Biodegradable, Strong, and Hydrophobic Regenerated Cellulose Films Enriched with Esterified Lignin Nanoparticles.

The scientific community is pursuing significant efforts worldwide to develop environmentally viable film materials from biomass, particularly transparent, high-performance regenerated cellulose (RC) films, to replace traditional plastics. However, the inferior mechanical performance and hydrophilic nature of RC films are generally not suitable for use as a substitute for plastics in practical applications. Herein, lignin homogenization is used to synthesize high-performance composite films. The esterified lignin nanoparticles (ELNPs) with dispersible and binding advantages are prepared through esterification and nanometrization. In the presence of ELNPs, RC films exhibit a higher tensile strength (110.4 MPa), hydrophobic nature (103.6° water contact angle, 36.6% water absorption at 120 min, and 1.127 × 10-12 g cm cm-2 s-1 Pa-1 water vapor permeability), and exciting optical properties (high visible and low ultraviolet transmittance). The films further display antioxidant activity, oxygen barrier ability, and thermostability. The films completely biodegrade at 12 and 30% soil moisture. Overall, this study offers new insights into lignin valorization and regenerated cellulose composite films as novel bioplastic materials.

Preparation and Characterization of Size-Controlled Lignin Nanoparticles with Deep Eutectic Solvents by Nanoprecipitation.

Lignin nanomaterials have wide application prospects in the fields of cosmetics delivery, energy storage, and environmental governance. In this study, we developed a simple and sustainable synthesis approach to produce uniform lignin nanoparticles (LNPs) by dissolving industrial lignin in deep eutectic solvents (DESs) followed by a self-assembling process. LNPs with high yield could be obtained through nanoprecipitation. The LNPs were characterized by dynamic light scattering (DLS), transmission electron microscopy (TEM), scanning electron microscopy (SEM), Fourier transform infrared spectroscopy (FTIR), and gel permeation chromatography (GPC). Distinct LNPs could be produced by changing the type of DES, lignin sources, pre-dropping lignin concentration, and the pH of the system. Their diameter is in the range of 20-200 nm and they show excellent dispersibility and superior long-term stability. The method of preparing LNPs from lignin-DES with water as an anti-solvent is simple, rapid, and environmentally friendly. The outcome aids to further the advancement of lignin-based nanotechnology.

Phlorotannins from Undaria pinnatifida Sporophyll: Extraction, Antioxidant, and Anti-Inflammatory Activities.

Undaria pinnatifida sporophyll (U. pinnatifida) is a major byproduct of U. pinnatifida (a brown algae) processing. Its phenolic constituents, phlorotannins, are of special interest due to their intrinsic ability to precipitate proteins. Herein, a high-temperature extraction procedure was used to isolate these biologically active compounds. The heating temperature, heating time, and extraction solvent (ethanol) concentration were examined with response surface analysis to determine the optimal conditions to achieve the maximum extraction rate. The analysis revealed the optimal conditions to be: 170 °C of heating temperature, 5.2 h of heating time, and 52% ethanol concentration for a yield of 10.7 ± 0.2 mg gallic acid equivalent/g dry weight (GAE/g DW) of sample. Compared to epigallocatechin gallate (EGCG), the extracted phlorotannins displayed higher antioxidant activity on H2O2-induced RAW 264.7 cells with improved efficiency. Furthermore, the compounds exhibited strong anti-inflammatory activity. These findings potentially can be utilized to guide development of novel functional foods and food supplements from sea-originated resources such as brown algae.

Hydrocolloid-based nutraceutical delivery systems: Effect of counter-ions on the encapsulation and release.

Nutraceuticals provide health benefits, especially for the prevention and treatment of chronic diseases such as diabetes, obesity, cardiovascular disease and cancer. Their incorporation in food supplements, functional foods and medicinal foods is a major technological challenge due to lower water solubility, instability during processing and storage conditions. Carriers that can effectively overcome these predicaments and protect them during product development, consumption and delivery are in high demand. Toward this end, our research approach is to entrap nutraceuticals in the ordered networks of hydrocolloids. We have examined the effect cations in regulating the encapsulated amounts and release characteristics. Iota-carrageenan and eugenol have been chosen as models of hydrocolloid and nutraceutical, respectively, in the presence of Na and Ca ions. The results suggest that carrageenan maintains its network organization even after encapsulating the eugenol molecules. Increased eugenol amounts are found in the Na carrageenan complex compared to the Ca complex, and the release rate is faster from the former but it is more controlled from the latter. These differences highlight the vital role of cations on the encapsulation efficiency and release profiles of hydrocolloid-based nutraceutical carriers. The outcome offers an elegant opportunity for developing novel and value-added food systems employing low-in-cost, nontoxic and heavily consumed food grade hydrocolloids.

Biodegradable, UV-blocking, and antioxidant films from alkali-digested lignocellulosic residue fibers of switchgrass.

The development of bio-friendly materials to replace single-use plastics is urgently needed. In this regard, cellulosic material from plants is a promising alternative. However, due to the risk of forest depletion, agricultural biomass stands out as a favorable choice. Toward this end, switchgrass, an underutilized grass, presents itself as a viable source of lignocellulose that can be turned into a bio-friendly material. Herein, lignocellulosic residue from switchgrass has been extracted using two different concentrations of NaOH (20% and 50% w/v), solubilized in aqueous ZnCl2 solution, and crosslinked with CaCl2 (200, 300, 400, and 500 mM) to prepare biodegradable films. The color, thickness and moisture, water solubility, water absorption, water vapor permeability, tensile strength and elongation, biodegradation, UV transmittance, and antioxidant activity of films have been studied. The films possess a high tensile strength of 14.7 MPa and elongation of 4.7%. They block UVB-radiation and hold antioxidant properties. They display good water vapor permeability of 1.410-1.6 × 10-11 gm-1s-1Pa-1 and lose over 80% of their weight at 30% soil moisture within 40 days. An increase in the CaCl2 amount decreased the water vapor permeability, elongation, UV transmittance, and biodegradation but increased the transparency, tensile strength and antioxidant property. Overall, films of alkali-digested lignocellulosic residue of switchgrass showed excellent potential to be used against lightweight plastics and support the circular economy.

Porous corn starch granules as effective host matrices for encapsulation and sustained release of curcumin and resveratrol.

Type 2 Diabetes Mellitus (T2DM) is a carbohydrate-rich diet-regulated ailment with carbohydrates digested and absorbed rapidly. Hence, modulating carbohydrate digestion is warranted; to this end, polyphenols from plant sources are handy. However, polyphenols' instability and low bioavailability limit their wholesome use, and thus, encapsulating them into an inexpensive and suitable wall material would be the best strategy. Herein, the potential of porous starch granules is demonstrated. Curcumin and resveratrol were chosen as the test polyphenols due to their proven health benefits, and porous corn starch granules were chosen as the wall material. Porous corn starch granules were prepared through enzymatic modification with 11, 22, and 33 units of amyloglucosidase at three reaction times of 2, 4, and 6 h. The polyphenols were loaded at 100, 200, and 500 mg concentrations in 1 g of starch for 21 days and were characterized through Scanning Electron Microscope (SEM) and Fourier Transform Infrared spectroscopy (FTIR) analyses. The encapsulation efficiency was determined, the rate of starch digestion was calculated through the Englyst test, and polyphenols' in vitro release behavior in gastric and intestinal fluids was measured. Results suggest that 33 enzyme units for a 2 h reaction time were optimal for forming spherical-oval pores on corn starch granules with the maximum encapsulation efficiency of 80.16 % and 88.33 % for curcumin and resveratrol, respectively. The FTIR results suggest the entrapment of polyphenols inside the starch matrix. The inclusion significantly reduced starch digestion and increased the percentage of resistant starch up to 41.11 % and 66.36 % with curcumin and resveratrol, respectively. The in vitro release behavior demonstrated good stability in the simulated gastric fluids and sustained release in simulated intestinal fluids. The encapsulated polyphenols showed a complex Fickian type of diffusion mechanism. Overall, the results suggest that porous corn starch granules could be a potential delivery system for curcumin and resveratrol and will aid in developing novel functional foods to address the T2DM concerns.

Hydrocolloid-based nutraceutical delivery systems: Potential of κ-carrageenan hydrogel beads for sustained release of curcumin.

This study investigates the potential of κ-carrageenan hydrogel beads as a delivery system for curcumin, a bioactive compound with various health benefits. Hydrogel beads were prepared using the extrusion technique with a hypodermic needle. The encapsulation efficiency of curcumin in the κ-carrageenan hydrogel beads was found to be 74.61 ± 3.2 %. FTIR spectroscopy analysis revealed shifts in absorption peaks, indicating possible hydrogen bonding and/or ionic interactions between the polymer and salt. An increase in the melting point of curcumin, by 25 °C, in curcumin- κ-carrageenan beads suggests the heat protection offered by the carrageenan chains to curcumin molecules. The in vitro release of curcumin from the beads suggests a sustained and pH-dependent release nature. The release kinetics follow the first order and the Korsmeyer-Peppas model. The outcome offers value-added delivery systems of bioactive compounds toward developing novel food and pharmaceutical applications.

Corncob-derived biodegradable packaging films: A sustainable solution for raspberry post-harvest preservation.

Plastic food packaging, with its harmful migration of microplastics and nanoplastics into food, presents significant ecological imbalance and human health risks. In this regard, using food and agricultural byproducts as packaging materials reduces environmental and economic concerns and supports their sustainable management. Herein, cellulosic residue from corncob was employed as a renewable source for developing biodegradable packaging films. It was solubilized in ZnCl2 solution, crosslinked with Ca2+ ions, and plasticized with sorbitol to form films and used to improve the shelf-life of raspberries. The optimized film possesses water vapor permeability, tensile strength, and elongation at break of 1.8(4) x10-10 g-1 s-1 Pa-1, 4.7(1) MPa, and 15.4(7)%, respectively. It displays UV-blocking and antioxidant properties and biodegrades within 29 days at 24% soil moisture. It preserves raspberries for 7 and 5 more days at room temperature and refrigeration conditions, respectively, compared to polystyrene film. Overall, more value addition could be envisioned from agricultural residues to minimize post-harvest losses and food waste through biodegradable packaging, which also aids in mitigating plastic perils.

Biodegradable films from the lignocellulosic fibers of wheat straw biomass and the effect of calcium ions.

Plastics are hazardous to human health, and plastic waste results in environmental pollution and ecological catastrophe. Biobased polymers from renewable sources have recently become promising for developing biodegradable packaging films. Among them, lignocellulosic residue from agricultural biomass is inexpensive, renewable, and biodegradable. This study aims to develop biodegradable films using lignocellulosic residue from wheat straw biomass. The methodology is a green process that solubilizes lignocellulosic chains using Zn2+ ions and crosslinks with Ca2+ ions of different concentrations (200-800 mM). The results reveal that the increase of Ca2+ ions significantly decreases moisture content, water solubility, water vapor permeability, transparency, and elongation of films. The tensile strength is recorded as 6.61 ± 0.07 MPa with the addition of 800 mM of CaCl2, which is approximately 2.5 times higher than commercial polyethylene films. Around 90 % of films biodegrade within a month in soil containing 20 % moisture content. Overall, lignocellulosic residue from wheat straw biomass could be an excellent replacement for synthetic polymer to fabricate strong, transparent, and biodegradable plastic films.

Biodegradable, UV-blocking, and antioxidant films from lignocellulosic fibers of spent coffee grounds.

Plastics are strong, flexible, and inexpensive and hence desirable for packaging. However, as they biodegrade very slowly, their waste remains a global burden and pollution, warranting a search for safer alternatives. Towards this end, residual fibers from biowaste, such as spent coffee grounds (SCGs), stand out for creating biodegradable packaging materials. Herein, lignocellulosic fibers from SCG were extracted, and various amounts (0.6, 0.8, 1.0, and 1.2 g) were solubilized using 68 % ZnCl2 and crosslinked with salt (CaCl2) amounts 0.1, 0.2, 0.3 and 0.4 g and prepared biodegradable films. The films were characterized for their color, thickness, moisture content, tensile strength, elongation at break, water vapor permeability, transmittance of electromagnetic radiation, biodegradability, and antioxidant properties. The results reveal that the films possess the highest tensile strength of 26.8 MPa. The tensile strengths are positively correlated to salt and SCG extract amounts. The percentage of elongation decreased with an increase in the calcium ions but increased with SCG residue increment. The films biodegraded in the soil, and most lost >80 % of their initial weight in 45 and 100 days, respectively, at 30 % and 12 % soil moisture. Biodegradability and water vapor permeability decreased with an increase in salt content. Films also showed antioxidant properties and blocked UV and IR radiation significantly. Overall, this research involving green and recyclable chemicals in preparation of SCG residue fibers is a promising, economical, and sustainable route to produce strong biodegradable films to replace petrochemical plastics and thus is an attractive contribution to the circular bioeconomy.

Complexing curcumin and resveratrol in the starch crystalline network alters in vitro starch digestion: Towards developing healthy food materials.

Starch is an abundant and common food ingredient capable of complexing with various bioactive compounds (BCs), including polyphenols. However, little information is available about using native starch network arrangement for the starch-BCs inclusion. Herein, two BCs, curcumin, and resveratrol, were undertaken to delineate the role of different starch crystalline types on their encapsulation efficiency. Four starches with different crystalline types, botanical sources, and amylose content were examined. The results suggest that B-type hexagonal packing is necessary to encapsulate curcumin and resveratrol successfully. The increase in XRD crystallinity while maintaining the FTIR band at 1048/1016 cm-1 suggests that BCs are likely entrapped inside the starch granule than attaching to the granule surface. A significant change in starch digestion is seen only for the B-starch complexes. Embedding BCs in the starch network and controlling starch digestion could be a cost-effective and valuable approach to designing and developing novel starch-based functional food ingredients.

Role of metal chlorides in the gelation and properties of fucoidan/κ-carrageenan hydrogels.

Metal ions play a crucial role in forming hydrogels, and their effects on fucoidan (FUC): κ-carrageenan (KC) mixed gels were investigated. The results indicated that the FUC: KC mixed gels (FC) were promoted by K+ and Ca2+ but destroyed by Fe3+. The gel strength of FC was enhanced by K+ and Ca2+, with G' and G″ being highest at 50 mmol/L KCl and 25 mmol/L CaCl2, respectively. Water mobility was weakened after the addition of KCl and CaCl2 in accordance with the decrease in T23 relaxation time (free water, 100-1000 ms). After addition of KCl and CaCl2, the FC groups presented a typical three-dimensional network structure in contrast to the lamellar, disordered, and broken structure of FUC. Moreover, the FT-IR spectrum certified the enhancement of hydrogen bonds and the occurrence of electrostatic interactions during gel formation by the red-shift of the OH stretching vibration of the Ca2+ group and the blue-shift of the COS vibrations. The XRD results confirmed that the binding of Ca2+ to FC was tighter than that of K+ at the same charge content. These results provide a theoretical basis for understanding the interaction mechanism of FC with metal ions.

Preparation and characterization of corn flours with variable starch digestion.

Several grains such as wheat, rice, corn, oat, barley and rye are cultivated throughout the world. They are converted to variety of food products using a multitude of processing technologies to quench the growing organoleptic demands and consumers' preferences. Among them, corn, ranking third in wide consumption, is cost-effective and has long-term storability. Herein, ready-to-eat corn flours with variable starch digestion have been developed by processing at high temperature with shear using a twin screw continuous processor. The influence of processing temperature (121, 145 and 160°C) and moisture (25, 30 and 35%) has been studied. Results suggest both processing temperature and moisture modulate the rapidly digestible starch (RDS), slowly digestible starch (SDS) and resistant starch (RS) amounts of the flours. The presence or absence of oil in the flour further controls the starch digestion. The outcome is deemed to be helpful to design and develop healthy and palatable functional food products in addition to furthering the current market share for corn and other grains.

Lignin Nanoparticles and Alginate Gel Beads: Preparation, Characterization and Removal of Methylene Blue.

A novel and effective green system consisting of deep eutectic solvent (DES) was proposed to prepare lignin nanoparticles (LNPs) without any lignin modification. The LNPs are obtained through the dialysis of the kraft lignin-DES solution. The particle size distribution, Zeta potential and morphology of the LNPs are characterized by using dynamic light scattering (DLS), scanning electron microscopy (SEM) and transmission electron microscopy (TEM). The average diameter of LNPs is in the range 123.6 to 140.7 nm, and the LNPs show good stability and dispersibility in water. The composite beads composed of LNPs and sodium alginate (SA) are highly efficient (97.1%) at removing methylene blue (MB) from the aqueous solution compared to 82.9% and 77.4% by the SA/bulk kraft lignin composite and pure SA, respectively. Overall, the LNPs-SA bio-nanocomposite with high adsorption capacity (258.5 mg/g) could be useful in improving water quality and other related applications.

Starch digestibility and ß-carotene bioaccessibility in the orange- fleshed sweet potato puree-wheat bread.

Vitamin A is essential for vision, human health, growth, immune function, and reproduction. Its deficiency leads to anemia, xerophthalmia, and growth reduction in children. Foods enriched with naturally occurring carotenes have the potential, in this regard, and orange-fleshed sweet potato (OFSP) stands out tall as it is rich in ß-carotene (ßC), a provitamin A carotenoid. In view of developing OFSP-based functional foods to address the vitamin A deficiency (VAD) issues, herein, OFSP puree-wheat composite breads have been prepared at 10% to 50% OFSP puree concentrations and bioaccessibility of ßC has been estimated. The total ßC is found to be 4.3, 9.2, 16.5, 23.3, and 33.6 µg/g in 10, 20, 30, 40, and 50% OFSP bread, respectively. The corresponding calculated retinol activity equivalents (RAE) are 30.9, 66.4, 119.5, 170.4, and 246.2 RAE/100 g. The efficiency of micellarization of all-trans-ßC, 13-cis ßC, and 9-cis ßC after simulated oral, gastric, and small intestinal digestion are 1.4% to 6.4%, 1.4% to 7.2%, and 1.1% to 6.9%, respectively. The amount of micellarized ßC correlates linearly with the OFSP concentration in the bread. Furthermore, in vitro starch digestion decreases with significant reduction in the Rapidly Digestible Starch (RDS) amount coupled with increase in the Slowly Digestible Starch (SDS) and Resistant Starch (RS) fractions. Overall, OFSP-wheat composite bread holds adequate amount of provitamin A carotenoids. The amount of bioaccessible ßC coupled with altered starch digestion of the OFSP wheat breads highlight their usefulness as novel functional foods that could address the VAD as well as glycemic issues toward improving human health.

Fucoidan hydrogels induced by κ-carrageenan: Rheological, thermal and structural characterization.

Fucoidan (FUC) is a non-gelling polysaccharide but could interact with κ-carrageenan (KC) to form a stable gel blend. However, their interaction mechanism is unclear. Herein, FUC and KC blended gels are prepared by mixing FUC (10 and 20 mg/mL) and KC (6, 7 and 8 mg/mL) solutions, and characterized through LF-NMR, rheology, DSC, Cryo-SEM, and FTIR. The FTIR analysis confirms the formation of hydrogen bonds between FUC and KC chains. The KC addition to FUC significantly improves the water retention and frost resistance. The viscoelastic measurements reveal higher gelling nature of the FUC-KC binary mixtures, and the DSC results confirm the higher thermal stability. The Cryo-SEM images clearly reveal the gel network structure. The outcome of this study deemed to further the FUC use in food and non-food applications.

The functionality of laccase- or peroxidase-treated potato flour: Role of interactions between protein and protein/starch.

Potato flour is used in bakery products, extruded products and snacks. However, it displays weaker gel strengths and thus the wholesome utility is curtailed significantly. To improve viscoelastic properties and stability of potato gels, herein potato flour was treated with laccase and peroxidase to create a protein network structure leading to stable gels. The results revealed that the secondary structure of potato proteins altered upon the enzyme treatment. The gels of peroxidase-treated potato flour (PPF) and laccase-treated potato flour (LPF) displayed larger anti-shear ability, thermal stability and stronger three-dimensional network structure compared to the native potato gel. The PPF and LPF gels exhibited stronger viscoelastic properties and structural stability compared to peroxidase-treated potato protein and laccase-treated potato protein gels. The outcome serves as a theoretical basis to improve the properties of potato gels and to promote the designing and the development of novel potato flour based functional food.

Innovative production of lignin nanoparticles using deep eutectic solvents for multifunctional nanocomposites.

A green and simple lignin nanoparticles (LNPs) production strategy was developed using deep eutectic solvents (DES). The LNPs were formed with corncob alkali lignin by sequential DES dissolution and self-assembling process. Uniform size and spherical shape of LNPs were observed by scanning electron microscopy (SEM), transmission electron microscopy (TEM), dynamic light scattering (DLS), zeta potential analyzer and gel permeation chromatography (GPC). Less than 100 nm of LNPs were formed, and these particles were preserved without significant size-increase or precipitation within 30 days. The nanocomposite films prepared by incorporating the LNPs into biodegradable poly(vinyl alcohol) (PVA) matrix display good mechanical properties (tensile strength of 82.5 MPa and breaking strain of 103.3%), excellent UV-blocking (100% shielding of the UV spectrum region), strong hydrophobicity (static contact angle of 117.0°) and relatively high thermal stability (the maximum thermal weight loss temperature increased by 40 °C). Overall, this study not only facilitates the advancement of lignin-based nanotechnology by DES but also paves the way for the PVA polymer composites as potential food and medical packaging materials.

Comparison of functional properties of porous starches produced with different enzyme combinations.

To obtain porous starch granules with higher absorption capacities, three types of enzyme combinations were adopted to modify wheat and maize starches: (1) sequential α-amylase (AA) â†’ glucoamylase (GA); (2) sequential branching enzyme (BE) â†’ GA; and (3) sequential AA→BE→GA. The results indicated that AA→BE→GA treatment had a most optimal influence on porous starches. Compared to AA→GA and BE→GA, the mesopores in wheat starch granules treated with AA→BE→GA decreased by 52.82 and 48.70%, respectively. Conversely, the macropores increased by 216.68 and 138.18%, respectively. While for maize starch, the percentages of mesopores and macropores hardly changed after three enzyme combinations. Comparing the three enzyme treatments showed that pore volume (0.005 and 0.007 cm3/g) and pore size (36.35 and 26.54 nm) were largest in the AA→BE→GA treated wheat and maize starches, respectively. Compared to the AA→GA and BE→GA, the adsorption capacities for oil, dye and heavy metal ions, wheat starch treated with AA→BE→GA increased by 46.61 and 242.33%, and 44.52 and 134.41%, and 28.83 and 271.72%, respectively. Correspondingly, that of maize starch increased by 29.71 and 133.29%, and 42.92 and 79.93%, and 28.16 and 161.43%, respectively. These results may provide a new and valuable enzyme combination for optimising porous starch granules with higher absorption capacities.

Further insights into the evolution of starch assembly during retrogradation using SAXS.

A new and effective method for evaluating the reassembly of starch molecules at large scale (>2 nm) during retrogradation has been developed based on the small angle X-ray scattering (SAXS) technique. The SAXS curves fitted by the Cauchy plus Power-law functions are decomposed into peak- and non-peak-derived sub-patterns. The peak-derived patterns are used for calculating (i) the size of ordered aggregate structures (d) using Lorentz correction and (ii) the proportion of ordered structures within starch samples (Rpeak) by estimating the ratio of the area under the peak-derived sub-pattern (Speak) to the total area under SAXS curve. The Imax and fractal-like dimension (α) of the scattering aggregates (the fitted parameters of SAXS curve), d, Speak, Snon-peak (the area under the non-peak-derived sub-pattern) and Rpeak change as a function of retrogradation time. Importantly, the Snon-peak interrogates the continuous reduction of amorphous starch molecules during the aging, SAXS parameters including α and d describe starch ordered aggregate structures with larger scale than 2 nm are fitted well with pseudo Avrami equation. The SAXS in this study can be used to unravel the evolution of both amorphous starch structures and ordered aggregates with larger scale during retrogradation.