are also on the rise [29,117–120]. On this basis, TEM is typically used to characterize the dispersibility of GFMs in water or cement pore solutions.
![Figure 5
TEM images of graphene obtained by the aqueous phase dispersion technique and the Hummer method [116].](/document/doi/10.1515/rams-2025-0147/asset/graphic/j_rams-2025-0147_fig_005.jpg)
TEM images of graphene obtained by the aqueous phase dispersion technique and the Hummer method [116].
However, TEM characterization faces several inherent limitations. The primary challenge lies in sample preparation: depositing GFMs’ dispersions onto TEM grids typically involves drying, which may induce aggregation or restacking that misrepresents the original dispersion state. Additionally, the vacuum environment required for TEM operation can cause the evaporation of solvents, potentially altering the dispersion state of GFMs. Moreover, the small field of view in TEM limits the ability to obtain statistically significant data on the dispersion state, as it may not be representative of the entire sample. Therefore, while TEM provides valuable insights, these limitations must be carefully considered when interpreting results regarding the dispersibility of GFMs within the cement matrix.
3.1.3 AFM
AFM is a high-resolution imaging technique that assesses the dispersion state of GFMs in solutions by scanning a sharp tip across the sample surface. The fundamental principle of AFM involves scanning a sharp tip, typically made of silicon or silicon nitride, across the surface of sample. As the tip moves, it interacts with the surface forces, causing the cantilever to deflect. These deflections are measured using a laser beam reflected off the top of the cantilever into a photo detector. The resulting data are then processed to generate a topographical map of the sample surface at the nanoscale.
In contrast to conventional electron microscopy, AFM offers significant advantages for characterizing GFMs’ dispersions due to its operational capability in ambient and liquid environments, preserving the native dispersion state. First, this capability enables direct nanoscale observation of dispersion state, providing accurate information about their lateral dimensions, thickness, and overall morphology without the need for extensive sample preparation that could alter the original dispersion state [121–124]. Luo et al. [125] reported an efficient “surfactant”-GO that effectively disperses graphene through π–π interactions in acidic aqueous solutions, without the need for any additives. As demonstrated in Figure 6 AFM analysis, they found that GO’s size is significantly larger in acidic solutions due to agglomeration. GO tends to aggregate into bilayer stacks with a thickness of approximately 2 nm in acidic solutions, while it disperses evenly as monolayers with a thickness of about 1 nm in slightly acidic solutions. Conversely, in alkaline solutions, GO’s size remains like that under slightly acidic conditions, but the average thickness increases, suggesting the formation of multilayer nanosheet stacks. Second, AFM can provide detailed information on the surface topography and roughness of graphene-family/cement composites, which is crucial for understanding the state of dispersion. It can accurately measure the thickness and size of graphene sheets, facilitating a more precise assessment of their distribution within the cement matrix [126]. For example, a detailed characterization using both TEM and AFM suggested that graphene which consists of a limited number of layers has an average size of approximately 3.2 μm [125]. Furthermore, AFM can detect the interaction between GFMs and cement matrix, providing insights into the mechanisms of CBMs improved by GFMs [123,127].
![Figure 6
AFM images of GO in solutions with different pH values: (a) acidic (pH = 2), (b) slightly acidic (pH = 6), and (c) alkaline (pH = 12) [125].](/document/doi/10.1515/rams-2025-0147/asset/graphic/j_rams-2025-0147_fig_006.jpg)
AFM images of GO in solutions with different pH values: (a) acidic (pH = 2), (b) slightly acidic (pH = 6), and (c) alkaline (pH = 12) [125].
While AFM provides high-resolution surface characterization, it cannot fully resolve the three-dimensional distribution of GFMs within cement matrix. The technique also struggles to distinguish closely stacked graphene layers or detect small sheets. Additionally, sample preparation may affect dispersion characterization, particularly when capturing thin or small GFMs. Given these limitations, reliance on any single characterization method proves inadequate. Consequently, complementary techniques are typically integrated to comprehensively assess dispersibility of GFMs in CBMs [128–131].
3.2 Spectroscopy techniques
Spectroscopic techniques, including UV-visible (UV-Vis), Fourier-transform infrared (FTIR), and Raman spectroscopy, provide complementary approaches for characterizing the dispersibility of GFMs within the cement matrix. Their key applications and distinctive capabilities are discussed here.
3.2.1 UV-Vis spectroscopy
UV-Vis spectroscopy is a widely employed analytical technique based on the absorption or transmission of ultraviolet and visible light by a material as a function of wavelength. This technique leverages the principle that molecules or particles interact with light at specific wavelengths corresponding to electronic transitions, providing a unique spectral fingerprint [132]. For GFMs’ dispersions, UV-Visible is utilized to monitor the uniformity of dispersion by analyzing the absorption spectra, which reflects the extent of agglomeration or disaggregation of GFMs [133]. This capability facilitates optimization of dispersion protocols and interrogation of graphene-cement matrix interactions. Empirical evidence confirms UV-Vis efficacy in evaluating dispersion enhancements achieved via various methods [95,134–136]. As depicted in Figure 7, the resulting spectroscopy reveals two distinct characteristic absorption peaks when ultrasonic treatment is combined with PCs as the dispersion method. The primary absorption peak, attributed to the π → π* transitions of C═C bonds, is observed near 230 nm, while a weaker peak, corresponding to the n → π* transitions of carboxyl group, appears around 300 nm [137]. A higher absorption peak in the GO dispersion indicates a greater concentration of GO, reflecting effective dispersion, particularly when ultrasonic and PCs are employed.
![Figure 7
UV-Vis spectra of the different GO dispersion solutions [137].](/document/doi/10.1515/rams-2025-0147/asset/graphic/j_rams-2025-0147_fig_007.jpg)
UV-Vis spectra of the different GO dispersion solutions [137].
Although UV-Vis spectroscopy offers a convenient, non-destructive approach for assessing GFMs’ dispersions, its application to CBMs faces significant limitations due to light scattering, opacity, and inadequate spatial resolution. Light scattering effects in cement suspensions substantially compromise the measurement accuracy. Cement particles, which are heterogeneous and of varying sizes, scatter light and interfere with GFMs’ absorbance signals, and this effect is more prominent with increasing cement particle concentration, resulting in distorted or unreliable spectra. Additionally, the inherent gray or dark coloration of cement further absorbs and scatters light, obscuring GFMs’ characteristic absorption peaks and complicating the accurate assessment of its content and dispersion state. As low GFMs dosages, weak absorption signals become obscured by background interference from impurities, presenting particular challenges for precise analysis.
3.2.2 FTIR
FTIR identifies functional groups and chemical bonds by measuring material-specific infrared absorption. This technique provides critical insights into molecular structures and interfacial interactions of GFMs, making it essential for characterizing their dispersion behavior and chemical compatibility within the cement matrix.
FTIR can identify functional groups on the surface of GFMs, such as hydroxyl (–OH), carboxyl (–COOH), or epoxy (–C–O–C) groups [138–140]. These groups play a critical role in determining the compatibility and interaction between GFMs and cement hydration products. As demonstrated in Figure 8, the area size of the C–S–H IR peak for GO-doped cement is dependent on curing methods: microwave cured GO-cement > both water and microwave cured GO-cement > water cured GO-cement > GO-cement. The 1,629 cm−1 absorption peak in GO indicates the presence of alkene bonds. By contrast, the IR peaks at 3,300 and 1,735 cm−1 confirm hydroxyl (–OH) and carbonyl (C═O) groups, indicating the presence of –COOH group [141]. Critically, uniform dispersions of GFMs reduce agglomeration, yielding enhanced spectral resolution with reduced noise interference in FTIR analysis. Consequently, improved dispersions correlate directly with targeted chemical functionalization of GFMs, as evidenced by distinct FTIR spectral signatures. Moreover, FTIR can help assess the role of GFMs during cement hydration reaction [142–145]. For instance, GO can significantly accelerate the cement hydration rate since its oxygen-containing functional groups offer adsorption sites for water molecules and cement components [146]. While FTIR effectively identifies functional groups and their role in the hydration process, it lacks the spatial resolution needed to directly evaluate the uniformity of graphene distribution within the cement matrix. Additionally, signal overlaps from the complex matrix of cement hydration products can obscure subtle changes related to GFMs. These limitations suggest that FTIR necessitates complementing FTIR with other analytical techniques to achieve robust characterization of GFMs’ dispersions.
![Figure 8
FTIR spectrum of (a) 0.5 wt% GO-doped cement cured by different methods and (b) GO before and after microwave treatment [141].](/document/doi/10.1515/rams-2025-0147/asset/graphic/j_rams-2025-0147_fig_008.jpg)
FTIR spectrum of (a) 0.5 wt% GO-doped cement cured by different methods and (b) GO before and after microwave treatment [141].
3.2.3 Raman spectroscopy
Raman spectroscopy serves as an effective technique for characterizing GFMs, providing structural insights such as layer number, defect density, and doping state. This method probes molecular vibrations through analysis of inelastically scattered light. For graphene dispersions, Raman spectrum can identify key peaks, such as the G peak (corresponding to the in-plane vibration of sp2-hybridized carbon atoms) and the 2D peak (corresponding to double-phonon scattering and indicating the number of graphene layers) [147,148]. The intensity ratio between the D-band and G-band is crucial for assessing the structure of GFMs’ dispersion. A higher ratio suggests greater disorder or defects, while a lower ratio indicates superior order degree and material quality [149–152]. While Raman spectroscopy cannot directly measure the dispersibility of GFMs in CBMs, it can characterize the number of layers, defects, and order degree of GFMs by the intensity ratio and thus can be used as a supplementary means to deeply reveal the dispersion mechanism of different GFMs, which can provide a strong support for the further application of GFMs in CBMs.
Moreover, Raman spectroscopy is typically employed to evaluate the interaction mechanism between GFMs and cement. For instance, Figure 9 exhibits notable Raman shifts in D-band and G-band. The D-band of GO embedded in cement matrix shifted from 1337.06 to 1349.51 cm−1, and the G-band shifted from 1574.46 to 1598.62 cm−1, indicating a wavenumber shift of 12.45 cm−1 for the D-band and 24.16 cm−1 for the G-band [153]. These shifts suggest an increased bonding force constant, implying weakened covalent C–C bonds in the graphitic plane due to interactions with the cement matrix. Therefore, both the crystalline and amorphous structures of GO may be squeezed by the cement matrix, leading to the broadening of Raman modes D and G.
![Figure 9
Raman spectra of pure GO and GO embedded in cement matrix after curing for 28 days [153].](/document/doi/10.1515/rams-2025-0147/asset/graphic/j_rams-2025-0147_fig_009.jpg)
Raman spectra of pure GO and GO embedded in cement matrix after curing for 28 days [153].
In summary, Raman spectroscopy provides a comprehensive and non-destructive approach for characterizing GFMs through the analysis of characteristic peaks such as the G and 2D peaks, Raman mapping, and the examination of peak intensity ratios. The technique delivers critical insights into the distribution state of GFMs within the cement matrix, thus playing an essential role in facilitating the application of GFMs in CBMs.
4 Effect of dispersibility of GFMs on the properties of CBMs
GFMs exhibit exceptional properties that make them promising additives for enhancing CBMs. However, their tendency to agglomerate and poor dispersibility significantly limit practical application. While numerous reviews comprehensively address the substantial improvements in mechanical and functional properties of CBMs modified by GFMs [27,154–157], this section specifically examines the influence of GFMs’ dispersibility on CBM performance. The analysis focuses on the roles of surfactants (including the chemical and mineral admixtures detailed in Table 3) and the types of GFMs. This focused approach aims to provide insights for advancing the practical implementation of GFMs in CBMs.
4.1 Effect of GFMs dispersed by chemical admixtures on the properties of CBMs
Optimal dispersion of GFMs within CBMs is essential for maximizing their enhancement of mechanical and functional properties. Two chemical admixtures commonly used to achieve this are superplasticizers and SDBS, which employ differing dispersion mechanisms.
Superplasticizers, particularly polycarboxylate ether (PCE)-based variants, are extensively utilized as high-performance water-reducers to improve the workability of CBMs. Their unique comb-like molecular structure, characterized by a hydrophilic backbone and hydrophobic side chains, enables effective adsorption onto GFMs. This adsorption mechanism employs steric hindrance and electrostatic repulsion to prevent agglomeration of GFMs, thereby promoting their dispersion within the cement matrix. Moreover, studies demonstrate that PCE-based superplasticizers, when employed as surfactants in conjunction with ultrasonication, significantly enhance the properties of graphene/cement composites. For instance, Liu et al. [158] directly mixed GO and PCE into water and applied ultrasonic treatment to prepare the PCE/GO dispersion. Their study revealed that incorporating 0.2 wt% PCE/GO (ratio of 1:1) in mortars increased the 28-day flexural strength by 9 and 16.9%, and the compressive strength by 11.6 and 17.6%, respectively. In contrast, Zhou and Li [159] synthesized the PCE/GO dispersion using a dropwise addition method. Their results showed that the 28-day compressive strength of mortars with the same dosage of PCE/GO increased by 10.7%, suggesting that the synthesis method of PCE/GO dispersions contributes to the improvement of CBMs. Furthermore, Elbatanouny et al. [59] investigated the effects of ultrasonication on graphene/cement composites through two strategies: ultrasonication with surfactant coating and mechanical blending with surfactant coating. They observed that the 28-day compressive strength of mortars containing 0.3 wt% PCE/graphene (ratio of 9:1) improved by 17.5 and 13.7%, respectively, highlighting the critical role of ultrasonication in graphene/cement composites. And similar conclusions have been drawn by other studies [57,160,161].
It is widely accepted that the dosage of superplasticizer is a crucial factor influencing the dispersibility of GFMs within cement matrix. Ragstogi et al. [162] and Yu et al. [163] reported an optimum dosage that ensures uniform graphene dispersion, which depends on both the superplasticizer type and applied sonication energy. Extensive studies have therefore investigated strategies to optimize superplasticizer dosage and sonication energy synergistically. Metaxa and Kourkoulis [164] prepared Type II cement paste reinforced with 0.1 wt% GNPs and varying PCE dosages, demonstrating significant improvements in electrical and mechanical properties. The optimum dosage was determined to be 0.7 wt%, resulting in the lowest electrical resistivity and a 25% increase in 28-day flexural strength. Under this dosage, applying ultrasonic energy of 400 kJ further enhanced performance, achieving the lowest electrical resistivity and the highest flexural strength. Their findings confirm that a combination of 0.7 wt% PCE and 400 kJ ultrasonic energy is optimal for uniform graphene dispersion and maximizing composite performance. Similarly, Yan et al. [110] investigated the GO dispersion modified by six types of PCE, examining the effects of ultrasonication energy, PCE dosage, and type on the dispersibility. The results showed that Sika-PCE achieved the best dispersibility, with optimal parameters of 30% ultrasonication energy and a GO/PCE ratio of 1:1. At these parameters, GO increased the 3-day flexural and compressive strengths of mortars by 15.48% (0.02 wt% GO) and 14.39% (0.04 wt% GO), respectively.
Despite extensive research focused on determining the optimal PCE dosage for dispersing GFMs, establishing this parameter remains a significant challenge due to inconsistent findings in the literature [93,165]. Rios et al. [165] explored the relationship between GO dispersion and the inconsistent properties of CBMs, indicating that while PCE reduce agglomeration, they cannot fully eliminate irregular GO aggregates. This limitation underscores the inherent difficulty in achieving homogeneous GFMs’ dispersions using PCE alone, as agglomeration in alkaline cement environments remains a persistent barrier to optimal performance enhancement. Consequently, recent research has expanded to explore alternative chemical admixtures and synergistic strategies. Taking SDBS as an example, studies have shown that homogeneous graphene dispersion can be obtained using SDBS as surfactant. It has been reported that cement paste samples containing 0.025 wt% GO and 0.15% SDBS showed an increase in compressive strength by 14.9 and 10.0% at 7 and 28 days, respectively, and an increase in flexural strength by 23.6 and 16% at 7 and 28 days, respectively [115]. Additionally, Jiang et al. [95] compared the effectiveness of SDBS with PCE, sodium cholate (SC), and Pluronic F-127 to optimize GNPs’ dispersion in mortars, applying ideal solution principles and component analysis methods. Compressive strengths and permeable void tests for GNPs-modified mortars (Figure 10) revealed that adding 0.05 and 0.1 wt% graphene increased compressive strength by 32.4 and 31.4%, respectively, when the graphene/SDBS ratio was 1:2. These results indicate that higher graphene concentrations may lead to increased agglomeration, weakening the interfacial bond between graphene and hydration products and limiting further strength enhancement in mortars.
![Figure 10
Properties of GNPs-modified mortars change with different dispersion agents [95].](/document/doi/10.1515/rams-2025-0147/asset/graphic/j_rams-2025-0147_fig_010.jpg)
Properties of GNPs-modified mortars change with different dispersion agents [95].
4.2 Effect of GFMs dispersed by mineral admixtures on the properties of CBMs
Among all mineral admixtures serving as dispersing agents for graphene in CBMs, silica fume and fly ash are favored for their low cost and effectiveness. Although both enhance properties of graphene/cement composites, they operate through distinct dispersion mechanisms.
Silica fume, owing to its ultra-fine particle size and high pozzolanic reactivity, effectively reduces GFMs agglomeration and promotes strong interfacial bonding between GFMs and cement matrix. Its nano-sized particles fill the voids within the matrix and chemically react with calcium hydroxide to form additional C–S–H gel, which not only enhances the overall matrix density but also stabilizes the dispersed GFMs. The synergy between silica fume and GO has been a focal point of research. For example, Li et al. [81] investigated the combined effects of GO and silica fume on cement paste, finding that optimal proportions of GO (0.02 wt%) and silica fume (5.0 wt%) significantly improved mechanical properties. Their study demonstrated that the dispersibility of GO, which governs the mechanical properties of cement paste, is closely related to the silica fume content. It further suggested that the optimal silica fume dosage can be determined by matching its total surface area to that of the GO sheets, as shown in Figure 11. Similarly, Lu et al. [166] explored the co-effects of GO and silica fume on the rheological properties of cement paste. They proposed a method of synthesizing GO-coated silica fume to promote the utilization of GO in CBMs. Their results revealed that this approach effectively reduced yield stress and plastic viscosity, indicating improved workability of the fresh mixture. Furthermore, Roy et al. [167] showed that adding silica fume and metakaolin together significantly increased the strength of GO/cement mortars compared to the plain samples, due to the reduced porosity and improved interfacial bonding between GO and the cement matrix. Specifically, the optimal compressive strength was achieved with 0.05 wt% GO when silica fume (14.3 wt%) and metakaolin (28.6 wt%) were used as dispersants, resulting in increases of 72.41, 84.61, and 90.90% after 3, 7, and 28 days, respectively. Similarly, the tensile strength reached its maximum with 0.1 wt% GO, exhibiting significant enhancements of 132, 178.6, and 181.2% over the same periods.
![Figure 11
Schematic diagram of GO covered with silica fume particles [81].](/document/doi/10.1515/rams-2025-0147/asset/graphic/j_rams-2025-0147_fig_011.jpg)
Schematic diagram of GO covered with silica fume particles [81].
In contrast, fly ash consists primarily of spherical particles and exhibits lower pozzolanic reactivity than silica fume. Nevertheless, its smooth surface and spherical morphology form a physical barrier that impedes GFMs from agglomerating. Generally, the use of fly ash as a dispersing agent helps mitigate this issue by promoting GFMs uniformly dispersed into cement matrix, thus enhancing the workability of CBMs. For instance, Wang et al. [86] indicated that fly ash can offset the reduction in fluidity by GO. At 0.01 wt% GO and 20 wt% fly ash, the yield stress of the paste decreased by 85.81%, and the plastic viscosity reduced by 29.53% compared to the control sample without fly ash or GO. Actually, the synergistic use of fly ash and graphene not only enhances the workability but also improves the mechanical strength of CBMs. A study by Reddy and Prasad [168] investigated the static and dynamic mechanical properties of concrete containing GO and fly ash. The results indicated that 0.15% GO and up to 20% fly ash replacement increased compressive strength by 19.7 and 28.5% on 7 and 28 days, respectively. Similarly, Nguyen et al. [169] concluded that incorporating 10 wt% FA and 0.036 wt% GO optimizes the physical and mechanical properties of cement mortar while maintaining essential characteristics such as workability.
In summary, silica fume and fly ash function as multifunctional additives in graphene/cement composites, serving simultaneously as fillers, pozzolanic materials, and dispersion aids. However, silica fume demonstrates superior chemical reactivity and dispersion stability, while fly ash offers enhanced cost-effectiveness and workability. Although studies have been given to explore which one is more beneficial for enhancing the properties of graphene/cement composites, the conclusions remain unconvincing due to insufficient data [82,85]. Consequently, the choice between these additives depends on specific project requirements, such as cost constraints or the desired improvement in material properties.
4.3 Effect of the type of GFMs on the properties of CBMs
Fundamental differences in atomic structure and surface chemistry across GFMs directly dictate their dispersibility in cementitious environments, ultimately leading to divergent performance enhancement effects in CBMs.
Studies demonstrate that GO and rGO surpass graphene in enhancing CBMs, primarily owing to their superior dispersibility within the cement matrix enabled by surface functionalization via ionic modifiers and surfactants [170–173]. Specifically, GO demonstrates remarkable performance enhancements because its abundant oxygen-containing functional groups promote better dispersion, hydration, and interfacial bonding. Studies have indicated that GO can improve compressive strength and flexural strength by 30 and 84%, respectively, while rGO showed slightly lower but comparable improvements of 28 and 81%. By contrast, although graphene elevates compressive strength substantially (39% improvement), its limited dispersibility restricts flexural strength gains to 38%, demonstrating the critical role of nanomaterial dispersibility in CBMs [34]. However, the performance-enhancing superiority of GO in CBMs is contested by studies showing that advanced functionalization of rGO and graphene can achieve superior dispersibility and composite performance. For instance, TiO2-functionalized rGO exhibits dispersion quality exceeding that of GO, consequently delivering mortar strength precisely double that of GO-modified mortars at equivalent nanomaterial dosage [38]. Qureshi and Panesar [174] indicated that the 28-day compressive strength of cement pastes increased by approximately 10 and 15% with 0.06 wt% GO and rGO, respectively, compared to the control sample. The highest flexural strength was observed with 0.04 wt% GO (75.7% improvement) and 0.06 wt% rGO (33.7% improvement). Additionally, electrical resistivity increased with GO and rGO incorporation, while water absorptivity decreased by 24.8 and 4.7%, respectively. Similar results have been observed with other modified rGO and graphene, suggesting that tailored modifications can outperform GO under specific conditions [175–177]. These findings emphasize that while GO sets a high standard for performance enhancement, innovative functionalization approaches for other GFMs and hybrid materials may unlock even greater potential in CBMs, paving the way for advanced cement composites with superior strength and durability.
Furthermore, the reinforcement efficacy of GFMs in CBMs is intricately linked to their lateral dimensions, specific surface area, and oxygen content [178–180]. For instance, by utilizing two types of GNPs with distinct lateral sizes (<2 μm and 25 μm) and specific surface areas (300 and 120 m2·g−1), Jiang et al. [181] observed that smaller lateral sizes and larger specific surface areas of graphene significantly enhance their ability to prevent water penetration into CBMs. Similarly, Lavagna et al. [107] demonstrated that reinforcements with the highest oxygen content tend to aggregate, whereas the highest cement strength is achieved with functionalized graphene containing 5% oxygen. This level of oxygen provides an optimal balance, offering sufficient polar groups on the surface to ensure proper dispersion and effective interaction with the hydrated cement matrix.
5 Challenges and prospects
The integration of GFMs into CBMs has attracted significant research interest due to their exceptional mechanical, electrical, and thermal properties. Nevertheless, critical challenges impede widespread application. Foremost is dispersibility limitation: graphene’s hydrophobicity and strong van der Waals forces induce agglomeration, constraining reinforcement potential. Achieving homogeneous dispersion is further challenged by cement matrix’s high alkalinity and calcium-rich environment (Figure 12) [182]. Poor dispersibility not only reduces the effective surface area of GFMs but also introduces weak points that weaken the CBM’s overall performance. Addressing this issue requires a multi-pronged approach. Functionalization of graphene with hydrophilic groups, such as hydroxyl or carboxyl groups, has shown promise in enhancing dispersion stability. However, excessive functionalization can compromise graphene’s intrinsic properties, such as electrical conductivity and mechanical strength [183,184]. Therefore, it is necessary to find a balance between improving compatibility and preserving functionality. Furthermore, advanced mixing techniques, such as the use of high-shear mixers or ultrasonic homogenizers, can enhance dispersion but are challenging to scale for industrial applications.
![Figure 12
Cluster model of GO under high alkalinity and high calcium conditions. (a) High calcium environment, (b) high alkalinity environment, and (c) combined effect [182].](/document/doi/10.1515/rams-2025-0147/asset/graphic/j_rams-2025-0147_fig_012.jpg)
Cluster model of GO under high alkalinity and high calcium conditions. (a) High calcium environment, (b) high alkalinity environment, and (c) combined effect [182].
Graphene’s interaction with cement matrix is a double-edged sword. Positively, graphene acts as nucleation sites for hydration products, refining microstructural morphology and enhancing mechanical properties. Conversely, preferential bonding with specific hydrates (e.g., C–S–H over Portlandite) causes uneven distribution, diminishing reinforcement efficiency. For instance, studies have shown that GO can accelerate the hydration of Portland cement through a seeding effect, while temporarily retarding clinker hydration due to its interaction with the surface of hydrating grains [185]. Moreover, graphene’s impact on hydration kinetics is not yet fully understood. Accelerated hydration may improve early-age strength but could also lead to undesirable effects, such as increased shrinkage or cracking. Advanced computational models and molecular dynamics simulations could play a crucial role in unraveling these complex interactions, providing insights that are difficult to obtain through experimental methods alone.
The inherent complexity of cement systems poses significant challenges to the accurate characterization of GFMs and interfacial interactions within the cement matrix. Traditional imaging techniques, such as SEM and TEM, provide valuable qualitative insights but the results may be non-representative due to poor stochasticity of samples. Spectroscopic methods, such as Raman spectroscopy, offer a more accessible alternative but require significant expertise to interpret results in the context of CBMs. Developing new characterization techniques that combine speed, accuracy, and affordability is crucial. Real-time monitoring methods, such as DLS or in situ spectroscopy, could provide immediate feedback during mixing and curing processes, enabling researchers to optimize dispersion on the fly [31,59]. Additionally, the integration of advanced imaging techniques with machine learning algorithms could automate the analysis of dispersion quality, making it more accessible for both academic and industrial applications.
A further significant challenge stems from the lack of standardized experimental methodologies, which has resulted in a fragmented research landscape that impedes reliable comparison of findings across studies. For instance, the use of different functionalization methods, solvent types, or dispersion techniques often results in conflicting findings regarding graphene’s effectiveness. Additionally, the variability in cement types, water-to-cement ratios, and curing conditions further complicates comparisons across studies. Therefore, establishing standardized protocols for GFMs’ incorporation and performance evaluation in CBMs is imperative. Such standards should include guidelines for functionalization, dispersion techniques, and characterization methods. Furthermore, the cost of GFMs and functionalization represents another significant barrier. High-quality material synthesized via chemical vapor deposition or mechanical exfoliation is expensive and energy intensive. These costs make it challenging to justify GFMs in large-scale applications, particularly in the cost-sensitive construction industry.
While GFMs demonstrate significant potential for enhancing CBMs, addressing persistent challenges (dispersibility limitations, characterization complexities, experimental inconsistencies, and economic barriers) necessitates targeted research efforts, as depicted in Figure 13. Successful application will depend on the development of optimized functionalization techniques to improve graphene-family dispersions, a deeper understanding of their role in hydration, and the establishment of standardized testing protocols to ensure consistency and reproducibility across studies. Moreover, balancing cost-effective production methods with performance enhancements will be crucial for the large-scale application of GFMs into CBMs.
Dispersion research and challenge when applying GFMs into CBMs.
6 Conclusion
GFMs exhibit substantial potential for enhancing the properties of CBMs, including mechanical strength, durability, and smart performance. However, their practical implementation is hindered by several challenges, particularly the achievement of homogeneous dispersion within the complex cement environment. Due to strong van der Waals forces and hydrophobic nature, GFMs tend to agglomerate, reducing its effectiveness in enhancing performance of CBMs.
Although physical modification, chemical functionalization, and synthetic approaches have demonstrated notable progress in addressing dispersion issues, scaling these techniques for large-scale engineering applications remains a critical obstacle.
Moreover, the long-term impacts of GFMs on cement hydration and the development of cost-effective manufacturing methods require further research.
Future advancements in dispersion technologies, a more profound comprehension of hydration mechanisms, and the establishment of standardized experimental frameworks will be critical for unlocking the full potential of GFMs in CBMs. Additionally, the development of novel dispersant materials and the integration of computational modeling offer innovative strategies to optimize graphene-family incorporation. Addressing these challenges would enable GFMs to assume a pivotal role in fabricating more durable, sustainable, and high-performance construction materials, thereby driving transformative progress in the construction industry.
Acknowledgments
The authors acknowledge the support by Natural Science Foundation of Zhejiang Province (LQ23D010002), Scientific Research Fund of Zhejiang Provincial Education Department (Y202248582, Y202455558), Special Fund of Hangzhou Iron and Steel Group Co., Ltd (XKZ202212027), Shaoxing Science and Technology Plan Project (2023A13006), and Scientific Research Projects of Shaoxing University (2022LG008).
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Funding information: This study was supported by Natural Science Foundation of Zhejiang Province (LQ23D010002), Scientific Research Fund of Zhejiang Provincial Education Department (Y202248582, Y202455558), Special Fund of Hangzhou Iron and Steel Group Co., Ltd (XKZ202212027), Shaoxing Science and Technology Plan Project (2023A13006), and Scientific Research Projects of Shaoxing University (2022LG008).
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Author contributions: Hongyan Zeng: writing – original draft, methodology, investigation, funding acquisition, and conceptualization. Junbin Chen: writing – original draft and investigation. Xiaofeng Luo: writing – review and editing, and supervision. Shen Qu: funding acquisition and formal analysis. Yunan Li: investigation. Yunjin Hu: resources and funding acquisition. Yun Tian: resources. All authors have accepted responsibility for the entire content of this manuscript and approved its submission.
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Conflict of interest: The authors state no conflict of interest.
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Data availability statement: Data sharing is not applicable to this article as no datasets were generated or analyzed during the current study.
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- Study of feasibility of using copper mining tailings in mortar production
- Shear and flexural performance of reinforced concrete beams with recycled concrete aggregates
- Advancing GGBS geopolymer concrete with nano-alumina: A study on strength and durability in aggressive environments
- Leveraging waste-based additives and machine learning for sustainable mortar development in construction
- Study on the modification effects and mechanisms of organic–inorganic composite anti-aging agents on asphalt across multiple scales
- Morphological and microstructural analysis of sustainable concrete with crumb rubber and SCMs
- Structural, physical, and luminescence properties of sodium–aluminum–zinc borophosphate glass embedded with Nd3+ ions for optical applications
- Eco-friendly waste plastic-based mortar incorporating industrial waste powders: Interpretable models for flexural strength
- Bioactive potential of marine Aspergillus niger AMG31: Metabolite profiling and green synthesis of copper/zinc oxide nanocomposites – An insight into biomedical applications
- Preparation of geopolymer cementitious materials by combining industrial waste and municipal dewatering sludge: Stabilization, microscopic analysis and water seepage
- Seismic behavior and shear capacity calculation of a new type of self-centering steel-concrete composite joint
- Sustainable utilization of aluminum waste in geopolymer concrete: Influence of alkaline activation on microstructure and mechanical properties
- Optimization of oil palm boiler ash waste and zinc oxide as antibacterial fabric coating
- Tailoring ZX30 alloy’s microstructural evolution, electrochemical and mechanical behavior via ECAP processing parameters
- Comparative study on the effect of natural and synthetic fibers on the production of sustainable concrete
- Microemulsion synthesis of zinc-containing mesoporous bioactive silicate glass nanoparticles: In vitro bioactivity and drug release studies
- On the interaction of shear bands with nanoparticles in ZrCu-based metallic glass: In situ TEM investigation
- Developing low carbon molybdenum tailing self-consolidating concrete: Workability, shrinkage, strength, and pore structure
- Experimental and computational analyses of eco-friendly concrete using recycled crushed brick
- High-performance WC–Co coatings via HVOF: Mechanical properties of steel surfaces
- Special Issue on Recent Advancement in Low-carbon Cement-based Materials - Part II
- Investigating the effect of locally available volcanic ash on mechanical and microstructure properties of concrete
- Flexural performance evaluation using computational tools for plastic-derived mortar modified with blends of industrial waste powders
- Foamed geopolymers as low carbon materials for fire-resistant and lightweight applications in construction: A review
- Autogenous shrinkage of cementitious composites incorporating red mud
- Mechanical, durability, and microstructure analysis of concrete made with metakaolin and copper slag for sustainable construction
- Special Issue on AI-Driven Advances for Nano-Enhanced Sustainable Construction Materials
- Advanced explainable models for strength evaluation of self-compacting concrete modified with supplementary glass and marble powders
- Analyzing the viability of agro-waste for sustainable concrete: Expression-based formulation and validation of predictive models for strength performance
- Special Issue on Advanced Materials for Energy Storage and Conversion
- Innovative optimization of seashell ash-based lightweight foamed concrete: Enhancing physicomechanical properties through ANN-GA hybrid approach
- Production of novel reinforcing rods of waste polyester, polypropylene, and cotton as alternatives to reinforcement steel rods
Articles in the same Issue
- Eco-friendly green synthesis of silver nanoparticles with Syzygium aromaticum extract: characterization and evaluation against Schistosoma haematobium
- Mechanical properties and fatigue analysis of rubber concrete under uniaxial compression modified by a combination of mineral admixture
- Predictive modeling assessment of advanced concrete materials incorporating plastic waste as sand replacement
- Nanotechnology for calcium aluminate cement: thematic analysis
- Experimental study of flexural performance of solid wood beams strengthened with CFRP fibers
- Self-compacting mortar overlays using expanded polystyrene beads for thermal performance and energy efficiency in buildings
- Review Articles
- Utilization of steel slag in concrete: A review on durability and microstructure analysis
- Technical development of modified emulsion asphalt: A review on the preparation, performance, and applications
- Recent developments in ultrasonic welding of similar and dissimilar joints of carbon fiber reinforcement thermoplastics with and without interlayer: A state-of-the-art review
- Unveiling the crucial factors and coating mitigation of solid particle erosion in steam turbine blade failures: A review
- From magnesium oxide, magnesium oxide concrete to magnesium oxide concrete dams
- Properties and potential applications of polymer composites containing secondary fillers
- A scientometric review on the utilization of copper slag as a substitute constituent of ordinary Portland cement concrete
- Advancement of additive manufacturing technology in the development of personalized in vivo and in vitro prosthetic implants
- Recent advance of MOFs in Fenton-like reaction
- A review of defect formation, detection, and effect on mechanical properties of three-dimensional braided composites
- Non-conventional approaches to producing biochars for environmental and energy applications
- Review of the development and application of aluminum alloys in the nuclear industry
- Advances in the development and characterization of combustible cartridge cases and propellants: Preparation, performance, and future prospects
- Recent trends in rubberized and non-rubberized ultra-high performance geopolymer concrete for sustainable construction: A review
- Cement-based materials for radiative cooling: Potential, material and structural design, and future prospects
- A comprehensive review: The impact of recycling polypropylene fiber on lightweight concrete performance
- A comprehensive review of preheating temperature effects on reclaimed asphalt pavement in the hot center plant recycling
- Exploring the potential applications of semi-flexible pavement: A comprehensive review
- A critical review of alkali-activated metakaolin/blast furnace slag-based cementitious materials: Reaction evolution and mechanism
- Dispersibility of graphene-family materials and their impact on the properties of cement-based materials: Application challenges and prospects
- Research progress on rubidium and cesium separation and extraction
- A step towards sustainable concrete with the utilization of M-sand in concrete production: A review
- Studying the effect of nanofillers in civil applications: A review
- Studies on the anticorrosive effect of phytochemicals on mild steel, carbon steel, and stainless-steel surfaces in acid and alkali medium: A review
- Research Articles
- Investigation of the corrosion performance of HVOF-sprayed WC-CoCr coatings applied on offshore hydraulic equipment
- A systematic review of metakaolin-based alkali-activated and geopolymer concrete: A step toward green concrete
- Evaluation of color matching of three single-shade composites employing simulated 3D printed cavities with different thicknesses using CIELAB and CIEDE2000 color difference formulae
- Novel approaches in prediction of tensile strain capacity of engineered cementitious composites using interpretable approaches
- Effect of TiB2 particles on the compressive, hardness, and water absorption responses of Kulkual fiber-reinforced epoxy composites
- Analyzing the compressive strength, eco-strength, and cost–strength ratio of agro-waste-derived concrete using advanced machine learning methods
- Tensile behavior evaluation of two-stage concrete using an innovative model optimization approach
- Tailoring the mechanical and degradation properties of 3DP PLA/PCL scaffolds for biomedical applications
- Optimizing compressive strength prediction in glass powder-modified concrete: A comprehensive study on silicon dioxide and calcium oxide influence across varied sample dimensions and strength ranges
- Experimental study on solid particle erosion of protective aircraft coatings at different impact angles
- Compatibility between polyurea resin modifier and asphalt binder based on segregation and rheological parameters
- Fe-containing nominal wollastonite (CaSiO3)–Na2O glass-ceramic: Characterization and biocompatibility
- Relevance of pore network connectivity in tannin-derived carbons for rapid detection of BTEX traces in indoor air
- A life cycle and environmental impact analysis of sustainable concrete incorporating date palm ash and eggshell powder as supplementary cementitious materials
- Eco-friendly utilisation of agricultural waste: Assessing mixture performance and physical properties of asphalt modified with peanut husk ash using response surface methodology
- Benefits and limitations of N2 addition with Ar as shielding gas on microstructure change and their effect on hardness and corrosion resistance of duplex stainless steel weldments
- Effect of selective laser sintering processing parameters on the mechanical properties of peanut shell powder/polyether sulfone composite
- Impact and mechanism of improving the UV aging resistance performance of modified asphalt binder
- AI-based prediction for the strength, cost, and sustainability of eggshell and date palm ash-blended concrete
- Investigating the sulfonated ZnO–PVA membrane for improved MFC performance
- Strontium coupling with sulphur in mouse bone apatites
- Transforming waste into value: Advancing sustainable construction materials with treated plastic waste and foundry sand in lightweight foamed concrete for a greener future
- Evaluating the use of recycled sawdust in porous foam mortar for improved performance
- Improvement and predictive modeling of the mechanical performance of waste fire clay blended concrete
- Polyvinyl alcohol/alginate/gelatin hydrogel-based CaSiO3 designed for accelerating wound healing
- Research on assembly stress and deformation of thin-walled composite material power cabin fairings
- Effect of volcanic pumice powder on the properties of fiber-reinforced cement mortars in aggressive environments
- Analyzing the compressive performance of lightweight foamcrete and parameter interdependencies using machine intelligence strategies
- Selected materials techniques for evaluation of attributes of sourdough bread with Kombucha SCOBY
- Establishing strength prediction models for low-carbon rubberized cementitious mortar using advanced AI tools
- Investigating the strength performance of 3D printed fiber-reinforced concrete using applicable predictive models
- An eco-friendly synthesis of ZnO nanoparticles with jamun seed extract and their multi-applications
- The application of convolutional neural networks, LF-NMR, and texture for microparticle analysis in assessing the quality of fruit powders: Case study – blackcurrant powders
- Study of feasibility of using copper mining tailings in mortar production
- Shear and flexural performance of reinforced concrete beams with recycled concrete aggregates
- Advancing GGBS geopolymer concrete with nano-alumina: A study on strength and durability in aggressive environments
- Leveraging waste-based additives and machine learning for sustainable mortar development in construction
- Study on the modification effects and mechanisms of organic–inorganic composite anti-aging agents on asphalt across multiple scales
- Morphological and microstructural analysis of sustainable concrete with crumb rubber and SCMs
- Structural, physical, and luminescence properties of sodium–aluminum–zinc borophosphate glass embedded with Nd3+ ions for optical applications
- Eco-friendly waste plastic-based mortar incorporating industrial waste powders: Interpretable models for flexural strength
- Bioactive potential of marine Aspergillus niger AMG31: Metabolite profiling and green synthesis of copper/zinc oxide nanocomposites – An insight into biomedical applications
- Preparation of geopolymer cementitious materials by combining industrial waste and municipal dewatering sludge: Stabilization, microscopic analysis and water seepage
- Seismic behavior and shear capacity calculation of a new type of self-centering steel-concrete composite joint
- Sustainable utilization of aluminum waste in geopolymer concrete: Influence of alkaline activation on microstructure and mechanical properties
- Optimization of oil palm boiler ash waste and zinc oxide as antibacterial fabric coating
- Tailoring ZX30 alloy’s microstructural evolution, electrochemical and mechanical behavior via ECAP processing parameters
- Comparative study on the effect of natural and synthetic fibers on the production of sustainable concrete
- Microemulsion synthesis of zinc-containing mesoporous bioactive silicate glass nanoparticles: In vitro bioactivity and drug release studies
- On the interaction of shear bands with nanoparticles in ZrCu-based metallic glass: In situ TEM investigation
- Developing low carbon molybdenum tailing self-consolidating concrete: Workability, shrinkage, strength, and pore structure
- Experimental and computational analyses of eco-friendly concrete using recycled crushed brick
- High-performance WC–Co coatings via HVOF: Mechanical properties of steel surfaces
- Special Issue on Recent Advancement in Low-carbon Cement-based Materials - Part II
- Investigating the effect of locally available volcanic ash on mechanical and microstructure properties of concrete
- Flexural performance evaluation using computational tools for plastic-derived mortar modified with blends of industrial waste powders
- Foamed geopolymers as low carbon materials for fire-resistant and lightweight applications in construction: A review
- Autogenous shrinkage of cementitious composites incorporating red mud
- Mechanical, durability, and microstructure analysis of concrete made with metakaolin and copper slag for sustainable construction
- Special Issue on AI-Driven Advances for Nano-Enhanced Sustainable Construction Materials
- Advanced explainable models for strength evaluation of self-compacting concrete modified with supplementary glass and marble powders
- Analyzing the viability of agro-waste for sustainable concrete: Expression-based formulation and validation of predictive models for strength performance
- Special Issue on Advanced Materials for Energy Storage and Conversion
- Innovative optimization of seashell ash-based lightweight foamed concrete: Enhancing physicomechanical properties through ANN-GA hybrid approach
- Production of novel reinforcing rods of waste polyester, polypropylene, and cotton as alternatives to reinforcement steel rods
