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Application Progress of Hydrogels as Food Matrices
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This entry is adapted from the peer-reviewed paper 10.3390/gels9010068

Food hydrogels are biopolymeric materials made from food-grade biopolymers with gelling properties (proteins and polysaccharides) and a 3D network capable of incorporating large amounts of water.  Hydrogels present a wide range of properties (including high water content, flexibility, softness, and compatibility), making their application highly tunable for different food systems. Protein–polysaccharide composites have been so far successfully used only in the food packaging industry as they possess an oil barrier, water solubility, and tastelessness. The commercially used edible films are produced mostly from cellulose and whey protein biopolymers, or alginate and collagen. The most recent trend in using hydrogels is the development of matrices that can replace animal-based food products in terms of texture and nutritional aspects. The food sector is increasingly becoming more concerned with providing enough nutritious food for everyone while protecting natural resources. 

proteins polysacharides hydrogels food binary hydrogels

1. Encapsulation and Delivery Systems of Bioactive Compounds

Hydrogels are increasingly used as encapsulating and delivery agents because of their high encapsulation efficiency, biocompatibility, low cost, and environmentally friendly properties. These properties can be achieved due to their porous nature caused by the three-dimensional structures in which crosslinked polymers form large interstitial spaces that are densely packed with water. These interstitial spaces can also incorporate various nutrients and bioactive compounds [1]. That is why these spaces can be utilized to overcome some challenges related to adding health-beneficial substances to food products; for example, low thermal and chemical stability, poor solubility, and undesirable flavor organoleptic profile. Encapsulating the bioactive substances in hydrogels makes it possible to protect them from external environmental factors during production, storage, and even after consumption. Such factors include oxygen, heat, light, pH, enzymes, etc. [2][3][4].
Moreover, by mixing proteins and polysaccharides, it is possible to obtain improved structural and functional properties, which can be explained by the formation of protein–polysaccharide complexes via covalent and noncovalent interactions. These binary protein–polysaccharide hydrogels can be used as a matrix for embedding hydrophilic and hydrophobic compounds [5]. Hydrophobic compounds can be embedded into a hydrogel by first preparing an emulsion containing these bioactive substances and then introducing the biopolymers to the emulsion, resulting in an emulsion-filled hydrogel [6]. Both hydrophilic and hydrophobic compounds can either form the gel network, contributing to the strength and stability of the final hydrogel—such compounds are called active fillers. However, the embedded compound might not interact or can interact minimally with the gel network—such compounds are called inactive fillers.
Protein and polysaccharide hydrogels can be used as delivery systems for polyphenols, a group of compounds (over 8000 phenolic compounds) with a range of physiological functions, including antioxidant, anti-inflammatory, anti-virus, antibacterial, and immunity enhancement. These functional properties are mainly related to the phenolic groups and the conjugated double bonds [7]. Polyphenols are widely used in the food industry, but their bioavailability still imposes challenges because of their poor solubility and stability [8]. That is why many researchers are involved in designing a food-grade hydrogel carrier that can protect those compounds from oxygen, heat, light, and pH degradation. The latest finding regarding the use of hydrogels as delivery systems for phenolic compounds and vitamins are mentioned below.
Curcumin, a phenolic compound extracted from turmeric (Curcuma longa Linn.), has been well known for its health-promoting properties (antimicrobial, anti-inflammatory, antirheumatic, immunomodulatory, anti-carcinogenic). However, it exhibits poor water solubility and low bioavailability after ingestion [9]. Recently, proteins and polysaccharides-based hydrogels were developed to improve curcumin’s stability and bioavailability. George et al. [10], in their research on cellulose-chitosan-zinc oxide composite hydrogels for the encapsulation of curcumin, reported that the loading efficiency reached 89.68%. In addition, the obtained hydrogel exhibited an antimicrobial effect on Trichophyton rubrum and Staphylococcus aureus and a controlled release at pH 7.4. In another study, curcumin was embedded in a chitosan/lotus root pectin hydrogel with an efficiency of 90.3% and improved solubility and stability [7]. Moreover, a nanoparticles-in-microparticles hydrogel system was fabricated by electrospray technology for curcumin colon-targeting oral delivery, which enabled curcumin release and entry to the macrophages [11]. Kour et al. [12] studied the effect of nanoemulsion-loaded hybrid biopolymeric hydrogel beads on the release kinetics, antioxidant potential, and antibacterial activity of encapsulated curcumin. They found that the high structural stability of the obtained carriers and their effective delivery of curcumin can provide a novel and tailored formulation out of polymers for oral drug delivery.
Epigallocatechin gallate (EGGG) is a catechin phenolic active compound with several health-beneficial properties, such as antioxidant, anti-tumor, antiviral, antibacterial, and cardio cerebral vessel protective. The polyhydroxy structure of catechins makes them unstable in neutral and alkaline pH. Additionally, they can be glucosylated or methylated by gastrointestinal tract enzymes, making them highly unstable and biologically unavailable [13]. To improve the stability and release of EGGG, Wang et al. [14] prepared a composite protein–polysaccharide hydrogel using carboxymethyl konjac glucomannan and gelatin. Authors reported that obtained hydrogels had better pH-sensitive properties, which enhanced the encapsulation and the bioavailability of EGGG. Furthermore, Yu et al. [15] reported that EGGG added to collagen hydrogels acted as an active filler by narrowing the pore size and strengthening the collagen fiber network. This effect was due to the formation of covalent bonds between lysine and EGCG. What is more, the incorporation of nanofiber particles coated with epigallocatechin-gallate (EGCG) into gelatin methacryloyl hydrogel reduced the free-radical-derived cellular damage when using 3D tissue fabrication (ex vivo) [16]. Wu et al. [17] demonstrated that using konjac galactomannan with the addition of oxidized hyaluronic acid enhances the stability and control release of EGGG. Other studies also reported the positive effect of EGGG on the structural remodeling of soy protein-derived amyloid fibrils hydrogel [18].
Resveratrol is another poorly water-soluble polyphenolic compound that exhibits various physiological properties (e.g., oxidative stress, anti-inflammatory, anti-obesity, anti-cancer, etc.) [19]. Additionally, to its poor water solubility, resveratrol is characterized by a fast metabolism in the gastrointestinal environment, which affects bioavailability. Fan et al. [20] prepared pea protein particles with calcium-induced cross-linking in which they encapsulated resveratrol. This encapsulation led to enhancing the physicochemical stability of the compounds, as well as led to a better antioxidant ability. Other studies on the improvement of resveratrol stability included the preparation of a resveratrol-loaded nanostructured lipid carrier hydrogel that significantly enhanced anti-UV irradiation and anti-oxidative activity in vitro and in vivo [21]. Currently, Pickering emulsion presents a high potential in the encapsulation of resveratrol. Based on Wu et al.’s [22] reports, it is possible to conclude that Pickering emulsion prepared using sodium alginate and pectin has a promising potential in developing low-calorie food products while contributing to the delivery of resveratrol to the gastrointestinal tract.
Anthocyanins are water-soluble flavonoids with high antioxidant activity. Their use in the food industry is limited due to their rapid degradation triggered by the pH value. They also have a low bioavailability and recovery rate after ingestion because of their low resistance to environmental changes [23]. Additionally, Jin et al. [24], in their study, prepared a konjac glucomannan and xanthan gum hydrogel in which they embedded anthocyanins. They reported that this synergistic hydrogel enhanced the thermal stability of anthocyanins at various pH values (3.0, 6.0, and 9.0). Ćorković et al. [25] also reported that the use of carboxymethylcellulose hydrogel as polyphenol carriers, specifically anthocyanins, helped preserve their antioxidant capacity. These findings showcased that proper formulation of food hydrogel, including the proper selection of biopolymers, can significantly maximize the retention of anthocyanins. In the current study conducted by Liu et al. [26], it was reported that the efficiency of anthocyanin encapsulation in gelatin/gellan hydrogel was high because of the high density of the formed structure. Moreover, the gelatin/gellan hydrogel protected the embedded anthocyanins during digestion, increasing its bioavailability in the small intestine. However, the proper selection of hydrogel building components is critical because anthocyanins may be degraded rather than protected, as observed in the studies of Kopjar et al. [27], in which the fortification of anthocyanins-loaded pectin hydrogel with apple fibers caused a substantial degradation in the retention of the anthocyanins. Furthermore, hydrogel loaded with anthocyanins can also be utilized as a colorimetric pH indicator to monitor, for example, the freshness of food products [28][29][30].
Quercetin, a flavonoid with beneficial properties, such as exhibited antioxidant, anti-inflammatory, anticancer, and cardioprotective, also exhibits low solubility and physicochemical instability, making it hard to be absorbed and utilized by the human body [31]. Several hydrogel systems have been recently prepared to protect this compound from the environment and raise its bioavailability. Quercetin-loaded pH-sensitive gellan gum hydrogels were induced using an ionotropic gelation method, and it was found that the obtained hydrogel beads had a pH-responsive release behavior. This release behavior improved the intestinal stability of this bioactive substance [32]. Moreover, Liu et al. [33] developed a lotus root amylopectin-coated whey protein hydrogel to protect quercetin. They reported that the obtained hydrogel enhanced the stability of quercetin while improving its bioavailability (in mice). In another study, linseed oil and quercetin were co-loaded to liposome-chitosan hydrogel beads. Based on the obtained results, the authors found that the chemical stability of quercetin could be improved by loading liposomes into hydrogel beads [34]. Moreover, Hu et al. [35] studied the co-encapsulation of epigallocatechin and quercetin in double-emulsion hydrogel beads and reported that obtained hydrogel beads inhibited oil digestion while increasing quercetin bioavailability.
Hydrogels obtained using food-grade biopolymers (proteins and polysaccharides) have been utilized for vitamin protection and delivery. The complexation of vitamin A and milk protein has been proven to increase the water-solubility and the light and heat stability of this vitamin [36]. Moreover, Rana et al. [37] also reported that vitamin A-loaded caseinate complexes improved vitamin A bioavailability. Similarly, Kaur et al. [38] highlighted the potential of chitosan and gelatin-based hydrogel to deliver vitamin B1. A chemically crosslinked cellulose–hemicellulose-based vitamin B12-loaded hydrogel was also reported to be effective in releasing this vitamin when the in vitro release is performed in successive buffers (from pH 1.2 to 7.4) [39]. Furthermore, β-cyclodextrin-soy soluble polysaccharide-based hydrogel was used to encapsulate and deliver vitamin E, showcasing the tunability of the swelling release properties of this vitamin both in-vitro and in-vivo [40]. Moreover, Martinez et al. [41] reported that the incorporation of vitamin E into a bigel (a combination of a hydrogel and an organogel) increased the diameter of the inner phase and the strength of the obtained structure. Mir et al. [42], in their research on glycerol-crosslinked guar gum monoaldehyde-based superabsorbent hydrogels for vitamin B6, concluded that the release of vitamin B6 depended on the pH of the medium (at pH 7, the concentration of the released vitamin was 79.2%).

2. Bioactive Substances Targeted Transport and Controlled Release

Because of the ability of hydrogels to hold large amounts of water or biological fluids, they can be used as carriers for bioactive substances, which can be embedded in the 3D hydrogel’s structure. Hydrogels have significant potential in developing targeted release systems, which can release the embedded substances into the digestive tract. When choosing biopolymers such as building blocks, what needs to be taken into consideration is their digestibility [43][44][45]. Proteins are known to be very efficiently digestible because of multiple peptidases in the digestive system. Additionally, denatured proteins in hydrogels obtained using heat induction are even more digestible [46]. On the other hand, polysaccharides have diverse digestion pathways, which depend on their type. For example, starch digestibility varies from rapidly digestible to indigestible. Some starches can be rapidly hydrolyzed by amylase in the mouth or the small intestine [47]. However, some polysaccharides, such as inulin, pectin, alginate, etc., can only be fermented by the microbiota in the colon [48][49].
Binary protein–polysaccharide hydrogels that deliver bioactive compounds to specific areas of the digestive tract can be developed based on the properties of the biopolymers used as hydrogel building blocks. These hydrogels can be designed to deliver the bioactive substance in the right place and time under the influence of factors such as pH, temperature, enzyme, or microbiota. These factors affect the hydrogel’s 3D structure, leading to its swelling or shrinkage and the release of the compound [50][51]. Based on the physiological conditions in different parts of the human digestive tract, it is possible to design a suitable hydrogel to deliver the bioactive compound to the targeted delivery site. The embedded bioactive substances can be released via swelling (change in volume), disintegration (dissociation of electrostatic coacervates), change in the molecular interactions (e.g., change in the electrostatic interaction between the bioactive compound and the polymeric building blocks), erosion (fermentation by the microbiota, digestion by enzymes) of the hydrogel’s carriers [52]. For the hydrogels to deliver the embedded compound to the oral cavity, stomach, or small intestine, they should be pH- and enzyme-sensitive. When the targeted site is the colon, the used hydrogel should be pH-sensitive and fermentable by the microbiota [44].
Certain hydrogels can respond to chemical changes in the pH and ionic composition in the environment surrounding them. This response leads to changes in the structure of the polymer network. Such hydrogels are called pH- and ion-responsive [53]. Xie et al. [54] reported that they synthesized a hydrogel using Chinese quince seed gum, which has promising potential for the oral delivery of drugs. Furthermore, Sarıyer et al. [55] developed pH-responsive alginate and κ-carrageenan hydrogels for the targeted release of bovine serum albumin. The targeted delivery of albumin to the intestines was achieved through diffusion and polymer structure relaxation. Temperature-responsive hydrogels are another type of carrier that respond to the changes in the temperature of the environment they are in by swelling or shrinking, which allows for the bioactive compounds to be released from the gel structure [56]. Temperature-responsive hydrogels might not be used to deliver bioactive substances to the stomach, small intestine, and colon but instead for oral (buccal) delivery. The such hydrogel can be developed to release the embedded substance at a temperature of 37 °C. Baus et al. [57] assessed in-vitro methods for the characterization of mucoadhesive hydrogels prepared using biopolymers, such as hydroxyethyl cellulose, carboxymethyl cellulose, xanthan gum, hyaluronic acid, and sodium alginate. They found out that xanthan gum had the highest resistance to the removal by artificial saliva. They also reported that based on the residence time of hydrogels, it is possible to develop a formulation with the best mucoadhesive properties for the delivery of bioactive compounds to the buccal area. Another type of hydrogel undergoes changes in its structure because of the activity of a specific enzyme. These hydrogels are enzyme-responsive and can be used to deliver a compound to a specific region of the digestive tract—where the concentration of enzymes, such as proteases or amylases, are the highest. The microbiota can also release the embedded compounds since it also produces enzymes that are not produced by the human gastrointestinal tract and can hydrolyze specific bonds of the biopolymers present in the 3D structure of the hydrogel. Wang et al. [58] developed an intestine enzyme-responsive polysaccharide-based hydrogel using carboxymethyl chitosan embedded with an antitumor-selective kinase inhibitor. They reported that the obtained hydrogel was able to enhance the therapeutic efficiency.
Because of the wide range of possibilities in developing protein–polysaccharide hydrogels, it is possible to design hydrogels that can be responsive to multiple stimuli depending on the targeted delivery area. Zhao and Li [59] obtained pH- and temperature-responsive hydrogels using Tremella polysaccharides, carboxymethyl cellulose, and nonionic surfactants as the main hydrogel building blocks. Whereas Liao and Huang [60] obtained a pH- and magnetic-responsive hydrogel using carboxymethyl chitin, for which the swelling structure degree can be regulated depending on the concentration levels of Fe3O4, the release mechanism is triggered by pH modulation.

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Subjects: Food Science & Technology
Contributors MDPI registered users' name will be linked to their SciProfiles pages. To register with us, please refer to https://encyclopedia.pub/register :
Adonis Hilal
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Anna Florowska
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Małgorzata Wroniak
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Revisions: 2 times (View History)
Update Date: 07 Feb 2023
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