Food Hydrocolloids 154 (2024) 110089

Contents lists available at ScienceDirect

Food Hydrocolloids
journal homepage: www.elsevier.com/locate/foodhyd

Bigels as emerging biphasic systems: Properties, applications, and prospects

in the food industry
Erpeng Chao a, Jinwei Li a, Zhenhua Duan b, **, Liuping Fan a, b, c, *
a
State Key Laboratory of Food Science and Resources, Jiangnan University, 1800 Lihu Avenue, Wuxi, Jiangsu, 214122, China
b
Guangxi Key Laboratory of Health Care Food Science and Technology, Hezhou University, Hezhou, 542899, China
c
Collaborat Innovat Ctr Food Safety & Qual Control, Jiangnan University, 1800 Lihu Avenue, Wuxi, Jiangsu, 214122, China

A R T I C L E I N F O A B S T R A C T

Keywords: Bigels, as emerging biphasic systems, have garnered significant attention owing to their advantages encom­
Bigels passing both hydrogels and oleogels. The performance and application of bigels in food systems depend strongly
Mechanical properties on their mechanical properties. Therefore, acquiring a rational understanding of bigels with varied mechanical
Influencing factors
properties for distinct application scenarios is crucial for expanding their practical applications. This review
Applications
emphasizes the intrinsic characteristics and extrinsic factors influencing the mechanical properties of bigels. This
insight enables the design of the mechanical properties of bigels for specific food-related applications, with a
particular focus on their use as nutrient delivery systems, fat replacers, food packaging, and 3D printing food.
The mechanical properties of bigels depend on intrinsic characteristics, such as the ratio between oleogel and
hydrogel, and types of organogelators/hydrogelators, as well as extrinsic factors, including the incorporation of
additives/emulsifiers and pH. The changes in intrinsic characteristics could alter the interfacial area, structural
arrangement, and degree of crosslinking and the polymer strength of phases. Moreover, extrinsic factors play
crucial roles in modifying the mechanical properties of bigels by influencing the interactions between the oleogel
and hydrogel and enhancing the interfacial and structural stabilization of bigels. Understanding these factors
allows for more precise design of bigels characteristics, thereby enhancing their suitability in various food
industries.

1. Introduction suitable for delivering hydrophobic compounds. Oleogels, on the other

hand, are defined as semi-solid mixtures containing an organic liquid
Gels are classically defined as soft matter, typically composed of at phase trapped within a 3D network, achieved by adding a small amount
least one component with low molecular mobility, known as structuring of a gelling agent to liquid vegetable oil (Qiu, Qu, Zhang, & Eun, 2023).
agents, and another predominant compound, usually a solvent (Evans & Indeed, while oleogels offer several advantages, such as the ability to
Wennerstrm, 1999). Gels can be categorized depending on the gelation restrict the flow of liquid fat and provide thermal reversibility, they do
of either polar or apolar liquid phases, resulting in hydrogels and oleo­ come with certain drawbacks that need to be considered including their
gels, the latter being a subcategory of organogels (Fig. 1). Hydrogels softer texture and lower plasticity compared to traditional solid fats (Li,
primarily consist of water, and their network is formed through the Liu, Bogojevic, Pedersen, & Guo, 2022).
crosslinking of biopolymer chains via chemical crosslinking with cova­ Bigels are innovative biphasic systems consisting of two gelled
lent bonds, physical crosslinking through non-covalent interactions, or a phases, typically formed through mechanical mixing under specific
combination of both (Okuro, Santos, & Cunha, 2021). Hydrogels can temperature and gel-setting conditions (Liu et al., 2021). The fabrication
serve as delivery systems that respond to environmental stimuli, such as of bigels offers the advantages of both hydrogels and oleogels, including
changes in temperature and pH, and as ingredients to improve various the capacity to deliver both hydrophilic and hydrophobic components,
food properties, including elasticity and stability during food product thermodynamic stability, hydrating and cooling effects, and controlled
manufacturing (Okuro et al., 2021). Nevertheless, hydrogels are not release characteristics (Martins et al., 2019; Shakeel et al., 2019;

* Corresponding author. School of Food Science and Technology, Jiangnan University, Wuxi, 214122, China.
** Corresponding author. Guangxi Key Laboratory of Health Care Food Science and Technology, Hezhou University, Hezhou, 542899, China
E-mail address: [email protected] (L. Fan).

https://doi.org/10.1016/j.foodhyd.2024.110089
Received 4 March 2024; Received in revised form 2 April 2024; Accepted 8 April 2024
Available online 9 April 2024
0268-005X/© 2024 Elsevier Ltd. All rights reserved.
E. Chao et al. Food Hydrocolloids 154 (2024) 110089

2. Fabrication and categories of bigels

2.1. Fabrication of bigels

The preparation methods of bigels mainly include the heat-set gel­

ling method and the cold-set gelling method, which are also called the
one-step mixing method and the two-step mixing method, respectively
(Fig. 2). The heat-set gelling method and the cold-set gelling method are
based on different gelation mechanisms. The heat-set gelling method
leads to a decrease in the interfacial tension between the water phase
and the oil phase and a decrease in the viscosity of the system (Kupi­
kowska, Barbara, Jacek, & Mirosław, 2024). Compared with the heat-set
gelling method, the cold-set gelling method can produce a more ordered
network structure, higher mechanical strength, and stability (Yiu et al.,
2023). Therefore, gels prepared by the heat-set gelling method generally
appear as rubber-like gels, while gels prepared by the cold-set gelling
method act as squeezing gels (Clímaco & Fasolin, 2024). In the one-step
mixing method, vigorous mixing is required to generate non-equilibrium
and bicontinuous structures by shearing the droplets of the two
Fig. 1. Schematic representation of hydrogel, oleogel, and bigels. immiscible liquids. The two-step mixing method involves independently
preparing and storing oleogels and hydrogels, followed by their subse­
Shakeel, Lupi, Gabriele, Baldino, & De Cindio, 2018). Key properties of quent mixing (Shakeel et al., 2019). The mixing parameters, particularly
bigels encompass their unique thermodynamic behavior, texture char­ mixing speeds and temperatures, play a crucial role in determining the
acteristics, and versatility in material preparation. These properties can final properties of bigels. Universally, a higher mixing speed causes the
be finely adjusted through various factors, including material combi­ formation of finer droplets, accompanied by the increasing viscous
nations (Habibi, Kasapis, & Truong, 2022; Shakeel, Farooq, Gabriele, modulus (G″). Conversely, a lower mixing speed results in a stronger
Marangoni, & Lupi, 2021), formulation ratios (Nutter, Shi, Lamsal, & system characterized by higher values of the complex modulus (G′) and
Acevedo, 2023a, 2023b; Richa & Roy Choudhury, 2023; Saffold & improved consistency. The formation of weaker structures in bigels at
Acevedo, 2021), the types of gelling agent (Nutter et al., 2023a, 2023b; higher mixing speeds can be attributed to the phenomenon of oil/water
Yang, Zheng, Mo, Gao, & Mao, 2022), and the inclusion of additives droplet formation due to structural breakup (Fasolin & Vicente, 2017).
(Saffold & Acevedo, 2022; Xie, Hu, Huang, & Lu, 2023a, 2023b), among The complex physical arrangement in the bigels network depends solely
other factors. Consequently, bigels have garnered significant attention on the composition and process conditions that influence the particle
from researchers, particularly in the field of controlled release of size, thereby affecting the mechanical properties of the bigels. Previous
bioactive compounds, such as coenzyme Q10 (CoQ10) (Zulfakar, Chan, literature suggested that the one-step mixing method, known as the hot
Rehman, Wai, & Heard, 2018), lycopene (Zhu et al., 2021), β-carotene melt emulsification process, was performed at temperatures above 40 ◦ C
(Zheng, Mao, Cui, Liu, & Gao, 2020) and, omega-3 fatty acids (Rehman, (Behera, Sagiri, Singh, Pal, and Anis (2014) at 50 ◦ C, Samui, Goldenisky,
Mohd Amin, & Zulfakar, 2014). Notably, bigels have found diverse ap­ Rosen-Kligvasser, and Davidovich Pinhas (2021) at 70◦ C, Zheng et al.
plications in the food industry, contributing to the enhancement of the (2020) at 80 ◦ C. In the two-step mixing method, the pre-set gels were
stability, taste, safety, and health benefits of food products. They mixed at room temperature (Martinez et al., 2021; Martins et al., 2019).
contribute to improvements in the nutritional composition and func­ The ideal homogenization temperature should be below the crystalli­
tional properties of food products (Machado et al., 2022; Zhuang, Clark, zation onset of the wax and oleogel phase. Higher temperatures lead to
& Acevedo, 2021). Besides, their versatility and unique structural the formation of a grainy texture, resulting in poor spreadability, while
properties make them serve as fat replacers (Li et al., 2024; Qiu et al., lower temperatures will induce a softer gel texture.
2024; Tian et al., 2023), intelligent food packaging (Kanelaki, Zam­ Some assistive technologies have also been employed in gel prepa­
pouni, Mourtzinos, & Katsanidis, 2022; Zhai et al., 2022), innovative 3D ration. Microwave-assisted heating is promising for obtaining oleogel
printing food production (Chen, Bian, Cao, Shi, & Meng, 2023; Guo, Gu, components of bigels with desired characteristics. In contrast to con­
Du, & Meng, 2023; Guo, Li, Song, & Meng, 2024). ventional heating, which relies solely on conduction, microwave-
While some recent review articles have offered insights into the key assisted heating combines both dielectric polarization and conduction
characteristics and drug delivery applications of bigels (Shakeel et al., mechanisms (Kumar, Kuang, Liang, & Sun, 2020). When molecules are
2021; Shakeel et al., 2019; Shakeel et al., 2018), the summary of factors exposed to microwaves, they develop permanent dipole moments, align,
influencing the characteristics of bigels remains inadequately compre­ and undergo various motions, including rotation, friction, and collision.
hensive. Additionally, limited research has been dedicated to designing These motions result in rapid heating in solvents that absorb microwaves
bigels with varied gel properties tailored for distinct application sce­ (Yang et al., 2021). Consequently, microwave-assisted heating can
narios. The design of gel properties in bigels for specific food-related reduce both time and energy consumption, particularly in gel prepara­
applications holds substantial practical importance in the food in­ tion within the pharmaceutical field. Algin Yapar, Tuncay Tanriverdi,
dustry. To foster broader utilization of bigels and establish a robust Aybar Tural, Gumus, Turunc, and Gokce (2020) employed microwave
foundation for novel food gels, this review provides insights into the radiation as an alternative heat source to conventional heating when
examination of intrinsic characteristics and extrinsic factors influencing working with Carbopol 974 P NF (C974) oleogel. After just 2 min of
their gel properties. By regulating both intrinsic and extrinsic factors, exposure to microwave irradiation, the mixtures became transparent,
bigels can be tailored to meet diverse application needs. Recent ad­ indicating the formation of apparently more viscous formulations. The
vancements in utilizing bigels as carriers for nutrient delivery systems, potential of gamma radiation technology in the synthesis of biomedical
fat replacers, food packaging, and in 3D printing food are summarized. polymers has been extensively explored and is regarded as a sustainable
Finally, we present perspectives on the future challenges of bigels and environmentally friendly approach for designing biomedical mate­
development, with the anticipation of offering valuable insights for the rials. Gamma radiation-induced crosslinking was utilized to produce
design and development of food gels with desired gel-related both hydrogels and the final bigels for these drug delivery systems. This
performance. technology involved the formation of hydrogels through gamma

2
E. Chao et al. Food Hydrocolloids 154 (2024) 110089

Fig. 2. Fabrication process and categories of bigels.

irradiation of polysaccharide gum, offering enhanced application pos­ combinations (i.e., the ratio between oleogel and hydrogel, types of
sibilities (Singh & Kumar, 2019). These advanced technologies organogelators and hydrogelators), and extrinsic factors, such as the
contribute to the efficient and controlled production of bigels, making incorporation of additives/emulsifiers and pH. By regulating both
them more suitable for various applications in the food and pharma­ intrinsic and extrinsic factors, bigels can be tailored to meet diverse
ceutical industries. application needs.

2.2. Categories of bigels 3.1. Intrinsic characteristics

Incorporating two gelled phases into a bigel system can result in 3.1.1. The ratio between oleogel and hydrogel
different structures, each with its unique properties and applications, The ratio of oleogel/hydrogel is a fundamental parameter that
namely hydrogel-in-oleogel, oleogel-in-hydrogel, and bicontinuous gels significantly influences the gel structure and, consequently, the gel
(Zheng et al., 2020). The type of bigels formed depends on the con­ properties of bigels, such as firmness, adhesiveness, viscosity, cohe­
centration of oleogel and hydrogel components (Fig. 2). siveness, and stickiness. Generally, changes in the ratio of oleogel/
Oleogel-in-hydrogel type: The bigels exhibit the oleogel-in-hydrogel hydrogel could impact the interfacial area of bigels, which is related to
type when the oleogel concentration is below 50%. Bicontinuous type: interaction sites between the dispersed phase and the matrix. When the
Bigels transform into a bicontinuous type when the oleogel and hydrogel hydrogel serves as the dominant phase (continuous phase), the oleogel
contents are equal. Hydrogel-in-oleogel type: Further increasing the acts as the dispersion phase. As the oleogel ratio increases, more oil
oleogel concentration to 70% leads to the bigels becoming a droplets are generated. These oil droplets lead to a higher total inter­
hydrogel-in-oleogel type (Qiu et al., 2022). These bigels systems hold facial area of bigels, providing more interaction sites between the
promising applications in the food industry due to their solid-like dispersed phase and the matrix. Hashemi, Varidi, and Jafari (2023) and
behavior and resistance to phase separation over time (Bollom, Clark, Lu et al. (2022) have observed that the dispersed oil droplets tend to
& Acevedo, 2020). However, if the gel network is disrupted by shearing aggregate. The resulting proximity of the droplets induces intense in­
action, phase separation in the bigels might occur (Zheng et al., 2020). teractions among them, forming a tighter three-dimensional network,
Bicontinuous gels possess a unique combination of high surface area and ultimately strengthening the bigels network. According to a report by
a bicontinuous morphology, making them promising materials for ap­ Zheng et al. (2020), the bigels with the stronger network continuity and
plications in various fields, such as catalysis, energy storage, separation, firmness could be achieved by increasing the number of oil droplets as
biomedical implants, and coatings. However, the stability of bicontin­ active fillers. Additionally, closer packing of dispersed droplets is asso­
uous gels is one of the limiting factors in their application, as even slight ciated with increased bigels stability (Singh, Anis, et al., 2014). Intro­
agitation or changes in temperature and solution conditions can disrupt ducing protein-based oleogels into bigels enhances stability through
the bicontinuous morphology. The disruption of bicontinuous interactions between the protein and oleogel phases. Oil droplets in
morphology due to changes in temperature, pH, and ionic strength bigels act as numerous cross-linking units, filling gaps between aggre­
presents a significant challenge in effectively utilizing these materials. gated protein particles (Hashemi et al., 2023).
Applications like separations and catalysis often demand a delicate On the other hand, the ratio changes of oleogel/hydrogel could cause
balance between maintaining a two-phase liquid state and ensuring a more ordered structural arrangement. Martins et al. (2019) demon­
excellent mechanical, thermal, and chemical stability. The challenge lies strated that the structural arrangement of bigels became more ordered
in creating materials or systems that can preserve these characteristics with the introduction of oleogel. The crystalline arrangement remained
under various operating conditions. consistent during bigels production due to the introduction of more
crystalline particles (i.e., a higher oleogel fraction) into the bigels sys­
3. Factors affecting the mechanical properties of bigels tem. The structural arrangement within bigels plays a pivotal role in
determining their gel properties and overall stability (Fasolin, Martins,
Factors affecting the mechanical properties of bigels mainly include Cerqueira, & Vicente, 2021).
intrinsic characteristics, such as formulation adjustments and material In bigel-based foam emulsions, an increase in the proportion of

3
E. Chao et al. Food Hydrocolloids 154 (2024) 110089

oleogel improves the integrity of the fat crystal network, thereby oil phase (Guo, Chen, & Meng, 2023). This process relies on the
increasing the mechanical strength of the system. Additionally, a higher temperature-controlled formation of physical interactions between
oleogel ratio also enhances foaming ability. Fat crystals adsorbed on the small molecules, i.e. van der Waals, hydrophobic, and hydrogen bonds.
air/oil interface can prevent the coarsening and coalescence of bubbles. Due to the role of these physical interactions in structure formation and
Fat crystals with a three-dimensional network structure inside can the use of small molecule building blocks, low molecular weight gelling
reduce agglomeration and coalescence (Zheng et al., 2023). Further­ agents are highly sensitive to temperature and shear (Davidovich
more, Saffold and Acevedo (2021) confirmed that an increase in the Pinhas, 2019). In this category, wax types like beeswax beeswax (Mar­
oleogel/hydrogel ratio led to enhanced stability in the gelatin-rice bran tins et al., 2019; Rehman et al., 2014), rice bran wax (Nutter et al.,
wax-based bigels system. A higher oleogel/hydrogel ratio consistently 2023a, 2023b), sorbitan monostearate (Singh, Banerjee, et al., 2014),
resulted in higher elastic modulus (G′) values compared to bigels with a stearic acid (Senggam Wakhet et al., 2015a, 2015b), and glyceryl stea­
lower oleogel/hydrogel ratio, reflecting increased oleogel droplet in­ rate (Lupi et al., 2016) are commonly found. Exactly, the gelling ca­
teractions and improved mechanical properties. The complex modulus, pacity of organogelators in oleogels depends on achieving a delicate
as demonstrated by frequency sweep tests of pectin/olive oil-based balance between interactions among the gelator molecules themselves
bigels, is influenced by the oleogel-to-hydrogel ratio and its proper­ (gelator-gelator interactions) and interactions between the gelator
ties. As the ratio of oleogel/hydrogel increases, the complex modulus molecules and the oil phase (gelator-oil interactions).
increases non-linearly and the phase angle decreases non-linearly, High molecular weight gelators are polymeric structures capable of
which is related to the increasing consistency and structuring of the forming three-dimensional networks. High molecular weight gelling
bigels and degree of structuration of bigels (Lupi et al., 2016). An agents such as proteins and polysaccharides form polymeric network
increased oleogel/hydrogel ratio enhances firmness and spreadability structures through physical interactions (i.e., hydrogen bonding).
while decreasing gel adhesivity and cohesiveness. Increased stiffness Because of their polymeric nature, these oleogels exhibit viscoelastic
and fracture stress of bigels were observed with higher oleogel fractions, properties, which are strongly influenced by the molecular weight,
establishing a clear linear relationship between oleogel fraction and conformation, and concentration of the polymer. When considering a
stiffness. Their relative proportions play a critical role in determining fixed oleogel/hydrogel ratio, different gelling agents can result in
the viscoelasticity of the resulting material (Zhu et al., 2021). Bigels various types of bigels. Beeswax-based bigels exhibit greater strength
composed of guar gum-based hydrogel and sorbitan compared to glycerol monostearate-based bigels as the content of the
monostearate-sesame oleogel exhibited higher viscosity and firmness oleogelator increases. In glycerol monostearate-based bigels, the water
when they contain higher proportions of oleogel. The ability of bigels to and oil holding capacity improves with increasing glycerol mono­
resist harsh temperature treatments and maintain their structural stearate content (Yang et al., 2022). Singh, Banerjee, et al. (2014)
integrity and organization is a significant advantage in various appli­ highlighted the influence of the length of the alkyl hydrocarbon chain of
cations (Singh, Banerjee, et al., 2014). Moreover, Singh, Anis, et al. sorbitan monostearate on the stability of bigels composed of guar gum
(2014) and Singh, Banerjee, et al. (2014) found that bigels with a higher and sesame oil, and they likely found that the length of the alkyl hy­
volume of oleogel possessed higher yield stress values. Additionally, the drocarbon chain in sorbitan monostearate played a crucial role in sta­
oleogel/hydrogel ratio in the system could also influence the surface bilizing the bigels. The research by Lupi et al. (2016) demonstrated that
morphologies of the bigels. Gellan/κ-carrageenan bigels with a 1:2 the organogelator content had a significant impact on the consistency
oleogel/hydrogel ratio displayed a rough surface morphology, with and structuration of pectin/policosanol/olive oil-based bigels. The
corrugations localized to some regions of the bigels. In contrast, bigels increasing the organogelator amount induced an increase in consistency
with equal or higher proportions of organogel exhibited significantly and degree of structuration of bigels. Notably, bigels with different
smoother surfaces (Richa & Roy Choudhury, 2023). Interestingly, the organogelator content displayed a similar droplet size distribution.
use of bigels composed of citrus fiber particle-based hydrogel and
policosanol-based oleogel offers an intriguing approach to studying the 3.1.2.2. Hydrogelators. The choice of hydrogelators plays a crucial role
relationship between rheological properties and the volume fraction of in determining the textural and rheological properties of bigels. A large
the dispersed phase. As the oleogel/hydrogel ratio increases, the com­ number of reports illustrated that varying hydrogelators have more
plex modulus also increases. The Kerner model and the S-shaped obvious influence on the texture of bigels than organogelators (Behera,
Boltzmann model were established as tools for predicting food products Singh, et al., 2015; Martin Illana, Notario Perez, Cazorla Luna, Ruiz
such as fat substitutes, sauces, dressings, etc (Bruno, Lupi, Mammolenti, Caro, & Veiga, 2019). Different hydrogelators can lead to variations in
Baldino, & Gabriele, 2024). viscosity, spreadability, hardness, and deformation resistance of bigels.
Here are some key observations and examples of how various hydro­
3.1.2. Type of gelators gelators can impact the properties of bigels:
The inherent strength of both phases within bigels, namely the Various biopolymers are the most commonly used gelling agents in
oleogel phase and the hydrogel phase, is fundamental in determining the the manufacture of hydrogel. Polysaccharides like sodium alginate
mechanical strength and overall texture of these complex materials. The (Behera et al., 2014), guar gum (Sahoo et al., 2015), gelatine (Beauty
structure of bigels relies on the degree of crosslinking and the polymer Behera, Singh, et al., 2015), pectin (Lupi, De Santo, Ciuchi, Baldino, &
strength of both phases. Gabriele, 2017), hydroxypropyl-methylcellulose (Ibrahim, Hafez, &
Mahdy, 2013) and agar-gelatin mixture (Wakhet et al., 2015a, 2015b)
3.1.2.1. Organogelator. Oleogels are structured systems stabilized by are commonly used hydrogelators in bigels formulations. During the
the formation of a three-dimensional network created by organo­ formation of polysaccharide-based bigels, the interaction between water
gelators. Organogelators are compounds that have the ability to molecules and these hydrogelators leads to the formation of an ordered
immobilize the nonpolar phase (usually an oil or a hydrophobic liquid) structure around the polysaccharide molecules, contributing to struc­
within a gel-like structure. Adding a gelling agent is considered a viable tural stabilization. For example, when guar gum is dispersed in water,
strategy for creating carriers with more compact structures. Oil struc­ the interaction of galactose side chains with water molecules results in
turing gelling agents are generally classified into two major groups: low intermolecular chain entanglement, leading to increased viscosity in
molecular weight gelling agents and high molecular weight gelling bigels. As the concentration of guar gum increases, the entanglement or
agents (Davidovich Pinhas, 2019). degree of intermolecular chain reaction enhances, leading to increased
Low molecular weight gelling agents can self-assemble and create a viscosity of bigels. Besides, Behera et al. (2014) compared the effects of
stable crystalline network of small molecules, effectively stabilizing the starch polysaccharides (maltodextrin and starch soluble) and non-starch

4
E. Chao et al. Food Hydrocolloids 154 (2024) 110089

polysaccharides (sodium alginate and sodium carboxy methyl cellulose) arrangement of gelant molecules or strengthening the structural
on the mechanical properties of the bigels, and they found that the bigels network within the bigels (Martins et al., 2023). Therefore, the addition
with maltodextrin and starch soluble possesssed the highest firmness of exogenous additives is an effective strategy to modulate the gel
and strength, which was related to the incorporation of branched structure of bigels.
polysaccharides. Branched polysaccharides have a more complex Emulsifiers can enhance the stability of bigels by increasing the
structure compared with linear counterparts. The presence of branching thickness of the interfacial layer. For example, stearic acid and sorbitan
points and side chains causes increased molecular entanglement within monostearate act as mixed emulsifiers in bigels and can adsorb on oil
the polymer network (Behera et al., 2014). This enhanced entanglement droplets to form a thicker interfacial layer due to the amphiphilic nature
results in a denser and more interconnected network, which contributes of the molecules. Importantly, multilayer structures are fabricated
to higher mechanical strength and stiffness. In practical applications, through droplet aggregation, which occurs due to adhesion between
branched and linear polysaccharides can be tailored as hydrogelators in solid lipid particles and hydrophilic gels. This enables uniform and
bigels formulations to achieve specific structural and mechanical prop­ efficient loading of drugs of varying solubility (Kouider et al., 2024). In a
erties. When a firmer or solid-like texture is desired, branched poly­ recent study, researchers used three different emulsifiers, namely pol­
saccharides are generally preferred, whereas for softer or gel-like yglycerol polyricinoleate (PGPR), monoglycerides, and lecithin, to tailor
properties, linear polysaccharides may be selected. The choice depends physical and printing properties of bigels as 3D printable materials. They
on the intended application of the final product and the desired sensory found that emulsifier molecules could significantly influence the in­
attributes. The observation that the gel containing sodium alginate teractions between the oleogel and hydrogel, which, in turn, have a
possessed higher stiffness compared to the gel containing hydroxypropyl direct impact on the formation of the three-dimensional structure of the
methylcellulose (HPMC) can be attributed to the distinct molecular bigels matrix. For example, PGPR was found to have a disruptive effect
structures and properties of these two linear polysaccharides (Rehman on the crystalline process of candelilla wax, resulting in a weaker me­
et al., 2014). chanical strength of the oleogel and phase separation in the bigels. In
Sodium alginate is often used when a firmer and more structured gel contrast, monoglycerides and lecithin were observed to act as crystalline
is required, especially in applications like food and pharmaceuticals particles and self-assembly fibers to promote the formation of oleogel,
where controlled release and stability are required. The non-ionic nature respectively. The addition of monoglycerides and lecithin contributes to
of HPMC makes it more suitable for applications where softer gels are a stable and homogenous gel system with a bicontinuous emulsion
preferred. The differences in critical strain, strength, and firmness structure, ultimately improving the 3D printing performance of bigels.
observed between guar gum-based bigels and those based on acacia gum In addition to changing additive/emulsifier types, adjusting the additi­
and xanthan gum can be attributed to the unique properties of these ve/emulsifier concentration could be also a texture modification method
hydrocolloids (Sahoo et al., 2015). The superior properties of guar of bigels. The interaction between gellan gum and polysorbate 80 can
gum-based bigels, attributed to strong interactions between guar gum lead to variations in the texture and technological characteristics of gels,
and the organogelator (Span 40) molecules, highlight the importance of such as their hardness or softness, depending on the surfactant con­
molecular interactions in determining the characteristics of these centration (Fasolin, Picone, Santana, & Cunha, 2013). At the low poly­
biphasic systems. These strong interactions between the organogelator sorbate concentration, the gellan gum properties were predominant and
and hydrogelator molecules played a crucial role in enhancing the the gellan gum underwent the conformational coil–helix transition. This
rheological and mechanical properties of guar gum-based bigels. The transition leads to the formation of harder gels, even at elevated tem­
study conducted by Lupi et al. (2017) investigated the impact of peratures. With increasing polysorbate concentration above 30% (w/w),
hydrogelator content, particularly pectin, on the rheological properties the surfactant micelles prevented the gellan–gellan aggregation and
of bigels systems. The key finding of the study was that an increase in interaction, forming the softer gels. This change in gel texture offer
pectin content led to improvements in both consistency and the degree opportunities for the application of these gels in various products across
of structuration in the bigels. Besides, some studies have explored the industries such as food, pharmaceuticals, and cosmetics.
use of composite hydrogelators, such as κ-carrageenan and gelatin, to Additionally, controlling the interface content of emulsifiers in O/W
create bigels. In summary, the combination of κ-carrageenan and gelatin bigel systems is crucial for modulating the bulk properties of bigels. Two
in bigels systems results in the formation of cross-linked polyelectrolyte common preparation procedures for bigels are suggested, and they differ
complexes due to hydrogen bonding and electrostatic interactions in the state of the phases during mechanical stirring. The first procedure
(Derkach, Voron’ko, Maklakova, & Kondratyuk, 2014). This complex­ involves the direct mixing of the two gels at room temperature. In
ation leads to changes in the swelling behavior of the bigels, making it contrast, the second approach is performed with both phases in a liquid
less prone to swelling and expansion. The strong electrostatic in­ state. The latter method relies on the ability of emulsifiers to stabilize
teractions between protein and polysaccharide chains indeed play a the interface between water and oil, two immiscible liquids. This
significant role in influencing the fluidity and network structure of approach offers an effective means of altering and controlling the bulk
composite hydrogels (Zampouni, Mouzakitis, Lazaridou, Moschakis, & properties of bigels by adjusting the interface content of emulsifiers in
Katsanidis, 2023). These findings have implications for tailoring the O/W bigels systems. Golodnizky and Davidovich Pinhas (2020) reported
properties of bigels for specific applications by manipulating the in­ that the bigel containing sucrose esters (SEs) with HLBs of 1 and 2
teractions between hydrogelators. exhibited a higher elastic and solid-like behavior in comparison with the
bigel containing SEs with an HLB of 6. They found that mono-esterified
3.2. Extrinsic factors SEs exhibit the stronger ability to diffuse and adsorb compared to fully
esterified SEs. The lower molar mass of mono-esterified SEs causes a
3.2.1. Incorporation of additives/emulsifiers higher SE content at the oil-in-water (O/W) interface, as opposed to
The stability of a biphasic matrix relies on the equilibrium between being predominantly present in the bulk oil phase. This difference in the
attractive and repulsive forces acting among its components (Con­ diffusion kinetics contributes to different droplet size, further altering
treras-Ramirez et al., 2022). Although organogelators and hydrogelators gel properties. Moreover, Guo, Gu, et al. (2023) found that the edible
have the ability to immobilize the oil-water components, phase sepa­ Spirulina platensis protein nanoparticle nanoparticle-based bigel exhibi­
ration may still occur during sample preparation and prior to gelation. ted the better technological and functional outputs compared to the
The high temperatures applied during the thermal emulsification pro­ bigels consisting of wax-based oleogel due to the dual stability mecha­
cess increase the mobility of molecules within the system (Con­ nism, both nanoparticles interfacial adsorption and bulk stabilization in
treras-Ramirez et al., 2022). The addition of exogenous additives in a one system.
bigel system plays a significant role in promoting the structural It is worth noting that some emulsifiers, such as mono-diglycerides,

5
E. Chao et al. Food Hydrocolloids 154 (2024) 110089

could act as both emulsifiers and fat crystal modifiers in bigels systems. lower release of lycopene (Zhu et al., 2021), lutein, ascorbic acid (Kai­
The addition of these emulsifiers could improve interfacial and struc­ mal & Singhal, 2023a, 2023b) and β-carotene (Zheng et al., 2020)
tural stabilization by the formation of crystals traps the oil phase and occurred during the gastric digestion phase and slowly sustained release
solidifies the oleogel. In the other words, they have the dual effect of during the intestinal digestion phase. This is related to the interfacial
adjusting mechanical properties and improving physical stability (Saf­ properties of the oleogel component, namely hydrophobicity, lower
fold & Acevedo, 2022). Nutter et al. (2023a, 2023b) found that the swelling ratio, and higher dispersed phase particle size (Kaimal & Sin­
formation of compact networks of mixed-sized crystals in binary ghal, 2023a, 2023b). Zhu et al. (2021) developed high acyl gellan
monoglycerides and wax-based oleogels is a significant factor contrib­ gum/glycerol monostearate-beeswax bigels as carriers for lycopene.
uting to their enhanced oil binding capacity. Samui, Goldenisky, Rosen This phenomenon where lycopene release decreases as the oleogel
Kligvasser, and Davidovich Pinhas (2021) prepared a novel in-situ bigel fractions increase can be attributed to the inhibitory effect of the oleogel
system depending on glycerol monostearate oleogels and gelatin on the penetration of gastric juices into the interior of the bigels
hydrogels with the addition of lecithin and glycerol as surfactant and network. However, in simulated intestinal fluid, the percentage release
co-surfactant, respectively. Glycerol mono-stearate plays a dual role in of lycopene from the bigels continued to increase. This is because the
stabilizing the studied bigels: on the one hand, glycerol mono-stearate structure of bigels collapses in the simulated intestinal fluid, allowing
contributes to the solidification of oleogels within the bigels system. lipase to directly attack the oleogel particles and promoting the release
This occurs through the process of crystallization and network forma­ of lycopene. Furthermore, κ-carrageenan/monoglyceride-based bigels
tion; on the other hand, it possesses emulsification characteristics, were prepared as carriers for β-carotene (Zheng et al., 2020). The results
allowing it to interact with both water and oil phases. indicated that increasing oleogel fractions improved the thermal sta­
bility and light stability of β-carotene. The bigels with 75% oleogel re­
3.2.2. pH tains 70% of the original β-carotene content after 8 h of UV-light
Many biological macromolecules are sensitive to pH changes. In this exposure. The release of bigels in simulated gastric juice exhibited a
case, adjusting the pH is a versatile technique that can be used to affect decrease, while the release ratios in simulated intestinal juice were
the physical and chemical interactions within bigels, ultimately allow­ greatly increased, with higher oleogel content promoting these release
ing for the modulation of their microstructural and textural properties. ratios. Notably, the structure of bigels exhibits advantages in slow
The study conducted by Cui et al. (2022) demonstrated how pH can play release of bioactive substances and colonic phase delivery compared to
a critical role in the fabrication of chitosan-cinnamaldehyde-glycerol single oleogel or hydrogel. The chemical stability of curcumin encap­
monolaurate bigels, particularly by influencing the extent of the sulated in bigels is significantly improved, but the bioaccessibility is
Schiff-base reaction. At the low pH (3.8), the homogenous bigel was reduced compared with oleogel, which is related to the hydrogel
formed, while at a higher pH, the phase separation of bigels were inhibiting the digestion of oleogel and thereby reducing the curcumin
occurred. Besides, Richa and Roy Choudhury (2023) found that the release ability (Gonçalves, Zhou, Vicente, Pinheiro, & McClements,
interaction between hydrogen ions and carboxylate groups in carra­ 2024). Additionally, the study by Lu et al. (2022) highlights the po­
geenan reduces electrostatic repulsion in carrageenan at lower pH. Due tential of bigels to co-delivery lipophilic (curcumin) and hydrophilic
to the formation of a stable junction region, the interaction between (epigallocatechin gallate) functional ingredients while considering the
carrageenan molecules is enhanced, thereby enhancing the stability of structural properties of the bigels and the digestive process. During
carrageenan based bigesl at lower pH and reducing swelling. gastric digestion, the bigels were able to maintain their intact structure
effectively. However, gels with higher gel-strength inhibited the release
4. Application of bigels in food system of curcumin to a greater extent during this stage. Notably, EGCG, a
hydrophilic component distributed within the external hydrogel
The application of bigels in the food industry is vast and diverse, (gelatin), was susceptible to attack by pepsin. The hydrolysis of gelatin
encompassing various aspects of food production and innovation, from caused the structural breakdown of the hydrogel, resulting in the rapid
serving as fat replacers to acting as efficient delivery systems for degradation of EGCG. Interestingly, a higher content of glycerol mon­
bioactive ingredients and enabling innovative 3D printing food pro­ ostearate (oleogelator) significantly the release of curcumin during
duction. Table 1 and Table 2 provide an overview of the primary ap­ digestion, while having little effect on the release of EGCG. Interestingly,
plications of bigels in the food industry. new gel beads with a bigel structure also demonstrate the advantage of
encapsulating EGCG and curcumin simultaneously. The hydrogel
4.1. Bigels used as delivery systems network structure (alginate gel) not only plays a strong barrier role
during the encapsulation process but also improves the effective diffu­
4.1.1. Bigels-based delivery systems for bioactive compounds sion of EGCG through the hydrogel microstructure. Due to the relatively
Co-delivery systems, capable of encapsulating two or more bioactive loose alginate network structure, it helps to increase intestinal release
compounds simultaneously, have emerged as valuable tools to improve rate. Additionally, the encapsulation efficiency of lipophilic and hy­
health benefits and nutritional value of food products (Hashemi, drophilic substances in gel beads can be controlled by changing the ratio
Assadpour, & Jafari, 2024). Bigels, characterized by structured aqueous of oleogel and hydrogel. Specifically, the encapsulated curcumin can
and oil phases, have gained prominence as favorable delivery systems hydrophobically bind to the palisade layer of Tween 20 micelles and can
for both lipophilic and hydrophilic bioactive compounds (Fig. 3 and diffuse from the beads. During the syneresis process, the increase in the
Table 1). The cross-linked network structures of bigels act as effective proportion of oleogel will lead to a reduction in the effective content of
shields against adverse environmental pressures. Notably, the structural the emulsifier, thereby reducing the release of micelle-bound curcumin
variations among different bigels systems influence their disintegration (Yang, Song, Miao, Gao, & Mao, 2024). In O/W bigels, lipophilic
properties, thereby impacting the release characteristics of functional bioactive substances, such as coenzyme Q10 (CoQ10) and fish oil,
ingredients. This demonstrates that the release of bioactive compounds incorporated into the oleogel phase have demonstrated the ability to
can be modulated by the structural properties of the bigels. significantly enhance stability. Concurrently, the surrounding hydrogel
Generally, bigels with higher gel strength could provide enhanced phase facilitates the penetration of these bioactive substances through
protection for encapsulated bioactive compounds. Bigels with a higher the skin membrane. The combination of adhesive properties, appro­
ratio of oleogel/hydrogel possess higher gel strength, which can inhibit priate viscosity, and the lipophilic nature of the fish oil-based bigel
the penetration of gastric juices inside the bigels network. During the system makes it an effective vehicle for delivering CoQ10 across the skin
intestinal digestion stage, the oleogel network slowly collapsed, membrane. CoQ10 exhibits a strong binding affinity between EPA and
enabling a slow release of the encapsulated bioactive compounds. The DHA, resulting in the formation of complexes between EPA, DHA, and

6
 E. Chao et al.
Table 1
Applications of bigels in delivery systems for bioactive ingredients.
Delivered target Bigels Key findings Ref.

Oleogel Hydrogel Oleogel/ Synthesis Emulsifier/Additives The highest

Hydrogel parameters release rate (%)
ratio (w/w)

Curcumin/ Glycerol monostearate sodium alginate 10: 90 Two-step Tween-20 70% of curcumin was retained after 40 days / Yang et al.
epigallocatechin (GMS) (10% w/w)-corn (1%, w/w) 15: 85 method: 500 (2024)
gallate (EGCG) oil 20: 80 rpm
25: 75
30: 70
Curcumin/EGCG GMS-corn oil Gelatin 50: 50 Two-step Tween-20 1. Higher GMS content contributed to lower 85 (EGCG) Lu et al. (2022)
method: 300 release of curcumin.
rpm 2. GMS content exhibited little effect on the
60 ◦ C release of EGCG. 36.3 (Curcumin)
20 min
Catechin/quercetin Candelilla wax-high oleic fish gelatin 30: 70 Two-step Stearate monoglyceride/Soy 1. The release of quercetin from bigels 53.37 ± 0.47 Xie et al.
acid sunflower seed oil method: 300 lecithin containing monoglyceride and lecithin was (catechin) (2023a, 2023b)
rpm positively associated with the extent of FFAs 11.08 ± 2.84
50: 50 90 ◦ C release (quercetin)
70: 30 10 min 2. The bigel with 50% oleogel and soy
lecithin possessed the highest release of
catechin.
Curcumin Candelilla wax-coin oil 30: 70 70: 30 One-step / The stability of curcumin embedded by bigel 16.3 ± 3.9 Gonçalves et al.
method: 1300 was 43.8% (2024)
rpm
50: 50 90: 10 25 ◦ C
70: 30 10 min
7

β-carotene Monoglyceride-corn oil κ-carrageenan 25: 75 Two-step / 1 0.08%–0.11% of β-carotene was released 89.2 Zheng et al.
method: 300 in simulated gastric juice. (2020)
rpm 2 The bigels (25% oleogel) exhibted the
40: 60 80 ◦ C highest release of β-carotene.
50: 50 20 min 3 Oleogel fractions↑ the release rates and
60: 40 the released percentage↑
75: 25 4 The bigel (75% oleogel) possessed the
highest release of β-carotene.
Sunflower oil-ethyl xanthan-guar gum 25: 75 One-step / 1 Good thermal stability 87 Kaimal and
cellulose method: 2 Encapsulation rat is greater than 97% Singhal (2023a,
10000 rpm 2023b)
50: 50 70 ◦ C
75: 25 5 min
Lycopene Glycerol monostearate gellan gum 10: 90 Two-step / 1 Increased oleogel ratio was beneficial for 85 Zhu et al.
-beeswax -soybean oil method: retarding the release of lycopene. (2021)
10000 rpm 2 Bigel with 60% oleogel exhibited the
20: 80 60 ◦ C lowest release percentage (60%) of
30: 70 1 min lycopene after a complete digestion

Food Hydrocolloids 154 (2024) 110089

40: 60 process.
50: 50
60: 40
Lutein Sunflower oil -ethyl xanthan gum-guar 25: 75 Two-step Tween 80 1 Hydrogel fraction↑Swelling ratio and 83.2 Kaimal and
acetate gum method: lutein release↑ Singhal (2023a,
10000 rpm 2 The bigel (25% oleogel) possessed the 2023b)
50: 50 75 ◦ C highest release of lutein (83.2%)
75: 25 5 min
(continued on next page)
E. Chao et al. Food Hydrocolloids 154 (2024) 110089

CoQ10 that further enhance its permeation through the skin. Addi­
tionally, the binding energy between fatty acids and CoQ10 has been

Martinez et al.
Mousavi et al.

Zulfakar et al.

Behera et al.
found to influence the drug permeation flux (Zulfakar et al., 2018).
Additionally, the type of gelators have an impact on the delivery of

(2021)

(2018)

(2014)

(2021)
bioactive compounds. Bigels with hydrogelators containing branched
Ref.

polysaccharides release less bioactive compounds, which is related to

the fact that the branching of these polysaccharides can strengthen the
gel matrix, thereby hindering the release of bioactive compounds.

(metronidazole)
release rate (%)

0.514 ± 0.072
Behera et al. (2014) developed bigels using Span-40 oleogels and
The highest

(mg/cm2)
various hydrocolloid hydrogels (CMC, sodium alginate, starch, and
13.91

maltodextrin) for co-delivery of a lipophilic drug and probiotics.

58.3
Branched polysaccharides (e.g., maltodextrin and starch) were found to

/
enhance probiotics’ viability within bigels. The entrapment and survival
1 The release rate of CoQ10 bigels was 1.46
and 1.47 times higher than that of oleogel

The oxidative stability of bigels maintained

Quercetin entrapment in the bigels delayed

viability of 9 × 108 cfu/g after 60 days. of Lactobacillus plantarum 299v in bigels exceeded 108 CFU/g after 60
2 The drug flux of CoQ10 bigels was 1.41
and 1.52 times higher than oleogel and

significantly better probiotics viability

compared with other polysaccharides.
the release time and prevented its pro-

2 Branched polysaccharides produced days of storage, indicating improved tolerance in simulated gastroin­
1 Maltodextrin-based bigels showed a
oxidant property due to high doses.

testinal fluids compared to free cells. Besides, different emulsifiers have

different effects on the delivery efficiency of bigels. For example,

for 90 days in 40 ◦ C of storage

and hydrogel, respectively.

monoglyceride presented greater effect on improving the stability of

hydrogel, respectively.

bigels compared with lecithin, which was related to different emulsifiers

exhibited different effects on the microstructure of bigels (Xie et al.,
2023a, 2023b). An interesting study by Lang Liu, Abdullah, Tian, Chen,
Huang, and Xiao (2023) involved the design of novel bigels that incor­
Key findings

porate a binary hydrogel composed of different mass ratios of konjac

glucomannan to gelatins with stearic acid oleogel. The observation that
the total release of free fatty acids and quercetin decreased with an
increased ratio of konjac glucomannan to gelatins in a bigel system
Triethanolaminebutylated

suggests that the compositional changes within the bigel have a direct
Benzalkonium chloride

impact on the release of these bioactive compounds. The observation

that enhanced gel strength resulted in a delay in the digestion of lipids
Emulsifier/Additives

Calcium carbonate

Hydroxianisole

and subsequently delayed the release of encapsulated bioactive

Phenoxyethanol

Caprylyl glycol

substances.
Carbopol
Tween 80

The release of bioactive compounds is also linked to the swelling

Span-40

capacity of the bigels. A recent study on lutein-loaded bigels exhibited

that the release of lutein increased with an augmented hydrogel fraction
1
2
3
4

in the bigels in gastric digestion stage (Kaimal & Singhal, 2023a, 2023b).
method: 50 ◦ C

This increase in lutein release can be attributed to the enhanced the

method: 800

method: 600
parameters

swelling of hydrogel resulted in a marginal leaking of the oleogel.

Synthesis

Two-step

Two-step

Two-step
500 rpm
20 min

15 min

15 min
25 ◦ C

25 ◦ C
rpm

rpm

4.1.2. Bigels used as delivery systems to encapsulate and release food

nutrients
Bigels have demonstrated significant potential as versatile delivery
ratio (w/w)

systems for encapsulating and releasing food nutrients. Interestingly, a

Hydrogel
Oleogel/

50: 50

50: 50

bigel with both heat-triggered natural pigment release properties and

5: 95

heat-responsive color-changing properties was developed, providing the

/

food industry with a new way to stably and precisely regulate the release
Sodium polyacrylate

of natural pigments by adjusting the concentration of candelilla wax in

Sodium alginate-

Polysaccharides:

methyl cellulose
Sodium alginate
Sodium carboxy

the oleogel (Lee, Baek, Jeong, & Lee, 2024). In addition, the relationship
Starch soluble
Maltodextrin

between color changes and the bioactivity embedded in bigels was

ferula gum
Hydrogel

Carbopol

established through a classical kinetic model, enabling the development

of a new method for real-time monitoring of bioactive content in
4D-printed bigels products. The loss of structural stability in 3D-printed
bigel products is closely related to the high degree of water freedom in
sunflower oil-mineral oil

the hydrogel and the fluidity of the oleogel, which subsequently affects
Stearic acid-cottonseed

hydroxystearic acid-

the color change and molecular movement of curcumin and β-carotene.

Candelilla wax-12-
Fish oil-Bees wax

(Qiu et al., 2024). In a study conducted by Machado et al. (2022), a

oil/cannabis oil

Sunflower oil

novel avocado oil-functionalized yogurt with anti-obesity potential was

developed, and bigels samples of these yogurts exhibited significantly
Oleogel
Bigels

higher levels of total fatty acids compared to yogurts with free-form

avocado oil. Additionally, yogurts with avocado bigels demonstrated
better stability throughout the gastrointestinal tract and increased the
Table 1 (continued )

lipolytic rate in adipocytes. This suggests that bigels serve as a protective

encapsulation process for avocado oil, preventing the deterioration of
Delivered target

Metronidazole/

major fatty acids during production and digestion. Furthermore, diges­

probiotics

Vitamin E
Quercetin

ted samples were found to modulate obesity-related cellular metabolites

CoQ10

in vitro (Machado et al., 2022). In another study by Zhuang et al. (2021),

a soy lecithin-stearic acid oleogel emulsion and a whey protein hydrogel

8
 E. Chao et al.
Table 2
Applications of bigels in real food system.
Applications Bigels Advantages Disadvantages Ref.

Oleogel Hydrogel Optimal Synthesis Emulsifier/

oleogel/ parameters Additives
hydrogel
ratio (w/w)

Cream analogues 30 wt% corn oil, 5 wt% 2 wt% xanthan gum 40: 60 One-step / 1 Oleogel-hydrogel ratio of The flavor of bigel is Qiu et al. (2024)
whey protein isolate method: 10000 40: 60 presented best somewhat different from
rpm thermal stability that of commercially
25 ◦ C 2 Mixing commercial cream available cream
3 min and bigel 1:1 not only
resembles commercial
cream in texture and taste,
but also has higher stability
food spread Walnut oi/l Candelilla Chitosan/sodium 60: 40 Two-step Mono- and Uniform structure, good / Li et al. (2024)
wax tripolyphosphate method: 6000 diglycerides of texture, rheological
rpm fatty acids/ properties and thermal
25 ◦ C γ-oryzanol/ stability
3 min β-sitosterol
Sustainable Cinnamaldehyde/ Chitosan 33: 67 Two-step Span 80 Bigels formed at pH 4.3 Compared with the Cui et al. (2022)
alterative to glycerol monolaurate/ method: 200 exhibited good thermal commercial creams, the
plastic fats like medium chain rpm reversibility. melting temperature↓
cream triglyceride 60 ◦ C
20 min
9

Fat replacer Low-fat beef Sunflower oil/ Wheat starch 75: 25 Two-step sodium azide 1 Compared to the control After replacement of 75% (Ghiasi & Golmakani,
burgers Ethylcellulose method: 2000 sample with animal fat, all animal fat with bigel, 2022),
rpm low-fat burgers showed hardness, gumminess, and
25 ◦ C better cooking chewiness↑
2 min characteristics.
2 Bigels containing higher
oleogel were thermally
more stable.
Semi-dry sausage Olive oil/15% w/w 2% w/w 80:20 Two-step 2.125% w/w 1 Compared with pork back The dehydration rate Zampouni, Filippou,
monoglycerides κ-carrageenan method: 12000 Tween 20 fat, the bigel contains 20% decreased during Papadimitriou, and
rpm less energy and 27% less fermentation. Katsanidis (2024)
25 ◦ C fat, respectively.
2 min 2 The bigel formula has the
lowest cholesterol content.
Compound Grape seed oil/ Sodium alginate 95: 5 Two-step / The compound chocolate Low adhesiveness Ghorghi et al. (2023)
chocolate Beeswax method: 600 replaced by the bigel at 15%
rpm had and the most similarity to
25 ◦ C the control regarding

Food Hydrocolloids 154 (2024) 110089

45 min hardness and flow behavior.

Low fat cookies Canola oil/Candelilla Gelatinized starch 50: 50 Two-step / 1 Lower hardness and higher Vitro digestibility of starch (Barragan-Martinez
wax method: 10000 firmness. (43%)↑ et al., 2022)
rpm 2 Total fat and saturated fat
90 ◦ C content↓
5 min
(continued on next page)
 E. Chao et al.
Table 2 (continued )
Applications Bigels Advantages Disadvantages Ref.

Oleogel Hydrogel Optimal Synthesis Emulsifier/

oleogel/ parameters Additives
hydrogel
ratio (w/w)

Cookies Alginate/ Rice bran wax/ 80: 20 One-step 1 Improved fatty acid profile, Limited ductility Nutter et al. (2023a,
κ-carrageenan soybean oil n method: 15000 free of palm oil and animal 2023b)
rpm ingredients
85 ◦ C 2 The texture is softer than
1 min butter.
cheese sticks Soybean oil/stearic Konjac One-step Lower viscosity, igher creep / Tian et al. (2023)
acid (3.00 % w/w) glucomannan & method: 9000 recovery and enhanced
gelatin rpm mouthfeel during minimal
75 ◦ C oral chewing
3 min
Encapsulation Avocado oil Carboxymethyl Geleol / One-step Tween 80 1 Protect the avocado oil / Machado et al. (2022)
fortified yogurts cellulose avocado oil method: 10000 during the yogurts
rpm manufacture and avoid its
60 ◦ C oxidation
1 min 2 Thrombogenic indexes
(0.69 ± 0.03)↓
3 Higher recovery
percentage of oleic acid in
the intestine (47.2%)
4 The highest lipolytic effect
Probiotic bigels Soy lecithin stearic Whey protein 75: 25 Two-step / L. acidophilus or B. lactis The mechanism by which Zhuang et al. (2021)
in yogurt acid method: 13500 survived better bigels protect probiotics is
10

rpm unclear.
85 ◦ C
2 min

Dysphagia diet Carnauba wax Collagen 60: 40 One-step Lecithin 1 Higher elasticity and 1 An increase in firmness. (Eisinaite, Jasutiene,
product method: 10000 higher complex viscosity 2 Due to the higher fat and Vinauskiene, &
rpm 2 Higher cohesiveness values wax content, bigels Leskauskaite, 2023)
60 ◦ C containing 60% of
1 min oleogel fraction were less
sensually acceptable
Intelligent food In-situ and real- Sunflower oil/ Agar/purple sweet 80: 20 Two-step / 1 Best sensitivity to alkali Poor color recovering Zhai et al. (2022)
packaging time monitoring beeswax/glyceride potato method: 12000 and color stability under ability of the bigels
of beef and monooleate anthocyanins rpm pH 6.5
salmon freshness 70 ◦ C 2 Good color stability in
2 min water
3 Excellent anti-leaching
ability
Coatings on fresh Sunflower oil/ Agar/anthocyanins 80: 20 Two-step / 1 More effective oxygen / Kanelaki et al. (2022)

Food Hydrocolloids 154 (2024) 110089

sardine fillets beeswax/glyceride method: barrier than the plain
monooleate 300 rpm hydrogel coating
70 ◦ C 2 Prevent dehydration of the
15 min fillet surface
3 Protecting the sardine
fillets from oxidative
deterioration.
The combination of 3D printing Sunflower seed oil/ Fish gelatin 70: 30 One-step / Bigel with great printing 1 The printed bigel strings Xie et al. (2023a,
technology and bigels candelilla wax method: 300 performance could be were still rigid and could 2023b)
rpm obtained by adjusting the not well adhere to
90 ◦ C previous printed layers.
(continued on next page)
 E. Chao et al.
Table 2 (continued )
Applications Bigels Advantages Disadvantages Ref.

Oleogel Hydrogel Optimal Synthesis Emulsifier/

oleogel/ parameters Additives
hydrogel
ratio (w/w) hydrogel/oleogel ratio and
types of emulsifiers.
10 min 2 The texture was too soft
to self-support the prin­
ted layers and retain the
designed three-
dimensional structure
3 Some oil leakage
4 The semi-bicontinuous
state bigels exhibited the
worst extrusion ability
due to the inhomogeneity
of the system.
Soybean oil/Beeswax/ Hydroxypropyl 50: 50 Two-step / A lubricious and glossy / Chen et al. (2023)
Polyglycerol methylcellulose method: 8000 surface
polyricinoleate rpm
85 ◦ C
1 min
Beeswax Litchi homogenate/ / One-step / 1 Smooth extrusion / Tian et al. (2021)
carrageenan/ method: 30 min 2 Fast gelation
11

xanthan gum 3 High deformation

resistance
4 The accuracy, shape
retention and stability of
3D printed food materials.
Beeswax Carrageenan/ 80: 20 Two-step / 1 Suitable consistency and / Qiu et al. (2022)
xanthan gum method: 3000 fluidity
rpm- 2 Rapid recoverability
2min+6000 3 Outstanding mechanical
rpm-3min properties
80 ◦ C
Sunflower waxes/ Xanthan gums 56: 44 Two-step / 1 Promising formability for / Guo, Gu, Du, and Meng
soybean oils method: 12000 decorating (2023)
rpm 2 Good appearance integrity
85 ◦ C to cream flowers
2 min
Ethyl cellulose/ Gelatin 60: 40 Two-step / 1 Excellent fluidity / Jiang et al. (2022)
glycerol method: 8000 2 Ideal rheological properties

Food Hydrocolloids 154 (2024) 110089

monostearate/soybean rpm and hardness
oils 70 ◦ C
2 min
E. Chao et al. Food Hydrocolloids 154 (2024) 110089

Fig. 3. Bigels-based delivery systems for bioactive ingredients. Conjugated linolenic fatty acids-CLNA, medium-chain fatty acids-MCFA, curcumin-CUR, epi­
gallocatechin gallate-EGCG, simulated gastric juice-SGF, simulated intestinal juice-SIF, the ratio of oleogel and hydrogel-OG: HG, glycerol monostearate-GMS.

were mixed to manufacture the probiotic bigels, and Lactobacillus aci­ oleogel-to-hydrogel ratio decreased the hardness and adhesion of the
dophilus (L. acidophilus) and Bifidobacterium lactis (B. lactis) were incor­ bigel. A bigel developed based on walnut oil-based oleogel and chitosan
porated and suspended in milk. Compared with the free bacteria, the hydrogel demonstrated good sensory properties by replacing 75% of
total amount of L. acidophilus and B. lactis entrapped in bigels was commercial spreads (Li et al., 2024). Interestingly, an increase in the
significantly higher after 3–5 weeks, suggesting that probiotics could be oleogel-to-hydrogel ratio induced a decrease in the release of oil-soluble
embedded and their survival rate significantly enhanced. This suggests a flavor substances in cheese (Tian et al., 2023). A bigel formula butter
promising future for the application of bigels in commercial yogurt that contains unsaturated fatty acids with rich nutritional value and
production, with the aim of improving probiotic survival. Additionally, encapsulated probiotics has been developed (Hashim, El Sayed, & El
Eisinaite, Jasutiene, Vinauskiene, and Leskauskaite (2023) developed a Sayed, 2023). Besides, Cui et al., 2022 also fabricated chitosan-based
bigel with strong shear-thinning behaviour and high protein concen­ bigels (chitosan-cinnamaldehyde-glycerol monolaurate bigels),
tration (16%–36%) oriented to the dysphagia diet. In the providing a healthy and sustainable alternative to plastic fats like cream.
dysphagia-oriented food products, thermally treated collagen was used Bigels fabricated at pH 4.3 showed great thermal reversibility and dis­
as a gelator for hydrogel phase and as source of proteins. The concen­ played similar textural attributes and appearances to commercial
tration of collagen significantly affected the structural properties and creams. The findings regarding the thermal reversibility of bigels with
visual appearance of the bigels. Bigels composed of the highest collagen different gelling agents and vegetable oils have important implications
concentration exhibited higher viscosity, viscoelasticity, and cohesion for potential future applications in low-fat foods. A novel bigel butter
values, indicating that collagen played a dominant role in the formation spread was developed as a fat replacer using sesame/beeswax oleogels
of the bigel structure. The use of bigels in ensuring a safe swallowing and sodium alginate/whey protein hydrogels. The resulting bigels
process and reducing the risk of malnutrition is a significant advance­ showed a balanced fatty acid composition, high oxidative stability, and
ment, particularly in the context of food products for individuals with maintained probiotic viability above recommended levels. This butter
swallowing difficulties or those at risk of malnutrition. spread bigel has the potential as a new carrier system for probiotic de­
livery. However, further studies are needed to investigate viability and
counts.
4.2. Use of bigels as fat replacers
The potential of bigels with starch and ethylcellulose as a fat replacer
was first demonstrated in food products by Ghiasi and Golmakani
Obesity, a global health issue, is often associated with high con­
(2022), who found that low-fat beef burgers using bigels offers improved
sumption of saturated fats (Henney et al., 2024). This highlights the
cooking properties in comparison with those with animal fat. Among
need for healthier fat replacers. They can be incorporated into products
them, the bigels with a 75% oleogel fraction displayed the highest values
such as cream, burgers, cookies, and chocolate to reduce saturated fat
for hardness, gumminess, chewiness, springiness, and cohesiveness,
content. The mechanical properties and structural stability of the bigels
making it the most effective fat replacer. The increased hardness,
as fat replacers were mostly affected by the ratio between oleogel and
gumminess, and chewiness observed after replacing 75% of animal fat
hydrogel. Bigels with higher ratio between oleogel and hydrogel were
with the bigels can be attributed to the strong and compact gel network
thermally more stable according to their greater viscoelastic behavior.
formed by the bigels within the burger matrix (Herrero, Ruiz-Capillas,
Recent studies indicate that oleogels and hydrogels developed from
Jimenez-Colmenero, & Carmona, 2014). Besides, the reduction in
whey proteins and polysaccharides were prepared as bigels and devel­
cooking shrinkage observed when using bigels as a replacement for
oped as trans-fat substitutes with similar appearance, flavor, stability,
animal fat in burgers can be attributed to the high melting point of
and rheological properties to commercially available creams. Further­
ethylcellulose oleogel. The high melting point of ethylcellulose oleogel
more, a higher oleogel-to-hydrogel ratio induces protein folding and
and the thermal-irreversible nature of the starch hydrogel work together
exposure of hydrophobic groups, strengthening the network structure
to maintain the shape, structural integrity, and thermal stability of
and gel behavior (Qiu et al., 2024). Similarly, increasing the

12
E. Chao et al. Food Hydrocolloids 154 (2024) 110089

burgers during the cooking process. Furthermore, sensory panelists re­ bigels as protective coatings for enhancing the shelf life and quality of
ported no significant differences in overall acceptability between the food products.
control group and the low-fat burgers, indicating a significant role for
bigels in the development of healthier food formulations. In another 4.4. 3D printing food
study by Nutter et al. (2023a, 2023b), a promising plant-based semi-­
solid fat substitute with an enhanced ratio of saturated to unsaturated Indeed, emulsions and emulsion gels have been extensively
fatty acids was developed. Notably, the bigel with an 80:20 oleo­ researched in the context of food 3D printing; however, they come with
gel/hydrogel ratio containing 2% monoglycerides exhibited the most inherent challenges such as instability and weak self-supporting prop­
suitable rheological properties for commercial semisolid fats. erties. These limitations make them prone to deformation during key
Different oleogel-hydrogel ratios will affect the properties of the stages of 3D printing, including extrusion, recycling, and providing
dough and, consequently, the properties of the biscuits produced. A structural support (Li, Fan, Liu, & Li, 2021). A promising development in
lower oleogel-to-hydrogel ratio restricts the mobility of water molecules the food industry is the integration of 3D printing technology with
in the dough, thereby limiting the hydration of the flour particles. bigels. This combination holds great significance for several reasons.
Conversely, a higher oleogel-to-hydrogel ratio reduces sugar solubility, Firstly, bigels consist of two phases, allowing them to encapsulate both
resulting in a dough with increased viscosity, i.e., higher crystalline hydrophilic and oleophilic nutrients, thereby enhancing nutritional
sucrose concentration, compared to dough made with butter. Therefore, diversity-an important objective in the future of food 3D printing. Sec­
adjusting the ratio of oleogel to hydrogel allows for modification of the ondly, 3D printing technology has the potential to enhance the food
viscosity of dough and, consequently, the texture of the biscuits (Nutter industry by offering personalized food and nutritional choices, enabling
et al., 2023a, 2023b). Cookies made with bigels as a fat replacer have a customization of food products to meet individual preferences, dietary
similar firmness and significantly higher crispness to those containing restrictions, and nutritional needs (Zhao, Zhang, Chitrakar, & Adhikari,
original shortening (Quilaqueo et al., 2022). In another study by Bar­ 2021). For instance, it can be used to create specialized food for elderly
ragan-Martinez, Roman-Guerrero, Vernon-Carter, and Alvarez-Ramirez patients with dysphagia or to craft healthy snacks with creative shapes
(2022), up to 50% of the fat in sugar-snap cookies was replaced with and enriched with essential vitamins for teenagers and children.
bigels. The cookies prepared with bigels tended to have lower hardness Furthermore, bigels exhibit excellent rheological properties, making
and higher firmness than the control group made with commercial them ideal materials for 3D printing applications. Thus, the develop­
shortening. This increase in biscuit hardness may be attributed to the ment of bigels for the field of 3D printing is not only justified but also
gelling effect of the dextrinated starch within the bigels biscuits, which holds immense potential to revolutionize the food industry.
interacts with solid components like sugar and non-dextrinated starch Adjusting the oleogel/hydrogel ratio and incorporating emulsifiers
granules, imparting mechanical stability to the biscuit structure. Ghor­ can significantly improve the 3D printing properties of bigels through
ghi et al. (2023) found that replacing Cocoa Butter Substitute with bigels promoting positive interactions among organogelators, hydrogelators,
at a 15% level was the optimal choice for the production of composite and emulsifier molecules. This fine-tuning of the oleogel/hydrogel ratio
chocolate. This replacement showed roughly similar hardness and flow is essential for achieving optimal printing performance. Increasing the
behavior to the control, and there is no fat or sugar bloom was in the oleogel fraction has a notable impact on the rheological characteristics
samples during storage. The increased melting point resulting from fat of bigel inks, thereby influencing their printability. The latest research
replacement with bigels offers numerous advantages, from improved indicates the development of a novel whippable bigel system. Increasing
heat resistance and extended shelf life to new product opportunities. The the ratio of oil gel to hydrogel results in a reduction in the self-
high resistance to deformation observed in products with fat replace­ supporting force of the foam but an increase in the smoothness of the
ment using bigels can be attributed to the unique three-dimensional printed surface. Consequently, inks with a high oleogel-to-hydrogel ratio
network, intermolecular interactions, crystalline structures, and the are suitable for printing small-area single-layer models (Guo, Song, &
overall stability that bigels provide (Sarika, Prasad, & Kumar, 2023; Meng, 2024). In bigels inks containing oleogel fractions ranging from
Somali, Miguel, Doman, & Kunal, 2024). Future studies could explore 20% to 70%, oleogel and hydrogel particles tended to aggregate to
enhancing the thermal resistance of similar products using bigel struc­ varying degrees after extrusion. However, in bigel inks with an 80%
tures with appropriate concentrations and ratios. This technology holds oleogel fraction, these aggregates remained stable. Notably, bigel inks
significant promise and potential for future exploration and for use as fat comprising 80% oleogel fraction exhibited excellent extrusion proper­
replacers in various dairy, baked goods, and meat products. ties, allowing for smooth nozzle flow within just 2 s. This remarkable
performance can be attributed to the characteristics of the
4.3. Intelligent food packaging beeswax-based oleogel, which lacks strong connectivity between crys­
tals in the oleogel network. As a result, the system can rapidly rebuild its
Bigels offer several notable advantages, one of which is their ability structure after experiencing high shear forces. In contrast, bigels with
to act as physical barriers, providing improved stability to encapsulated lower O/W ratios tend to experience disruption in the network structure
bioactive compounds in challenging external environments, as observed of the hydrogel when subjected to strong shear. This disruption neces­
in a study by Lee, Tan, Ravanfar, and Abbaspourrad (2019). In another sitates the re-establishment of hydrogen bonding, leading to a longer
study by Zhai et al. (2022), bigels were extruded onto polyvinylidene recovery time to restore viscosity (Qiu et al., 2022). Indeed, the research
fluoride film to create a composite film using 3D printing technology. by Qiu et al. (2022) supports the notion that an 80% oleogel fraction is
This innovative approach addressed the issue of anthocyanins leaching ideal for 3D printing applications, as it enhances the stability of printed
in most sensors under humid packaging conditions. The use of a com­ samples. Guo, Gu, Du and Meng (2023) also found the similar result that
posite film for in-situ and real-time monitoring of beef and salmon the bigels with higher oleogel/hydrogel ratio led to the less likely to
freshness is an innovative application. The presence of an oleogel layer collapse, which indicated that the appropriate amount of oleogel
in the bigels acted as a hydrophobic barrier, significantly reducing the enhanced the stability of printed samples. They also observed that
diffusion of external water into the internal hydrogel, thus preventing moisture content significantly influences printing behavior, with slightly
anthocyanins leaching. Furthermore, Kanelaki et al. (2022) utilized higher moisture content playing a crucial role in achieving a smooth
bigels as coatings for fresh sardine fillets with rosemary extract to structure. The study by Jiang et al. (2022) highlights the importance of
evaluate their effectiveness as delivery systems. The results demon­ thixotropy in ethyl cellulose oleogels, which contributes to good 3D
strated that incorporating rosemary extract into the oleogel phase of the printing ability in W/O bigels. These bigels reduce the oil phase content
bigels inhibited oxidative changes and the production of total volatile required for 3D printing compared to high oil phase emulsions. The
basic nitrogen within the coated fillets. This highlights the potential of research showed that bigels containing 60% oleogels exhibited the best

13
E. Chao et al. Food Hydrocolloids 154 (2024) 110089

3D printing effect. Additionally, the choice of continuous phase material 5.2. Future trends
also affects bigel properties, with gelatin hydrogel providing higher
hardness than glycerol monostearate-enhanced ethyl cellulose oleogel. 5.2.1. Environmentally responsive bigels-based nutraceutical delivery
However, an excessive hydrogel content (80%) was found to hinder systems
system fluidity. In addition, Chen et al. (2023) regarding the impact of The delivery systems based on bigels can adapt their properties in
the extrusion process on different types of bigels and their suitability for response to specific environmental triggers is a promising development
3D printing offer some insights. They discovered that the extrusion with potential applications in the food industry. Bigels that can respond
process had a strong destructive effect on W/O bigels and to environmental triggers, such as changes in pH, temperature, ionic
semi-bicontinuous bigels but not on O/W bigels. W/O bigels were strength, or enzyme activity, offer a dynamic approach to controlled
deemed more suitable for printing flat stacked models (e.g., cylinders release of bioactive compounds in food systems. While the concept of
and snowflakes), while O/W bigels were preferable for printing models environmentally responsive bigel-based delivery systems is intriguing, it
with small single-layer structures (e.g., cones). This versatility opens up is important to acknowledge that such systems have received limited
possibilities for replacing traditional solid fats and designing specific attention within the food industry. Further exploration and research in
appearance food products. Furthermore, Xie et al. (2023a, 2023b) found this area are necessary for future advancements.
that bigels containing monoglycerides or lecithin exhibit homogeneity,
stability, and high deformation resistance, which enhances their 3D 5.2.2. Evaluating the bioavailability of bioactive compounds through in vivo
printing performance. However, polyglycerol polyricinoleate was found experiments
to prevent bigel formation due to its interference with the crystalline While bigel-based nutritional delivery systems hold significant
process of candelilla wax in the oleogel phase. Tian et al. (2021) re­ promise for the development of functional foods, the metabolic fate of
ported that the addition of beeswax improved the 3D printing behavior the components constituting these delivery systems remains to be fully
of bigels. Beeswax’s orthorhombic structure melted during the incuba­ studied. Presently, nearly all bigel-based nutritional delivery systems
tion process, forming more hydrocarbon/monoester compounds that developed for food have been assessed solely through in vitro studies.
improved the shear-thinning effect of the bigels. These hydro­ However, conducting in vivo experiments is imperative to establish
carbon/monoester compounds then re-stacked to form more ortho­ long-term metabolic mechanisms accurately. To achieve this, it is
rhombic structures during the self-support stage, thereby enhancing the essential to consider more practical models, including cell cultures,
gel strength of the bigels. animal models, and human experiments, to precisely evaluate the
bioavailability of encapsulated bioactive compounds. Undoubtedly,
5. Challenges, perspectives and future trends addressing these issues will require substantial further research.

5.1. Challenges and perspectives CRediT authorship contribution statement

Currently, bigels have become the focus of research due to its dual Erpeng Chao: Writing – original draft, Resources, Methodology.
advantages of oleogel and hydrogel. Additionally, this system has Jinwei Li: Writing – review & editing, Resources. Zhenhua Duan:
demonstrated effectiveness in co-delivering bioactive substances due to Writing – review & editing, Resources. Liuping Fan: Writing – review &
its hydrophilic and lipophilic properties. However, some issues closely editing, Validation, Supervision, Conceptualization.
related to food industry applications remain and need to be explored
over time.
One significant gap in current research lies in the limited investiga­ Declaration of competing interest
tion of multi-component interactions between bigels and food matrices.
When bigel-based bioactive ingredient delivery systems are incorpo­ The authors declare that they have no known competing financial
rated into food matrices to form more diverse systems, whether the interests or personal relationships that could have appeared to influence
bioactives embedded in the bigel still perform as expected in the pres­ the work reported in this paper.
ence of multi-component interactions is crucial for further application.
Therefore, assessing the performance of bigels within real food systems Data availability
and verifying their suitability as delivery vehicles will greatly facilitate
the advancement of bigels within practical food applications. For Data will be made available on request.
instance, it is imperative to explore whether multi-component in­
teractions may adversely affect the bioactive functions of these in­ Acknowledgments
gredients. These investigations merit further attention and
investigation. The authors acknowledge financial support of the Chongzuo science
Furthermore, a comprehensive understanding of the metabolic fate and technology project of Guangxi province (Chongke 2021021479),
of bigels within the human body is imperative, necessitating an eluci­ key research and development program of Xinjiang Autonomous Region
dation of the complete metabolic mechanism. Regrettably, there re­ (2022B02026-5), Inner Mongolia Autonomous Region Science and
mains a dearth of detailed information concerning the specific digestive Technology Plan Project (2023YFHH0002), which have enabled us to
fate and metabolic processes involving bigels. Existing studies have accomplish this study.
elucidated that bigels exhibit minimal degradation within the stomach,
whereas the gel network of bigels undergoes collapse when exposed to
References
intestinal fluids due to direct lipase attacks on oleogel particles (Zhu
et al., 2021). Additionally, the swelling behavior of bigels within the Algin, Y. E., Tuncay, T. S., Aybar, T. G., Gumus, Z. P., Turunc, E., & Gokce, E. H. (2020).
intestine outpaces that within the stomach. Consequently, the intestinal An examinatio of carbopol hydrogel/organogel bigels of thymoquinone prepared by
fluids further compromise the structural integrity of bigels following the microwave irradiation method. Drug Development and Industrial Pharmacy, 46(10),
1639–1646. https://doi.org/10.1080/03639045.2020.1820031
initial swelling within the stomach, leading to erosion (Zhu et al., 2021). Barragan-Martinez, L. P., Roman-Guerrero, A., Vernon-Carter, E. J., & Alvarez-
It is evident that the scarcity of in vivo trials represents a notable limi­ Ramirez, J. (2022). Impact of fat replacement by a hybrid gel (canola oil/candelilla
tation within the body of research and should be a prominent focus for waxoleogel and gelatinized corn starch hydrogel) on dough viscoelasticity, color,
texture, structure, and starch digestibility of sugar-snap cookies. International Journal
future investigations. of Gastronomy and Food Science, 29, Article 100563. https://doi.org/10.1016/j.
ijgfs.2022.100563

14
E. Chao et al. Food Hydrocolloids 154 (2024) 110089

Behera, B., Sagiri, S. S., Pal, K., Pramanik, K., Rana, U. A., Shakir, I., et al. (2015). Habibi, A., Kasapis, S., & Truong, T. (2022). Effect of hydrogel particle size embedded
Sunflower oil and protein-based novel bigels as matrices for drug delivery into oleogels on the physico-functional properties of hydrogel-in-oleogel (bigels).
applications-characterization and in vitro antimicrobial efficiency. Polymer-Plastics LWT-Food Science and Technology, 163, Article 113501. https://doi.org/10.1016/j.
Technology and Engineering, 54(8), 837–850. https://doi.org/10.1080/ lwt.2022.113501
03602559.2014.974268 Hashemi, B., Assadpour, E., & Jafari, S. M. (2024). Bigels as novel carriers of bioactive
Behera, B., Sagiri, S. S., Singh, V. K., Pal, K., & Anis, A. (2014). Mechanical properties and compounds: Applications and research trends. Food Hydrocolloids, 147, Article
delivery of drug/probiotics from starch and non-starch based novel bigels: A 109427. https://doi.org/10.1016/j.foodhyd.2023.109427
comparative study. Starch, 66(9), 865–879. https://doi.org/10.1002/ Hashemi, B., Varidi, M., & Jafari, S. M. (2023). Fabrication and characterization of novel
star.201400045 whey protein-based bigels as structured materials with high-mechanical properties.
Behera, B., Singh, V. K., Kulanthaivel, S., Bhattacharya, M. K., Paramanik, K., Food Hydrocolloids, 145, Article 109082. https://doi.org/10.1016/j.
Banerjee, I., et al. (2015). Physical and mechanical properties of sunflower oil and foodhyd.2023.109082
synthetic polymers based bigels for the delivery of nitroimidazole antibiotic – a Hashim, A. F., El Sayed, S. M., & El Sayed, H. S. (2023). Bigel formulations based on
therapeutic approach for controlled drug delivery. European Polymer Journal, 64, sesame oleogel with probiotics alginate hydrogel: A novel structure for nutritious
253–264. https://doi.org/10.1016/j.eurpolymj.2015.01.018 spreadable butter. International Journal of Biological Macromolecules, 242, Article
Bollom, M. A., Clark, S., & Acevedo, N. C. (2020). Development and characterization of a 124782. https://doi.org/10.1016/j.ijbiomac.2023.124782
novel soy lecithin-stearic acid and whey protein concentrate bigel system for Henney, A. E., Gillespie, C. S., Alam, U., Hydes, T. J., Boyland, E., & Cuthbertson, D. J.
potential edible applications. Food Hydrocolloids, 101, Article 105570. https://doi. (2024). Ultra-processed food and non-communicable diseases in the United
org/10.1016/j.foodhyd.2019.105570 Kingdom: A narrative review and thematic synthesis of literature. Obesity Reviews. ,
Bruno, E., Lupi, F. R., Mammolenti, D., Baldino, N., & Gabriele, D. (2024). Development Article e13682. https://doi.org/10.1111/obr.13682
and rheological modeling of dietary fiber and policosanol plant-based bigels for Herrero, A. M., Ruiz-Capillas, C., Jimenez-Colmenero, F., & Carmona, P. (2014). Raman
potential food applications. Food Hydrocolloids, 150, Article 109733. https://doi. spectroscopic study of structural changes upon chilling storage of frankfurters
org/10.1016/j.foodhyd.2024.109733 containing olive oil bulking agents as fat replacers. Journal of Agricultural and Food
Chen, Z., Bian, F., Cao, X., Shi, Z., & Meng, Z. (2023). Novel bigels constructed from Chemistry, 62(25), 5963–5971. https://doi.org/10.1021/jf501231k
oleogels and hydrogels with contrary thermal characteristics: Phase inversion and Ibrahim, M. M., Hafez, S. A., & Mahdy, M. M. (2013). Organogels, hydrogels and bigels as
3D printing applications. Food Hydrocolloids, 134, Article 108063. https://doi.org/ transdermal delivery systems for diltiazem hydrochloride. Asian Journal of
10.1016/j.foodhyd.2022.108063 Pharmaceutical Sciences, 8(1), 48–57. https://doi.org/10.1016/j.ajps.2013.07.006
Clímaco, G. N., & Fasolin, L. H. (2024). Effect of the gelling mechanism on the physical Jiang, Q., Wang, Y., Du, L., Li, S., Liu, Y., & Meng, Z. (2022). Catastrophic phase
properties of bigels based on whey protein isolate. Food Research International, 176, inversion of bigels characterized by fluorescence intensity-based 3D modeling and
Article 113784. https://doi.org/10.1016/j.foodres.2023.113784 the formability for decorating and 3D printing. Food Hydrocolloids, 126, Article
Contreras-Ramirez, J. I., Patel, A. R., Gallegos-Infante, J. A., Toro-Vazquez, J. F., Perez- 107461. https://doi.org/10.1016/j.foodhyd.2021.107461
Martinez, J. D., Rosas-Flores, W., et al. (2022). Organogel-based emulsified systems, Kaimal, A. M., & Singhal, R. S. (2023a). A bigel based formulation protects lutein better
food applications, microstructural and rheological features-A review. Biointerface in the gastric environment with controlled release and antioxidant profile than other
Research in Applied Chemistry, 12(2), 1601–1627. https://doi.org/10.33263/ gel based systems. Food Chemistry, 423, Article 136304. https://doi.org/10.1016/j.
BRIAC122.16011627 foodchem.2023.136304
Cui, H., Tang, C., Wu, S., Julian McClements, D., Liu, S., Li, B., et al. (2022). Fabrication Kaimal, A. M., & Singhal, R. S. (2023b). Bigels for controlled gastric release of ascorbic
of chitosan-cinnamaldehyde-glycerol monolaurate bigels with dual gelling effects acid: Impact on rheology, texture, thermal stability and antioxidant activity. Food
and application as cream analogs. Food Chemistry, 384, Article 132589. https://doi. Hydrocolloids for Health, 4, Article 100171. https://doi.org/10.1016/j.
org/10.1016/j.foodchem.2022.132589 fhfh.2023.100171
Davidovich Pinhas, M. (2019). Oil structuring using polysaccharides. Current Opinion in Kanelaki, A., Zampouni, K., Mourtzinos, I., & Katsanidis, E. (2022). Hydrogels, oleogels
Food Science, 27, 29–35. https://doi.org/10.1016/j.cofs.2019.04.006 and bigels as edible coatings of sardine fillets and delivery systems of rosemary
Derkach, S. R., Voron’ko, N. G., Maklakova, A. A., & Kondratyuk, Y. V. (2014). The extract. Gels, 8(10), 660. https://doi.org/10.3390/gels8100660
rheological properties of gelatin gels containing κ-carrageenan. The role of Kouider, A. M., Rahal, S., Laidi, M., Kouar, I., Bourahla, R. F., Akouche, Y., et al. (2024).
polysaccharide. Colloid Journal, 76, 146–152. https://doi.org/10.1134/ Balancing competing objectives in bigel formulations using many-objective
S1061933X14020021 optimization algorithms and different decision-making methods. European Journal of
Eisinaitė, V., Jasutienė, I., Vinauskienė, R., & Leskauskaitė, D. (2023). Development of Pharmaceutics and Biopharmaceutics, 195, Article 114167. https://doi.org/10.1016/j.
bigel based dysphagia-oriented products, structured with collagen and carnauba ejpb.2023.12.007
wax: Characterisation and rheological behaviour. International Journal of Food Kumar, A., Kuang, Y., Liang, Z., & Sun, X. (2020). Microwave chemistry, recent
Science and Technology, 58(1), 145–153. https://doi.org/10.1111/ijfs.16181 advancements, and eco-friendly microwave-assisted synthesis of nanoarchitectures
Evans, D. F., & Wennerstrm, H. (1999). The colloidal domain: Where physics, chemistry, and their applications: A review. Materials Today Nano, 11, Article 100076. https://
biology, and technology meet. VCH Publishers: Wiley-VCH. doi.org/10.1016/j.mtnano.2020.100076
Fasolin, L. H., Martins, A. J., Cerqueira, M. A., & Vicente, A. A. (2021). Modulating Kupikowska, S. B., Jacek, D., & Mirosław, M. K. (2024). Critical review of techniques for
process parameters to change physical properties of bigels for food applications. food emulsion characterization. Applied Sciences, 14(3), 1069. https://doi.org/
Food Structure, 28, Article 100173. https://doi.org/10.1016/j.foostr.2020.100173 10.3390/app14031069
Fasolin, L. H., Picone, C. S. F., Santana, R. C., & Cunha, R. L. (2013). Production of hybrid Lee, G. R., Baek, Y., Jeong, E., & Lee, H. G. (2024). Development and characterization of
gels from polysorbate and gellan gum. Food Research International, 54(1), 501–507. a novel bigel system based on candelilla wax oleogel and guar gum hydrogel for
https://doi.org/10.1016/j.foodres.2013.07.026 heat-triggered release properties. Food Hydrocolloids, 152, Article 109892. https://
Fasolin, L. H., & Vicente, A. A. (2017). Evaluation of process conditions in the bigels doi.org/10.1016/j.foodhyd.2024.109892
production: A multivariate analysis. In Poster session presentation at the meeting of the Lee, M. C., Tan, C., Ravanfar, R., & Abbaspourrad, A. (2019). Ultrastable water-in-oil
19th gums & Stabilisers for the food industry Conference: Hydrocolloid Multifunctionality, high internal phase emulsions featuring interfacial and biphasic network
Berlin, BE. stabilization. ACS Applied Materials & Interfaces, 11(29), 26433–26441. https://doi.
Ghiasi, F., & Golmakani, M. T. (2022). Fabrication and characterization of a novel org/10.1021/acsami.9b05089
biphasic system based on starch and ethylcellulose as an alternative fat replacer in a Li, X., Fan, L., Liu, Y., & Li, J. (2021). New insights into food O/W emulsion gels:
model food system. Innovative Food Science & Emerging Technologies, 78, Article Strategies of reinforcing mechanical properties and outlook of being applied to food
103028. https://doi.org/10.1016/j.ifset.2022.103028 3D printing. Critical Reviews in Food Science and Nutrition, 63(11), 1564–1586.
Ghorghi, Z. B., Yeganehzad, S., Hesarinejad, M. A., Faezian, A., Kutsenkova, V., Gao, Z., https://doi.org/10.1080/10408398.2021.1965953
et al. (2023). Fabrication of novel hybrid gel based on beeswax oleogel: Application Li, L., Liu, G., Bogojevic, O., Pedersen, J. N., & Guo, Z. (2022). Edible oleogels as solid fat
in the compound chocolate formulation. Food Hydrocolloids, 140, Article 108599. alternatives: Composition and oleogelation mechanism implications. Comprehensive
https://doi.org/10.1016/j.foodhyd.2023.108599 Reviews in Food Science and Food Safety, 21(3), 2077–2104. https://doi.org/10.1111/
Golodnizky, D., & Davidovich Pinhas, M. (2020). The effect of the HLB value of sucrose 1541-4337.12928
ester on physiochemical properties of bigel systems. Foods, 9(12), 1857. https://doi. Li, C., Xu, Y., Zhang, Y., Shen, Y., Deng, X., & Wang, F. (2024). Novel bigels based on
org/10.3390/foods9121857 walnut oil oleogel and chitosan hydrogel: Preparation, characterization, and
Gonçalves, R. F. S., Zhou, H., Vicente, A. A., Pinheiro, A. C., & McClements, D. J. (2024). application as food spread. International Journal of Biological Macromolecules, 260,
Plant-based bigels for delivery of bioactive compounds: Influence of hydrogel: Article 129530. https://doi.org/10.1016/j.ijbiomac.2024.129530
oleogel ratio and protein concentration on their physicochemical properties. Food Liu, K., Chen, Y. Y., Zha, X. Q., Li, Q. M., Pan, L. H., & Luo, J. P. (2021). Research
Hydrocolloids, 150, Article 109721. https://doi.org/10.1016/j. progress on polysaccharide/protein hydrogels: Preparation method, functional
foodhyd.2023.109721 property and application as delivery systems for bioactive ingredients. Food Research
Guo, Z., Chen, Z., & Meng, Z. (2023). Bigels constructed from hybrid gelator systems: International, 147, Article 110542. https://doi.org/10.1016/j.foodres.2021.110542
Bulk phase-interface stability and 3D printing. Food & Function, 14, 5078–5089. Liu, L. A., Tian, W., Chen, М., Huang, Y., & Xiao, J. (2023). Oral sensation and
https://doi.org/10.1039/D3FO00948C gastrointestinal digestive profiles of bigels tuned by the mass ratio of konjac
Guo, J., Gu, X., Du, L., & Meng, Z. (2023). Spirulina platensis protein nanoparticle-based glucomannan to gelatin in the binary hydrogel matrix. Carbohydrate Polymers, 312,
bigels: Dual stabilization, phase inversion, and 3D printing. Food Hydrocolloids, 135, Article 120765. https://doi.org/10.1016/j.carbpol.2023.120765
Article 108160. https://doi.org/10.1016/j.foodhyd.2022.108160 Lu, Y., Zhong, Y., Guo, X., Zhang, J., Gao, Y., & Mao, L. (2022). Structural modification of
Guo, Z., Li, Y., Song, X., & Meng, Z. (2024). Stabilization models of foams prepared from O/W bigels by glycerol monostearate for improved co-delivery of curcumin and
whippable bigels: Crystal absorption and droplet stability. Food Hydrocolloids, 147, epigallocatechin gallate. ACS Food Science & Technology, 2(6), 975–983. https://doi.
Article 109383. https://doi.org/10.1016/j.foodhyd.2023.109383 org/10.1021/acsfoodscitech.2c00044

15
E. Chao et al. Food Hydrocolloids 154 (2024) 110089

Lupi, F. R., De Santo, M. P., Ciuchi, F., Baldino, N., & Gabriele, D. (2017). A rheological Sarika, Prasad, K., & Kumar, A. (2023). Physiochemical, thermal, textural, functional, and
modelling and microscopic analysis of bigels. Rheologica Acta, 56, 753–763. https:// microstructural characterization of the developed shelf stable bigel using hydrogel and
doi.org/10.1007/s00397-017-1030-3 oleogel. IOP Publishing, Article 012029. https://doi.org/10.1088/1742-6596/2663/
Lupi, F. R., Shakeel, A., Greco, V., Oliviero Rossi, C., Baldino, N., & Gabriele, D. (2016). 1/012029
A rheological and microstructural characterisation of bigels for cosmetic and Shakeel, A., Farooq, U., Gabriele, D., Marangoni, A. G., & Lupi, F. R. (2021). Bigels and
pharmaceutical uses. Materials Science and Engineering: C, 69, 358–365. https://doi. multi-component organogels: An overview from rheological perspective. Food
org/10.1016/j.msec.2016.06.098 Hydrocolloids, 111, Article 106190. https://doi.org/10.1016/j.
Machado, M., Sousa, S., Morais, P., Miranda, A., Rodriguez-Alcalá, L. M., Gomes, A. M., foodhyd.2020.106190
et al. (2022). Novel avocado oil-functionalized yogurt with anti-obesity potential: Shakeel, A., Farooq, U., Iqbal, T., Yasin, S., Lupi, F. R., & Gabriele, D. (2019). Key
Technological and nutraceutical perspectives. Food Bioscience, 50, Article 101983. characteristics and modelling of bigels systems: A review. Materials Science and
https://doi.org/10.1016/j.fbio.2022.101983 Engineering: C, 97, 932–953. https://doi.org/10.1016/j.msec.2018.12.075
Martin Illana, A., Notario Perez, F., Cazorla Luna, R., Ruiz Caro, R., & Veiga, M. D. Shakeel, A., Lupi, F. R., Gabriele, D., Baldino, N., & De Cindio, B. (2018). Bigels: A unique
(2019). Smart freeze-dried bigels for the prevention of the sexual transmission of hiv class of materials for drug delivery applications. Soft Materials, 16, 77–93. https://
by accelerating the vaginal release of tenofovir during intercourse. Pharmaceutics, 11 doi.org/10.1080/1539445X.2018.1424638
(5), 232. https://doi.org/10.3390/pharmaceutics11050232 Singh, V. K., Anis, A., Banerjee, I., Pramanik, K., Bhattacharya, M. K., & Pal, K. (2014).
Martinez, R. M., Magalhaes, W. V., Sufi, B.d. S., Padovani, G., Nazato, L. I. S., Preparation and characterization of novel carbopol based bigels for topical delivery
Velasco, M. V. R., et al. (2021). Vitamin E-loaded bigels and emulsions: of metronidazole for the treatment of bacterial vaginosis. Materials Science and
Physicochemical characterization and potential biological application. Colloids and Engineering: C, 44, 151–158. https://doi.org/10.1016/j.msec.2014.08.026
Surfaces B: Biointerfaces, 201, Article 111651. https://doi.org/10.1016/j. Singh, V. K., Banerjee, I., Agarwal, T., Pramanik, K., Bhattacharya, M. K., & Pal, K.
colsurfb.2021.111651 (2014). Guar gum and sesame oil based novel bigels for controlled drug delivery.
Martins, A. J., Guimarães, A., Fuciños, P., Sousa, P., Venâncio, A., Pastrana, L. M., et al. Colloids and Surfaces B: Biointerfaces, 123, 582–592. https://doi.org/10.1016/j.
(2023). Food-grade bigels: Evaluation of hydrogel:oleogel ratio and gelator colsurfb.2014.09.056
concentration on their physicochemical properties. Food Hydrocolloids, 143, Article Singh, B., & Kumar, R. (2019). Designing biocompatible sterile organogel-bigel
108893. https://doi.org/10.1016/j.foodhyd.2023.108893 formulations for drug delivery applications using green protocol. New Journal of
Martins, A. J., Silva, P., Maciel, F., Pastrana, L. M., Cunha, R. L., Cerqueira, M. A., et al. Chemistry, 43(7), 3059–3070. https://doi.org/10.1039/C8NJ05480K
(2019). Hybrid gels: Influence of oleogel/hydrogel ratio on rheological and textural Somali, D., Miguel, A. C., Doman, K., & Kunal, P. (2024). Bigels: An innovative hybrid of
properties. Food Research International, 116, 1298–1305. https://doi.org/10.1016/j. hydrogels/oleogels for food applications. Advances in Oleogel Development,
foodres.2018.10.019 Characterization, and Nutritional Aspects, 122, 327–348. https://link.springer.com/ch
Mousavi, S. N., Hosseini, E., Dorraji, M. S. S., Mohammadi, S. S., Pourmansouri, Z., apter/10.1007/978-3-031-46831-5_14.
Rasoulifard, M. H., et al. (2021). Synthesis of a green bigel using cottonseed oil/ Tian, W., Huang, Y., Song, Z. A., Yu, Y., Liu, J., Cao, Y., et al. (2023). Flexible control of
cannabis oil/alginate/ferula gum for quercetin release: Synergistic effects for bigel microstructure for enhanced stability and flavor release during oral
treating infertility in rats. International Journal of Biological Macromolecules: Structure, consumption. Food Research International, 174, Article 113606. https://doi.org/
Function and Interactions, 177, 157–165. https://doi.org/10.1016/j. 10.1016/j.foodres.2023.113606
ijbiomac.2021.02.121 Tian, H., Wang, K., Lan, H., Wang, Y., Hu, Z., & Zhao, L. (2021). Effect of hybrid gelator
Nutter, J., Shi, X., Lamsal, B., & Acevedo, N. C. (2023a). Designing and characterizing systems of beeswax-carrageenan-xanthan on rheological properties and printability
multicomponent, plant-based bigels of rice bran wax, gums, and monoglycerides. of litchi inks for 3d food printing. Food Hydrocolloids, 113, Article 106482. https://
Food Hydrocolloids, 138, Article 108425. https://doi.org/10.1016/j. doi.org/10.1016/j.foodhyd.2020.106482
foodhyd.2022.108425 Wakhet, S., Singh, V. K., Sahoo, S., Sagiri, S. S., Kulanthaivel, S., Bhattacharya, M. K.,
Nutter, J., Shi, X., Lamsal, B., & Acevedo, N. C. (2023b). Plant-based bigels as a novel et al. (2015a). Characterization of gelatin-agar based phase separated hydrogel,
alternative to commercial solid fats in short dough products: Textural and structural emulgel and bigel: A comparative study. Journal of Materials Science: Materials in
properties of short dough and shortbread. Food Bioscience, 54, Article 102865. Medicine, 26(2). https://doi.org/10.1007/s10856-015-5434-2
https://doi.org/10.1016/j.fbio.2023.102865 Wakhet, S., Singh, V. K., Sahoo, S., Sagiri, S. S., Kulanthaivel, S., Bhattacharya, M. K.,
Okuro, P. K., Santos, T. P., & Cunha, R. L. (2021). Compositional and structural aspects of et al. (2015b). Characterization of gelatin-agar based phase separated hydrogel,
hydro- and oleogels: Similarities and specificities from the perspective of emulgel and bigel: A comparative study. Journal of Materials Science: Materials in
digestibility. Trends in Food Science & Technology, 111, 55–67. https://doi.org/ Medicine, 26(2), 118. https://doi.org/10.1007/s10856-015-5434-2
10.1016/j.tifs.2021.02.053 Xie, D., Hu, H., Huang, Q., & Lu, X. (2023a). Development and characterization of food-
Qiu, R., Liu, X., Tian, H., Hu, Z., Wang, K., & Zhao, L. (2024). Exploration of bigel 4D grade bigel system for 3d printing applications: Role of oleogel/hydrogel ratios and
printing with spontaneous colour change for monitoring bio-actives kinetic emulsifiers. Food Hydrocolloids, 139, Article 108565. https://doi.org/10.1016/j.
behaviour based on the dual-units 3D printer. Journal of Food Engineering, 367, foodhyd.2023.108565
Article 111861. https://doi.org/10.1016/j.jfoodeng.2023.111861 Xie, D., Hu, H., Huang, Q., & Lu, X. (2023b). Influence of oleogel/hydrogel ratios and
Qiu, H., Qu, K., Zhang, H., & Eun, J. B. (2023). Characterization and comparison of emulsifiers on structural and digestion properties of food-grade 3D printed bigels as
physical properties and in vitro simulated digestion of multi-component oleogels carriers for quercetin and catechin. Food Hydrocolloids, 144, Article 108948. https://
with different molecular weights prepared by the direct method. Food Hydrocolloids, doi.org/10.1016/j.foodhyd.2023.108948
142, Article 108850. https://doi.org/10.1016/j.foodhyd.2023.108850 Yang, M., Gao, Y., Liu, Y., Yang, G. Z., Zhao, C. X., & Wu, K. J. (2021). Integration of
Qiu, R., Wang, K., Tian, H., Liu, X., Liu, G., Hu, Z., et al. (2022). Analysis on the microfluidic systems with external fields for multiphase process intensification.
printability and rheological characteristics of bigel inks: Potential in 3D food Chemical Engineering Science, 234. https://doi.org/10.1016/j.ces.2021.116450
printing. Food Hydrocolloids, 129, Article 107675. https://doi.org/10.1016/j. Yang, J., Song, J., Miao, S., Gao, Y., & Mao, L. (2024). Alginate-based gel beads with
foodhyd.2022.107675 bigel structures: Preparation, characterization and bioactive encapsulation. Food
Quilaqueo, M., Iturra, N., Contardo, I., Millao, S., Morales, E., & Rubilar, M. (2022). Hydrocolloids, 146, Article 109294. https://doi.org/10.1016/j.
Food-grade bigels with potential to replace saturated and trans fats in cookies. Gels, 8 foodhyd.2023.109294
(7), 445. https://doi.org/10.3390/gels8070445 Yang, J., Zheng, H., Mo, Y., Gao, Y., & Mao, L. (2022). Structural characterization of
Rehman, K., Mohd Amin, M. C. I., & Zulfakar, M. H. (2014). Development and physical hydrogel-oleogel biphasic systems as affected by oleogelators. Food Research
characterization of polymer-fish oil bigel (hydrogel/oleogel) system as a transdermal International, 158, Article 111536. https://doi.org/10.1016/j.foodres.2022.111536
drug delivery vehicle. Journal of Oleo Science, 63(10), 961–970. https://doi.org/ Yiu, C. C. Y., Liang, S. W., Mukhtar, K., Kim, W., Wang, Y., & Selomulya, C. (2023). Food
10.5650/jos.ess14101 emulsion gels from plant-based ingredients: Formulation, processing, and potential
Richa, & Roy Choudhury, A. (2023). Self-assembled ph-stable gellan/κ-carrageenan applications. Gels, 9(5), 366. https://doi.org/10.3390/gels9050366
bigel: Rheological studies and viscosity prediction by neural network. International Zampouni, K., Filippou, A., Papadimitriou, K., & Katsanidis, E. (2024). Evaluation of
Journal of Biological Macromolecules, 237, Article 124057. https://doi.org/10.1016/j. bigel systems as potential substitutes to partially replace pork backfat in semi-dry
ijbiomac.2023.124057 sausages. Meat Science, 208, Article 109392. https://doi.org/10.1016/j.
Saffold, A. C., & Acevedo, N. C. (2021). Development of novel rice bran wax/gelatin- meatsci.2023.109392
based biphasic edible gels and characterization of their microstructural, thermal, and Zampouni, K., Mouzakitis, C. K., Lazaridou, A., Moschakis, T., & Katsanidis, E. (2023).
mechanical properties. Food and Bioprocess Technology, 14, 2219–2230. https://doi. Physicochemical properties and microstructure of bigels formed with gelatin and
org/10.1007/s11947-021-02719-7 κ-carrageenan hydrogels and monoglycerides in olive oil oleogels. Food
Saffold, A. C., & Acevedo, N. C. (2022). The effect of mono-diglycerides on the Hydrocolloids, 140, Article 108636. https://doi.org/10.1016/j.
mechanical properties, microstructure, and physical stability of an edible rice bran foodhyd.2023.108636
wax-gelatin biphasic gel system. Journal of the American Oil Chemists’ Society, 99(11), Zhai, X., Sun, Y., Cen, S., Wang, X., Zhang, J., Yang, Z., et al. (2022). Anthocyanins-
1033–1043. https://doi.org/10.1002/aocs.12640 encapsulated 3D-printable bigels: A colorimetric and leaching-resistant volatile
Sahoo, S., Vinay, K. S., Uvanesh, K., Dibyajyoti, B., Arfat, A., Usman, A. R., et al. (2015). amines sensor for intelligent food packaging. Food Hydrocolloids, 133, Article
Development of ionic and non-ionic natural gum-based bigels: Prospects for drug 107989. https://doi.org/10.1016/j.foodhyd.2022.107989
delivery application. Journal of Applied Polymer Science, 132(38). https://doi.org/ Zhao, L., Zhang, M., Chitrakar, B., & Adhikari, B. (2021). Recent advances in functional
10.1002/app.42561 3D printing of foods: A review of functions of ingredients and internal structures.
Samui, T., Goldenisky, D., Rosen Kligvasser, J., & Davidovich Pinhas, M. (2021). The Critical Reviews in Food Science and Nutrition, 61, 3489–3503. https://doi.org/
development and characterization of novel in-situ bigel formulation. Food 10.1080/10408398.2020.1799327
Hydrocolloids, 113, Article 106416. https://doi.org/10.1016/j. Zheng, R., Chen, Y., Wang, Y., Rogers, M. A., Cao, Y., & Lan, Y. (2023). Microstructure
foodhyd.2020.106416 and physical properties of novel bigel-based foamed emulsions. Food Hydrocolloids,
134, Article 108097. https://doi.org/10.1016/j.foodhyd.2022.108097

16
E. Chao et al. Food Hydrocolloids 154 (2024) 110089

Zheng, H., Mao, L., Cui, M., Liu, J., & Gao, Y. (2020). Development of food-grade bigels Zhuang, X., Clark, S., & Acevedo, N. (2021). Bigels-oleocolloid matrices-as probiotic
based on κ-carrageenan hydrogel and monoglyceride oleogels as carriers for protective systems in yogurt. Journal of Food Science, 86(11), 4892–4900. https://
β-carotene: Roles of oleogel fraction. Food Hydrocolloids, 105, Article 105855. doi.org/10.1111/1750-3841.15928
https://doi.org/10.1016/j.foodhyd.2020.105855 Zulfakar, M. H., Chan, L. M., Rehman, K., Wai, L. K., & Heard, C. M. (2018). Coenzyme
Zhu, Q., Gao, J., Han, L., Han, K., Wei, W., Wu, T., et al. (2021). Development and Q10-loaded fish oil-based bigel system: Probing the delivery across porcine skin and
characterization of novel bigels based on monoglyceride-beeswax oleogel and high possible interaction with fish oil fatty acids. AAPS PharmSciTech, 19(3), 1116–1123.
acyl gellan gum hydrogel for lycopene delivery. Food Chemistry, 365, Article 130419. https://doi.org/10.1208/s12249-017-0923-x
https://doi.org/10.1016/j.foodchem.2021.130419

17