Pickering Multiphase Materials Enabled by Plant-Based Particles: Stabilization Mechanisms and Template-Directed Architectures

Abstract

Engineering forestry bioresources into high-value materials is central to achieving global sustainability goals, but requires innovative strategies, such as leveraging widely available forest-derived biopolymers and bioparticles. This review highlights pathways toward advanced biobased materials by exploiting their inherent interfacial activity to create multiphase functional systems. The distinctive interfacial behavior and physicochemical tunability of forestry-derived components enable robust performance across a wide range of architectures, with particular relevance to emulsion-based platforms. We show that plant-based Pickering emulsions provide versatile templates for applications spanning food formulations, nutrient delivery, and the fabrication of multidimensional structures, including microspheres, fibers, and porous scaffolds. Finally, we discuss emerging challenges and opportunities in interfacial engineering and scalable processing, outlining pathways that bridge biomass valorization with high-performance, sustainable material design.

Graphical abstract

Keywords

Forestry bioproducts / Plant-based nanoparticles / Plant-based biopolymers / Food emulsions / Packaging materials / Controlled release

Highlight

	● Forestry-derived particles are emerging as sustainable stabilizers for Pickering multiphase systems.
	● Particle wettability, charge density, and aspect ratio regulate emulsion structure and performance.
	● Plant-based Pickering emulsions enable applications ranging from food systems to nutrient delivery.
	● Pickering systems serve as versatile templates for multidimensional material fabrication.

1 Introduction

Forest has long served as a fundamental bridge between human society and natural ecosystems. From early wood-derived tools and fuels to architectural timber systems that enabled the rise of agrarian civilizations, the efficient use of forest resources has consistently reflected the depth of human–nature coexistence [1–4]. In the contemporary context of global carbon neutrality and green manufacturing, forestry engineering faces a renewed mandate: to move beyond the traditional perception of wood as a bulk structural material and to position forest-derived biomass as a strategic feedstock for high-value, functional, and sustainable advanced materials [5-12]. Achieving this transition is critical for upgrading the forestry sector and establishing a competitive bio-based economy within markets still largely dominated by standardized petrochemical products [13]. Compared with fossil-derived materials, forest biomass offers distinct advantages, including renewability, biocompatibility, biodegradability, low toxicity, and its function as a natural carbon sink [14]. These attributes make forestry-derived materials particularly attractive for applications related to human health, environmental remediation, packaging, and sustainable manufacturing [15-22].

A defining characteristic of many forestry-derived biopolymers is their intrinsic amphiphilicity, which arises from abundant surface functional groups, hierarchical morphologies, and partially crystalline structures [21,23,24]. These features enable forestry-derived micro- and nanoparticles to strongly, and often irreversibly, adsorb at fluid–fluid or gas–liquid interfaces, providing exceptional potential for stabilizing diverse multiphase systems [25]. Multiphase systems, including emulsions (liquid–liquid) and foams (gas–liquid), underpin a wide range of applications in the food, cosmetic, pharmaceutical, and materials industries [26-28]. As demonstrated initially by Ramsden and Pickering, colloidal particles can assemble at interfaces to form mechanically robust interfacial layers, stabilizing emulsions and foams through what is now known as Pickering stabilization [29,30]. Compared with conventional molecular surfactants, Pickering systems exhibit remarkable resistance to environmental stresses, including changes in pH, ionic strength, temperature, and shear. This robustness arises from the high desorption energy of interfacial particles combined with electrostatic and steric stabilization mechanisms [31-33]. As a result, Pickering emulsions are particularly promising for enhancing shelf-life and enabling new functionalities. [34,35]

Over the past two decades, research on Pickering stabilization has been dominated by synthetic particles, including silica and metal oxides, owing to their uniformity and tunable surface chemistry [36-39]. However, growing demand for sustainable, biocompatible, and environmentally benign stabilizers has driven increasing interest in naturally derived alternatives. Among these, plant-based colloids, particularly lignocellulosic nanoparticles such as cellulose nanocrystals (CNC), cellulose nanofibrils (CNF), and lignin nanoparticles (LNP), have attracted significant attention due to their biodegradability, structural diversity, and distinctive interfacial properties [40-43]. These particles have been widely explored for nutrient encapsulation and delivery [44-46], fat replacement [47,48], flavor retention [49], oxidative stabilization [50,51], controlled release [52-54], and environmental remediation. [55,56]

Beyond emulsion stabilization, Pickering emulsions also serve as versatile platforms for templating one-dimensional fibers, two-dimensional films, and three-dimensional porous architectures with tunable mechanical, transport, and functional properties [32,57–59]. Through phase-solidification processes such as drying, polymerization, or induced phase transitions, the microstructure of emulsions and foams can be translated into hierarchical biobased materials [16,20,25,36,60]. However, the complex interactions between biobased components and solvents, particularly water, introduce challenges in preserving porosity and structural integrity during processing, often leading to deformation or defects [34,61,62]. Addressing these challenges requires a deeper understanding of the interfacial stabilization mechanisms and structural resilience imparted by forestry-derived particles.

Although several excellent reviews have summarized Pickering emulsions, nanocellulose-based stabilizers, or food-related applications individually, a comprehensive perspective that connects forestry-derived particulate stabilizers, interfacial assembly mechanisms, and their emerging roles in hierarchical material fabrication remains limited. In particular, most existing reviews focus primarily on emulsion stabilization and delivery functions. Therefore, this review aims to bridge these areas by integrating recent advances in forestry-derived particles, their interfacial assembly behavior, stabilization mechanisms, and applications spanning both food systems and functional materials.

In this review, we first examine the physicochemical characteristics of plant-based particles, with emphasis on forestry-derived micro- and nanoparticles, that govern their interfacial behavior in Pickering emulsions. Unlike prior reviews that focus primarily on food emulsions or individual nanoparticle classes, we integrate forestry-derived particles across food and materials applications, emphasizing interfacial assembly as a unifying design principle and highlighting emerging routes toward scalable, multifunctional multiphase systems. We also discuss emerging challenges and future opportunities in leveraging lignocellulosic particles for sustainable multiphase structuring, material fabrication, and food applications (Fig. 1).

2 Plant-based Ingredients Suitable for Emulsions

Various plant-derived ingredients can be used for emulsion stabilization, which can be classified into particulate stabilizers, lipids, and additives. In most cases, these ingredients are extracted and separated from the bulk plants into specific structural elements, followed by controlled reassembly during emulsion formation and stabilization. In this section, we provide a brief summary of plant-derived ingredients that can be potentially used to form emulsions.

2.1 Plant-based stabilizers

Emulsion is a thermodynamically metastable system, while its kinetic stabilization can be enabled by emulsifiers or stabilizers via reducing the interfacial tension between phases and generating a protective surface coating on the droplets, offering electrostatic and/or steric repulsions [63]. Regarding plant-based emulsions, appropriate stabilizers should be identified and used accordingly (Table 1).

2.1.1 Plant-based polysaccharides

Plant-derived polysaccharides, in the form of surface-active biopolymers or insoluble (nano)particles, have been used as stabilizers for emulsions and as additives to adjust their water phase (e.g., as a thickening agent) [80,81]. They exhibit different molecular, physicochemical, biological, and functional properties depending on their biological origin and isolation procedures; for instance, they may be digestible or indigestible, depending on the resource [82]. Owing to the versatile and tunable properties of these carbohydrates, a variety of functional and nutritional attributes can be integrated into plant-based emulsions, which is therefore important to select appropriate carbohydrates in emulsion formulation to provide the required quality and attributes, which impact human health.

2.1.2 Plant-based proteins

Plant proteins are also used as emulsion stabilizers owing to their high surface activity, which is governed by the balance of polar and nonpolar groups on their surfaces [83]. These proteins can be derived from various botanical sources, leading to different characteristics not only because of their biological origin but also because of changes during isolation and purification. While most plant-derived proteins are present as complex multimers consisting of numerous different types of proteins held together by physical and/or chemical bonds, their lack of consistent properties is a major drawback for their use in emulsion formulation [84]. Consequently, identifying appropriate botanical sources and optimizing isolation procedures to produce reliable proteins suitable for emulsions is key to the practical use of plant proteins.

2.1.3 Plant-based phospholipids

Lecithin, a common phospholipid-based emulsifier, can be extracted from plant sources such as soybeans and rapeseed, and is widely used as an emulsifier in the food industry [85]. Food lecithin typically consist of mixtures of phospholipids with different head and tail groups, as well as other types of lipids, including triglycerides, glycolipids, and sterols [86]. Depending on the phospholipid composition and concentration, they can adsorb at oil–water interfaces to form interfacial layers that reduce interfacial tension and stabilize emulsion droplets, with the hydrophobic fatty acid tails oriented toward the oil phase and the hydrophilic headgroups extending into the aqueous phase. Under certain conditions, phospholipids may further self-assemble into multilamellar or lamellar liquid-crystalline structures, which can provide additional structural stability to the system. [87]

2.1.4 Plant-based small-molecular extracts

Small surface-active molecules can also be isolated from plant sources, which are referred to as plant-based biosurfactants [88]. Saponin, one of the most used biosurfactants in the food industry, is extracted from the bark of the Quillaja saponaria tree [89], bearing hydrophilic regions (e.g., sugar groups) and hydrophobic regions (e.g., phenolic structures) on the same molecule [90]. One advantage of this ingredient is that it can be processed into either powder or liquid forms, which are more conveniently used in food applications. However, saponin typically needs to be isolated from a complex mixture of other molecules and then purified before it can be used as a biosurfactant. Optimized procedures for the extraction and processing of saponin are therefore required for its industrial use in plant-based emulsions.

2.2 Plant-based lipids

Plant-based oils can be extracted from various lipid-rich botanical sources, including corn, soybean, sunflower, etc., each with its own unique characteristics. One of the main differences between these plant-based oils and animal fats is that the former contain more unsaturated fatty acids, which give them a more fluid nature at ambient temperature. The type of fatty acids present in these oils influences their nutritional profile. For instance, plant-derived oils containing high levels of polyunsaturated fatty acids, particularly omega-3 fatty acids, have been claimed to have beneficial health effects, e.g., the ability to reduce heart and brain diseases, [91] and can be used as an alternative to fish oil. However, oxidation of these oils during storage and processing, which would result in the generation of undesirable off-flavors and toxic reaction products [92], is a major challenge for their use. Emulsion technology is therefore a possible route to overcome some of these issues, [93] creating nutritionally fortified plant-based foods.

2.3 Plant-based additives

For food emulsions, additives are required to enable additional properties and functional attributes [94]. Thus, the formulation of plant-based food emulsions requires the use of various plant-derived additives [95], including colors, flavors, buffers, and preservatives. For instance, plant-derived pigments (e.g., carotenoids and anthocyanins) or preservatives (e.g., essential oils) have been used in food emulsions, [96] showing additional contributions to their properties. It is therefore important to identify new types of plant-based additives in future research to improve the nutritional and functional attributes of food emulsions.

Collectively, plant-derived stabilizers, including polysaccharides, proteins, phospholipids, biosurfactants, and their corresponding micro/nanoparticles, provide a versatile platform for the development of sustainable Pickering emulsions. Their diverse interfacial properties, renewable origins, and potential for structural and functional tailoring have stimulated growing interest in a wide range of food and material applications [97,98]. Among these stabilizers, plant-derived particulate systems have attracted particular attention because they combine the sustainability of biomass resources with the unique advantages of Pickering stabilization. Unlike molecular emulsifiers, these particles can irreversibly adsorb at fluid interfaces and, through their morphology, surface chemistry, and assembly behavior, provide opportunities for regulating emulsion structure and functionality. In particular, forestry-derived particles such as CNCs, CNFs, and LNPs have emerged as representative systems owing to their abundance, tunable interfacial properties, and ability to act as both emulsion stabilizers and structural building blocks. Therefore, the following sections focus on forestry-derived particulate stabilizers and discuss how their interfacial assembly behavior governs Pickering stabilization and enables emerging applications in food systems and functional materials.

3 Interfacial Assembly of Forestry-derived Particles in Pickering Systems

3.1 Theory of Pickering emulsions

Traditionally, emulsions are thermodynamically unstable systems [99], but they are widely used in food, pharmaceuticals, cosmetics, etc. The concept of particle-stabilized emulsions dates back to the early 20th century, when Ramsden first observed that water-insoluble solid particles could stabilize emulsions [29], followed by Pickering’s systematic investigations, from which the term Pickering emulsion originated. [30]

Pickering emulsion refers to an emulsion stabilized by solid or colloidal particles that adsorb at the oil–water interface. Effective stabilization requires partial wettability of the particles by both phases, sufficient interfacial adsorption energy, and a particle size significantly smaller than that of the emulsion droplets. Upon adsorption, particles form a rigid interfacial barrier that suppresses droplet coalescence, leading to the high kinetic stability characteristic of Pickering systems. The type of emulsion is judged according to the contact angle of the oil–particle–water interface. When the contact angle is less than 90°, it will form an oil-in-water (O/W) emulsion; on the contrary, a water-in-oil (W/O) emulsion will be formed [100,101], as shown in Figure 2A. Although the contact-angle criterion provides a useful framework for predicting emulsion type, experimental observations often reveal more complex behavior. In practice, particle aggregation, surface roughness, particle concentration, and phase volume ratio can significantly influence interfacial adsorption and emulsion morphology. Consequently, the contact angle should be regarded as a primary but not exclusive determinant of Pickering emulsion type and stability.

The theory of Pickering emulsion stabilization mechanism mainly includes two kinds: solid particles interface film theory and three-dimensional viscoelastic particle network mechanism [103]. The former was demonstrated by Bink and co-workers [104], they found that polystyrene nanospheres acted as emulsifiers to form an interfacial film on the surface of the emulsion droplet when observing water-in-oil emulsions prepared with cyclohexane as the oil phase. In other words, the solid particles were closely arranged between the interfaces to form a stable film, and the steric hindrance produced by the film prevented the aggregation and collision of the droplets, making it difficult for the two phases to contact. As a result, the synergistic effect of adsorption and repulsion makes the Pickering emulsion more stable. On the other hand, Lagaly et al. [105] found the formation of a three-dimensional network when studying the use of clay particles to stabilize the emulsion system, leading to an increase in emulsion viscosity and a slowdown in droplet moving speed. The droplet collision probability decreased, thereby improving emulsion stability.

The sources of Pickering stabilizers include inorganic particles, animal-based, plant-based, etc. In recent years, the use of plant-based particles has attracted attention due to the rise of plant-based foods, such as protein [106], polysaccharide [107,108], and protein-polysaccharide complex particles [109,110]. According to the aspect ratio and shape of the nanoparticles, these plant-based particles can be divided into uniform spherical and anisotropic nanoparticles [111], and the latter includes rod-shaped, disc-shaped, ellipsoidal, nano-fiber-shaped, peanut-shaped, and cubic-shaped. [112]

Zein, a nearly spherical particles (Fig. 2B) for example, can adsorb on the O/W interface to form a physical barrier, owing to a favorable three-phase contact angle of ~90°. Under low pH conditions, the emulsion is relatively stable. De Folter et al. [75] used the anti-solvent precipitation method to prepare zein particles to stabilize the Pickering emulsion. It further demonstrated the ability of zein particles to stabilize Pickering emulsions. The desorption energy required for the separation of a single spherical particle from the oil-water interface can be calculated according to formula (1):

(1)\mathrm{\Delta }{E}_{\mathrm{s}\mathrm{p}\mathrm{h}\mathrm{e}\mathrm{r}\mathrm{e}}\text{= π}{r}^2{\gamma }_{\text{o/w}}(1-\left|\cos {\theta }_{\text{w}}\right|{)}^2

In the formula, r is the particle radius, {\gamma }_{\text{o/w}} represents the oil–water interfacial tension, and {\theta }_{\text{w}} is the contact angle of the particle adsorbed on the oil–water interface. [112]

However, for near-fibrous particles (Fig. 2B), such as CNCs or CNFs, they are usually rod- or needle-shaped, with high crystallinity and high-aspect-ratio nanoscale dimensions. For CNCs, the high-aspect-ratio enables them to connect to one another and form a bridge-like structure at the oil–water interface via self-assembly, providing steric hindrance and preventing the agglomeration of emulsion droplets to stabilize the emulsion [113]. Similarly, CF stabilizes the water-in-oil emulsion by forming a layer of CF fiber network on the oil droplet surface, and the distribution of the CF fiber on the surface can be adjusted by varying the degree of CF fiber entanglement, thereby affecting emulsion formation and performance [114]. The detachment energy of rod-shaped particles at 0° ≤ θ_w ≤ 90° or 90° ≤ θ_w ≤ 180° can be calculated according to the following formulas (2) and (3), respectively:

(2)\begin{array}{rl}& \mathrm{\Delta }{E}_{\text{rod, w}}=\\ & {\gamma }_{\text{o/w}}{\text{π}{\text{b}}^2(1-\cos {\theta }_{\text{w}})}^2\left[1+\frac{4\left({\displaystyle \frac{a}{b}}-1\right)\left(\sin {\theta }_{\text{w}}-\cos {\theta }_{\text{w}}\right)}{{\text{π}(1-\cos {\theta }_{\text{w}})}^2}\right]\end{array}

(3)\mathrm{\Delta }{E}_{\text{rod,o}}=\mathrm{\Delta }{E}_{\text{rod, w}}+4{\gamma }_{\text{o/w}}\text{π}{b}^2\cos {\theta }_{\text{w}}\left(a/b\right)

where {\gamma }_{\text{o/w}}is the oil–water interfacial tension, {\theta }_{\text{w}} is the contact angle of the adsorbed particles at the oil–water interface, and a and b are the dimensions of the semi-major axis and semi-minor axis, respectively [115].

Comparing these energy expressions reveals that rod-shaped particles have significantly higher desorption energies than spherical particles (under the same wettability), indicating that emulsions stabilized by high-aspect-ratio nanoparticles generally exhibit superior stability. This arises from the larger interfacial contact area they provide and the stronger capillary interactions generated by anisotropic particle adsorption [116,117]. Experimental studies on nanocellulose-stabilized emulsions generally support this prediction. High-aspect-ratio particles such as CNCs and CNFs frequently exhibit enhanced resistance to coalescence and creaming due to their strong interfacial anchoring and network-forming capabilities. However, desorption-energy models are based on idealized assumptions involving isolated particles and equilibrium interfaces. In real systems, particle flexibility, aggregation, interparticle interactions, and dynamic interfacial rearrangement can substantially influence stabilization behavior. Therefore, desorption energy should be considered together with kinetic and collective assembly effects when evaluating Pickering emulsion stability.

3.2 Assembly of nanocellulose at the interfaces

Cellulose, an abundant and readily available biomass material, is naturally present not as isolated molecules but as hierarchical fibers composed of bundled microfibrils [21,118]. These fibers contain alternating ordered (crystalline) and disordered (amorphous) regions, which can be processed into two main types of nanocellulose: CNCs and CNFs. CNCs are rod-like nanoparticles with high crystallinity, derived predominantly from the ordered regions of cellulose fibers after selective removal of amorphous domains (Fig. 3A). In contrast, CNFs are longer and more flexible, containing alternating crystalline and amorphous segments (Fig. 3B).

As reported by Capron and Dri, the crystalline faces of cellulosic particles are structurally nonequivalent, with hydrophobic edges [e.g., the (200) face] tending to orient toward the oil phase upon interfacial adsorption (Fig. 3C) [119,120]. This difference in wettability among crystal faces endows nanocellulose with intrinsic amphiphilic properties, which are fundamental for stabilizing oil–water interfaces (Fig. 3D). In addition, nanocellulose is typically negatively charged, generating electrostatic repulsion that prevents droplet coalescence and contributes to long-term emulsion stability. The anisotropic shape of CNCs and CNFs further enables them to form three-dimensional networks in the continuous phase, simultaneously encapsulating and immobilizing dispersed droplets. Taken together, these characteristics allow unmodified, rod-like nanocelluloses to assemble at oil–water interfaces, creating highly stable Pickering emulsions. While the absence of discrete hydrophobic groups limits deep penetration into the oil phase and dynamic rearrangement of adsorbed particles, the combination of amphiphilicity, surface charge, and anisotropic network formation makes nanocellulose a promising stabilizer for next-generation functional Pickering emulsions.

Given that the hydrophilicity–hydrophobicity balance is a key determinant of how nanocellulose adsorbs and arranges at oil–water interfaces, tailoring surface wettability has emerged as an effective strategy to enhance Pickering emulsion stability. Chemical hydrophobization, typically achieved via covalent attachment of synthetic moieties such as ethers, esters, or acrylonitrile, provides a direct route to increasing interfacial wettability. For instance, Tang et al. [122] grafted hydrophobic polystyrene chains onto CNCs, substantially improving their ability to stabilize emulsions of nonpolar oils such as toluene and hexadecane. Similarly, Du Le et al. [123] employed octenyl succinic anhydride to introduce hydrophobic chains onto CNCs, which markedly enhanced their interfacial adsorption and yielded highly stable Pickering emulsions. Notably, although unmodified cellulosic particles generally lack sufficient interfacial activity to stabilize liquid foams [124], hydrophobization via grafting hydrophobic moieties can impart the amphiphilic character necessary for foam formation and stabilization [42].

In contrast to chemical modification, which may compromise the intrinsic green attributes of nanocellulose, physical strategies offer more sustainable means of enhancing interfacial assembly. Leveraging the surface charge of nanocellulose, electrostatic adsorption of oppositely charged species has proven particularly effective. For example, a food-grade cationic surfactant, laurate arginine ester (LAE), has been used to modulate CNC interfacial behavior [125]. Through electrostatic association, LAE binds to the CNC surface, with its hydrophobic tail increasing the overall hydrophobicity of the CNC-LAE complexes. By adjusting the LAE concentration, the structure and morphology of these complexes can be finely tuned, yielding emulsions with distinct droplet characteristics and significantly improved anti-coalescence stability (Fig. 4A).

Combining nanocellulose with other polysaccharide-based nanoparticles provides another pathway for modulating interfacial behavior without introducing synthetic chemicals [126]. Xia et al. [127] demonstrated that pairing negatively charged CNFs with oppositely charged chitin nanofibers (ChNFs) enables precise tuning of CNF interfacial localization. Depending on the ChNF level, CNFs transitioned from dispersed free fibrils in the aqueous phase to complete interfacial coverage of oil droplets (Fig. 4B). This cooperative assembly substantially strengthened the interfacial network, ultimately enabling the formation of long-term stable, high-internal-phase Pickering emulsions with oil contents as high as ~83%. Overall, these studies demonstrate that surface wettability is a primary determinant of nanocellulose interfacial adsorption. Enhancing the hydrophilic–hydrophobic balance generally promotes particle attachment at oil–water interfaces, resulting in higher interfacial coverage, smaller droplet sizes, and improved resistance to coalescence, thereby enhancing overall emulsion stability.

Beyond amphiphilicity, the surface charge density of nanocellulose plays a pivotal role in governing its interfacial adsorption behavior. Electrostatic repulsion between charged particles is widely recognized as a key stabilization mechanism in Pickering emulsions [128]. Capron and co-workers systematically investigated how CNC surface charge density affects their ability to adsorb at oil–water interfaces [129]. In their study, sulfate half-ester groups on CNCs, introduced during sulfuric acid hydrolysis, were partially removed by mild acidic treatments (2.5 M HCl or 5 M trifluoroacetic acid), generating a broad range of surface charge densities (0.123–0.017 e/nm [2]) while preserving the nanocrystals’ morphology. A clear threshold behavior was observed: CNCs with surface charge densities below ~0.03 e/nm [2] efficiently adsorbed at the interface and produced small droplets with high emulsion stability. In contrast, CNCs with charge densities above this threshold exhibited poor interfacial adsorption and generated unstable emulsions, owing to excessive electrostatic repulsion that hindered particle attachment, rearrangement, and network formation at the interface.

In addition to intrinsic charge density, external environmental factors such as pH and ionic strength exert a substantial influence on the electrostatic and aggregation behavior of nanocellulose. For example, CNCs can stabilize water-in-water (W/W) interfaces formed in thermodynamically phase-separated aqueous two-phase systems (ATPS) composed of polyethylene glycol (PEG) and dextran [130,131]. In such W/W emulsions, CNCs are distributed both at the droplet interface and within the continuous phase. When NaCl is introduced, non-adsorbed CNCs aggregate within the continuous (dextran-rich) phase, forming a weak gel-like network. This network restricts droplet movement and suppresses coalescence, resulting in improved overall stability. Similarly, CNC adsorption and distribution within W/W Pickering emulsions can be finely controlled by adjusting NaCl concentration [132]. Increasing ionic strength accelerates CNC aggregation in the continuous phase, and at sufficiently high aggregation rates, a robust emulsion gel forms due to the development of interconnected CNC networks both at the interface and in bulk. This tunable gelation process enables the formation of systems with controllable gelation kinetics and mechanical strength. Taken together, these findings highlight that surface charge density must be carefully balanced to achieve efficient interfacial adsorption and colloidal stability. Moderate charge densities facilitate particle dispersion while maintaining sufficient interfacial attachment, leading to smaller droplets and enhanced long-term stability. In contrast, excessive electrostatic repulsion can inhibit particle adsorption and network formation, resulting in poorer emulsion stability.

Nanocellulose typically exhibits an anisotropic geometry with a characteristic aspect ratio, and this morphological parameter plays a crucial role in determining its interfacial assembly behavior and, consequently, the properties of the resulting Pickering emulsions [25,133]. Ni et al. [134] extracted CNF from ginkgo seed shells and demonstrated that nanoparticle length strongly influences emulsion stabilization: Shorter nanocellulose provided higher surface coverage, while longer nanofibers readily formed entangled networks in the continuous phase. A representative study by Kalashnikova et al. [135] demonstrated that cellulosic nanorods with different aspect ratios exhibit distinct interfacial assembly behaviors. Specifically, lower-aspect-ratio CNCs achieved interfacial coverages exceeding 84%, indicating dense packing around oil droplets. In contrast, higher-aspect-ratio CNFs formed less compact interfacial layers with coverages below 44% and instead promoted the formation of interconnected networks within the continuous phase. These observations highlight how aspect ratio influences the balance between interfacial coverage and network formation in nanocellulose-stabilized Pickering emulsions. Similarly, Dai et al. [136] prepared lemon-seed-derived cellulose nanocrystals (LSCNC) and cellulose nanofibers (LSCNF) and used them to stabilize Pickering emulsions containing sunflower oil. Morphological analysis (Fig. 4C) revealed that emulsions stabilized solely by LSCNC displayed smaller droplets with densely distributed blue-stained regions, indicating effective CNC adsorption at the oil-water interface. As the proportion of LSCNF increased, bright blue regions and larger droplets appeared, accompanied by a more heterogeneous distribution. This behavior can be attributed to LSCNF aggregation and entanglement within the continuous phase, which reduces interfacial coverage and hinders droplet subdivision, ultimately yielding emulsions with larger droplet sizes. Collectively, aspect ratio governs the balance between interfacial coverage and network formation in nanocellulose–stabilized emulsions. Lower-aspect-ratio nanocelluloses generally favor dense interfacial packing and the formation of smaller droplets, which are suitable for applications requiring fine dispersion and smooth texture, such as food and beverage formulations. In contrast, higher-aspect-ratio nanofibers tend to establish continuous-phase networks that improve viscoelasticity and resistance to creaming or coalescence, resulting in gel-like or highly viscoelastic emulsions, which are advantageous for high-internal-phase emulsions (HIPPEs) and structured materials. Overall, these findings collectively demonstrate the versatile capacity of nanocellulose to stabilize and architect a wide range of unconventional biphasic systems through interfacial adsorption strategies.

It should be noted that, despite their growing interest, Pickering emulsions are not intended to universally replace molecular surfactants. Conventional emulsifiers remain dominant in many formulations due to their simplicity, scalability, and regulatory maturity. Instead, Pickering systems excel in applications where interfacial architecture and structural integrity are critical. This functional differentiation underpins the increasing use of forestry-derived Pickering emulsions in both food-grade formulations and multidimensional material fabrication, which are discussed in the following section.

4 Novel Applications of Plant-based Pickering Emulsions

Emulsion technology, particularly Pickering emulsification, has emerged as a versatile platform for constructing functional materials [137,138]. Leveraging the inherent advantages of plant-based particles, [139] the synergistic integration of Pickering stabilization with these bio-derived colloids has enabled the development of a wide range of multiphase materials with novel structures and functionalities. Representative plant-derived stabilizers, including CNCs, CNFs, LNPs and starch-based particles exhibit distinct interfacial assembly behaviors and functional characteristics. For example, rigid rod-like CNCs favor dense interfacial packing and structural control, CNFs promote network formation and mechanical reinforcement, starch-based particles provide food-grade stabilization, while LNPs impart additional functionalities such as antioxidant, UV-shielding, and photothermal properties. These complementary characteristics underpin their suitability for different application scenarios, ranging from food systems to hierarchical material fabrication.

Accordingly, this section summarizes recent advances in plant-based Pickering emulsions from two complementary perspectives: their applications in food systems and their roles in constructing functional materials with increasing structural complexity, including zero-dimensional, one-dimensional, two-dimensional, and three-dimensional architectures. Together, these examples illustrate how plant-based particles enhance the performance and expand the application potential of Pickering-stabilized multiphase systems.

4.1 Plant-based Pickering emulsions for food applications

The unique structural and compositional characteristics of Pickering emulsions confer novel physicochemical and functional attributes to food emulsions. Plant-derived ingredients are generally more compatible with food-related applications because of their sustainability, biocompatibility, and consumer acceptance. Accordingly, this section discusses some emerging applications of advanced plant-based food emulsions.

4.1.1 Encapsulation and delivery systems

Many nutraceuticals found in foods exhibit beneficial effects on human health, but their use is often limited by low solubility, chemical instability, and/or bioavailability. Emulsion technology has been widely used to encapsulate these bioactive ingredients, protecting them from degradation, improving their bioavailability, and controlling their release profiles [140]. This particularly applies to Pickering emulsions. The advantage of Pickering emulsions for encapsulation and delivery applications is their superior stability [141]. Curcumin is a pigment extracted from turmeric, which is often used in the food industry to dye meat products [142,143]. Bertolo et al. [144] used LNPs extracted from bagasse as a Pickering stabilizer to encapsulate curcumin, and the curcumin content remained 73% after 96 h of storage. Moreover, research on antibacterial emulsion systems is of great significance for extending shelf life in the food sector. Li et al. [145] prepared a Pickering emulsion loaded with thymol by using zein/gum Arabic compound particles as stabilizer, which had an obvious inhibitory effect on Escherichia coli. Based on the growth behavior of Escherichia coli, the sustained-release behavior of thymol further confirmed the encapsulation capacity of the Pickering emulsion.

4.1.2 Control of lipid digestion

Lipid digestion is a basic function of the internal organs of the human body, which is also a major difficulty in physiology to control the delivery of lipophilic nutrients by the oral route. In fact, lipid digestion is an interfacial process in which oil droplets come into contact with lipase through biosurfactants (bile salts) in the body and are eventually broken down into glycerol and fatty acids. In recent years, some researchers have manipulated the interface structure to control oil digestion [54], and the inherent particle absorbability of Pickering emulsions offers an opportunity for this research [146,147]. Bai et al. [53] used plant-based solid particles, CNCs, as a Pickering stabilizer to study the release of free fatty acids in corn oil through an in vitro gastrointestinal model, and compared it with the emulsion prepared by a conventional molecular emulsifier, gum Arabic. They found that the CNC coating on the oil droplets inhibited bile salt and lipase adsorption (Fig. 5A), resulting in a 40% reduction in free fatty acid release (Fig. 5B). Surprisingly, the free fatty acid release was lowest when the CNC content was lowest (0.1%), which was attributed to flocculation of oil droplets; the mechanism is shown in Figure 5C. Another report [113] on the use of CNCs as stabilizers also showed that CNCs were effective in controlling lipid absorption because the intestinal mucus layer in mice prevented CNCs from reaching epithelial cells. Miao et al. [114] proved that the composite interface layer between whey protein and CNCs could control the degradation rate of lipid. They believed that this could be attributed to two aspects: on the one hand, the electrostatic shielding and replacement effect of CNCs on bile salt; on the other hand, the encapsulation effect of CNCs’ shell on several small oil droplets reduced the surface area in contact with active substances. Moreover, the delayed effect of Pickering emulsions prepared with zein [106,115] and proanthocyanidin particles [108,148] on lipid digestion was also demonstrated.

4.1.3 Healthier foods

Researchers are developing strategies to produce healthier foods from advanced plant-based emulsions owing to their unique properties. Plant-based emulsions can be used as building blocks for creating novel structures and textures in foods [149]. In particular, they exhibit solid-like characteristics at much lower concentrations [150], which may be useful for creating reduced-calorie products that are viscous or gel-like. Control of lipid digestion in foods has been an attractive topic for the food industry, as it may help prevent metabolic or hormonal dysregulation [24]. To this end, the in vitro digestion of CNC-stabilized Pickering emulsions has been compared to the digestion of conventional gum-arabic-stabilized emulsions [53]. The final amount of free fatty acids released was around 40% less for CNC-coated lipid droplets than that of gum-arabic-coated lipid droplets, suggesting that forming a non-digestible CNC coating surrounding the oil droplets inhibited lipase adsorption and subsequent lipid digestion. Another function of plant-based Pickering emulsions is to develop an alternative to replace saturated and trans fats in many semi-solid foods, showing desirable textural attributes, which can lead to an increased risk of cardiovascular disease and diabetes [151]. For instance, HIPPE stabilized by wheat gluten particles were developed as a plant-based mayonnaise substitute, [152] showing similar textural properties to mayonnaise but a much better thermal stability. This technology may therefore be useful for creating high-quality plant-based foods.

4.1.4 Safety and commercialization considerations

The development of novel food systems inevitably introduces safety considerations, with potential risks arising at multiple stages, including ingredient selection, processing, and storage. As emerging categories in the food sector, next-generation plant-based foods require a comprehensive safety evaluation. Standard assessment protocols for milk and cream alternatives have been reported [153]. In addition to routine physicochemical and sensory analyses, safety testing of emulsion-based foods emphasizes particle characteristics and storage stability more than that of solid meat analogues. Furthermore, gastrointestinal evaluation methods, most notably the standardized INFOGEST protocol, have been established to assess macronutrient digestion, bioavailability, and overall digestive behavior (Fig. 6).

Recent advances have also improved the accuracy and reliability of plant-based food safety assessments. Kumar et al. [154] provided a detailed overview of analytical techniques for characterizing plant proteins and highlighted amino acid profiling as a key metric for determining protein quality. Bessaire et al. [155] developed a mass-spectrometry-based toxin screening library, including general procedures for sample preparation, chromatographic separation, and high-resolution mass spectrometry, which offers a valuable platform for the screening and selecting of safe plant-derived raw materials.

Despite the progress in safety research, a noticeable gap remains between scientific development and commercial implementation. Nevertheless, the rational application of Pickering emulsions presents new opportunities to bridge this gap. From the consumer perspective, acceptance of novel foods is critical to their successful commercialization. All-plant Pickering emulsions provide a highly stable structuring strategy that can protect sensitive nutrients while enabling the incorporation of health-promoting bioactives, thereby enhancing both nutritional value and consumer trust.

Compared with conventional low-molecular-weight emulsifiers (e.g., synthetic surfactants and lecithin-based systems) that rely primarily on dynamic adsorption–desorption equilibria at interfaces, forestry-based particle stabilizers stabilize emulsions through irreversible particle adsorption and the formation of robust interfacial layers. This distinction provides enhanced resistance to coalescence, improved long-term storage stability, and reduced reliance on high concentrations of surfactants. In addition, their biomass origin offers advantages in renewability, biodegradability, and food safety compliance, making them particularly attractive for next-generation clean-label food formulations. From the industry perspective, the low success rate of novel product launches remains a major challenge [156]. Favorably, Pickering emulsions offer practical advantages for manufacturing: they are simple to prepare, highly reproducible, and compatible with a wide range of established emulsification technologies, including rotor–stator homogenization, high-pressure homogenization, ultrasonication, microfluidic emulsification, and membrane emulsification [108,157]. These mature processing routes significantly enhance scalability and manufacturing robustness, accelerating the translation of plant-based Pickering emulsions from laboratory research to commercial food applications.

4.2 Plant-based Pickering emulsions for multidimensional materials

Plant-based emulsions are emerging not only as stabilized multiphase systems but also as versatile soft templates and structuring platforms for constructing multidimensional materials [25,158,159]. Owing to their unique interfacial assembly of solid particles, these emulsions enable precise control over droplet size, topology, and spatial organization, thereby providing powerful handles for engineering zero-dimensional (0D) microspheres, one-dimensional (1D) fibers, two-dimensional (2D) films, and three-dimensional (3D) porous or gel-like architectures. Importantly, the design requirements of Pickering emulsions vary with the dimensionality of the target material. For 0D microspheres and microcapsules, droplet size and interfacial shell integrity directly determine particle dimensions and encapsulation performance. In 1D fibrous materials, emulsion continuity and droplet-templated porosity govern filament morphology and transport properties. For 2D films, long-term emulsion stability and homogeneous droplet dispersion are essential for achieving uniform barrier and mechanical properties. In contrast, 3D porous materials typically require highly stable emulsion or foam templates with interconnected droplet networks to generate hierarchical porosity and structural integrity. Consequently, emulsion characteristics such as droplet size, interfacial robustness, viscoelasticity, and network-forming ability play distinct roles in directing the fabrication of multidimensional materials. The inherent advantages of plant-derived particles-renewability, biocompatibility, chemical tunability, and robust interfacial anchoring-further expand their utility in designing functional materials for food, packaging, biomedicine, and beyond. In this section, we summarize how plant-based Pickering emulsions serve as highly adjustable templates and structuring tools for fabricating multidimensional materials, with emphasis on the mechanisms, fabrication strategies, and emerging applications enabled by these bio-derived systems.

4.2.1 0D Microspheres and microcapsules

Plant-derived Pickering emulsions offer a versatile platform for constructing 0D microspheres and microcapsules, in which biomass nanoparticles adsorb at the oil–water interface to form robust colloidal shells. Among various plant-based stabilizers, LNPs are particularly attractive due to their intrinsic aromatic structures, UV-shielding capability, and chemical tunability [71]. Recent studies have demonstrated that LNP-stabilized Pickering droplets can be used as templating reactors to build functional microspheres with precisely programmable interfacial structures and release behaviors [160]. Grafting thermoresponsive poly(N-isopropylacrylamide) onto lignin enables the formation of self-assembled AL-g-PNIPAM nanoparticles that stabilize bioactive-loaded droplets and act as a protective interfacial barrier (Fig. 7A). The resulting microspheres exhibit markedly enhanced UV stability of encapsulated compounds and temperature-triggered modulation of droplet morphology and release kinetics, highlighting the feasibility of responsive lignin-based colloidosomes for storage and controlled delivery of light-sensitive nutraceuticals (Fig. 7B).

Beyond direct nanoparticle design, interfacial engineering strategies further expand the functional complexity of plant-based Pickering microcapsules. LNPs–stabilized emulsions can be coated via layer-by-layer (LbL) assembly of oppositely charged biopolymers such as chitosan (CH) and sodium lignosulfonate (SL), forming multilayered shells [(CH+SL)n@PE, where PE denotes Pickering emulsion templates] with tunable thickness and significantly improved physical stability [57]. These biomass-derived microcapsules provide high encapsulation efficiency, excellent UV protection (Fig. 7C), and finely adjustable release profiles, while also exhibiting pH- and enzyme-responsive behaviors relevant for targeted delivery in agricultural or biological environments (Fig. 7D). Collectively, these advances underscore the capacity of plant-based Pickering emulsions to serve as structurally controllable templates for constructing multifunctional 0D microspheres, offering eco-friendly, low-cost, and highly programmable carriers for bioactives, pesticides, and other sensitive hydrophobic agents. These examples demonstrate that precise control of droplet size and interfacial shell architecture is the key factor governing particle dimensions, encapsulation efficiency, and release behavior in 0D systems.

4.2.2 1D filaments

Pickering emulsions have recently emerged as a potential versatile soft template for constructing 1D fibrous materials. A representative advance is the development of interfacial polyelectrolyte-emulsion complexation (IPEC) spinning, in which ChNF-stabilized Pickering emulsions serve as both structural building blocks and functional carriers during fiber formation [58]. By drawing the emulsion into contact with an oppositely charged alginate solution, composite filaments with tunable diameters and highly adjustable internal porosity can be continuously produced (Fig. 8A). Importantly, the droplet size of the precursor Pickering emulsion directly dictates the pore size within the resulting filaments, demonstrating the unique ability of plant-derived and biomass-based particles to encode microstructural features into 1D architectures. The resulting filaments exhibit robust mechanical properties in both dry and wet states and can serve as controlled-release systems due to their emulsion-derived porous networks (Fig. 8B). Although reports on plant-based Pickering-templated 1D fibers remain scarce, this work highlights the significant potential of using biomass particles to produce sustainable, structurally programmable filaments and is expected to inspire broader exploration of Pickering-assisted spinning strategies for advanced fiber materials. [161-163]

4.2.3 2D films

Plant-based Pickering emulsions have also proven highly effective as structural and functional templates for engineering two-dimensional (2D) films, particularly in the field of food packaging where barrier performance, mechanical robustness, and controlled release of bioactive components are essential. Building upon their roles in nutraceutical encapsulation and delivery, Pickering emulsions also enable the integration of hydrophobic actives and renewable polymers into continuous film matrices in a highly uniform and stable manner. In a recent study [164], polyethylene imine was grafted onto TEMPO-oxidized CNCs. The nanoparticles could stabilize a Pickering emulsion of oregano essential oil and be used to produce a bacteriostatic food packaging film. Similarly, TEMPO-oxidized CNFs and carboxymethyl chitosan were used as hybrid stabilizers to encapsulate beeswax into a robust oil-in-water Pickering emulsion [59]. The strong interfacial complexation forms protective shells around wax particles, preventing aggregation and ensuring long-term emulsion stability. When applied as a coating on cellulose substrates, the Pickering emulsion yields hydrophobic, bacteriostatic paper films (Fig. 9A) that effectively slow fruit spoilage (Fig. 9B), demonstrating a green and solvent-free route for upgrading traditional wax barrier coatings.

Another prominent example uses LNPs to stabilize essential-oil-loaded Pickering emulsions, which are then embedded in gelatin matrices reinforced with CNCs [165]. This emulsion-assisted assembly results in biodegradable composite films with markedly enhanced UV shielding, mechanical strength, water and oxygen barrier properties, and thermal stability. Crucially, the Pickering structure enables controlled release of encapsulated essential oils, endowing the films with long-lasting antioxidant and antimicrobial activity, which are necessary attributes for active food packaging. These films not only exhibit rapid biodegradation but also demonstrate excellent performance in extending the shelf life of perishable foods such as pork. The pH is a key indicator of meat freshness and spoilage.

Together, these studies underscore the unique capability of plant-derived Pickering emulsions to translate interfacial stabilization principles into high-value 2D materials with multifunctional protective, antimicrobial, and sustainability features. These also highlight that emulsion stability and homogeneous droplet distribution are crucial for achieving uniform film structures and multifunctional barrier performance. This approach provides a powerful bridge between emulsion-based delivery systems and next-generation biodegradable packaging technologies.

4.2.4 3D porous materials

In the construction of three-dimensional architectures, plant-based Pickering emulsions are most commonly employed as structural templates or as regulators of phase behavior to achieve programmable microstructures, stable interfaces, and controlled release properties [27,166–168]. For example, Cheng et al. [169] embedded CNF/ChNF-stabilized PLA/CHCl₃ droplets into a CNF–PAA matrix, where shear-induced phase separation during extrusion printing drove the spontaneous formation of a continuous hydrophobic PLA film on the printed surface (Fig. 10A–C). This emulsion-triggered interfacial reconstruction endowed the printed constructs with hierarchical interfaces, long-term wet stability, and tailorable release behavior. As a demonstration, urea-loaded emulgel scaffolds exhibited substantially prolonged release in soil column experiments, with kinetics governed by both diffusion and matrix relaxation, highlighting a level of structural programmability unattainable for conventional slow-release fertilizers (Fig. 10D).

Alongside emulsions, Pickering foams have emerged as a powerful parallel templating strategy for constructing multiscale porous materials, owing to their extremely low density, high porosity, and the ability of their thin liquid films to transform into solid frameworks upon gas exchange or evaporation. Unlike the relatively encapsulated structure of emulsions, the more “open” and dynamic interfaces of Pickering foams facilitate the formation of particle networks across both film regions and Plateau borders, enabling the preservation of three-dimensional structures during drying. Rojas and colleagues demonstrated that combining high-aspect-ratio, hydrophilic CNF with low-aspect-ratio, hydrophobic silica particles yields exceptionally stable Pickering foams (Fig. 10E) [124,170,171]. Compared with foams stabilized solely by hydrophobic silica, the incorporation of CNF led to substantial improvements in foamability and extended foam lifetimes (up to a 350% increase) by promoting the formation of a fiber network that modulates particle interactions and effectively suppresses drainage, coarsening, and bubble coalescence. Upon drying, these complex fluids undergo a controlled transition into lightweight yet mechanically robust solid foams, with final properties strongly influenced by the surface energy of the CNF precursors. Overall, such plant-based Pickering foam systems exhibit that highly stable emulsion or foam networks are essential for generating interconnected porous architectures and achieving long-term structural robustness in 3D materials and provide a promising route for producing structurally robust, lightweight porous composites directly from their liquid counterparts.

5 Conclusion and Future Perspectives

This review provides a comprehensive account of the interfacial behavior, stabilization mechanisms, and potential applications of plant-derived, particularly forestry-based micro-/nano-particles in Pickering multiphase systems, together with their emerging applications in food formulations and template-directed functional material fabrication. Owing to their distinctive morphologies, tunable surface chemistries, and positive environmental impact, lignocellulosic particles can spontaneously adsorb and densely assemble at oil–water interfaces, generating high interfacial energy barriers that impart exceptional stability and structural control to Pickering systems. Moreover, their interfacial performance can be rationally tuned through physical or chemical modification, enabling broad applicability in nutrient delivery, reduced-fat formulations, and the fabrication of multidimensional functional materials.

Despite significant progress, several challenges remain at both the fundamental and engineering levels. First, the dynamic processes governing particle adsorption, spreading, rearrangement, and cooperative assembly at interfaces are not yet fully understood, limiting predictive control over interfacial stabilization. Second, batch-to-batch variability inherent to biomass-derived particles, arising from differences in botanical origin, extraction routes, and processing conditions, can result in variations in particle morphology and surface chemistry, affecting system reproducibility and performance. Third, systematic studies addressing safety, toxicology, and long-term behavior of these natural particles in food, personal care, and biomedical contexts remain limited, constraining their broader industrial translation.

Beyond stabilization, the secondary processing of Pickering systems into functional solid materials is still in its early stages. While approaches such as interfacial consolidation, freeze-drying, template solidification, and emerging fabrication methods including 3D printing have demonstrated promise, challenges persist in achieving precise architectural control, scalability, continuous processing, and multifunctional integration.

Looking ahead, the future development of plant-based Pickering systems need to rely not only on the discovery of new biomass-derived particles but also on a deeper understanding of how particle characteristics govern interfacial assembly and macroscopic functionality. Establishing quantitative relationships between particle wettability, surface charge, aspect ratio, and emulsion performance will be critical for moving from empirical formulation toward predictive design. Such understanding could further enable the rational regulation of droplet size, interfacial architecture, and network formation, thereby tailoring system properties for specific applications. In addition, as highlighted throughout this review, Pickering emulsions are increasingly being utilized as dynamic templates for constructing hierarchical materials rather than merely as stabilized multiphase systems. Future research should therefore place greater emphasis on coupling interfacial assembly with advanced manufacturing and material-processing strategies to achieve controllable architectures across multiple length scales. Finally, translating these systems into practical applications will require improved standardization of biomass-derived particles, comprehensive safety evaluations, and validation under realistic processing and storage conditions.

Overall, this review highlights that the performance of plant-based Pickering systems is fundamentally governed by the interfacial assembly behavior of biomass-derived particles. As discussed throughout the review, key particle parameters, including wettability, surface charge density, aspect ratio, and cooperative assembly behavior, collectively determine interfacial adsorption, droplet stabilization, and the resulting functionality of Pickering multiphase systems. Beyond their established roles in food formulations and nutrient delivery, these interfacial principles have enabled the fabrication of hierarchical materials spanning zero-, one-, two-, and three-dimensional architectures with tailored structures and functionalities. Therefore, plant-derived micro- and nanoparticles should be viewed not only as sustainable stabilizers but also as programmable interfacial building blocks for the rational design of advanced multiphase materials. Continued advances in interfacial characterization, assembly control, and scalable processing are expected to further expand their applications in food, packaging, agriculture, and functional materials.

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