Tough and Elastic Cellulose Composite Hydrogels/Films for Flexible Wearable Sensors.

Cellulose and its composites, despite being abundant and sustainable, are typically brittle with very low flexibility/stretchability. This study reports a solution processing method to prepare porous, amorphous, and elastic cellulose hydrogels and films. Native cellulose dissolved in a water-ZnCl2 mixture can form ionic gels through in situ polymerization of acrylic acid (AA) to poly(acrylic acid) (PAA). The addition of up to 30 vol % AA does not change the solubility of cellulose in the water-ZnCl2 mixture. After polymerization, the formation of interpenetrated networks, resulting from the chemical cross-linking of PAA and the ionic/coordination binding among cellulose/PAA and ZnCl2, gives rise to strong, transparent, and ionically conductive hydrogels. These hydrogels can be used for wearable sensors to detect mechanical deformation under stretching, compression, and bending. Upon removal of ZnCl2 and drying the gels, semitransparent amorphous cellulose composite films can be obtained with a Young's modulus of up to 4 GPa. The rehydration of these films leads to the formation of tough, highly elastic composites. With a water content of 3-10.5%, cellulose-containing films as strong as paper also show typical characteristics of elastomers with an elongation of up to 1300%. Such composite films provide an alternative solution to resolving the material sustainability of natural polymers without compromising their mechanical properties.

Effect of ultrasound assisted H2O2/Vc treatment on the hyperbranched Lignosus rhinocerotis polysaccharide: Structures, hydrophobic microdomains, and antitumor activity.

The effect of ultrasonic intensity (28.14, 70.35, and 112.56 W/cm2) on Lignosus rhinocerotis polysaccharide (LRP) degraded by ultrasound assisted H2O2/Vc system (U-H/V) was investigated. U-H/V broke the molecular chain of LRP and improved the conformational flexibility, decreasing the molecular weight, intrinsic viscosity ([η]) and particle size. The functional groups and hyperbranched structure of LRP were almost stable after U-H/V treatment, however, the triple helix structure of LRP was partially disrupted. With increasing ultrasonic intensity, the critical aggregation concentration increased from 0.59 mg/mL to 1.57 mg/mL, and the hydrophobic microdomains reduced. Furthermore, the LRP treated with U-H/V significantly inhibited HepG2 cell proliferation by inducing apoptosis. The increase in antitumor activity of LRP was closely associated with the reduction of molecular weight, [η], particle size and hydrophobic microdomains. These results revealed that U-H/V treatment facilitates the degradation of LRP and provides a better insight into the structure-antitumor activity relationship of LRP.

Glycerol/organic acid-based ternary deep eutectic solvents as a green approach to recover chitin with different molecular weight from seafood waste.

In this study, we designed a green and efficient approach for the fractionation of high-purity chitin with tunable molecular weights from seafood waste. This was achieved by using ternary deep eutectic solvents (TDESs) composed of choline chloride as a hydrogen bond acceptor, glycerol as the polyol-based hydrogen bond donor, together with lactic acid or malic acid. Two binary DESs and four TDESs were evaluated for their ability to recover chitin. The extracted chitin exhibited not only high yield with excellent protein and mineral removal, but also high purity with similar crystallinity patterns as standard chitin. However, the average molecular weights, viscosity behavior and morphology of chitin extracted by DESs were varied and influenced by organic acid to glycerol molar ratios. The molecular weights of chitin extracted by lactic acid-based TDES ranged from 264 kDa to 541 kDa, but malic acid-based TEDS displayed a stronger depolymerization effect, resulting in chitin with a smaller molecular weight of less than 300 kDa. Lactic acid-based TDES revealed that the purity of chitin remained higher than 92 % after three cycles. This sustainable and environmentally friendly extraction system holds great potential to recover chitin from seafood waste, opening a new era for chitin extraction and applications.

Physicochemical and functional properties of RG-I enriched pectin extracted from thinned-young apples.

The demand for obtaining pectin from new sources has been continuously increasing. The abundant but underutilized thinned-young apple is a potential source of pectin. In this study, an organic acid (i.e., citric acid) and two inorganic acids (i.e., hydrochloric acid and nitric acid) commonly used in commercial pectin production were applied to extract pectin from three varieties of thinned-young apples. The physicochemical and functional properties of the thinned-young apple pectin were comprehensively characterized. The highest pectin yield (8.88 %) was obtained from Fuji apple using citric acid extraction. All pectin was high methoxy pectin (HMP) and rich in RG-I regions (>56 %). The citric acid extracted pectin had the highest molecular weight (Mw) and lowest degree of esterification (DE) values, and exhibited great thermal stability and shear-thinning property. Furthermore, Fuji-apple pectin possessed significantly better emulsifying properties compared to pectin obtained from the other two varieties of apples. Thus, pectin extracted with citric acid from Fuji thinned-young apples has great potential to be applied in the food industry as a natural thickener and emulsifier.

Removal of anionic and cationic dyes using porous chitosan/carboxymethyl cellulose-PEG hydrogels: Optimization, adsorption kinetics, isotherm and thermodynamics studies.

Chitosan (CS)/carboxymethyl cellulose (CMC) porous hydrogels chemically crosslinked by epichlorohydrin were synthesized using polyethylene glycol (PEG) as a pore-forming agent for anionic (Congo red, CR) and cationic (methylene blue, MB) dyes removal from aqueous solutions. The swelling ratio of hydrogels prepared with 2 % CS and 2 % CMC (CS2/CMC2) exhibited optimal performance at different pHs. The addition of PEG into hydrogels (denoted as CS2/CMC2-PEG1.25) exhibited a significantly higher adsorption for CR and MB, increasing from 117.83 to 159.12 mg/g and 110.2 to 136 mg/g, respectively. The comprehensive analyses of Fourier transform infrared spectroscopy, thermalgravimetric study and scanning electron microscopy showed that CS2/CMC2-PEG1.25 hydrogels became more porous with no significant changes in intermolecular and intramolecular interactions, compared with CS2/CMC2 hydrogels. The adsorption process for CR and MB conformed to the pseudo-second-order and pseudo-first-order kinetics models, respectively. The results of adsorption isotherm for CR followed both Freundlich and Langmuir models with the maximum adsorption capacities of 1053.88 mg/g, whereas the isotherm for MB fitted the Langmuir model better with the maximum adsorption capacities of 331.72 mg/g. The thermodynamic study results proved that the CR and MB adsorption by hydrogels was spontaneous, but the CR adsorption was endothermic and the MB adsorption was exothermic.

Recent development of egg protein fractions and individual proteins as encapsulant materials for delivery of bioactives.

Egg proteins, as one of the most abundant animal protein sources, have received considerable attention for developing delivery systems. Among all egg proteins, egg white (ovalbumin) is the most promising encapsulant due to its excellent properties such as gelling, digestibility, self-assembly, amphiphilic nature. In this review paper, we focused particularly on egg protein-based delivery systems with superior encapsulation and delivery functions, including polymeric nanoparticles, emulsions, hydrogels and aerogels. Egg protein-based delivery systems across a wide range of geometry and dimensions have been applied to protect or control-release bioactive small molecules and macromolecules, probiotics and metal nanostructures. However, there are challenges that must be carefully addressed for advancing the practical applications of egg protein-based delivery system in foods, including allergenicity from ovalbumin and ovotransferrin, intolerance to environmental conditions, limited processing technologies. More efforts are warranted to fill knowledge gaps related to fabrication, utilization and digestive mechanisms of egg protein-derived delivery systems.

A Comprehensive Review of Nanoparticles for Oral Delivery in Food: Biological Fate, Evaluation Models, and Gut Microbiota Influences.

Edible nanoparticles are being developed for the oral delivery of nutrients to improve human health and well-being. Because of the extremely demanding conditions foods experience within the gastrointestinal tract, fundamental knowledge about the biological fate of encapsulated nutrients must be constantly revised. In this review, we first provide an overview of the fundamental absorption pathways of ingested foods and then discuss the evaluation models available to test and predict the biological fate of nutrient-loaded nanoparticles. Then, owing to their importance for human health, the impacts of nanoparticles on the gut microbiota are evaluated. Lastly, the limitations of current evaluation methods are highlighted and future research directions on the study and application of edible nanoparticles for the oral delivery of bioactive food compounds are discussed.

Effect of four plant oils on the stability of high internal phase Pickering emulsions stabilized by ovalbumin-tannic acid complex.

The poor interfacial stability of protein-stabilized high internal phase Pickering emulsions (HIPEs) is a major hurdle to realize their practical applications in food processing. The emulsifying stability is not only related to the protein itself, but also dependent upon the oil phases. In this study, four plant-based oils were studied to understand their respective effects on the interfacial stability of HIPEs prepared by ovalbumin (OVA) and ovalbumin-tannic acid complex (OVA-TA). Our findings revealed that the interfacial activities were closely related to the physicochemical properties of the oil phase, such as the number of carbon­carbon double bonds in the unsaturated fatty acids, melting point, and polarity. The emulsifying abilities were ranked as palm oil > soybean oil > olive oil > perilla oil. OVA-TA stabilized HIPEs exhibited excellent emulsifying stability compared with free OVA stabilized ones. This work provided a unique insight into understanding the interfacial stabilization mechanisms for protein-stabilized HIPEs with different kinds of oil phases.

Mechanisms of carotenoid intestinal absorption and the regulation of dietary lipids: lipid transporter-mediated transintestinal epithelial pathways.

Dietary lipids are key ingredients during cooking, processing, and seasoning of carotenoid-rich fruits and vegetables, playing vitals in affecting the absorption and utilization of carotenoids for achieving their health benefits. Besides, dietary lipids have also been extensively studied to construct various delivery systems for carotenoids, such as micro/nanoparticles, micro/nanoemulsions, and liposomes. Currently, the efficacies of these techniques on improving carotenoid bioavailability are often evaluated using the micellization rate or "bioaccessibility" based on in vitro models. However, recent studies have found that dietary lipids may also affect the carotenoid uptake via intestinal epithelial cells and the efflux of intracellular chyle particles via lipid transporters. An increasing number of studies reveal the varied impact of different dietary lipids on the absorption of different carotenoids and some lipids may even have an inhibitory effect. Consequently, it is necessary to clarify the relationship between the addition of dietary lipids and the intestinal absorption of carotenoid to fully understand the role of lipids during this process. This paper first introduces the intestinal absorption mechanism of carotenoids, including the effect of bile salts and lipases on mixed micelles, the types and regulation of lipid transporters, intracellular metabolizing enzymes, and the efflux process of chyle particles. Then, the regulatory mechanism of dietary lipids during intestinal carotenoid absorption is further discussed. Finally, the importance of selecting the dietary lipids for the absorption and utilization of different carotenoids and the design of an efficient delivery carrier are emphasized. This review provides suggestions for precise dietary carotenoid supplementation and offere an important reference for constructing efficient transport carriers for liposoluble nutrients.

Chitosan-based oral colon-specific delivery systems for polyphenols: recent advances and emerging trends.

Oral colon-targeted delivery systems (OCDSs) have attracted great attention in the delivery of active compounds targeted to the colon for the treatment of colon and non-colon diseases with the advantages of enhanced efficacy and reduced side effects. Chitosan, the second-most abundant biopolymer next to cellulose, has great biocompatibility, is non-toxic, is sensitive to colonic flora and shows strong adhesion to colonic mucus, making it an ideal biomaterial candidate for the construction of OCDSs. Being rich in functional groups, the chitosan structure is easily modified, both physically and chemically, for the fabrication of delivery systems with diverse geometries, including nanoparticles, microspheres/microparticles, and hydrogels, that are resistant to the harsh environment of the upper gastrointestinal tract (GIT). This review offers a detailed overview of the preparation of chitosan-based delivery systems as the basis for building OCDSs. A variety of natural polyphenols with potent biological activities are used to treat diseases of the colon, or to be metabolized as active ingredients by colonic microorganisms to intervene in remote organ diseases after absorption into the circulation. However, the poor solubility of polyphenols limits their application, and the acidic environment of the upper GIT and various enzymes in the small intestine disrupt their structure and activity. As a result, the development of OCDSs for polyphenols has become an emerging and popular area of current research in the past decade. Thus, the second objective of this review is to systematically summarize the most recent research findings in this area and shed light on the future development of chitosan-based OCDSs for nutritional and biomedical applications.

Preparation and characterization of carboxymethyl cellulose capped zinc oxide nanoparticles: A proof-of-concept study.

Zinc oxide (ZnO) is one of the promising food additives, which adds nutrients and provides antimicrobial properties when incorporated into various food matrices. In this study, carboxymethyl cellulose capped ZnO (ZnO-CMC) were developed via a low-energy and cost-effective technique without calcination or grinding. The fabrication involved two steps: crosslinking Zn2+ ions with CMC through electrostatic interactions and generation of ZnO nanoparticles with CMC as capping agent. After mild heating, the crystalline structure of ZnO-CMC was confirmed by WAXS. Both FTIR and AFM studies illustrated that ZnO was physically trapped by CMC molecules, resulting in a physical barrier to prevent aggregation. SEM verified that the ZnO-CMC had a size of 50-80 nm with comparable morphology to commercial ZnO. Overall, CMC played a key role in controlling growth and inhibiting agglomeration of ZnO. Given the small and uniform particle size, the obtained ZnO-CMC is ready to be incorporated into different food matrices.

Facile synthesis of water-dispersible poly(3-hexylthiophene) nanoparticles with high yield and excellent colloidal stability.

There has been growing interest in water-processable conjugated polymers for biocompatible devices. However, some broadly used conjugated polymers like poly(3-hexylthiophene) (P3HT) are hydrophobic and they cannot be processed in water. We herein report a facile yet highly efficient assembly method to prepare water-dispersible pyridine-containing P3HT (Py-P3HT) nanoparticles (NPs) with a high yield (>80%) and a fine size below 100 nm. It is based on the fast nanoprecipitation of Py-P3HT stabilized by hydrophilic poly(acrylic acid) (PAA). Py-P3HT can form spherical NPs at a concentration up to 0.2 mg/mL with a diameter of ∼75 nm at a very low concentration of PAA, e.g., 0.01-0.1 mg/mL, as surface ligands. Those negatively charged Py-P3HT NPs can bind with metal cations and further support the growth of noble metal NPs like Ag and Au. Our self-assembly methodology potentially opens new doors to process and directly use hydrophobic conjugated polymers in a much broader context.

Antimicrobial effects of thymol-loaded phytoglycogen/zein nanocomplexes against foodborne pathogens on fresh produce.

In this study, thymol-loaded hydrophobically modified phytoglycogen/zein nanocomplexes with a particle size around 100 nm were developed for improving microbial safety of fresh produce. The antimicrobial activities, including the determination of minimum inhibitory and bactericidal concentration, growth kinetic curves, and inhibition zone of the nanocomplexes against foodborne pathogens (Listeria monocytogenes, Salmonella enteritidis, and Escherichia coli) were evaluated. The results showed that the antimicrobial activities of the nanocomplexes were significantly stronger than that of free thymol control (without encapsulation), and the antimicrobial efficacy remained unchanged after storage at 4 °C for 60 days. The morphological results from atomic force microscope revealed that small micellar blebs were formed at the surface of bacteria after treatment with nanocomplexes and the gradual disappearance of the cell boundary indicated the occurrence of cytolysis. The potential applications of this nanocomplex as disinfectant agent in wash water were evaluated on different types of fresh produce (lettuce, cantaloupe, and strawberries). Notably, the nanocomplexes also demonstrated efficacy in biofilm removal. Findings from this study clearly demonstrated that the thymol-loaded nanocomplexes hold promising potential for the disinfection of fresh produce to improve their microbial safety and quality.

The Efficacy of Conventional Spray, Electrostatic Spray, and Dip with a Combination of Hydrogen Peroxide and Peroxyacetic Acid To Inactivate Listeria monocytogenes on Apples.

ABSTRACT: This study aimed to evaluate the efficacy of a hydrogen peroxide (H2O2) and peroxyacetic acid (PAA) mixer delivered by conventional garden spray (GS), electrostatic spray (ES), and dip methods to inactivate Listeria monocytogenes on apples. Organic Honeycrisp, Fuji, and Pink Lady apples were dip inoculated with L. monocytogenes (two strains, serotype 1/2b), which were then kept untreated (control), sprayed with water only, or treated with the H2O2-PAA mixer (0.0064, 0.1, 0.25, and 0.50%) for 20 s via GS, ES, or dip, followed by draining (for 2 min) on aluminum foil. Surviving bacteria were recovered on modified Oxford agar. Atomic force microscopy was used to detect the structural changes of inactivation of L. monocytogenes in broth medium by the H2O2-PAA mixer solution. Data (two replicates, with six samples per replicate) were analyzed using the mixed model procedure of SAS (P = 0.05). Initial counts of L. monocytogenes on untreated apples were 6.80 to 6.90 log CFU per apple. The dip method was the most effective treatment (P < 0.05) for pathogen reductions (2.31 to 2.41 log CFU per apple), followed by GS (1.44 to 1.70 log CFU per apple) and then ES (0.84 to 1.20 log CFU per apple). Reductions of L. monocytogenes were greatest (P < 0.05) when apples were treated with H2O2-PAA mixer -0.25 and -0.50%. Atomic force microscopy analyses indicated that inactivation of L. monocytogenes cells in H2O2-PAA mixer solutions resulted from disruption of the outer membrane. The H2O2-PAA mixer-treated cells had increased width and height and decreased roughness compared with the untreated cells. Results suggested that applying a H2O2-PAA mixer by dip or GS methods is better for pathogen reduction than ES on apples.

High internal phase Pickering emulsions stabilized by egg yolk low density lipoprotein for delivery of curcumin.

Egg yolk low density lipoprotein (LDL) was used to prepare high internal phase Pickering emulsions (HIPEs) and its role as a stabilizer was comprehensively studied in this work. LDL exists as homogenous nanoparticles with an average size of 49 nm and amphiphilic nature, having a contact angle close to 90°. HIPEs were studied by varying compositions of 75%-90% oil phase and 25%-10% aqueous phase containing 0.5%-2% LDL. Rheological measurement, confocal laser scanning and optical microscopes imaging together with digital photos revealed the solid gel network, the strength of which was dependent upon oil volume fraction and LDL concentration. Optimal formulation of HIPEs was found as 80% oil and 2% LDL concentration, which exhibited small droplets under 10 µm with negligible aggregations, even after four weeks storage under refrigeration or heating at 90 â„ƒ for 30 min. After three freeze-thawing cycles, the HIPEs were demulsified losing their gel structure, but a simple re-homogenization was able to reconstitute the gel network identical to original microstructure. Encapsulation of curcumin into Pickering HIPEs provided exceptional photostability (around 80% retention rate) against ultraviolet radiation and improved its bioaccessibility from 10% to 50% during in vitro digestion. Our findings may bring new opportunities to design semi-solid foods using natural and edible ingredients.

Self-assembled caseinate-laponite® nanocomposites for curcumin delivery.

In this study, novel self-assembled protein-clay nanocomposites were developed for curcumin delivery. Experimentally, curcumin was dissolved and deprotonated in sodium caseinate-laponite® (NaCas-LAP) dispersion at pH 12.0 for 30 min followed by neutralization to pH = 7. Due to the pH-mediated dissociation and re-association process, curcumin was successfully encapsulated into NaCas-LAP nanocomposites. The colloidal properties and encapsulation capabilities of NaCas-LAP nanocomposites were investigated, including particle size, zeta potential, encapsulation efficiency, release profile in simulated gastrointestinal tract, as well as nanoscale morphology. The results indicated that upon neutralization, NaCas-LAP nanocomposites were re-associated into smaller particles due to strong hydrophobic interactions among NaCas, LAP and curcumin. Specifically, 0.10% curcumin loaded nanocomposites prepared with 2% NaCas and 0.5% LAP showed improved encapsulation performance (73.4%) with smaller particle size (100 nm). The as-prepared protein-clay nanocomposites hold promising potential to deliver lipophilic bioactive compounds, such as curcumin.

Partition and stability of folic acid and caffeic acid in hollow zein particles coated with chitosan.

The carriers for hydrophobic bioactives have been extensively studied, while those for hydrophilic bioactives are still challenging. The partition of bioactives in the particles depends greatly on their solubility, interaction with carrier materials, as well as structure of carriers. In this study, chitosan-coated hollow zein particles using calcium phosphate as a sacrificing template (CS-HZ) were fabricated to co-encapsulate folic acid (FA) and caffeic acid (CA). Partition, photostability, and antioxidant capacity of bioactive compounds were also studied. The size, polydispersity index and ζ-potential of optimized CS-HZ were 176.3 nm, 0.14 and +39.3 mV, respectively, indicating their small and uniform dimension with excellent colloidal stability. FA interacted with chitosan to form complexes and then coated on the zein particles where CA was encapsulated. After co-encapsulation in CS-HZ, the photostability of both FA and CA was improved in comparison with encapsulation of single compound, with 85% of FA remaining after 240 min of UVA irradiation, and 90% of CA remaining after 80 min. Antioxidant activity of CA decreased upon encapsulation, but significantly increased after irradiation. Findings in this study shed some light on the design of carriers for co-delivery of hydrophilic compounds in acidic condition.

Protein deamidation to produce processable ingredients and engineered colloids for emerging food applications.

With the ever-increasing demands for functional and sustainable foods from the general public, there is currently a paradigm shift in the food industry toward the production of novel protein-based diet. Food scientists are therefore motivated to search for natural protein sources and innovative technologies to modify their chemical structure for desirable functionality and thus utilization. Deamidation is a viable, efficient, and attractive approach for modifying proteins owing to its ease of operating, specificity, and cost-effective processes. Over the past three decades, the knowledge of protein deamidation for food applications has evolved drastically, including the development of novel approaches for deamidation, such as protein-glutaminase and ion exchange resin, and their practices in new protein substrate. Thanks to deamidation, enhanced functionalities of food proteins from cereals, legumes, milk, oil seeds and others, and thereby their processabilities as food ingredients have been achieved. Moreover, deamidated proteins have been used to fabricate engineered food colloids, including self-assembled protein particles, protein-metallic complexes, and protein-carbohydrate complexes, which have demonstrated tailored physicochemical properties to modulate oral perception, improve gastrointestinal digestion and bioavailability, and protect and/or deliver bioactive nutrients. Novel bioactivity, altered digestibility, and varied allergenicity of deamidated proteins are increasingly recognized. Therefore, deamidated proteins with novel techno-functional and biological properties hold both promise and challenges for future food applications, and a comprehensive review on this area is critically needed to update our knowledge and provide a better understanding on the protein deamidation and its emerging applications.

Chemically modified phytoglycogen: Physicochemical characterizations and applications to encapsulate curcumin.

Phytoglycogen (PG), a water-soluble glycogen-like α-d-glucan, exists as natural dendritic nanoparticles which are known as a promising solubility enhancer and delivery vehicle for lipophilic compounds. However, the practical applications of PG in food and pharmaceutical fields are limited by their high hydrophilicity and relatively low encapsulation efficiency compared with other delivery systems. The objectives of this work were to chemically modify native PG nanoparticles with hydrophobic groups and to characterize their physicochemical properties, as well as to evaluate the application feasibility of modified PG (mPG) nanoparticles as a carrier for hydrophobic bioactive compounds. The surface hydroxyl groups of PG nanoparticles were capped with various anhydrides, e.g., acetic, valeric, and N-caprylic, to obtain the PG nanoparticles with different hydrophobicity. Successful modification by acyl groups was evidenced by both Fourier-transform infrared and nuclear magnetic resonance spectroscopies. The mPG nanoparticles exhibited a more compact structure and homogeneous size distribution as revealed by dynamic light scattering measurement and visualized by transmission electron microscope, while their size slightly increased with the chain length of anhydride. Rheological measurement revealed that the viscosity of mPG at low shear rate was increased with the increase of degree of substitution due to the intermolecular hydrophobic association. A novel pH-driven method to load curcumin showed significantly higher encapsulation efficiency and greater antioxidant activity compared with traditional ethanol mediated loading method. Hydrophobic modification of natural dendritic PG nanostructures demonstrates promising potential to develop food-grade nanocarriers for lipophilic bioactive compounds with improved bioactivity.