The persistent gap between hemostasis and tissue repair in wound care demands new biomaterials. To address this, we engineered an electrospun polysaccharide-based multilayer composite nanofiber membrane (MCNM) designed t...The persistent gap between hemostasis and tissue repair in wound care demands new biomaterials. To address this, we engineered an electrospun polysaccharide-based multilayer composite nanofiber membrane (MCNM) designed to transform early blood clots into bioactive, pro-regenerative interfaces. The MCNM integrates distinct carbohydrate polymer functionalities: a wound-contacting layer of pullulan/tannic acid/tranexamic acid nanofibers for hemostasis and fibrinolysis suppression; a polydopamine/CaCl-modified cellulose acetate intermediate layer for platelet adhesion and fibrin nucleation; and a chitosan-composited cellulose spunlace backing for directional exudate management. When applied, this structure quickly concentrates blood to create a stable clot that acts as both hemostatic barrier and reservoir or regenerative factors. Proteomic analysis confirmed significant upregulation of extracellular matrix organization, focal adhesion, and actin cytoskeleton remodeling pathways within the clot microenvironment. In vivo, the MCNM accelerated wound closure, improved re-epithelialization and collagen deposition, and promoted anti-inflammatory macrophage polarization. This work establishes an example for leveraging polysaccharide-driven clot bioengineering to seamlessly bridge hemostasis and tissue regeneration in advanced wound care.
Spinal cord injury (SCI) causes severe neurological deficits and remains difficult to treat with current strategies such as surgical decompression or corticosteroids, which offer limited benefits. Hydrogels represent a p...Spinal cord injury (SCI) causes severe neurological deficits and remains difficult to treat with current strategies such as surgical decompression or corticosteroids, which offer limited benefits. Hydrogels represent a promising alternative because they provide structural support and serve as therapeutic carriers. Quaternized chitosan (QCS), a derivative of chitosan, shows improved solubility and anti-inflammatory properties but lacks crosslinking ability and degrades rapidly, restricting its application in SCI. To overcome these limitations, we introduced methacrylate groups into QCS (QCS-MA), enabling photo-crosslinking, faster gelation, and enhanced mechanical stability while preserving bioactivity. QCS-MA was blended with type I collagen to form an interpenetrating hydrogel (QCS-MA/COL) through hydrogen bonding, then loaded with progranulin (PGRN), a multifunctional growth factor known to promote neuronal survival and modulate immune responses. The resulting PGRN@QCS-MA/COL hydrogel displayed favorable mechanical properties, injectability, and biocompatibility, while inducing macrophage polarization toward a reparative M2 phenotype. In a mouse SCI model, it significantly improved motor recovery, reduced lesion cavity formation, attenuated chronic inflammation, and enhanced axonal and neural regeneration. These findings highlight the potential of QCS-MA as a tunable immunomodulatory delivery platform, synergizing with PGRN and collagen to provide a biomimetic strategy for neural repair.
Aharodnikau UE, Kisliuk MV, Yedchyk AV
… +11 more, Pristromova YI, Bychkovsky PM, Salamevich DA, Cai Y, Sun Y, Shauchenka MA, Panibrat AV, Pavalanski EI, Yurkshtovich TL, Jiang G, Solomevich SO
Phosphorylated polysaccharides are emerging as biodegradable, biocompatible and hydrogel-forming materials with growing relevance in biomedical applications, yet controlled phosphorylation of pullulan and the resulting s...Phosphorylated polysaccharides are emerging as biodegradable, biocompatible and hydrogel-forming materials with growing relevance in biomedical applications, yet controlled phosphorylation of pullulan and the resulting structure-property relationships remain insufficiently explored. Here, pullulan was phosphorylated in a multicomponent organic system containing tributyl phosphate, orthophosphoric acid, phosphorus pentoxide and chloroform, yielding water-soluble and hydrogel-forming derivatives with phosphorus contents from 1.2 to 19.9 wt%. FTIR, H/C/P NMR, GPC, SEM, rheology and TGA/DSC showed that increasing phosphorylation enabled tuning of swelling capacity (1.6-370 g/g) and viscoelastic properties, with storage moduli up to 40 kPa, while shifting the onset of thermal degradation from ∼320 °C (native pullulan) to 180-240 °C and increasing the residual mass at 600 °C to 69%. Enzymatic degradation with pullulanase (pH 6.9, 37 °C) led to complete loss of low-phosphorus soluble derivatives within 3 days, whereas crosslinked hydrogels retained approximately 30% and 10% of their mass after 7 days, depending on network density. All derivatives induced <2% hemolysis and maintained ≥80% fibroblast viability at concentrations up to 2 mg/mL. Collectively, these findings demonstrate that multicomponent phosphorylation affords pullulan derivatives with tunable composition, mechanics, degradation behavior and in vitro biocompatibility, highlighting their potential for drug delivery, wound dressings and soft tissue engineering.
Hydrogels have garnered considerable attention in wearable devices due to their tunable mechanical properties. However, their applications are constrained by limited conductivity and inadequate freeze-resistance. In this...Hydrogels have garnered considerable attention in wearable devices due to their tunable mechanical properties. However, their applications are constrained by limited conductivity and inadequate freeze-resistance. In this study, we develop a physical-chemical dual network eutectogel (PECA/CMC) through a synergistic enhancement strategy combining the multiple hydrogen bonds of carboxymethyl cellulose sodium (CMC) with metal-ion coordination within a deep eutectic solvent (DES). The eutectogel incorporates a physically cross-linked CMC network with a chemically cross-linked polyacrylamide (PAM) network via multiple non-covalent interactions (e. g., hydrogen bonds) and covalent bonds formed through free-radical polymerization. PECA/CMC eutectogel exhibits superior mechanical properties, a fracture toughness (29.22 kJ·m) and a high tensile stress (23.8 kPa). Owing to the carboxyl-metal ions coordination and the freezing-point depression effect of DES, the eutectogel maintains a high conductivity of 0.35 S·m at -20 °C. When employed as an electrolyte in a supercapacitor, it exhibits stable cycling performance, retaining 79.4% of its initial capacitance and a Coulombic efficiency of 92.3% after 2000 cycles. As a strain sensor, the eutectogel achieves a gauge factor (GF) of 1.06 over a range of 40-200%. This work introduces a sustainable synergistic design strategy for multifunctional eutectogel suitable for flexible electronic devices under extreme conditions.
Cellulose shows limited solubility in conventional solvents due to its strong hydrogen-bonding network. Ionic liquids (ILs) are promising alternatives, yet the role of aryl substituent flexibility remains unclear. Here,...Cellulose shows limited solubility in conventional solvents due to its strong hydrogen-bonding network. Ionic liquids (ILs) are promising alternatives, yet the role of aryl substituent flexibility remains unclear. Here, two aryl- and benzyl-functionalized ILs-1-benzyl-3-methylimidazolium benzylphosphonate ([CBnzIm][P-Bnz]) and 1-phenyl-3-methylimidazolium phenylphosphonate ([CPhIm][P-Ph])-were synthesized with matched substituents on both ions. The benzyl-substituted IL exhibited superior cellulose dissolution, attributed to enhanced flexibility and stronger ion-cellulose interactions. COSMO-RS analysis revealed higher hydrogen-bond basicity and more favorable polarity interactions for this system. The best-performing IL was further evaluated with co-solvents, where dimethyl sulfoxide outperformed 1-methylimidazole. Variations in viscosity and ionic conductivity correlated well with cellulose dissolution efficiency. Characterization of regenerated cellulose by FTIR, XRD, SEM, and TGA confirmed successful dissolution and structural modification.
This study proposed an acid-assisted lignin enrichment strategy for the preparation of high-lignin cellulose nanofibrils (HLCNF, defined here as lignin-containing CNFs with lignin contents exceeding that of the native fe...This study proposed an acid-assisted lignin enrichment strategy for the preparation of high-lignin cellulose nanofibrils (HLCNF, defined here as lignin-containing CNFs with lignin contents exceeding that of the native feedstock). Through dilute sulfuric acid pretreatment of the applewood sample, hemicellulose and amorphous cellulose were preferentially removed, progressively increasing the relative lignin fraction from 23% in the raw material to ∼60%. The lignin-enriched substrate, together with the pretreatment-induced matrix loosening, facilitated fiber dissociation and enabled efficient mechanical fibrillation, resulting in nanofibrils with average diameters of 11.5-13.5 nm. Further characterization revealed that surface-associated lignin promoted markedly improved thermal stability, enhanced organic solvent compatibility, excellent ultraviolet absorption and hydrophobicity of the resulting HLCNF. As a performance demonstration, HLCNF was coated onto paper surfaces. The more hydrophobic and compact HLCNF coating enabled the paper substrate to achieve excellent barrier performance. Under optimized conditions (20 g/m coating content with hot-pressing), the coated paper showed a Cobb value of 3.3 g/m, a WVTR of 12.1 g/(m·d), and no detectable edible oil penetration. This work provided a framework for elevating lignin fractions beyond the native level while retaining a nanofibrillar network and contributing to the development of a sustainable bio-based material.
Developing low-cost, high-efficiency, and reusable absorbents for oil spill remediation is critical yet challenging. In this work, an eco-friendly and facile approach was implemented to construct ultralight cattail fiber...Developing low-cost, high-efficiency, and reusable absorbents for oil spill remediation is critical yet challenging. In this work, an eco-friendly and facile approach was implemented to construct ultralight cattail fiber/cellulose composite cryogels (CF/CNF-CGs) through freeze-drying and silane-based functionalization. The resulting CF/CNF-CGs possessed a hierarchical porous architecture with ultralow density (5.84-6.47 mg/cm) and ultrahigh porosity (99.55-99.58%). The hydrophobic cryogels (water contact angle up to 149.1°) demonstrated exceptional oil absorption capacities (109.2-121.4 g/g), retention (95.6%) capacity and excellent selective sorption property. Moreover, CF/CNF-CGs exhibited good reusability, retaining an oil absorption capacity of 82.0 g/g and oil-water separation efficiency of 99.6% after 10 cycles. The adsorption behavior of CF/CNF-CGs was quantitatively analyzed using quasi-first, quasi-secondary, and intraparticle diffusion models, which indicated that the adsorption of oil by cryogel was predominantly governed by physisorption driven by capillary action and pore filling, and involved both surface and internal diffusion mechanisms. These superior properties underscore the potential of CF/CNF-CGs as a promising and sustainable alternative for large-scale maritime oil cleanup.
Cartilage degradation after joint injury often leads to post-traumatic osteoarthritis, a process accompanied by a drop in synovial pH. Traditional dynamically crosslinked hydrogels overlook how their mechanical and tribo...Cartilage degradation after joint injury often leads to post-traumatic osteoarthritis, a process accompanied by a drop in synovial pH. Traditional dynamically crosslinked hydrogels overlook how their mechanical and tribological properties change in such acidic, inflammatory environments. Here, we report an arthritis-responsive, injectable hydrogel designed to both regenerate articular cartilage and inhibit its further degradation. The hydrogel is formed via Schiff base chemistry between aldehyde groups of oxidized hyaluronic acid (OHA) and amino groups of adipic acid dihydrazide-grafted chondroitin sulfate (Chs-ADH) and carboxyethyl chitosan (CEC). Under neutral pH, the imine bonds remain stable, allowing precise defect filling and minimizing stress-induced debris; under acidic conditions, their reversible nature enhances lubrication and resists wear. The hydrogel formulation was optimized using molecular dynamics simulations to achieve excellent injectability, shear-thinning behavior, and low friction without impeding normal joint motion. In vitro, the hydrogel exhibited outstanding biocompatibility and stimulated cell migration. In vivo, it accelerated cartilage repair, prevented cartilage degradation, and restored the lubrication of newly formed tissue to levels comparable with healthy cartilage. Together, these findings demonstrate that the pH-sensitive hydrogel is a promising candidate for effective cartilage repair and prevention of cartilage degradation.
Octenyl succinic anhydride (OSA) starch is a prominent particle stabilizer for Pickering emulsions, yet it often fails to protect polyunsaturated lipids effectively due to its lack of intrinsic antioxidant activity and t...Octenyl succinic anhydride (OSA) starch is a prominent particle stabilizer for Pickering emulsions, yet it often fails to protect polyunsaturated lipids effectively due to its lack of intrinsic antioxidant activity and the uneven distribution of interfacial hydrophobic groups. We hypothesized that quercetin's (QR) hydrophobic nature would allow it to assemble with OSA-modified adlay seed starch (OSA-ASS), thereby improving emulsifying properties and providing antioxidant capacity. To verify this hypothesis, we prepared OSA-ASS/QR complexes containing 0.5%-3.5% QR to stabilize walnut oil emulsions. The interaction mechanisms were elucidated via fluorescence spectroscopy, isothermal titration calorimetry (ITC), and molecular dynamics (MD) simulations. The results revealed that QR spontaneously bound to OSA-ASS, an entropy-driven process dominated by hydrophobic interactions, while hydrogen bonding and van der Waals forces provided structural specificity and supplementary enthalpic stabilization. The 2.5% QR complex facilitated the formation of a compact interfacial barrier that restricted water mobility. Ultimately, the system achieved dual protection: the dense physical barrier hindered pro-oxidant permeation, while interfacial QR chemically scavenged free radicals. These findings clarify the entropy-driven assembly of starch-polyphenol complexes, offering a robust strategy for encapsulating unsaturated oils.
Bacterial cellulose (BC) has emerged as a promising sustainable material for food packaging due to its biocompatibility, high mechanical strength, and versatile functionalization capability. However, its inherent lack of...Bacterial cellulose (BC) has emerged as a promising sustainable material for food packaging due to its biocompatibility, high mechanical strength, and versatile functionalization capability. However, its inherent lack of antimicrobial and antioxidant properties, together with its hydrophilic nature, limits its protective efficacy and broader practical application in food preservation. Covalent grafting offers a powerful approach to overcome these drawbacks by permanently anchoring functional agents onto BC, thereby boosting its food preservation capabilities. In this review, we discuss various covalent modification strategies for immobilizing active compounds - including biocidal agents, antioxidants, and hydrophobic agents - onto the BC structure. These modifications address key challenges of BC films in food packaging such as microbial and oxidative spoilage and moisture sensitivity. Representative examples are highlighted in which covalently modified BC has been successfully employed to extend the shelf-life of foods. Antimicrobial modifications can achieve >95% pathogen inactivation; hydrophobic agents such as silanes increase contact angles to 150°; antioxidant functionalization with dopamine enables 90% radical scavenging. Modified BC extends the shelf life of fruits and meat by 10-14 days with minimal impact on BC's biodegradability.
Ulcerative colitis (UC) is a chronic inflammatory bowel disease for which effective and durable therapeutic strategies remain limited. In this study, an acetylated glucomannan polysaccharide, Aloe barbadensis polysacchar...Ulcerative colitis (UC) is a chronic inflammatory bowel disease for which effective and durable therapeutic strategies remain limited. In this study, an acetylated glucomannan polysaccharide, Aloe barbadensis polysaccharide 7 (ABPA7), was isolated and purified from the gel of Aloe barbadensis with a purity of 97.65%. Structural characterization revealed that ABPA7 is a highly homogeneous β-(1 → 4)-linked mannan, low branching, site-specific O-acetylation at the O-2/O-2,3 positions, and a high molecular weight of approximately 647 kDa. Functionally, ABPA7 markedly alleviated disease severity in a dextran sulfate sodium (DSS)-induced mouse colitis model. Mechanistic investigations demonstrated that ABPA7 reinforced intestinal barrier integrity by restoring tight junction protein expression and suppressing pro-inflammatory cytokine production. In parallel, ABPA7 was associated with alterations in gut microbiota composition and microbial metabolic networks. Transcriptomic analyses further indicated that ABPA7 upregulates the extracellular matrix (ECM) related gene expression of the intestinal. Collectively, these findings support the involvement of a coordinated "microbiota-metabolism-host" regulatory framework underlying the anti-colitis effects of ABPA7, encompassing inflammation attenuation, barrier reinforcement, and controlled ECM remodeling. This study underscores the therapeutic potential of structurally defined aloe polysaccharides and provides a mechanistic reference for the rational development of polysaccharide-based interventions for ulcerative colitis.
Understanding how molecular architecture dictates the bioactivity of functional oligosaccharides remains a major challenge. Here, mannan oligosaccharides (MOS) were prepared from yeast cell wall mannan, and Gleditsia sin...Understanding how molecular architecture dictates the bioactivity of functional oligosaccharides remains a major challenge. Here, mannan oligosaccharides (MOS) were prepared from yeast cell wall mannan, and Gleditsia sinensis Lam. endosperm galactomannan, to investigate structure-function relationships in preventing inflammatory bowel disease. The protective effects of yeast-derived MOS (Y-MOS) and Gleditsia-derived MOS (G-MOS) were comparatively evaluated using a dextran sodium sulfate (DSS)-induced colitis mice model. Structural analysis revealed that Y-MOS primarily consisted of α-1,6 linked mannose with α-1,2/α-1,3 linked side chains, whereas G-MOS featured a β-1,4 linked mannose backbone with α-1,6 linked galactose branches. Furthermore, both MOSs mitigated colitis symptoms, preserved colonic epithelial barrier integrity, and suppressed inflammatory cytokines, primarily through suppressing JAK2-STAT3 and NF-κB signaling pathways, regulating gut microbiota, and promoting short-chain fatty acid production. Notably, G-MOS was more effective than Y-MOS, particularly in immune regulation and modulation of gut microbiota. Molecular docking further revealed that the rigid β-linked conformation of G-MOS exhibited stronger binding affinity toward inflammatory receptors, leading to more effective pathway inhibition, as validated in LPS-treated RAW264.7 cells. These findings elucidate a glycosidic topology-dependent molecular mechanism underlying MOS bioactivity, and identify β-linked G-MOS as a promising, sustainable candidate for inflammation management.
Fructans play important roles in plant physiology and have been reported to have several technological applications. They are complex fructose oligo- and polysaccharides with varying Degrees of Polymerization (DPs) and b...Fructans play important roles in plant physiology and have been reported to have several technological applications. They are complex fructose oligo- and polysaccharides with varying Degrees of Polymerization (DPs) and branching types. These features have made it difficult to determine the structure of the plant's different isomers. This work introduces a combined experimental and computational approach, in which we compare experimentally derived Collision Cross-Section (CCSe) values with a computationally generated CCS (CCSt) database of potential fructans based on reported characteristics. We identified 34 CCSe values corresponding to fructans up to DP12, of which 24 (70%) matched entries in the CCSt database with an average error of 0.29%, and were successfully assigned a structure. This approach offers promising possibilities for analysing different molecules and sample types.
Parkinson's disease (PD) is characterized by progressive dopaminergic neuron loss, chronic neuroinflammation, and α-synuclein aggregation. Blood-brain barrier (BBB)-penetrable, dual-target nanomedicines for microglial in...Parkinson's disease (PD) is characterized by progressive dopaminergic neuron loss, chronic neuroinflammation, and α-synuclein aggregation. Blood-brain barrier (BBB)-penetrable, dual-target nanomedicines for microglial inflammation and neuronal degeneration remain challenging. In this study, we fabricated a brain-targeted, pH- and reactive oxygen species (ROS)-responsive nanogel (NG) platform using dextran (Dex) as the main polysaccharide backbone, crosslinked with inflammation-targeting fibronectin (FN), and loaded with neuroprotective quercetin (Que). Dex-FN/Que NGs exhibited a uniform spherical morphology with an average diameter of 187 nm, favorable colloidal stability, and stimuli-triggered drug release behavior. Abundant hydroxyl groups on Dex enabled efficient BBB penetration, while FN mediated integrin-dependent internalization in microglia and neurons. These NGs suppressed the nuclear factor-kappa B (NF-κB) signaling pathway, scavenged ROS, promoted favorable microglial polarization, and balanced oxidative stress. Meanwhile, mitophagy flux activated by the NGs in neurons exerted strong neuroprotection effect. In a mouse model of PD, Dex-FN/Que NGs effectively crossed the BBB and accumulated in injured brain regions, significantly protecting dopaminergic neurons, improving motor function, and relieving depressive-like behaviors. Therapeutic benefits arose from normalized microglial polarization, reduced oxidative stress, and inhibited neuronal ferroptosis. This Dex-based stimuli-responsive nanoplatform provides a promising brain-targeted strategy for the treatment of PD and other neurological disorders.
Starch nanofibers hold promise for food-packaging but scalable production is hindered by limited spinnability understanding and conventional spinning challenges. Here, solution blow spinning (SBS) was employed to fabrica...Starch nanofibers hold promise for food-packaging but scalable production is hindered by limited spinnability understanding and conventional spinning challenges. Here, solution blow spinning (SBS) was employed to fabricate nanofibers from pure high-amylose starches (HI55 and HI70, with 56% and 72% amylose content, respectively) dissolved in aqueous NaOH, as model systems. Quantitative spinnability windows (non-spinnable, C < C, overlap; onset, C < C < C; stable, C > C, entanglement) were quantitatively established by correlating fiber morphology with rheological transitions. Stable fibers formed only at C > C, where sufficiently entangled starch chains formed a viscoelastic network capable of sustaining flow-induced extensional deformation under the combined shear and stretching fields of SBS. The transition from the non-spinnable regime to stable spinnability was accompanied by coordinated rheological responses, including increased consistency index, zero-shear viscosity, critical strain, and structural viscosity index, together with reduced non-Newtonian index, modulus-frequency dependence, and surface tension. In addition, fiber diameter scaled with both surface tension and C/C, highlighting the coupled roles of interfacial effects and chain entanglement in fiber morphology. Compared with HI55, HI70 exhibited superior spinnability at lower concentrations due to greater amylose-induced chain entanglement.
Acetylated mannan (PTPS-W-2) was isolated from Typha angustifolia Pollen through hot-water extraction followed by ion-exchange and size-exclusion chromatography. Structural characterization indicated that PTPS-W-2 is a h...Acetylated mannan (PTPS-W-2) was isolated from Typha angustifolia Pollen through hot-water extraction followed by ion-exchange and size-exclusion chromatography. Structural characterization indicated that PTPS-W-2 is a homogeneous polysaccharide with an average molecular weight of approximately 42 kDa, composed exclusively of mannose residues. The backbone consists predominantly of →4-β-Manp-(1→4)-β-Manp-(1→ linkages, with partial O-acetyl substitution at the C-2 and C-3 positions. Notably, this represents the first report of isolating a plant-derived acetylated mannan with a high degree of purity and structural homogeneity. In vivo administration for two weeks demonstrated that PTPS-W-2 selectively modulated the gut microbiota community by significantly enriching Lactobacillus johnsonii and enhancing intestinal phenyllactic acid production, which was further confirmed using an in vitro monoculture fermentation model. Notably, deacetylated PTPS-W-2 exhibited a markedly weaker growth-promoting effect on L. johnsonii. Comparative physicochemical analyses further showed that deacetylation markedly reduced the aqueous solubility of the mannan. These findings suggest that acetylation-associated structural and physicochemical features, particularly those related to hydration and substrate accessibility, may contribute to the microbial responsiveness of PTPS-W-2. Overall, this study highlights the potential importance of acetylation-associated structural features in shaping the physicochemical properties and microbiota-modulating behavior of plant-derived mannans, providing new insights into their structure-property-function relationships.
β-glucan is a valuable polysaccharide that has garnered attention for its nutraceutical and diverse biological applications. The present study involved the pilot-scale cultivation of Euglena gracilis, followed by β-gluca...β-glucan is a valuable polysaccharide that has garnered attention for its nutraceutical and diverse biological applications. The present study involved the pilot-scale cultivation of Euglena gracilis, followed by β-glucan extraction, purification, characterization, and cytotoxicity assessment. The extracted β-glucan has a white, granular, discoidal shape with an erythrocyte-like appearance, and an average particle size of 3.15 ± 2.11 μm. The presence of β-linkage was evident from the occurrence of a band at 889.07 in the IR spectra. UV-Visible spectroscopy and the Congo red test showed that the extracted β-glucan is pure with a triple-helical structure. XRD spectra revealed the crystalline nature with clear peaks and varying amorphous content. The extracted β-glucan is linear, with β-1,3 linkages, and has a molecular weight of 480-500 kDa, as indicated by HPLC, NMR (H, C, COSY, HMBC, HMQC) GC-MS, and MALDI-TOF spectra. The MTT, Neutral Red Uptake (NRU), and Alamar Blue-based cytotoxicity studies on L929 (mouse fibroblast) cell line showed that the extracted β-glucan is safe and biologically non-toxic at concentrations up to 50 mg/mL. The present study established a basis for the production and extraction of β-glucan from microalgae at pilot scale, presenting opportunities for the commercialization of this important nutraceutical compound.
Herein, core-shell nanofibers loaded with α-linolenic acid (ALA), a highly unsaturated polyunsaturated fatty acid (PUFA) sensitive to oxygen, were fabricated by emulsion electrospinning using peanut protein isolate-pullu...Herein, core-shell nanofibers loaded with α-linolenic acid (ALA), a highly unsaturated polyunsaturated fatty acid (PUFA) sensitive to oxygen, were fabricated by emulsion electrospinning using peanut protein isolate-pullulan (PPI-PUL) Maillard conjugates as emulsion stabilizers. Emulsion electrospinning enables the encapsulation and provides a protective barrier and efficient delivery. This work aims to elucidate the relationship between the covalent grafting and emulsion interfacial viscoelasticity, lipid protection, and bioaccessibility. These results showed that the conjugates prepared at 80 °C (PU11H) exhibited the highest degree of grafting (13.48%), an emulsifying activity index of 462.89 m/g, and the smallest ALA droplet size (0.839 μm). These interfacial properties suppressed droplet mobility and delayed phase separation, so the bead-free nanofiber with a core-shell structure was obtained after electrospinning. PU11H achieved the highest encapsulation efficiency (>95%), and showed the lowest POV and TBARS among all samples after 9 days at 40 °C, confirming that higher grafting density improved the oxidative stability. In vitro digestion indicated that PU11H had a final bioaccessibility of 63.5% in the intestinal phase (vs 25.5% for free ALA). Overall, these findings indicate that controlling the degree of grafting of protein-Maillard conjugates offers facile strategies to enhance oxidative stability and intestinal delivery of PUFAs.
Bacterial cellulose (BC) is a high-purity, biodegradable polysaccharide commercialized in foods and promising for biomaterials. Yet BC composites face challenges achieving high yields with mechanical strength and thermal...Bacterial cellulose (BC) is a high-purity, biodegradable polysaccharide commercialized in foods and promising for biomaterials. Yet BC composites face challenges achieving high yields with mechanical strength and thermal stability. Here, we move beyond "add-a-polysaccharide" approaches by leveraging konjac glucomannan (KGM) acetylation as a design parameter coupling fermentation operability with BC-polysaccharide interfacial co-assembly. Partially deacetylated KGM (DKGM, deacetylation degree 30.37%) was prepared to reduce viscosity and incorporated into BC via one-step in situ fermentation, while physical-mixture controls (BC-KGM-M and BC-DKGM-M) distinguished simple mixing from co-deposition. Under identical conditions, DKGM alleviated viscosity limitations and increased BC yield by 16.9% vs KGM, whereas native KGM showed no gain. FT-IR deconvolution and solid-state NMR revealed strengthened hydrogen bonding via deacetylation and more intimate associations in in situ composites than in mixture controls, while XRD confirmed retention of the cellulose Iα crystalline form. As a result, BC-DKGM exhibited a more compact architecture, enhanced tensile strength (0.37 MPa; ∼236.36% over BC) and thermal stability, superior viscoelasticity and recovery upon thermal cycling/creep, and a more immobilized water population. These findings demonstrate that tuning KGM acetylation enables predictable process-structure-property control in BC-based composite hydrogels via one-step strategy, expanding BC's applications in food and biomedical fields.
Chitosans are versatile and promising functional biopolymers with diverse bioactivities that are strongly influenced by three characteristic structural parameters: the degree of polymerization (DP), the fraction of acety...Chitosans are versatile and promising functional biopolymers with diverse bioactivities that are strongly influenced by three characteristic structural parameters: the degree of polymerization (DP), the fraction of acetylation (F), and the pattern of acetylation (PA). However, limited understanding of these structure-function relationships and of the underlying mechanisms compromises reproducibility and effective applications. To address this, we have produced a set of 16 different chitosans from a single parent chitosan (DP 1237, F 0.01) yielding chitosans with defined DP and F, and random (Bernoullian) PA. We analyzed the antimicrobial activity of selected chitosans against four phytopathogens, Pseudomonas syringae pv. tomato, Clavibacter michiganensis, Fusarium graminearum, and Ustilago maydis, observing strong antimicrobial activities for all chitosans. Detailed analysis including more chitosans against P. syringae revealed no consistent trend linking a low F or a specific DP alone to enhanced antibacterial activity. Instead, the influence of F on antibacterial efficacy was dependent on DP, and vice versa. There seems to be a complex interplay between DP and F, and single-parameter interpretations seem insufficient. Further studies will have to show whether this conclusion can be generalized beyond P. syringae.