Jerky-Inspired Fabrication of Anisotropic Hydrogels with Widely Tunable Mechanical Properties.

Jerky is a type of meat product traditionally produced using a hang-drying process to achieve desirable textural properties. Inspired by the jerky processing, we present a strategy for fabricating strong alginate hydrogels with highly anisotropic structures via stretching and drying under constant stress. The tunable stretching process endowed the alginate hydrogels with adjustable mechanical properties and structural features by promoting the orientation and aggregation of the constituent polymers. At a high water content of about 80%, the tensile strength of the obtained hydrogel was increased to 20 MPa, which was 10 times higher than that of the hydrogel without the stretching process. Moreover, these hydrogels can be favorably compared with other common structural materials. This paper introduces a facile strategy to tune the structural alignment and mechanical properties of hydrogels, which will expand the applicability of the natural hydrogels formed by non-covalent interactions.

Recent advances in the structure, synthesis, and applications of natural polymeric hydrogels.

Hydrogels, polymeric network materials, are capable of swelling and holding the bulk of water in their three-dimensional structures upon swelling. In recent years, hydrogels have witnessed increased attention in food and biomedical applications. In this paper, the available literature related to the design concepts, types, functionalities, and applications of hydrogels with special emphasis on food applications was reviewed. Hydrogels from natural polymers are preferred over synthetic hydrogels. They are predominantly used in diverse food applications for example in encapsulation, drug delivery, packaging, and more recently for the fabrication of structured foods. Natural polymeric hydrogels offer immense benefits due to their extraordinary biocompatible nature. Hydrogels based on natural/edible polymers, for example, those from polysaccharides and proteins, can serve as prospective alternatives to synthetic polymer-based hydrogels. The utilization of hydrogels has so far been limited, despite their prospects to address various issues in the food industries. More research is needed to develop biomimetic hydrogels, which can imitate the biological characteristics in addition to the physicochemical properties of natural materials for different food applications.

Natural biopolymer masks the bitterness of potassium chloride to achieve a highly efficient salt reduction for future foods.

Potassium chloride (KCl) can be considered as the most ideal salt replacer to reduce dietary sodium intake and ease various health risks of a high-sodium diet. However, a high proportion of sodium chloride (NaCl) replacement with KCl remains a challenge, because KCl has an inherent metallic bitterness. This study demonstrates a strategy for this bitterness-masking using a natural polysaccharide kappa-carrageenan to specifically bind with K+ and reduce the amount of free K+ as bitter stimulant. The results show that carrageenan can significantly slow down the release and diffusion of K+, leading to a reduced bitter taste of KCl in the mouth. Up to 50% replacement of NaCl by KCl can be achieved. Furthermore, the use of carrageenan-KCl-NaCl complex as salt substitutes can regulate mineral absorption (Na, K, Ca) and reduce hypertension and renal injury risks in the animal tests. In conclusion, this natural biopolymer-based strategy successfully masks the bitter of salt-replacer KCl, opening a route to the universally applicable salt-reduction in future foods.

Comparison of cellulose derivatives for Ca2+ and Zn2+ adsorption: Binding behavior and in vivo bioavailability.

Cellulose with distinct colloidal states exhibited different adsorption capability for ions and whether the intake of cellulose would bring positive or negative influence on the mineral bioavailability is inconclusive. This work investigated the binding behavior of carboxymethyl cellulose (CMC), TEMPO-oxidized nanofibrillated/nanocrystalline cellulose (TOCNF/TOCNC), and microcrystalline cellulose (MCC) with Ca2+and Zn2+ and compared their effects on mineral bioavailability in vitro and in vivo. The results suggested that CMC displayed a higher adsorption capability (36.6 mg g-1 for Ca2+ and 66.2 mg g-1 for Zn2+) than the other types of cellulose because of the strong interaction between carboxyl groups of cellulose and the ions. Although the cellulose derivatives had adverse effects on ion adsorption in vitro, the fermentability endowed by TOCNF/TOCNC counterbalanced the negative impacts in vivo. The findings suggested that the colloidal states of cellulose affected the bioavailability of minerals and could provide useful guidance for applications of specific cellulose.

In Vitro Colonic Fermentation Profiles and Microbial Responses of Cellulose Derivatives with Different Colloidal States.

Although cellulose derivatives are widely applied in the food industry, the effects of their structural properties on colonic health is unknown. Here, four types of cellulose derivatives, including microcrystalline cellulose (MCC), TEMPO-oxidized nanofibrillated cellulose (TOCNF), TEMPO-oxidized nanocrystalline cellulose (TOCNC), and carboxymethyl cellulose (CMC) were selected to investigate their in vitro fermentation profiles. TOCNF exhibited the highest production of total short-chain fatty acids (SCFAs), followed by TOCNC. The results suggested that reduced particle size and increased aspect ratio improved the fermentability of insoluble cellulose derivatives. MCC and CMC were barely fermented with similar total SCFAs production as the blank. 16S rRNA sequencing revealed that the fermentation of cellulose derivatives resulted in divergent microbial community structures. Moreover, Bacteroides cellulosilyticus showed high specificity to utilize TOCNF and TOCNC. The findings demonstrated that the colloidal states of cellulose derivatives, such as size and solubility, were important factors governing microbial community composition and metabolites.

Cellulose and cellulose derivatives: Different colloidal states and food-related applications.

Development of new sources and isolation processes has recently enhanced the production of cellulose in many different colloidal states. Even though cellulose is widely used as a functional ingredient in the food industry, the relationship between the colloidal states of cellulose and its applications is mostly unknown. This review covers the recent progress on illustrating various colloidal states of cellulose and the influencing factors with special emphasis on the correlation between the colloidal states of cellulose and its applications in food industry. The associated unique colloidal states of cellulose like high aspect ratio, crystalline structure, surface charge, and wettability not only promote the stability of colloidal systems, but also help improve the nutritional aspects of cellulose by facilitating its interactions with digestive system. Further studies are required for the rational control and improvement of the colloidal states of cellulose and producing food systems with enhanced functional and nutritional properties.

Identifying the phase behavior of biodegradable poly(hexamethylene succinate-co-hexamethylene adipate) copolymers with FTIR.

Whether a phase separation or a cocrystallization occurs in poly(hexamethylene succinate-co-hexamethylene adipate) (P(HS-co-HA)) copolymers was studied with a combination of wide-angle X-ray diffraction (WAXD) and Fourier transform infrared (FTIR) spectroscopy. With HA as the majority, the presence of HS comonomers leads to weakening and broadening of (10l) peaks in the X-ray fiber diffraction patterns, while a crystal structure similar to PHS is formed in the copolymer with HS as the majority. The X-ray diffraction patterns imply possible cocrystallization between HS and HA comonomers, but cannot lead to an unambiguous conclusion, which was clarified with the compensative tool of FTIR. Following the characteristic absorption bands of crystals, cocrystallization of HS and HA comonomers was observed in copolymers with HA comonomer as the majority during which HA initiated the nucleation at high temperatures. With HA as minority, cocrystallization of HS and HA can still be achieved with a fast quenching to below 0 degrees C, while a phase separation occurs and only HS comonomer crystallizes at high temperatures. This demonstrates that P(HS-co-HA) has an asymmetric phase diagram. Because of the sensitivity to local conformations, FTIR spectroscopic method is demonstrated to be a powerful tool on study phase behaviors of polymers with similar crystal structure.

Perception and measurement of food texture: Solid foods.

There is still a gap between instrumental measurement and sensory evaluation because of the complexity of food texture in spite of many efforts. In sensory evaluation, the terms describing the texture should be well understood by panelists, which poses a problem of establishing lexicons and training panelists. In the instrumental measurement, more efforts are required to understand the large deformation and fracture behavior of foods. The texture profile analysis (TPA) proposed by Alina Szczesniak, Malcolm Bourne, and Sherman has been applied to many foods, and was useful to develop the understanding of textures. But sometimes confusion of the interpretation of TPA parameters appeared. Many new techniques have been introduced to quantify TPA parameters. Recent efforts to fill the gap between sensory evaluation and instrumental measurements, human measurements, or physiological measurements have been introduced. This endeavor is an effort of synthesizing the dentistry and biomedical approach, sensory and psychological approach, and material science approach, and therefore, the collaboration among these disciplines is necessary. This manuscript mainly discusses texture studies for solid foods. PRACTICAL APPLICATIONS: To fill the gap between the sensory evaluation and the instrumental measurement of texture, it is necessary to examine the physical change of foods during the oral processing. This will give us the designing principle of palatable and safe foods.

Characterization of konjac glucomannan-ethyl cellulose film formation via microscopy.

Konjac glucomannan-ethyl cellulose (KGM-EC, 7:3, w/w) blended film shows good mechanical and moisture resistance properties. To better understand the basis for the KGM-EC film formation, optical microscopy, scanning electron microscopy (SEM), transmission electron microscopy (TEM), and atomic force microscopy (AFM) were used to observe the formation of the film from emulsion. Optical microscopy images showed that EC oil droplets were homogeneously dispersed in KGM water phase without obviously coalescence throughout the entire drying process. SEM images showed the surface and cross-sectional structures of samples maintained continuous and homogeneous appearance from the emulsion to dried film. AFM images indicated that KGM molecules entangled EC molecules in the emulsion. Interactions between KGM and EC improved the stability of KGM-EC emulsion, and contributed to uniformed structures of film formation. Based on these output information, a schematic model was built to elucidate KGM-EC film-forming process.

Thermosensitive injectable in-situ forming carboxymethyl chitin hydrogel for three-dimensional cell culture.

Injectable hydrogels have gained great attentions for cell therapy and tissue regeneration as a result of the applications in minimally invasive surgical procedures with the ease of handling and complete filling of the defect area. Here, a novel biodegradable, thermosensitive and injectable carboxymethyl chitin (CMCH) hydrogel was developed for three-dimensional (3D) cell culture. The obtained CMCH solution remained transparent liquid flowing easily at low temperatures and gelled rapidly at 37°C. The gelation time of CMCH hydrogels could be easily tuned by varying temperature and the degree of carboxymethylation, which facilitates the cell encapsulation process at room temperature and in-situ forming hydrogel at body temperature. Moreover, the CMCH-14 hydrogels in PBS buffer remained stable and continuous porous structure and could be degraded in the presence of lysozyme or hyaluronidase. HeLa cells proliferated sustainably and self-assembled to form 3D multicellular spheroids with high cell activity on the surface of CMCH-14 hydrogel. Encapsulation of COS-7 cells within the in-situ forming CMCH hydrogel demonstrated that CMCH hydrogels promoted cell survival and proliferation. In vivo mouse study of the CMCH hydrogels showed good in-situ gel formation and tissue biocompatibility. Thus, the biodegradable thermosensitive injectable CMCH hydrogels hold potential for 3D cell culture and biomedical applications. STATEMENT OF SIGNIFICANCE: Biodegradable hydrogels have been widely studied for cell therapy and tissue regeneration. Herein, we report a novel thermosensitive injectable carboxymethyl chitin (CMCH) hydrogel for 3D cell culture, which was synthesized homogeneously from the bioactive natural chitin through the "green" process avoiding using organic solvent. The CMCH solutions exhibited rapid thermoresponsive sol-to-gel phase transition behavior at 37°C with controllable gelation times, which facilitates the cell encapsulation process at room temperature and in-situ forming hydrogel at body temperature. Importantly, in vitro 3D cell culture and in vivo mouse study of the CMCH hydrogel showed promotion of cell survival and proliferation, good in-situ gel formation and biocompatibility. We believe that such thermosensitive injectable CMCH hydrogels would be very useful for biomedical applications, such as tumor model for cancer research, post-operative adhesion prevention, the regeneration of cartilage and central nervous system and so on.

Competitive adsorption between sugar beet pectin (SBP) and hydroxypropyl methylcellulose (HPMC) at the oil/water interface.

The emulsification performance, stability and competitive adsorption of two natural food emulsifiers, sugar beet pectin (SBP) and hydroxypropyl methylcellulose (HPMC) have been investigated. Both can reduce the surface tension and emulsify oil in water. However, due to their different structure and conformation they operate via different mechanisms. Using 15% middle chain triglycerides (MCTs) oil, the amounts of SBP and HPMC adsorbed in emulsions made with these individually and in mixtures were determined. The interfacial concentration (Γ) for SBP stabilized emulsion was ∼1.25mg/m(2) and for HPMC 3.5mg/m(2). The higher adsorption of HPMC was due to multilayer adsorption, whereas SBP adsorbed as a monolayer. Competitive adsorption between SBP and HPMC was also investigated. When the HPMC concentration approached that of adsorbed SBP, the effect of HPMC became dominant and at 1.5wt.% controlled the behavior of the mixed emulsions, which were then almost independent of SBP. The minor role of SBP was mainly to decrease the proportion of large droplets in the emulsion. A model to describe the competitive adsorption between SBP and HPMC is proposed.

Protein/polysaccharide cogel formation based on gelatin and chemically modified schizophyllan.

In the work, aldehyde groups were quantitatively introduced into schizophyllan (SPG) side chains through periodate oxidation. The periodate-oxidized SPG (POSPG) forms an elastic gel with gelatin. The cogel formation is based on the Schiff-base reaction between the amino groups of gelatin chains and the aldehyde groups of POSPG chains. The POSPG/gelatin cogel has an elastomeric character with a very small value of loss tangent. The gelation kinetics and gel properties were discussed as a function of POSPG concentration, gelatin concentration, oxidation degree, temperature, and pH. This method can be used to design a large variety of cogels between SPG and proteins.