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Frontiers in Soft Matter ·

Volume 6 - 2026 | https://doi.org/10.3389/frsfm.2026.1908524

Pickering emulsions: emulsion polymerization and systems stabilized with carbon allotropes or carbon-rich materials

  • Miguel Rosales-Guzmán1
  • María Esther Treviño Martínez2
  • Enrique Saldívar-Guerra1*corresponding author
  1. 1Department of Polymerization Processes, Centro de Investigación en Química Aplicada, Saltillo, Mexico
  2. 2Department of Macromolecular Chemistry and Nanomaterials, Centro de Investigación en Química Aplicada, Saltillo, Mexico
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Abstract

The use of Pickering emulsions (PEs) has recently expanded considerably in academia and industry due to their ease of preparation, remarkable stability, and versatility in applications. This review focuses on PEs stabilized by carbon-rich particles, such as functionalized graphene and graphene oxide (GO), among others. It includes general PE production and applications along with the stabilization of emulsions in which an emulsion polymerization occurs to generate a polymer that plays a key role in the final application. Novel aspects of this study compared to others consist of its focus on carbon-rich stabilizers and its inclusion of emulsion polymerization applications. The key factor to obtain a stable PE with these materials is to guarantee that they exhibit an amphiphilic nature (which is tunable in many cases) to stabilize the emulsion. The majority of the applications in recent literature use GO as a PE stabilizer due to its inherent amphiphilicity and versatility for further chemical modification. The most significant challenge for final applications is the scaling up of the production process of GO or other carbon-based materials as stabilizers so that they can perform reproducibly as PE stabilizers, as these processes are subject to significant variability. Future research will diversify and consolidate applications, focusing more on the practical implementation of these developments involving aspects such as scaling up, efficiency, and recyclability.

Keywords

1 Introduction

According to the IUPAC (2026), a colloidal dispersion is a dispersion of small particles (approximately 1–1000 nm in size) in a continuous phase that is of a different composition or nature than the particles. When the particles and the continuous phase are both in a liquid state, these dispersions are called emulsions, and the particles are usually called droplets. Due to the different chemical natures of the droplets and the continuous medium, there is an interfacial tension between the surface of the droplets and the continuous medium, and therefore a significant tendency for the droplets to flocculate and coalesce to minimize the free energy of the system. Emulsions will eventually destabilize, primarily through Ostwald ripening, flocculation, and coalescence. As a result, emulsions need to be stabilized to increase their kinetic stability. This can be achieved in various ways, but the use of surfactants is the most common one. Ionic surfactants are most commonly used and act via electrostatic repulsion between particles (droplets) through the interaction of the double layer of ions formed around them, as explained in detail by the DLVO (Derjaguin, Landau, Verwey, and Overbeek) theory (Hiemenz and Rajagopalan, 1997). Non-ionic surfactants, on the other hand, create a physical barrier around the particles (droplets) that prevents them from coalescing (Rapp, 2017).

A completely different form of stabilization is provided by solid particles dispersed in the medium that adsorb onto the surfaces of the emulsion droplets; this forms a barrier that impedes their coalescence. Emulsions stabilized in this way are called Pickering emulsions (PEs). Ramsden (1904) and Pickering (1907) were the first to describe the stabilization of droplets with solid particles. PEs have a wide variety of applications, primarily industrial. They can be used in catalysis, filtration membranes, drug delivery, antibacterial applications, protein recognition, cosmetics, nutraceuticals, food technology, and more (Herrera-Ordóñez et al., 2026; González Ortiz et al., 2020; Cassani and Gomez-Zavaglia, 2024). PEs can also be used as stabilizers in emulsion polymerization, a process with many applications that is widely used in industry to synthesize commercial and high-tech polymers for advanced applications. In summary, PEs can be defined as emulsions stabilized by solid particles (Herrera-Ordóñez et al., 2026).

The most common particles used in PEs are inorganic (Ribeiro et al., 2023), such as silica (Björkegren et al., 2017; Zhu et al., 2015; Wang and Wang, 2016; Heidari et al., 2022), nanoclays (Zheng et al., 2020), calcium carbonate (Huang et al., 2019), 2D boron nitride (Pakdel et al., 2011; Gonzalez Ortiz et al., 2019; Wang et al., 2023), graphene-based particles (Gonzalez Ortiz et al., 2019; Wang et al., 2023), and carbon nanotubes (Briggs et al., 2015; Briggs et al., 2018). Organic particles include proteins (Destribats et al., 2014; Bai et al., 2016) and polysaccharides (Yuan et al., 2017; Bai et al., 2016; Jug et al., 2021; Meng et al., 2023). Some materials are more suitable for certain applications; for example, proteins and polysaccharides are ideal for food applications. More recently, PE studies using carbon allotropes or carbon-rich materials have become popular due to recent discoveries related to these materials and their increased availability. Some carbon derivatives, in particular GO, are advantageous over other solid stabilizers due to their relatively easy preparation and tunable wettability, which can be adapted according to the application. Additionally, carbon derivatives enable the preparation of 3D structures after removing water and potentially the organic phase from O/W emulsions.

Over the last 20 years, the field of PEs has seen exponential growth. A Scopus search on Pickering emulsions has shown that the number of publications has increased year by year since 2000, reaching a maximum of 1,366 in 2025. Given the broad scope of PEs, this review will first discuss PE stabilization in general and the functionalization of carbon-rich particles for use as PE stabilizers. Then, it will present a brief analysis of polymerization in PEs stabilized with GO. To the best of our knowledge, the latter subject has not received sufficient attention, despite its relevance. This review is organized as follows: in the next section, the stabilization mechanism of emulsions via solid particles is briefly discussed; next, methods for modifying solid particles to provide better stabilization in PEs are reviewed and described; then, the subject of aqueous dispersion polymerizations, including emulsion polymerization, is introduced, and the use of solid particles as stabilizers in these systems is discussed; finally, a section on recent applications of carbon allotropes or carbon-rich materials as solid particles used in the preparation of PEs is provided.

2 Stabilization mechanism

According to Schulman and Leja (1954), solid particles can stabilize an emulsion by positioning themselves at the oil/water interface, where they are partially wetted by both phases (Herrera-Ordóñez et al., 2026). Wettability can be defined in terms of the three-phase contact angle, which determines the type of emulsion formed (O/W or W/O) and is similar to the hydrophilic-lipophilic balance (HLB) concept used for surfactants, which serves the same purpose. Figure 1A illustrates the three-phase contact angle Θ in a PE, which is formed at the intersection point where the solid particle meets the oil/water interface. If Θ < 90°, the solid particles are more hydrophilic and better suited for stabilizing O/W PEs. Conversely, if Θ > 90°, the solid particles are more hydrophobic and better suited for stabilizing W/O PEs. When solid particles are completely wetted by one of the phases (either oil or water), stabilization of emulsions is not possible (Herrera-Ordóñez et al., 2026; Zhang T. et al., 2022).

**(A)** Spherical solid particles at the oil-water interface, illustrating how the three-phase contact angle determines the type of emulsion formed: O/W or W/O. Taken from (Zhang T. et al., 2022a) and reproduced under license: [https://creativecommons.org/licenses/by-nc-nd/4.0/](https://creativecommons.org/licenses/by-nc-nd/4.0/); **(B)** Schematics of how isometric particles and two-dimensional materials cover the surface area of dispersed particles in a PE. Reprinted with permission from Creighton et al., 2014. Copyright 2014 American Chemical Society; **(C)** Illustration of the exfoliation and oxidation processes needed to obtain GO from graphite; **(D)** SEM and TEM images of PS-GO microspheres in a PE. Reprinted with permission from Song et al. (2011). Copyright 2011 American Chemical Society; **(E)** Sequence of steps involved in batch polymerization in a GO-stabilized PE: in stage 1, the organic phase (monomer) is brought into contact with the aqueous phase (GO has been previously dispersed in water); in stage 2, the organic phase is dispersed in the aqueous phase at a high shear energy; in stage 3, emulsion polymerization takes place (when a monomer-soluble initiator is used, it is usually added, dissolved in the monomer, before the emulsion is formed; however, if an aqueous-phase-soluble initiator is used, it can be added once the reaction temperature is reached); in stage 4, a latex containing hybrid particles is recovered, which generally consist of a polymer core surrounded by a GO shell; **(F)** Some common applications of Pickering emulsions.
Figure 1. (A) Spherical solid particles at the oil-water interface, illustrating how the three-phase contact angle determines the type of emulsion formed: O/W or W/O. Taken from (Zhang T. et al., 2022a) and reproduced under license: https://creativecommons.org/licenses/by-nc-nd/4.0/; (B) Schematics of how isometric particles and two-dimensional materials cover the surface area of dispersed particles in a PE. Reprinted with permission from Creighton et al., 2014. Copyright 2014 American Chemical Society; (C) Illustration of the exfoliation and oxidation processes needed to obtain GO from graphite; (D) SEM and TEM images of PS-GO microspheres in a PE. Reprinted with permission from Song et al. (2011). Copyright 2011 American Chemical Society; (E) Sequence of steps involved in batch polymerization in a GO-stabilized PE: in stage 1, the organic phase (monomer) is brought into contact with the aqueous phase (GO has been previously dispersed in water); in stage 2, the organic phase is dispersed in the aqueous phase at a high shear energy; in stage 3, emulsion polymerization takes place (when a monomer-soluble initiator is used, it is usually added, dissolved in the monomer, before the emulsion is formed; however, if an aqueous-phase-soluble initiator is used, it can be added once the reaction temperature is reached); in stage 4, a latex containing hybrid particles is recovered, which generally consist of a polymer core surrounded by a GO shell; (F) Some common applications of Pickering emulsions.

A useful quantity related to the stability of PEs is the energy Δ E required to remove a stabilizing solid particle from the oil/water interface. According to Binks (2002), for spherical particles and when the gravitational force is neglected, this energy is defined as:where R is the particle radius and γ O W is the interfacial tension between the oil and water phases. The sign of the cosine function is negative for the removal of the particle into the water phase, and positive for removal into the oil phase. This energy is usually significantly higher than thermal energy, resulting in remarkably stable emulsions compared to traditional ones stabilized by surfactants (Herrera-Ordóñez et al., 2026). Expressions for other particle geometries (e.g., disks and rod-like particles) are available (Vis et al., 2015; Peddireddy et al., 2016). Although the principle for the formation of PEs stabilized with non-spherical solid particles lies in the amphiphilic nature of these particles, the behavior of the emulsions will obviously differ for different particle types (Figure 1B), a factor that should be considered for applications (Creighton et al., 2014).

Δ E = π R 2 γ O W 1 ± cos θ 2

3 Functionalization of carbon-rich particles for pickering emulsion systems

In general, chemical modification of the particle surface is required for the improved stability of the prepared emulsion. This is particularly true for graphene and CNTs, which are considered hydrophobic materials. In the case of graphene, different approaches can be implemented to modify its amphiphilic properties and improve its dispersibility in water (Nikam et al., 2025; Rosales-Guzmán et al., 2025; Sali et al., 2019). The first and easiest method is direct exfoliation and functionalization of graphite to GO by one of the Hummers, Staudenmaier, Brodie, or Tour methods (Nikam et al., 2025; Sali et al., 2019). This procedure introduces functional groups, such as hydroxyl (-OH) and epoxy (C-O-C), into the graphene’s planar structure, along with carboxyl (-COOH) groups, primarily at the edges of the graphene flake (Figure 1C). As a result, GO is a material highly hydrophilic with localized hydrophobic zones, which makes it suitable for O/W PEs (Wang et al., 2023; Yan et al., 2024; Yu et al., 2021; Song et al., 2011; Wu et al., 2022; Zhang L. et al., 2014; Kim et al., 2014). In addition, these functional groups (on the surface or edges of GO) can be utilized to make further modifications to GO, changing its amphiphilic properties for applications in which W/O emulsions are required. Examples are listed in studies by Fei et al. (2016) (modification with hydrophobic alkyl amines), Yang et al. (2019) (edge functionalization), and others (Zhu et al., 2020; Xu et al., 2021).

Inorganic particles can also be directly attached to the surface of graphene using different methods (Xue et al., 2011; Tang et al., 2014; Wang et al., 2021a). For example, a redox reaction between GO and Fe2+ was proposed for the preparation of GO decorated with Fe3O4 nanoparticles for various purposes (Yu et al., 2021; Lin et al., 2015; Hu et al., 2015; Gu et al., 2014). Similar work has been reported for the preparation of reduced GO decorated with Au nanoparticles via a redox reaction between GO and chloroauric acid (HAuCl4) (Tang et al., 2014). In another study, a one-pot hydrothermal procedure was used to chemically reduce GO to graphene and at the same time functionalize the resulting graphene with amine moieties from polyacryloyl hydrazide (PAHz). This material was further used to prepare O/W PEs with olive oil and n-decane (Narukulla et al., 2022). Comparable approaches have been used for the preparation of graphene functionalized with poly (sodium 4-styrenesulfonate) for microencapsulated phase change materials (Zhao et al., 2019), bi-functional GO grafted with polyethylene glycol and 3-aminopropyltrimethoxysilane as a catalyst for aqueous nucleophilic substitution reactions (Yang et al., 2020), and GO modified with polystyrene and π-conjugated end groups (BPS), which was synthesized by reversible addition–fragmentation transfer polymerization for W/O PEs using toluene as the continuous phase (Mi et al., 2020). The functionalization of GO with sodium dodecylbenzene sulfonate and cetyltrimethylammonium bromide has also been reported (Zhang et al., 2021). In all the cases discussed so far, control of the functionalization is somewhat limited because the functionalization is not selective and affects the entire structure of the GO flakes. Selective functionalization of graphene can be performed, giving rise to the formation of Janus nanoparticles with asymmetric properties (Ma et al., 2020; Wu et al., 2015; Sharifzadeh and Parsnasab, 2021; Wu et al., 2015).

The contact angle of GO, and therefore its wettability, can be affected by the level of oxidation. In particular, contact angles of 63.6°, 55.8° and 90.6° can be obtained for oxidation degrees (O/C ratios) of 0.328, 0.469 and 0.295, respectively (Suhaimin et al., 2022).

Ball milling is another alternative to exfoliating graphene that produces relatively prominent results in terms of scalability. Hu et al. (2020) reported preparing zwitterionic graphene nanosheets using the ball milling technique with casein, a protein with amino and carboxyl groups that makes it soluble in acidic and alkaline media (Dhasmana et al., 2022).

Zwitterionic carbon materials can also be prepared from the pyrolysis of citric acid at 200 °C in the presence of air, which leads to the formation of hydrophilic graphene quantum dots (GQDs), typically nanometer-sized (Ma et al., 2021; Ma et al., 2022). Subsequent functionalization of these GQDs with dimethylaminopropylamine and dodecylamine changes the wettability of the carbonaceous material, making it suitable for the preparation of PEs of dodecane in water (Ma et al., 2022). In another study, GQDs functionalized with histidine were used for the preparation of PEs of styrene in water (Li et al., 2016).

In the case of CNTs, oxygen plasma treatment can be applied to modify their wettability for the preparation of PEs of cyclohexane in water (Chen et al., 2010). Additionally, the oxidation of CNTs with nitric acid has been reported as a method to introduce hydrophilic functional groups on their surface while achieving different degrees of wettability (Briggs et al., 2018).

4 Use of GO-stabilized PEs in emulsion polymerization

In recent years, graphene-reinforced polymer composites have attracted considerable interest due to their unique physicochemical and thermomechanical properties (Maity et al., 2025). Improving the dispersion of graphene in polymer matrices to optimize the properties of these composites has been a primary objective of numerous research projects.

Schrade et al. (2013) attributed the significant increase in the number of publications about PEs to their application as templates for obtaining hybrid particles (polymer/inorganic particles) with well-defined structures via heterogeneous polymerization techniques, such as emulsion, miniemulsion, dispersion, and suspension. According to López-Serrano and Fouconnier (2024), Pickering emulsion polymerization is a process in which colloidal stability is primarily imparted by fine solid particles that are adsorbed at the interface of polymer latex particles.

For specific PEs stabilized by GO, there are several options for their use as templates for the synthesis of microspheres, microcapsules, composite materials, and porous materials. Polymeric microspheres, with GO adsorbed on their surface, can be obtained by polymerizing monomers that act as the oil phase in normal PEs (O/W). Microcapsules are obtained by interfacial polymerization of GO adsorbed at the oil/water interface, which creates a protective shell that encapsulates the internal functional substance. Removing the continuous phase, for example, by evaporating water from latexes obtained by polymerization in normal PEs, results in a composite material with improved properties that can be obtained due to better GO dispersion within the polymer matrix. If both the oil and aqueous phases are removed from GO-stabilized PEs, porous materials with interconnected pore structures can be obtained (Liu et al., 2025).

An analysis of the literature about polymerization in normal PEs stabilized with GO to obtain microspheres or composites reveals that the polymerization mechanism does not correspond to that stipulated for polymerization in normal emulsions, where a primary characteristic is the diffusion of monomers and other reagents through the continuous phase during the emulsion polymerization reaction (Herrera-Ordóñez et al., 2026). The first investigations of polymerization in heterogeneous systems in the presence of GO were published at the end of the first decade of this century. Although this topic has not advanced as much as polymerization studies on PEs stabilized with other types of particles, such as silica (Whaval and Tiwari, 2025; Shen et al., 2024), the method’s viability has been confirmed by the production of polymeric PS microspheres surrounded by GO platelets (Song et al., 2011), as seen in Figure 1D. Polymerization studies in PEs stabilized with GO as the sole surfactant have been primarily focused on styrene (St) and methyl methacrylate (MMA) (Fadil et al., 2022). Figure 1E shows the basic sequence of steps that are followed in a PE polymerization. In the case of studies conducted on GO-stabilized PEs, the majority of works vary only one or two parameters, and the results are insufficient to draw conclusions about the polymerization mechanism. This is especially true since the emulsion preparation method often differs. In some cases, high-shear energy is used, as in the formation of miniemulsions; in others, only mechanical agitation is employed. In conventional emulsion polymerization, radical entry/exit phenomena between the particles and the aqueous phase determine the overall kinetics and growth of the polymer chains, which also determines their molecular weight. The initiator is soluble in the water phase, and the radicals must enter the particles, leading to the compartmentalization of these systems. This means that, at any given time, there are either zero or one radical in each particle. In contrast, in the few cases of emulsion polymerization reported in the presence of GO, the initiator is AIBN (Xu et al., 2021, and Li Y. et al., 2023), which is soluble in the organic phase; this suggests that the mechanism may be closer to that of miniemulsion polymerization instead of emulsion polymerization. Therefore, it is an open question whether the system is compartmentalized. In addition, the relatively large GO plaques covering the particles may hinder the radical exchange between the organic and the aqueous phases. In conclusion, at this point it is not possible to establish the mechanism of emulsion polymerization stabilized with solid particles, particularly with GO.

Reviewing the factors that affect the colloidal stability of GO-stabilized PEs could help to predict the colloidal stability of the system during the polymerization reaction: oil type, sonication time, GO concentration, oil-to-water ratio, and pH values (He et al., 2013). For example, Che Man et al. (2013) used GO nanosheets (with lateral dimensions smaller than 100 nm) to stabilize mini-emulsions using monomers with different polarity. Their results are consistent with those reported by Thickett and Zetterlund (2015), who studied the influence of oil phase polarity on the ability of GO nanosheets to stabilize normal PEs. GO adsorption at an oil/water interface must be thermodynamically favorable; therefore, high interfacial tension between non-polar oils and water is a driving force for GO adsorption at the interface. As the polarity of the oil increases, emulsions tend to become more unstable or simply fail to form.

5 Carbon materials used as solid particles in pickering emulsions

The subject of Pickering emulsions stabilized with different types of carbon allotropes or carbon derivatives has been recently reviewed by Liu et al. (2025), whose study focused on the stabilization mechanisms, preparation, characterization, and applications of GO-stabilized PEs. Additionally, Chen et al. (2025) reviewed the use of PEs stabilized with graphene derivatives (GDs) to create porous graphene materials after eliminating the liquid phases from the emulsion. In another recent review, Abu Zaid et al. (2024) discussed PEs that use GDs or CNTs, in addition to metal-organic frameworks (MOFs). Similarly, Zhang et al. (2022a) reviewed PEs stabilized by MOFs, GO, and graphitic carbon nitride, along with their applications. Table 1 contains a list of applications of PEs stabilized by graphene and GDs that were reported in the last 5 years (2021-2025) found via a Scopus search. The search criteria used were: i) Pickering emulsions and Graphene (in the title, 2020-26); ii) Pickering emulsions and carbon (in the title, 2020-26). Other search criteria used throughout the manuscript included (in Scopus): iii) Pickering emulsions and carbon nanotubes (in the title, abstract, or keywords, −2026). In SciFinder, the criteria were: i) Pickering emulsions, filtered by document type (journal or review) and search within results for graphene oxide. GO is the carbon-based material most frequently used in PE according to the literature review, primarily due to its amphiphilic nature with adjustable wettability.

TABLE 1. Last 5 years applications of graphene oxide, graphene, and other graphene derivatives as PE stabilizers.

Solid particlesPE componentsApplicationsCommentsReferences
Graphene oxideO/W emulsions of paraffin in water/ethanol solutionsFormation of paraffin-encapsulated porous GO for personal thermal management technology using paraffin as a phase-change materialPEs are an intermediate step to uniformly encapsulate small-sized paraffins inside a porous GO skeleton by freeze-drying PEs. Using 7.4 wt% GO achieves encapsulation efficiency of 100%, and a thermal conductivity of 1.3 W/(m·K) for the compositeFu et al. (2025)
GO (mixed with carbon nitride, g-C3N4)O/W emulsions of n-hexane in waterDevelopment of tunable catalytic systems for organic pollutant degradation and functional materials synthesisStabilization by concentrated solutions of solid nanoparticles; up to 6 mg/mL of g-C3N4 The zeta potential of the precursor g-C3N4 hydrosol of 6 mg/mL is −33 mVGorshkova et al. (2025)
GO/MWCNTsEmulsions of cross-linked silicone rubber (SR) in waterFormation of polymer composites with a segregated structure of reduced GO (RGO)/MWCNTs in a silicone rubber (SR) matrix for high electrical conductivity and high electromagnetic interference shieldingPEs stabilized with GO/MWCNTs particles are an intermediate step for the formation of the composites. PEs are freeze-dried to eliminate the water and hot-pressed. The final composite has an electrical conductivity of 12.5 S/m and an electromagnetic interference shielding effectiveness of 41.4 dBWang et al. (2025)
Cellulose nanocrystals (CNCs) and GO (coated with polydopamine and melamine formaldehyde (MF) resin)Emulsions of docosane (C22) and octadecane (C18) in waterEncapsulation of PCMs (phase-change materials) (C18 and C22) in polymers for energy storageFinal product: PCM microspheres with PDA-coated CNCs and reduced GO (rGO) as shells. The PCM@CNC/rGO/PDA/MF microcapsules have a high content of encapsulated PCMs (84.2%)Sun et al. (2024)
GOW/O emulsions of water in an oil phase of a solution of diamino-functionalized polydimethylsiloxane polymer in dimethyl silicone oilWater-in-oil pickering emulsion gel lubricant with good swelling and corrosion resistanceParticle size of the PE gel was approximately in the range of 50–120 nmYu et al. (2024)
Cellulose nanofibers (CNFs) and GOO/W emulsions of paraffin wax (PW) solution in 1,2-dichloroethane (oil phase) in waterCarbon aerogel films for lightweight smart devicesPEs are an intermediate step. After freeze-drying and carbonization to pyrolyze the paraffin, the aerogel is generated. The aerogel with 30% PW reaches 105 °C (20 s, 5 V) and 71.4 °C (25 s, 100 mW/cm2)Qiu et al. (2024)
H3PW12O40 (HPW) supported on graphene oxideSimulated sulfurated oil (thiophenes in n-octane) dispersed in acetonitrileCatalytic oxidative desulfurization (CODS) system for fuel oilHPW is the base of the catalytic system acting at the interface of the PE to reduce mass transfer limitations during oxidation reactions. The HPW catalyst enables a sulfur removal efficiency of 97.01%Dou et al. (2024)
Hexadecylamine-modified GODMSO (disperse phase) in a methyl polysiloxane (preceramic polymer precursor) solution in cyclohexane (continuous phase)Porous polymer-derived ceramic (PDC) monoliths as electrode materials for Li-ion batteriesPEs are used as a soft template precursor that is freeze-dried and pyrolyzed to generate silicon oxycarbide (SiOC) from the polymer precursor. An electrode containing 23% GO by mass, after pyrolysis at 900 °C, achieved insertion and extraction capacities of 2399 and 1176 mAh g-1, respectively, at a current density of 50 mA g-1Karamoko et al. (2024)
Graphene oxide (GO) nanosheets decorated with silver nanoparticles (AgNPs)Styrene and acrylate monomers/copolymer in waterPreparation of nanocomposites of Ag NP and GO in a poly (styrene-co-acrylate) matrix for antibacterial applicationsPEs originally contain monomers in the dispersed phase that are then converted into a copolymer by pickering-stabilized emulsion polymerization. The composite film exhibited higher thermal stability than the PSA film (T-degradation = 348 °C)Liao et al. (2023)
Spherical cellulose nanocrystals (S-CNCs) and GOn-hexadecane in water (O/W)Stability-tunable PEs by varying the S-CNCs/GO ratio for future biomedical and composite materials applicationsGO assembles into a 3D network. The PE reaches 100% stability at a GO concentration of 3.0 g/LChen et al. (2023)
GOLiquid paraffin in water (O/W)3D-printable ink and model for rheology studies of emulgelsCo-stabilized by didodecyldimethylammonium bromide (DDAB) as an auxiliary surfactant. The typical droplet size is ∼40–60 μmCui et al. (2023)
Quantum-dots GO (GOQD)Squalene in water (O/W)Adjuvant to increase immune responses to the Chlamydia trachomatis Pgp3 recombinant vaccineGOQDs are an effective loading platform for a variety of drugs and biomoleculesAverage droplet size 422 nm and zeta potential −52.7 mV of the PE Zhao et al. (2023a) Average droplet size of 1.8 μm and a zeta potential of −25.0 ± 1.3 mV for PEs (Zhao et al. (2023b)Zhao et al. (2023a), Zhao et al. (2023b)
Chitin/graphene oxide beadsIsooctane in water (O/W)Immobilized laccase in a porous chitin (Ch)/GO aerogel for synthetic dye removal from waterPorous Ch/GO aerogel beads obtained by the emulsion template method and freeze-drying for laccase immobilization. In the PE, droplet diameters ranged from ∼15 to ∼35 μmHuang et al. (2023)
Cellulose nanofibers (CNFs) and GOSolution of different polymers (PC, NBR, PS, ABS or PMMA) in 1,2-dichloroethane (oil phase) in water (O/W)Compressible multifunctional carbon aerogels as pressure sensors with different properties depending on the precursor polymerThe PE was freeze-dried to eliminate water and volatiles and then subjected to thermal annealing and pyrolysis to form the carbon aerogel Contact angles of CNF/GO nanogels with PC, PS, and PMMA were 93.9°, 105.9°, and 83.2°, respectively. The aerogel exhibited good thermal insulation, reaching 58.3 °C on a 160 °C hot plateLiao et al. (2022)
GOOil phase: Core/shell polymer in water; (O/W) emulsion. Core: (Poly (styrene-acrylate))+paraffin. Shell: PolysiloxaneProtective coatings for cementitious materials. PSA-siloxane composite emulsions are synthesized by making core-shell structures grafted together by cross-linking agentsThe PE originally contained the core monomers in the dispersed phase, which are then copolymerized by PE polymerization; then, silane monomers added in a semicontinuous fashion are polymerized into a shell.The mean particle size of the PEs was 113 nm with PDI = 0.26 nm. Grafting proportions: 85%–88%. The PE resulted in a contact angle >30° and reduced capillary water absorption of concrete by 98.3%Wu et al. (2022)
Fe3O4/GOStyrene monomer/polymer in water (O/W)Fabrication of magnetic and semiconducting composite particles of Fe3O4/GO-polystyreneThe PE originally contains styrene monomer in the dispersed phase, which is then polymerized by PE stabilized by the iron oxide/GO particles.The Fe3O4/GO particles were ∼10 nm, while the PE particles were approximately 30–50 nmLu et al. (2022)
GO (janus 2D nanosheets)Wax in water (O/W) emulsion as templatePreparation of janus nanosheets of GO decorated with styrene (St)-acrylamide (NIPAM) based copolymers for catalytic applications. PE used to prepare Wax-GO solid particles that are then used in solution to attach previously prepared polymers to the GO particlesTwo sets of copolymer-GO materials were prepared: PNIPAM-GO-p(VBTAC-co-St)@Pd and PSt-GO-p(NIPAM-co-MQ)@Pd, where VBTAC is vinylbenzyltrimethylammonium chloride and MQ is 5-(2-methacryloyl-ethyloxymethyl)-8-quinolinol.The diameter of the polymer-modified wax@GO particles was approximately 30 μmCui et al. (2022)
GO-TiO2Bisphenol a epoxy acrylate resin (BAEA) (oil phase) in water (O/W)Photo-responsive self-healing polymer composite based on BAEA resin @graphene oxide microcapsules (BAEA@GOMCs) applied as a coating of steel partsEmbedding of BAEA@GOMCs was carried out in a waterborne epoxy matrix.Particle size of PE 1–9 μm with an average ∼5 μm. Oil phase encapsulation was achieved using 4 wt% GO.Yu et al. (2022)
GO-g-polymerParaffin (oil) in water (O/W)Composite of a phase change material (paraffin) modified with GO-polymer for improving thermal conductivityThe leakage rate of paraffin was only 1.1%–1.3% after 1000 cycles. The thermal conductivity of the composite reached 3.968 W·m-1·K−1 with 0.4 wt% GO contentYang et al. (2022)
GOPhenacyl bromide (reactant) in toluene (oil phase) in water (O/W). The second reactant is thiourea (water soluble)PEs are used as a green reaction device (each emulsion droplet is a nanoreactor) for the synthesis of 2-aminothiazole from PB and thiourea (water soluble)After the reaction, the product was extracted with ethyl acetate, washed with water, and dried with sodium sulfate. The PE exhibited a zeta potential of −15 mV and a PDI value of 0.396. GO PEs resulted in isolated yields of 85%–90% for the synthesis of 2-amino-4-phenylthiazoleSadgar et al. (2021)
Amphiphilic GO (or SCGO: GO functionalized with two surfactants: DTAB and CTAB)Water in oil. Oil phase: PDMS in paraxylenePDMS composites with SCGO having gas barrier propertiesThe emulsion was freeze-dried to remove water and paraxylene to leave hollow GO shells in a PDMS matrix, which was then hot-pressed to form films.The contact angles of GO and SCGO were 30.7° and 94.5°, respectively. Droplet sizes in the PE ranged from 10 to 40 μm. At 3 phr of SCGO, the gas barrier properties of composites increased by 85.7% vs. PDMS aloneZhang et al. (2021)
GO/porphyrin-based MOFsTwo types: 1) oil in water. Oil phase: Porphyrins in chloroform; 2) n-hexane (non-polar) in porphyrin-containing DMSO (polar)Preparation of MOFs integrated with inorganic colloidal carriers for possible application in selective sorption and photocatalysisZinc acetate is used as an adhesion layer between the MOFs and GO. Average droplet size of the initial emulsion: 45 μmNugmanova and Kalinina (2021)
GO (janus nanoparticles)Melted wax (oil) in water (O/W emulsion)Preparation of janus GO nanoparticles for diverse potential applications: Drug delivery, sensors, compatibilizers, and so onSize of synthesized hollow GO particles was 50–242 nm. Three-phase contact angles of 58.14° for nano- and 130.85° for the microparticles in the PEsSharifzadeh and Parsnasab (2021)
GO and cellulose nanofibrilsNBR in 1,2-dichloroethane solution (oil) in water (O/W)Preparation of flexible/conductive nitrile rubber (NBR) composite films as electromagnetic interference (EMI) shielding materialsThe PE formed a gel that was then filtered, reduced with hydrazine hydrate, and hot pressed. Mean droplet size of the PEs was 73–89 μmWang et al. (2021b)
GO modified with iron oxide nanoparticlesGlycidyl methacrylate (GMA) (oil phase) in water (O/W)Preparation of GO microcapsules for self-healing epoxy resin coatingsA PE was prepared with GO microcapsules as the dispersed phase. The emulsions were further mixed with a waterborne epoxy matrix to get the liquid coating. The mean droplet size of the PE was 4.36–6.09 μmYu et al. (2021)
Chitin modified with GOOil phase: Paraffin wax and isophorone diisocyanate (polyurea precursor) in water (O/W). Water phase: Water and chitinFormation of microencapsulated phase change materials for thermal energy storage. GO contributes as a photothermal functional fillerOnce the PE is formed, the diisocyanate is reacted with ethylene diamine via interfacial polymerization to form polyurea in the oil phase. The mean particle size of PEs was approximately 10–40 μmMaithya et al. (2021)
GO modified with γ-methacryloxy propyl trimethoxy silaneOil phase: Paraffin, styrene, divinylbenzene (DVB) and AIBN, in water (O/W)Formation of microcapsules of paraffin with a PS + GO shell. Used as part of a multiprotective coating after being mixed with silicone resinThe PE is heated to obtain crosslinked PS (styrene + DVB with AIBN as initiator) in the core of microcapsules. GO is then reduced. Droplet size of the PE < 1 μmXu et al. (2021)
Double PE: hydrophilic partially reduced GO encapsulating W/O droplets stabilized by hydrophobic reduced GO quantum dots (r-GOQDs)Internal PE: W/O emulsion with oil phase containing L-Cysteine (L-Cy), stabilized by r-GOQDs. External (W/O)/W stabilized by GO. Oil phase consisting of toluene and monomers acrylic acid and ethylene glycol dimethacrylate with AIBN (initiator) + L-CyFabrication of hollow imprinted microspheres (H-IMMs) for the detection of L-CysteineThe PE is heated at 70 °C to generate crosslinked poly (acrylic acid) in the oil phase. The L-Cy (imprinting) and water (hollow sites) are then removed. Mean diameter of the PEs decreased from 48.2 to 16.7 μm when pH varied from 4 to 12Hosseinzadeh et al. (2021)
Self-assembled bromoacetic acid (BA) modified-amphipathic hydroxyethyl cellulose (MAHEC) and GOOlive oil (oil phase) in acrylamide + bisacrylamide and KPS solution in water (O/W)Hydrogel formation for pH-sensitive release of doxorubicin hydrochloride (DOX) (cancer treatment)The PE was heated at 60 °C to form polyacrylamide, followed by drying and extraction of the oil phase to form a hydrogel. Water contact angle in olive oil of GO/MAHEC: 88°. The mean particle size of PEs was 4.6–10.5 μmWang X. et al. (2021)
GO and lead tungstateParaffin (oil) in water (O/W)Fabrication of multifunctional microparticles of phase change materialsThe PE is co-stabilized by a styrene-maleic anhydride copolymer surfactant. The zeta potential of the PE was as high as −108.59 mV. Modes (peaks) of distribution sizes of microcapsules were between 700 and 1000 μmWei et al. (2021)
GOLinseed oil in water (O/W)Preparation of healing microcapsules in a self-healing coating systemContact angle of the prepared GO: 46.5°. The mean diameter of PEs ranged from 8.02 to 20.36 μm with coefficients of variation between 0.24 and 0.73Sahir et al. (2021)
Alkylated GO nanosheets (AmGO)Water in toluene (W/O)Encapsulation of ammonium dinitramide (a green oxidizer used in propellants) for hygroscopic inhibitionThe PE was subjected to vacuum-assisted solvent extraction to generate the final material. AmGO had a contact angle of 110° (hydrophobic). Average water droplet size 24.8 μmYan et al. (2021)
Graphene oxide/polyurethane/polyanilineIsophorone diisocyanate (IPDI) and 4,4′-methylene bis(phenyl isocyanate, MDI) (oil phase) in water (O/W)Fabrication of microcapsules for self-healing, anti-corrosive coatingsAfter forming the PE, 1,4-butanediol was added to react with MDI and form polyurethane by interfacial polymerization (IP). Then, the PANI was deposited on the surface of dried particles by IP of aniline. Average particle diameter 3.11 μm and encapsulation efficiency of 78.19%Yan et al. (2024)
Graphene oxiden-hexane (oil) in water (O/W)Fabrication of macroporous graphene aerogel (MGA) for high-performance pressure sensorsN-hexane was evaporated from the PE, and then water was removed by freeze-drying to obtain the MGA, which was finally combined with expanded thermoplastic polyurethane to build the flexible sensor. The aerogel had pore diameters of ∼100 μm. Resistivity of 33.664 Ω cm and electrical conductivity of 0.024 S/cmZhao W. et al. (2023)
Graphene quantum dots (GQD) modified with PdToluene (oil) in water (O/W)Electrooxidation in immiscible oil-water electrolytes, specifically of benzylamine to N-benzylidenebenzylamine (NBB)Average droplet diameter of the PE: 10.6–14.6 μm. High NBB selectivity >80%Huang et al. (2025)
Alkylamine (AA) functionalized graphene quantum dotsAlkylamines used: C8, C12 and C16Trichloromethane (CHCl3) (oil) in water (O/W). The oil phase may or may not contain poly-3-hexylthiophene (P3HT) dissolved in itPreparation of P3HT nanoparticles (photo-active conjugated polymer)To prepare the nanoparticles, CHCl3 was evaporated from the PE. The average diameter of PEs: 1.9–24.3 μm. Contact angle: 60°–113.5°, from C8 to C16 AA, respectivelySong and Im (2024)
Graphene nanosheets (GN)/pristine graphite (PG) = GNPGStyrene (oil) in water (O/W). The styrene phase also contained AIBN to be further polymerized at 70 °CPreparation of nanocomposites of polystyrene (PS) with GNPGThe solid (PS with GNPG) recovered from the PE was further mixed with commercial PS to produce the nanocomposite. The average particle diameter of PEs ranged from 115 to 760 μmLi et al. (2023a)
Sulfonated graphene (SG)N-octadecane (oil) in water (O/W)Microencapsulated phase change materials (MCPCMs) for energy storage with a shell made of SG + MUFAn emulsion of the melamine-urea-formaldehyde (MUF) prepolymer was added to the PE and further polymerized to obtain MCPCMs after drying.Contact angle of MCPCMs:116°Li et al. (2023b)
Ionic liquid-modified reduced graphene oxide (rGO-IL)Aniline (oil) in water (O/W)Fabrication of a graphene/polyaniline (PANI) hybrid hollow capsule for supercapacitorsThe aniline in the PE was interfacially polymerized to generate the PANI. The synthesized rGO-IL/PANI hollow spheres achieved a capacitance retention of 92.4%Li Y. et al. (2023)
Graphene with Pt nanoparticles on vulcan carbonHexane (oil) in acetonitrile (O/A) co-stabilized by a polymer of ethyl cellulosePreparation of graphene-Pt/Vulcan carbon (Pt/C) catalysts for the cathode oxygen reduction reaction in polymer electrolyte membrane fuel cellsHexane was evaporated from the PE, which was then filtered and dried to obtain the final material. Hexane phase 20% in volumePark et al. (2022)
Nanocomposite of poly (acryloyl-hydrazide)/reduced GOOlive oil or n-decane (oil) in water (O/W)Preparation of polymer-graphene nanocomposites (NC) in a single-pot process further used as a pickering stabilizerThe PE stabilizer exhibits -NH2 groups in the polymer for further reactions. The NC exhibited an average hydrodynamic size of ∼40 nmNarukulla et al. (2022)
Zwitterionic group-functionalized graphene quantum dots (ZGQD)Dodecane (oil) in water (O/W)pH-responsive pickering emulsions for controlled drug releaseFe3O4/rGO contained spherical Fe3O4 nanoparticles with sizes ranging from 4 to 10 nmMa et al. (2022), Xue et al. (2011)
Amphiphilic graphene quantum dots functionalized with alkyl groupsDodecane (oil) in water (O/W)pH-responsive pickering emulsion based on amphiphilic graphene quantum dots for potential application in enhanced oil recovery and oil/water separationReducing the content of hydrophobic groups increased the emulsion droplet size from 20 μm to >100 μmMa et al. (2021), Ma et al. (2022)
MnO2-decorated grapheneAniline in toluene (oil phase) in water (O/W). Water phase contained ammonium persulfate as polymerization initiatorFabrication of polyaniline/MnO2/graphene ternary hybrid hollow spheres for electrochemical supercapacitorsAniline was interface-polymerized in the PE; then the solvent and water were removed by freeze-drying. Emulsion droplet size: 20–50 μmWang et al. (2021a)
Graphene or PVA/grapheneO/WPreparation of two different kinds of graphene-based aerogels for organic adsorptionAverage emulsion droplet size increased from 12.49 μm to 41.68 μm as the O/W ratio increased from 1:5 to 4:5Liu et al. (2021)

Color code: Green: phase change materials, pink: catalysis or reaction-related application, light blue: composites with enhanced properties, dark blue: aerogels, lilac: electrochemical applications, yellow: drug delivery, light yellow: coatings.

The table is organized according to three criteria: 1) The first part of the Table shows GO-related PEs; the second part includes all other carbon derivatives as PE stabilizers; 2) Within each part, the most recent works are listed first (starting from 2025 down to 2021); 3) A color code is used to identify the area of application. The code explanation is above.

According to Table 1, some of the most common applications of GO-stabilized PEs include encapsulating phase change materials (PCMs), such as paraffins, for thermal energy storage to avoid the leaking of the encapsulated material (Fu et al., 2025; Sun et al., 2024; Yang et al., 2022; Maithya et al., 2021; Xu et al., 2021; Wei et al., 2021) (Figure 1F). In these cases, the stabilizing materials in the PEs eventually form an encapsulation shell with high retention of the PCM.

Other common applications include the preparation of self-healing coatings for use on diverse materials (Yu et al., 2022; Yu et al., 2021; Sahir et al., 2021; Yan et al., 2024); the preparation of composites (Wang et al., 2025; Liao et al., 2023; Chen et al., 2023; Lu et al., 2022; Yu et al., 2022; Zhang et al., 2022b; Wang et al., 2021b), some of them involving polymerization in PEs (Liao et al., 2023; Lu et al., 2022); the fabrication of porous aerogels using PEs as templates (Huang et al., 2023; Liao et al., 2022; Zhao W. et al., 2023; Qiu et al., 2024); and the preparation of materials for biomedical applications, such as vaccine adjuvants (Zhao et al., 2023a; Zhao et al., 2023b) or carriers for controlled drug release (Wang X. et al., 2021). In general, compared to other techniques for preparing materials for similar applications, the PE technique with GO presents the advantages of relative ease of preparation and tunability of GO (via intensity of chemical modification) as a stabilizer of PEs, depending on the requirements of further steps in the final material preparation process.

In a second set of carbon-based materials, we grouped graphene, functionalized graphene, reduced GO, and graphene quantum dots. Table 1 also shows applications of this second set of materials as PE stabilizers reported in the last 5 years. The main areas of application are similar to those described for PEs in the upper part of Table 1; that is, PCM encapsulation (Li et al., 2023b), composite preparation (Li Y. et al., 2023; Narukulla et al., 2022), aerogel fabrication (Liu et al., 2021), and controlled drug release (Ma et al., 2022).

Comparing the different carbon-based emulsion stabilizers, judging by the number of articles in the last decade, the most important ones in descending order are 1) GO, 2) other GDs, 3) CNTs, and 4) carbon quantum dots. GO already has an amphiphilic nature, which is necessary for it to be allocated at the W/O interface and act as a stabilizer; it also possesses functional groups that allow for further modification and versatility, making it hydrophilicity-tunable. It is also simpler to prepare. All these characteristics contribute to its importance for PEs. In fact, looking at Table 1, more than 75% of the entries correspond to GO PEs. The remaining (∼24%) entries correspond to all the other carbon materials. Other GDs can reach attributes similar to GO’s, but they usually require additional chemical steps (e.g., GO formation, reduction to graphene, and further chemical modification). CNTs are more difficult to synthesize than GO and require further complex chemical modifications to acquire amphiphilic characteristics since they are extremely hydrophobic. From an industrial point of view, CNTs are in a more mature stage of development with some well-identified areas of application, with their use as additives in Li-ion battery electrodes being their main growth driver. However, they are more difficult to produce in a reproducible way compared to graphene or GO. Although both GO and CNTs are produced on a large scale primarily by chemical vapor deposition, in both cases quality reproducibility is problematic (ACS Materials Team, 2025). In general, basic research on carbonaceous materials has shifted away from CNTs to GDs and GO in particular, due to the reasons discussed above. Although for some specialized applications CNTs may present advantages, the trend points to GO as the main carbon-derived material to be used as a stabilizer in PEs in the foreseeable future (Schuett, 2025).

Quantitative features of PEs or final materials are included in Table 1 (Comments column); however, it is difficult to make a systematic comparison of these features among the different applications given their variety and the fact that different authors include different information. Nonetheless, the reader can make some comparisons among similar applications with the information provided.

Regarding the production costs of GDs and CNTs, they are still relatively high, although they vary considerably depending on scale, application, and production efficiency. Costs are expected to decrease significantly in the next 5–10 years as production increases. Since these materials are used in relatively small proportions for some applications, the cost is not an issue, but this may not be the case for PEs. In short, the specific application will determine its economic viability (ACS Material LLC, 2025; Eco Zhang, 2025).

The health risks of these materials have been studied for more than a decade. They are known to present different levels of toxicity depending on their dimensions, modifications, and purity, although it seems that CNTs are potentially more harmful than GDs (Zhang Y. et al., 2014; Gendron and Bubak, 2023). This includes direct cell damage (to the membrane, mitochondria, and DNA) (Luan et al., 2015). Surface modification appears to attenuate the toxicity of these materials. The subject is still under study, and more research is needed to reach solid conclusions since there are still many unanswered related questions.

Finally, regarding the environmental effects of these materials, PE applications should be designed by taking into account their final fate once the associated product has reached its end of life, as is presently done with the majority of material developments. This is a complex challenge that has largely been overlooked in the literature thus far.

6 Conclusion

Among the different types of carbon-rich materials used as stabilizers in PE, GO is by far the most popular, due to its inherent amphiphilicity, which provides remarkable stability to PEs. Another, less common possibility is the use of chemically modified graphene (excluding GO) as an effective PE stabilizer. Regarding the mechanism of stabilization, this is only partially understood, assuming some idealized conditions, e.g., spherical particles, which are not always met. The mechanism of emulsion polymerization stabilized by solid particles, particularly graphene derivatives, is also poorly understood and remains an open scientific question. To advance in the elucidation of this mechanism, further studies on different types of monomers are required to establish the effects of variables such as the GO oxidation degree, GO sheet size, GO concentration, initiator type, and temperature on conversion vs. time, particle size and particle number evolution, Zeta potential, and TEM morphology. Additionally, the self-assembly of structures when the continuous phase is eliminated from a PE, which is key in the determination of the properties of the resulting material, is poorly understood and requires further studies to capture its key features and mechanisms. In the coming years, many new applications of carbon-rich materials as PE stabilizers will be developed, but extensive research is needed to improve our understanding of these systems.

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Footnotes

Edited by: Kamal Essifi, Chouaib Doukkali University, Morocco

Reviewed by: Vedanshu Malviya, GH Raisoni University, India

Statements

Conflict of interest

The author(s) declared that this work was conducted in the absence of any commercial or financial relationships that could be construed as a potential conflict of interest.

The author ES-G declared that they were an editorial board member of Frontiers at the time of submission. This had no impact on the peer review process and the final decision.

Funding

The author(s) declared that financial support was not received for this work and/or its publication.

Author contributions

MR-G: Investigation, Methodology, Writing – original draft. MT: Conceptualization, Investigation, Methodology, Writing – original draft, Writing – review and editing. ES-G: Conceptualization, Investigation, Methodology, Supervision, Writing – original draft, Writing – review and editing.

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Citation

Rosales-Guzmán, M., et al. (2026). Pickering emulsions: emulsion polymerization and systems stabilized with carbon allotropes or carbon-rich materials. Frontiers in Soft Matter, Volume 6. https://doi.org/
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Copyright © 2026 Rosales-Guzmán, Treviño Martínez and Saldívar-Guerra.

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*Correspondence: Enrique Saldívar-Guerra

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