基于天然生物大分子与多酚分子识别作用的自组装纳米体系：温和制备、结构可调、生物相容、较少依赖化学交联等优势

In this work, natural biopolymeric encapsulation structures were developed through the self-assembly of gelatin and ι-carrageenan in aqueous solutions. The interactions of this binary system and of a ternary system containing a polyphenol-rich extract were deeply explored for the development of intestinal delivery systems. The processing of the structures (extrusion vs. freeze-drying) greatly influenced release properties, explained by the specific interactions between gelatin and polyphenols, thus allowing for tuning the processing conditions depending on the desired target application. Release was further controlled by incorporating a divalent salt, giving raise to extract-loaded ι-carrageenan/gelatin capsules with adequate release profiles for intestinal targeted delivery. These results demonstrate the potential of exploiting biopolymer interactions for designing bioactive delivery systems using environmentally friendly processes which do not involve the use of toxic or harsh solvents or cross-linkers.

The efficacy of growth factor delivery-based therapies for bone tissue regeneration is frequently undermined by oxidative stress, especially under inflammatory conditions, which results in structure damage and function inactivation of growth factors. Herein, a straightforward and universal protective delivery strategy is proposed by employing the multiple physical interactions between epigallocatechin-3-gallate (EGCG) and growth factors (e.g., neuregulin-1/NRG-1) to efficiently form self-assembled particles (NE APs). NE APs provide sustained release of NRG-1 while protecting it from oxidative damage, preserving its biological functions of cell recruitment, migration, and angiogenesis. Additionally, NE APs leverage EGCG's ability to scavenge reactive oxygen species and maintain mitochondrial homeostasis, while synergistically enhancing TNF/NF-κB/JAK-STAT signaling pathways to support immune responses and osteogenic differentiation. In vivo experiments demonstrated that NE APs create a favorable microenvironment for bone regeneration through stem cell recruitment, angiogenesis, and immune modulation, effectively promoting the repair of inflammatory bone defects. This versatile protective delivery strategy, based on polyphenol and growth factor self-assembly, offers the potential to advance the application of growth factors in regenerative medicine.

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Regulation of different metal ions on the properties, structure, self-assembly and encapsulating capabilities of soybean globulin (SG)-tannic acid (TA) conjugates were investigated. Through coordination interactions, metal ions promoted the supramolecular self-assembly of SG, resulting in the efficient encapsulation of β-carotene in its hydrophobic domains. Fe3+ and Cu2+ enhanced particle integrity by forming stable metal–polyphenol networks, while Al3+ and Zn2+ achieved the highest β-carotene encapsulation efficiency due to their appropriate capability to interact with SG/TA and lower destructive effect on β-carotene. In the presence of TA, Fe3+/Cu2+ imparted strong pH stability to the carriers, Al3+/Mg2+/Zn2+ preserved β-carotene under light/heat/oxygen conditions, and Al3+/Zn2+ promoted superior antioxidant activity and β-carotene bioaccessibility during digestion. These findings demonstrate that metal ions with distinct coordination characteristics significantly influence the functionality of SG–TA conjugates, offering insights for the rational design of metal-induced protein–polyphenol delivery systems.

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Lignin has attracted wide attention in sustainable environment remediation, especially the polyphenol-metal-network (PMN) based on lignin that shows unique applicability. In this work, by self-assembly of double PMN formed by lignin, plant tannins (TA) and Fe ions, a universal gravel-like lignin catalysts were reported for cost-efficient water purification. A controllable self-assembly technique dependent in pH was developed, achieving the controllable synthesis of materials with highly uniformity. Driven by strong multiple intermolecular interactions and PMN mediated TA-Fe Fenton system, this bio-based material exhibited efficient interfacial capture (65.70 mg·g-1) and in-situ degradation performance (95.40 %), and removed ubiquitous dye contaminants through static and flowing operation. Benefiting from this, effective flowing purify platform that continuously purify large-scale dye-containing wastewater through flowthrough strategy was profiled, confirming the potential in real industrial system. The theoretical calculations including molecular dynamics simulation contributed to providing insightful comprehension for co-assembly of system and their intermolecular interaction with dye molecules. Additionally, this material also showed magnetic response ability, stable reusability performance, and extended preparation advantages. This work provided a facile strategy to develop advanced lignin-based double PMN derived materials to support water purification by utilizing solid-waste to repair liquid-waste.

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Nanogels formed by self-assembly of natural proteins and polysaccharides have attracted great interest as potential carriers of bioactive molecules. Herein, we reported that carboxymethyl starch-lysozyme nanogels (CMS-Ly NGs) were prepared using carboxymethyl starch and lysozyme by green and facile electrostatic self-assembly, and the nanogels served as epigallocatechin gallate (EGCG) delivery systems. The dimensions and structure of the prepared starch-based nanogels (i.e., CMS-Ly NGs) were characterized by dynamic light scattering (DLS), ζ-potential, Fourier transform infrared spectroscopy (FT-IR), X-ray diffraction (XRD) and thermal gravimetric analyzer (TGA). FT-IR and 1H NMR spectra together confirmed the formation of CMS; FT-IR spectra confirmed the formation of CMS-Ly NGs; XRD spectra confirmed the disruption of the crystal structure of lysozyme after electrostatic self-assembly with CMS, and further confirmed the formation of nanogels. TGA demonstrated the thermal stability of nanogels. More importantly, the nanogels showed a high EGCG encapsulation rate of 80.0 ± 1.4 %. The CMS-Ly NGs encapsulated with EGCG exhibited regular spherical structure and stable particle size. Under the simulated gastrointestinal environmental conditions, CMS-Ly NGs encapsulated with EGCG showed the controlled release potential, which increased its utilization. Additionally, anthocyanins can also be encapsulated in CMS-Ly NGs and showed slow-release properties during gastrointestinal digestion in the same way. Cytotoxicity assay also demonstrated good biocompatibility between CMS-Ly NGs and CMS-Ly NGs encapsulated with EGCG. The findings of this research suggested the potential application of protein and polysaccharides-based nanogels in the delivery system of bioactive compounds.

Herein, we used pH-shifted and pH-driven methods to assemble kidney-bean protein isolate (KPI) and luteolin (Lut) into a nanocomplex and subsequently investigated their binding mechanism, structure, and functional properties. Results showed that the nanocomplex prepared by the pH-driven method exhibited a better encapsulation effect and controlled release of Lut. Fluorescence spectroscopy and molecular docking analysis showed that the binding affinities under alkaline conditions were higher than those under acidic and neutral conditions. Various spectral techniques were used to determine the structural changes in the KPI-Lut nanocomplex, including the transformation of α-helices and β-sheets and alteration of specific amino acid microenvironments, which were more pronounced in the pH-driven nanocomplex. The structural changes in the nanocomplex further affected their surface hydrophobicity and thermal stability. Additionally, the combination of KPI and Lut significantly improved the antioxidant activity and α-glucosidase inhibitory ability of the resultant nanocomplexes, particularly the one prepared by the pH-driven method.

Self-assembled peptide and polysaccharide nanogels are excellent candidates for bioactive delivery vectors. However, there are still significant challenges in the application of nanogels as delivery tools for bioactive elements. This study aims to deliver, and control the release of a hydrophobic bioactive flavonoid hesperidin. Using the self-assembling peptide (SAP) Fmoc-FRGDF, extracellular matrix mimicking nanofibrils were fabricated, which were decorated and bolstered with immunomodulatory polysaccharide strands of fucoidan and infused with hesperidin. The mechanical properties, secondary structure, and microscopic morphologies of the composite hydrogels were characterized using rheometer, FTIR, XRD, and TEM, etc. The encapsulation efficiency (EE) and release behavior of hesperidin were determined. Coassembly of the SAP with fucoidan improved the mechanical properties (from 9.54 Pa of Fmoc-FRGDF hydrogel to 7735 Pa of coassembly hydrogel at 6 mg/mL fucoidan concentration), formed thicker nanofibril bundles at 4 and 6 mg/mL fucoidan concentration, improved the EE of hesperidin from 72.86 % of Fmoc-FRGDF hydrogel to over 90 % of coassembly hydrogels, and showed effectively controlled release of hesperidin in vitro. Intriguingly, the first order kinetic model predicted an enhanced hydrogel retention and release of hesperidin. This study revealed a new approach for bioengineered nanogels that could be used to stabilize and release hydrophobic payloads.

This study reports the development of a hierarchical arginine-based colloidal network within a Pickering nanoemulsions stabilized by basil extract polyphenols (PEMA). Heat-induced citric acid-polyphenol complexes drive colloidal self-assembly and adsorption at the oil-water interface. To refine the microstructure, polyol-surfactant co-stabilizers modulated interfacial tension and osmotic pressure, directing the assembly of a dense interfacial layer. Integrating arginine significantly enhances physical stability and antioxidant potency, facilitated by a network of hydrogen bonds and electrostatic interactions. The arginine-linked colloids exhibited pH-dependent mucoadhesive interactions with gastric mucin and maintained cellular redox balance in RAW 264.7 macrophages under oxidative and inflammatory stress. These results suggest that the structural properties of arginine, specifically its cationic guanidinium group and hydrophobic propyl moiety, provide a chemical basis for enhanced mucoadhesion, facilitating gastrointestinal retention and potential cytoplasmic delivery. Systemically, PEMA attenuated oxidative damage induced by gentamicin-piroxicam in vivo, as evidenced by a 37 % reduction in thiobarbituric acid reactive substances (TBARS) and an 88 % increase in cupric reducing antioxidant capacity (CUPRAC). Importantly, PEMA treatment attenuated renal and liver injuries, as demonstrated by decreased serum creatinine (SCr), blood urea nitrogen (BUN), and transaminase levels (AST/ALT). Histological periodic acid-Schiff (PAS) staining confirmed that PEMA supports the structural integrity of the renal brush border membrane (BBM). Even though tubular recovery was incomplete compared to controls, PEMA demonstrate potential as a promising colloidal formulation for treating oxidative stress-related conditions.

Bacterial infections and the resultant pyroptosis‐exacerbated inflammatory crises lead to a range of local or systemic diseases. Current therapeutic strategies are still constrained by host cellular barriers and biofilm, significantly impeding spatiotemporal precision, and functional robustness. Notably, residual pathogen‐ and damage‐associated molecular patterns can manipulate host cell biology even after antibacterial monotherapy. In this study, a modular self‐assembly strategy for the nano‐antibiotic system (EM NPs) is developed through stepwise construction design, leveraging non‐covalent interactions between polyphenol frameworks and antibiotic molecules. The assembled modules exhibit intrinsic protonation capability and strong intermolecular affinity, facilitating the dynamic modulation of molecular interactions and surface charge reversal of the EM NPs under acidic conditions. This enables intracellular delivery through adaptive drug release behavior, lysosomal escape, and efficient cytoplasmic distribution. In vitro, EM NPs leverage polyphenol‐mediated cellular barrier penetration and biofilm‐targeted accumulation, achieving superior intracellular bacterial eradication and biofilm clearance compared to free antibiotics. Furthermore, the data validates that EM NPs modulate the mitochondria‐inflammasome axis to effectively suppress pyroptosis and subsequent inflammatory responses. In mouse models of periodontitis and sepsis, EM NPs significantly alleviate inflammation and tissue damage. Overall, this work provides a promising therapeutic strategy for comprehensively managing bacterial infection‐induced inflammation.

Ellagic acid (EA) has limited utility due to its extremely low solubility. Inspired by the naturally high content of EA in Triphala, the research group discovered that there might be noncovalent self-assembled nanoaggregates centered on EA in natural polyphenols that could significantly improve EA's solubility and enhance its antibacterial activity. Therefore, seven polyphenols that we found were potentially involved in EA self-assembly were separated and identified from Triphala, and 18 binary, ternary, and quaternary self-assembly systems were constructed by combining them with EA. Finally, a ternary self-assembled solubilizing system centered on ellagic acid-gallic acid-catechin (EA-GA-CA) was established. The system could improve the solubility of EA from 0.95 to 171.345 μg·mL-1, leading to a notable 180-fold increase, and the stability of EA in water was increased 3 times compared with the mixture of EA, GA, and CA, which is currently the most effective carrier-free hydrotropic solubilizing method of EA. The in vitro release rate reached about 61%, which was about 60 times higher than that of EA. Exploring the formation mechanism of the self-assembled complex revealed that EA, GA, and CA were induced by hydrogen bonding and π-π stacking to form a solubilizing structure resembling a sandwich biscuit. In addition, in vitro antibacterial experiments, biofilm clearance experiments, and infected wound healing experiments demonstrated that the EA-GA-CA complex has a better inhibitory effect on Staphylococcus aureus (S. aureus) and methicillin-resistant S. aureus (MRSA) than EA, GA, CA, benzylpenicillin potassium, and the mixture of EA, GA, and CA (MIC = 12.5 mM). The inhibition rate of the EA-GA-CA complex against S. aureus reaches 82.68%, and it can rapidly promote the healing of infected wounds caused by S. aureus within 4-6 days (the healing rate increased from 15 to 75%). This study aims to provide new ideas for EA's natural small molecule carrier-free self-assembly solubilization and synergistic applications.

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The interaction of the polyphenol–protein–polysaccharide ternary system plays a critical regulatory role in many biological processes including cellular signal transduction, molecular recognition, and assembly. Moreover, the interactions of the three elements can form complex molecular structures and affect their respective functions and activities. It is necessary to clarify the correlation between the binding force and functional characteristics of polyphenols, proteins, and polysaccharides in the ternary system to effectively improve the sensory, functional, and nutritional properties of food. Hence, this paper systematically reviews the interactions of the ternary system composed of polyphenols, proteins, and polysaccharides. Moreover, this article also analyzes the interaction between the two components in the ternary system based on the functional characteristics of these components. Furthermore, this review comprehensively introduces the application of ternary systems. The findings are expected to provide important guidance for the polyphenol–protein–polysaccharide ternary system in biology, medicine, and food industry.

Our study investigates polyphenol-protein interactions, analyzing their structural diversity and dynamic behavior. Analysis of the entire Protein Data Bank reveals diverse polyphenolic structures, engaging in various noncovalent interactions with proteins. Interactions observed across crystal structures among diverse polyphenolic classes reveal similarities, underscoring consistent patterns across a spectrum of structural motifs. On the other hand, molecular dynamics (MD) simulations of polyphenol-protein complexes unveil dynamic binding patterns, highlighting the influx of water molecules into the binding site and underscoring limitations of static crystal structures. Water-mediated interactions emerge as crucial in polyphenol-protein binding, leading to variable binding patterns observed in MD simulations. Comparison of high- and low-resolution crystal structures as starting points for MD simulations demonstrates their robustness, exhibiting consistent dynamics regardless of the quality of the initial structural data. Additionally, the impact of glycosylation on polyphenol binding is explored, revealing its role in modulating interactions with proteins. In contrast to synthetic drugs, polyphenol binding seems to exhibit heightened flexibility, driven by dynamic water-mediated interactions, which may also facilitate their promiscuous binding. Comprehensive dynamic studies are, therefore essential to understand polyphenol-protein recognition mechanisms. Overall, our study provides novel insights into polyphenol-protein interactions, informing future research for harnessing polyphenolic therapeutic potential through rational drug design. Scientific contribution: In this study, we present an analysis of (natural) polyphenol-protein binding conformations, leveraging the entirety of the Protein Data Bank structural data on polyphenols, while extending the binding conformation sampling through molecular dynamics simulations. For the first time, we introduce experimentally supported large-scale systematization of polyphenol binding patterns. Moreover, our insight into the significance of explicit water molecules and hydrogen-bond bridging rationalizes the polyphenol promiscuity paradigm, advocating for a deeper understanding of polyphenol recognition mechanisms crucial for informed natural compound-based drug design.

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Intracellular protein therapeutics offer great promise for treating diseases involving intracellular targets, yet their clinical translation remains limited by inefficient delivery systems. Here, we report the development of a simple, versatile, and biocompatible protein delivery platform based on tea polyphenol nanoparticles (TPNs) formed via the oxidative self-polymerization of epigallocatechin gallate (EGCG). Through noncovalent interactions between EGCG and proteins, TPNs enable efficient encapsulation of proteins with diverse molecular weights and isoelectric points under mild conditions. Using urate oxidase (UOx) as a model therapeutic protein, we demonstrate that TPNs protect UOx from enzymatic degradation, preserve its native structure and enzymatic activity, and achieve effective cytosolic delivery via glutathione-triggered release. In disease models of hyperuricemia and gouty arthritis, TPNs/UOx significantly prolonged UOx circulation, lowered serum uric acid levels, reduced joint inflammation, and improved liver and kidney function, with favorable biocompatibility. This work establishes TPNs as a versatile and stimuli-responsive platform for intracellular protein delivery, offering new strategies for the clinical application of protein therapeutics.

Polyphenols are significant compounds that impact the winemaking process, influencing key attributes such as wine quality, color, astringency, bitterness, and chemical stability. Traditionally, the wine polyphenolic content is assessed through conventional analytical methods, which are costly and time‐consuming. Thus, developing novel strategies to overcome these limitations is highly desirable. Quartz Crystal Microbalance with Dissipation Monitoring (QCM‐D) is an electromechanical sensor that has gained broad recognition as a fast, reliable, and label‐free detection tool. The QCM‐D is employed to investigate Gelatin Type A (Gel‐A) and Mouse Proline‐Rich Protein 5 (MP5) as probes for analyzing polyphenols in red wines. The probes have been successfully immobilized on the sensor surface, yielding molecular densities of 2.1 × 1014 and 5.1 × 1012 molecules cm−2 for MP5 and Gel‐A, respectively. Both probes have shown promising performance in the analysis of polyphenols in wine, with both changes in the sensor's resonance frequency and dissipation with all tested samples. Notably, using MP5, a linear response of the dissipation has been observed with both the total polyphenol and hydroxybenzoic acid concentrations. These results indicate strong potential for developing a stand‐alone sensor platform to directly monitor polyphenols during the winemaking process.

Polyphenols are among the most versatile secondary metabolites of plants, with significant therapeutic potential, including anti-inflammatory, cardioprotective, and antioxidant properties. However, limited bioavailability impedes their clinical application. These improvements have led to the use of synthetic stabilizers, toxic solvents, and high-energy inputs, raising concerns about the sustainability, scalability, and environmental impact of these techniques. The bioavailability of polyphenolic bioactives is an emerging area of interest, and green strategies have been developed to address it. Recently, a series of carrier-free delivery systems have also been developed, such as edible colloidal architectures, biopolymer nanoparticles, self-assembled nanostructures, and protein/polysaccharide conjugate nanocarriers, which can enhance solubility, stability, gastrointestinal performance, and release profiles. This review offers a critical analysis of approaches to improve polyphenol bioavailability, as well as recent developments in sustainable formulation design, physicochemical characterization, and translational considerations. This review critically examines the potential, limitations, and future research directions for developing safe, scalable, and environmentally friendly polyphenol delivery systems for therapeutic applications.

Polyphenols, which are compounds characterized by the presence of phenolic hydroxyl groups, are abundantly found in natural plants and exist in highly complex forms within living organisms. As some of the most prevalent compounds in nature, polyphenols possess significant medicinal value due to their unique structural features, particularly their therapeutic efficacy in antitumor, anti-inflammatory, and antibacterial applications. In the context of inflammation therapy, polyphenolic compounds can inhibit the excessive release of inflammatory mediators from inflammatory cells, thereby mitigating inflammation. Furthermore, these compounds exhibit strong antioxidant properties, enabling them to scavenge free radicals and reactive oxygen species (ROS), reduce oxidative stress-related damage, and exert anti-inflammatory effects. Due to their multiple phenolic hydroxyl groups and their ability to chelate various metals, polyphenols are extensively utilized in the synthesis of self-assembled nanoparticles for the treatment of various diseases. Numerous studies have demonstrated that the therapeutic profile of nanoparticles formed through self-assembly with metal ions surpasses that of polyphenolic compounds alone. This Review will focus on the self-assembly of different polyphenolic compounds with various metal ions to generate nanoparticles, their characterization, and their therapeutic applications in inflammation-related diseases, providing researchers with new insights into the synthetic study of metal-polyphenol nanocomposites and their biological applications.

Natural polyphenol mixtures possess synergistic bioactivities but suffer from poor bioavailability and biological barrier penetration. Although nanoformulation offers a promising strategy, conventional carrier-dependent systems face limitations in biocompatibility, drug loading homogeneity, and scalability. To overcome these challenges, we developed carrier-free sugarcane polyphenol nanoparticles (SP-NPs) via hydrothermal-induced oxidative polymerization and supramolecular self-assembly of natural sugarcane polyphenol (SP) extract. SP-NPs was primarily composed of rutin, 2,4,6-trihydroxybenzoic acid, and gallic acid. It formed spherical nanoparticles via π-π stacking, hydrogen bonding, and hydrophobic interactions, with a particle size of 182.08 ± 35.40 nm and a zeta potential of -25.03 mV. It demonstrated markedly enhanced antioxidant activity via hydrogen atom transfer and favorable biosafety. Pharmacokinetic studies revealed substantially improved oral absorption of SP-NPs, with a shorter time to peak concentration (0.5 h), 71.07 % higher maximum plasma concentration, and 34.16 % greater systemic exposure compared to SP. SP-NPs also showed a 96.78 % plasma protein binding rate and specific enrichment in the brain, liver, and pancreas. This study provides a green and efficient carrier-free nanoassembly strategy for polyphenol mixtures, providing an experimental foundation for enhanced oral delivery and targeted therapy of oxidative stress-related diseases.

The breakdown of the blood-retinal barrier (BRB), which induces vascular leakage, represents a critical pathological hallmark underlying severe vision loss in uveitis. The inflammatory response triggers phenotypic alterations in microglia, driving excessive reactive oxygen species (ROS) production and initiating a pro-inflammatory cytokine storm involving multiple inflammatory mediators. This synergistic interaction establishes a self-amplifying pathological cascade that ultimately leads to BRB dysfunction. As a natural bioactive compound, epigallocatechin gallate (EGCG) demonstrates well-established ROS scavenging capacity, while metformin (MET), a clinically approved antidiabetic agent, effectively inhibits inflammatory responses. We used a self-assembly strategy to construct multifunctional nanoparticles (EM NPs) by combining EGCG and MET for the synergistic treatment of uveitis. In the inflammatory microenvironment, EM NPs promoted microglial polarization from M1 to M2 phenotype by suppressing the NF-κB signaling pathway and significantly reduced pro-inflammatory cytokine secretion. In addition, EM NPs suppressed apoptosis in retinal pigment epithelial (RPE) cells, a key constituent of the BRB, and preserved the integrity of tight junction proteins by scavenging ROS and inhibiting the mitochondrial apoptotic pathway, thereby exerting synergistic protective effects on the BRB. In experimental autoimmune uveitis (EAU) rat models, EM NP treatment markedly improved retinal and choroidal perfusion. Our findings demonstrate that EM NPs provide a novel therapeutic approach for uveitis management.

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Nanoformulation have been widely used in skin and transdermal drug delivery. However, the differences in integral nanoparticles absorption in healthy and diseased skin have not yet fully analyzed. The present study attempted to explore the percutaneous absorption of drugs via lesional skin by using atopic dermatitis (AD) as a model, dinitrochlorobenzene (DNCB) induced AD-like skin. In here, the small molecules of insoluble Licoricchalcone A (LA) and macromolecules glycyrrhizin polysaccharide were used to prepare LA-polysaccharide self-assembled nanoparticles (GPA-SANs) by micro-precipitation. An environment-responsive dye, P4, was loaded into SAN to track the transdermal translocation of the nanoparticles, while the drug marked with coumarin 6 (C6). Compared to healthy skin, the permeability of GPA-SANs on AD-like skin is stronger, which may be due to damage to the stratum corneum of the AD-like skin and increased intercellular spaces, resulting in an increased permeability coefficient. Therefore, the storage of nanoparticles and their diffusion at the lesion site also increased accordingly. CLSM shown that the fluorescence of P4 and C6 is observed to concentrate around the hair follicles and disseminate in the surrounding area in both AD-affected and healthy skin. It can be clearly seen that fluorescence signal of C6 in the intercellular spaces of the dermis and epidermis of AD-like skin, indicating that nano-drug on the disease skin can penetrate through the intercellular pathway to achieve therapeutic. The focus of the present study is to assess the permeability of healthy and disease skin, discuss their characteristics and discrepancy, aiming to provide a reference for the further study of nano-formulations in transdermal delivery.

The escalating global cancer burden has driven the development of nanomedicine‐based antitumor agents. Traditional Chinese herbal medicine (TCHM) provides a valuable source for drug discovery, with natural active product (NAP)‐based nanomaterials exhibiting excellent biocompatibility and potent therapeutic efficacy. This work develops a novel stimulus‐responsive antitumor nanoplatform (ISL@RLP‐Fe) based on polysaccharide‐flavonoid‐iron complexes. This system integrates multiple therapeutic modalities by combining the immunostimulatory activity of natural macromolecule Rosa laevigata polysaccharide (RLP), the chemotherapeutic potential of isoliquiritigenin (ISL), and the chemodynamic therapy (CDT) functionality of iron ions. ISL@RLP‐Fe exhibits dual pH/GSH‐responsive characteristics, enabling tumor microenvironment‐specific disintegration and drug release. In vivo studies using MCF‐7 xenograft models reveal that ISL@RLP‐Fe significantly reduces tumor mass and inhibits cancer cell migration. Mechanistically, ISL@RLP‐Fe exerts antitumor effects through multiple pathways. Fundamentally, it mediates reactive oxygen species generation and induces apoptosis. Concurrently, the iron ions within ISL@RLP‐Fe are reduced by GSH, catalyzing Fenton reactions that trigger lipid peroxidation and ferroptosis. Furthermore, RLP enhances immune responses by activating dendritic cells, collectively contributing to its antitumor efficacy. This study innovatively integrates TCHM components with modern nanotechnology to construct a fully active pharmaceutical ingredient (full‐API)‐based multifunctional system, providing a promising strategy for cancer combination therapy.

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Carrier-free self-assembled nanomedicines have emerged as promising alternatives to traditional nanocarrier-based systems due to their simpler fabrication, higher drug-loading efficiency, and better biocompatibility. Herein, we report a carrier-free polyphenol-metal coordinated nanoplatform composed of apigenin, tannic acid, and Cu2+ ions (AT-Cu NPs), synthesized through an oxidative-mediated coordination assembly. In this system, Cu2+ ions serve as coordination bridges between apigenin and tannic acid, forming a stable metal-phenolic network that facilitates spontaneous nanoparticle self-assembly. The obtained AT-Cu NPs exhibited good aqueous dispersibility, uniform spherical morphology, an average diameter of approximately 120 nm, and favorable structural stability. Density functional theory calculations were used to support the proposed coordination interactions and preferred binding geometries within the AT-Cu framework. Owing to the abundant phenolic and carbonyl coordination sites, AT-Cu NPs enabled efficient loading and stabilization of the near-infrared (NIR) dye IR-820. IR@AT-Cu NPs demonstrated effective photothermal conversion efficiency and singlet oxygen generation under 808 nm irradiation. In vitro studies showed that IR@AT-Cu NPs significantly enhanced cancer cell killing under NIR irradiation through a synergistic combination of chemotherapy, photodynamic therapy, and photothermal therapy. Mechanistic investigations suggested that the induced cell death was mainly associated with mitochondria-dependent apoptosis. Overall, this work presents a simple, biocompatible, carrier-free nanotherapeutic strategy that integrates polyphenol chemistry, metal coordination, and NIR-responsive multimodal therapy for potential combination cancer treatment.

Purpose Bone morphogenetic protein 7 (BMP7) plays a crucial role in the pathogenesis of hepatocellular carcinoma (HCC). Traditional therapies have severe side effects and cannot achieve the desired therapeutic effect. Delivery of small interfering RNA targeting BMP7 (siBMP7) can specifically down-regulate the expression of BMP7 and induce apoptosis of cancer cells, thereby achieving the effect of gene therapy. We aimed to use cationic safflower polysaccharide (SPS) as the basic carrier, and encapsulate it with synthetic hyaluronic acid (HA) and folic acid (FA) polymer to form a dual-targeting nano-carrier. After encapsulating siBMP7, we obtain dual-targeted self-assembled nanoparticles (NPs). This not only improves the delivery efficiency, maintains stability in the blood circulation, and enhances accumulation in the tumor site, but also achieves the effect of gene therapy for HCC. Methods We identified SPS, and then prepared and characterized the self-assembled NPs modified with polyethyleneimine (PEI), which can target the HA receptors and FA receptors on the surface of SMMC-7721 cells and deliver siBMP7 to hepatoma cells and induce cell apoptosis. The temperature stability, serum stability, cytotoxicity, buffering capacity, hemolytic properties, release behavior, uptake ability, and gene silencing effect of the NPs were evaluated in vitro. Further evaluation of their in vivo distribution, therapeutic effect, and safety was conducted in a nude rats model. Results The HA-FA polymer is light yellow and has strong water solubility. The blank NPs and self-assembled NPs have uniform particle size, physical stability, and stable release ability. HFSPNPs showed strong uptake ability and apoptotic effect in SMMC-7721 cells and LO2 cells. HFSPNPs could relatively effectively accumulate in the liver of rats and down-regulate the expression of BMP7 to induce apoptosis of hepatoma cells. Pathological analysis showed that the safety of HFSPNPs is better. Conclusion HFSPNPs have better tumor targeting properties, enabling siBMP7 to accumulate more in the tumor tissue and be released, thereby promoting apoptosis of hepatoma cells. This indicates that their potential for treating HCC is equivalent to that of gene therapy. This study highlights the potential of cationic SPS as a drug delivery material.

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In cancer therapy, addressing the tumor microenvironment remains a critical challenge. This study presented a novel drug delivery system based on thiolated fucoidan (FUC-SH), a marine-derived polysaccharide possessing immunomodulatory properties. FUC-SH was synthesized via cysteine conjugation and self-assembled with doxorubicin (DOX) to form stable nanoparticles through electrostatic interactions and disulfide crosslinking. These nanoparticles exhibited pH/GSH dual-responsive drug release properties, enabling selective drug release in tumor microenvironments. Characterization revealed an average particle size of 141.62 ± 16.94 nm, a Zeta potential of -23.1 ± 2.67 mV, and a high drug-loading efficiency (70.97 ± 1.70 %). Cellular assays demonstrated enhanced tumor-targeted cytotoxicity and immune-stimulating effects, including elevated ROS and cytokine production in RAW 264.7 macrophages. This study focused on in vitro evaluations and the findings highlighted the potential of FUC-SH/DOX nanoparticles as a multifunctional platform for tumor-targeted therapy, while the future studies planned to explore in vivo efficacy.

This study aimed to encapsulate lutein in high internal phase emulsions (HIPEs) stabilized by quinoa protein isolate (QPI), tannic acid (TA), and high-methoxy pectin (HMP) particles at varying concentrations to address its low delivery efficiency and bioavailability. High concentrations (3%-4%) of QPI-TA-HMP particles demonstrated strong interfacial adsorption, forming thick viscoelastic films around oil droplets. These interfacial properties imparted controllable rheological behaviors, textural characteristics, and stable 3D-printing scaffolds to the lutein-loaded HIPEs, achieving an encapsulation efficiency of 81.65 ± 2.36%. In vitro tests indicated that HIPEs enhanced lutein's resistance to storage, heat, and UV exposure while facilitating sustained intestinal release, resulting in a lutein bioaccessibility of 43.73 ± 1.44%. In vivo experiments further demonstrated that the HIPEs delivery system maintained high lutein concentrations in the small intestine, cecum, and colon, thereby significantly enhancing lutein accumulation in systemic circulation. These findings provide new insights into enhancing lutein's stability, delivery performance, and bioavailability.

Periodontitis is one of the most prevalent chronic inflammatory diseases and Polyphenols isolated from Turkish gall play a major role in the treatment of inflammatory diseases for their antibacterial, anti-inflammatory and antioxidant activities. In this work, Turkish Galls effective constituent (TGEC, T) was prepared into nanoparticles (T-NPs) by principle of oxidative self-polymerization. The pH-sensitive T-NPs was encapsulated into thermosensitive type in-situ hydrogel, and 42.29 ± 1.12% of effective constituent from T-NPs were continuously released within 96 h under the periodontitis environment. In addition, the weakly alkaline oral micro-environment of patients with periodontitis is more conducive to the sustained release of effective constituent, which is 10.83% more than that of healthy periodontal environment. The bacteriostatic test showed that T-NPs had stronger antibacterial activity on oral pathogens than that of TGEC. Compared with TGEC, the minimum inhibitory concentration (MIC) of T-NPs against P. gingivalis and A. viscosus was reduced by 50% and 25%, respectively. Interestingly, T-NPs induced bacteria lysis by promoting the excessive production of ROS without periodontal tissue damage caused by excessive oxidation reaction. In conclusion, a simple method of preparing microspheres with natural polyphenols was developed, which provides beneficial reference for one-step prepared drug carriers from effective components of natural product, likewise the method offers a green and effective solution to synthesis a new adjuvant therapy drugs for treatment of gingivitis associated with periodontal pockets.

Effective tumor treatment still faces tough challenges. Sonodynamic therapy (SDT) has gained recognition as a viable substitute for photodynamic therapy, providing enhanced tissue penetration and reduced skin damage by generating reactive oxygen species (ROS) via ultrasound-triggered sonosensitizers. Nonetheless, the therapeutic efficacy of SDT is often hindered by the intrinsic apoptosis resistance of cancer cells. Additionally, apoptosis-resistant cancer cells often exhibit susceptibility to ferroptosis, making the development of an iron enrichment ferroptosis strategy crucial for the combined apoptosis-ferroptosis antitumor therapy. However, tumor cells often counteract apoptosis and ferroptosis by upregulating autophagy; thus, interrupting the autophagic degradation process is vital for the enhancement of the therapeutic outcome. Accordingly, we designed a metal-organic synergistic nanotherapeutic platform (Fe-Rh@IAA NPs) by incorporating iron, rhein, and indole-3-acetic acid (IAA) to target apoptosis, ferroptosis, and autophagy inhibition. Following systemic administration, Fe-Rh@IAA NPs were preferentially gathered at the tumor location, leveraging the enhanced permeability and retention effect. When exposed to ultrasonic irradiation, Fe-Rh@IAA NPs induced apoptosis via SDT, while the Fe ions induced ferroptosis through ROS production and glutathione depletion. At the tumor microenvironment with high concentrations of H2O2, peroxidase-like activity of the nanoparticles converted IAA into the toxic molecule, 3-methylene-2-oxindole, which led to the suppression of autophagy activity and ultimately tumor cell death. In addition, Fe-Rh@IAA NPs could also provide magnetic resonance imaging capability, facilitating noninvasive real-time monitoring of material accumulation within tumor tissue. In vitro and in vivo studies demonstrated that Fe-Rh@IAA NPs exhibited excellent tumor-killing capabilities and favorable biosafety. This three-channel combined therapeutic strategy thus offers new insights and methodologies for tumor treatment.

Developing biocompatible, multi-target therapeutics remains a critical challenge in the management of inflammatory bowel disease (IBD). Herein, we engineered a carrier-free nanoplatform (Cur-Ant NPs) via the facile self-assembly of two natural polyphenols: curcumin (Cur) and anthocyanin (Ant). Spectroscopic analysis and molecular dynamics simulations confirmed that the assembly is stabilized by robust π-π stacking and hydrogen bonding networks, yielding uniform, spherical nanostructures with integrated functionality. In a dextran sulfate sodium (DSS)-induced colitis model, orally administered Cur-Ant NPs demonstrated superior therapeutic efficacy compared to both free polyphenols and the clinical standard, sulfasalazine (SASP). The nanoparticles' potent anti-inflammatory activity was initially validated in a zebrafish model, where they effectively inhibited neutrophil infiltration and scavenged reactive oxygen species (ROS). These protective effects were further substantiated in a murine model, where multi-omics analysis revealed a tripartite mechanism of action: reinforcing the intestinal epithelial barrier, mitigating pro-inflammatory cytokine responses, and remodeling the dysbiotic gut microbiome. Our findings establish Cur-Ant NPs as a potent, safe candidate for IBD prevention and highlight a scalable, green engineering strategy for designing next-generation nanomedicines based on the supramolecular co-assembly of natural bioactive agents.

Tannic acid (TA) can form stable complexes with proteins, attracting significant attention as protein delivery systems. However, its systemic application has been limited due to nonspecific interaction. Here, we report a simple technique to prepare systemically applicable protein delivery systems using sequential self-assembly of a protein, TA, and phenylboronic acid-conjugated PEG-poly(amino acid) block copolymers in aqueous solution. Mixing the protein and TA in aqueous solution led to covering of the protein with TA, and subsequent addition of the copolymer resulted in the formation of boronate esters between TA and copolymers, constructing the core-shell-type ternary complex. The ternary complex covered with PEG exhibited a small hydrodynamic diameter of ∼10-20 nm and prevented an unfavorable interaction with serum components, thereby accomplishing significantly prolonged blood circulation and enhanced tumor accumulation in a subcutaneous tumor model. The technique utilizing supramolecular self-assembly may serve as a novel approach for designing protein delivery systems.

In this study, a carrier system for encapsulating lycopene was established using soybean globulin (SG) and β-cyclodextrin as the primary carrier matrices. After pre-encapsulating lycopene with β-cyclodextrin, the supramolecular self-assembly of soybean globulin was induced by zinc ions (Zn2+). Then, the cyclodextrin-lycopene inclusion complexes bound to the surface of SG through non-covalent interactions were incorporated within the carrier particles. By covalently modifying SG to different extents with tannic acid (TA), the strength of the carrier particles was adjusted in a controlled manner. The results demonstrated that the pre-encapsulation of lycopene with cyclodextrin improved the encapsulation efficiency of the carrier matrices. Meanwhile, the addition of TA also enhanced the stability of carrier matrices under different pH conditions, as well as the stability of lycopene under light, heat, and oxygen conditions. The combined effect of TA and Zn2+ facilitated the formation of metal-polyphenol network structures and metal-protein coordination bonds, thereby strengthening the structure of the microparticles and providing antioxidant protection to lycopene. After cyclodextrin pre-treatment, the microparticles exhibited higher content of bio-accessible lycopene and antioxidant activity after in vitro digestion compared to the untreated group. The dual-layer encapsulation strategy using cyclodextrin and TA-Zn-induced SG contributed to the broader utilization of lycopene.

Protein-polyphenol composite particles are ideal carriers for bioactive substances. However, their tendency to aggregate and precipitate under weakly acidic conditions limits their broader application. This study investigated the effect of interfacial behavior of quinoa protein isolate-tannic acid (QPI-TA) particles regulated by high-methoxyl pectin (HMP) via self-assembly on the properties of Pickering high internal phase emulsions (HIPEs). Multispectral analysis demonstrated that HMP changed the hydrophobic microenvironment in QPI-TA (QT) particles, disrupted hydrogen bond structures, and triggered reassembly to form QPI-TA-HMP (QTH) composite particles. Interfacial adsorption kinetics, dilatational rheology, and quartz crystal microbalance with dissipation (QCM-D) analysis demonstrated that HMP significantly increased the interfacial pressure and adsorption rate of QT particles. The interfacial film formed by QTHs particles showed enhanced compactness, thickness, viscoelasticity, and mechanical strength relative to that of QT particles alone. Moreover, Pickering HIPEs stabilized by QTHs composite particles exhibited excellent stability and intelligent responsive properties under various oil phases, pH, centrifugation, temperature and storage conditions. Simulated in vitro digestion results demonstrated that both the release of free fatty acids and the bioaccessibility of hesperetin in hesperetin-loaded HIPEs were dramatically improved. This study demonstrates that incorporating anionic polysaccharides to optimize interfacial behavior in multi-responsive Pickering HIPEs provides a promising strategy for effective encapsulation and controlled delivery of hesperetin.

Cancer vaccines elicit responses of cytotoxic T lymphocytes (CTLs) and establish durable immune memory, offering promising cancer therapies. However, soluble tumor-associated antigens (TAAs) alone are rapidly cleared and poorly internalized by antigen-presenting cells (APCs), limiting cross-presentation and antitumor efficacy. Conventional nanoparticle-based delivery systems can prolong antigen retention but are often large (>100 nm), cationic, and cytotoxic, restricting their accumulation in lymph nodes (LNs) and impairing immune function. Here, to overcome these limitations, we report a sequentially self-assembled ternary complex composed of tannic acid (TA) and phenylboronic acid (PBA)-conjugated polymers for antigen delivery. Sequential coating of a protein antigen with TA and PBA-polymers generated a core-shell structure with a diameter of ∼20 nm and a neutral surface charge. Using ovalbumin (OVA) as a model protein antigen, we constructed the OVA-loaded ternary complex, and it exhibited significantly enhanced accumulation in draining LNs and uptake by APCs. Within APCs, PBA-conjugated polymers dissociated from the complex in response to the acidic pH of a late-endosome/lysosome and induced membrane destabilization through the hydrophobicity of deionized PBA and the cationic charge of residual lysine residues, enabling efficient endosomal escape and cross-presentation. Consequently, the ternary complex elicited potent CTL responses and inhibited the growth of OVA-expressing tumors with negligible adverse effects in mouse models. The ternary complex may be a promising antigen delivery platform.

Inspiration from the iron gall ink leads to the efficient formation of Fe(iii)-tannic acid coacervate particles inside the phase-separated microdroplets that are derived from the aqueous PEG/dextran liquid-liquid phase separation system. This hierarchical self-assembly, in aid of the protein affinity of tannic acid, makes it possible to compartmentalize and condense proteins into a localized, compact space in the microdroplets.

BACKGROUND Interface modification driven by supramolecular self-assembly has been accepted as a valuable strategy for emulsion stabilization enhancement. However, there has been a dearth of comparative research on the effect of simple complexation and assembly from the perspective of mechanism. RESULTS This work selected zein and tannic acid (TA) as representative protein and polyphenol modules for self-assembly (coined as TA-modified zein particle and TA-zein complex particle) to explore the surface properties, interfacial behavior, as well as the stability of constructed Pickering emulsions to obtain the regulation law of different modification methods on the interfacial behavior of colloidal particles. The results demonstrated that TA-modified zein colloidal particles stood a chance of improving emulsifying properties. When the TA concentration was 3 mmol/L, the optimized TA-modified zein particle was nano-sized (109.83 nm) and had advantageous interfacial properties, including sharply reduced surface hydrophobicity, and low diffusion rate at the oil/water interface. As a result, the shelf life of Pickering emulsion containing 50% oil phase was extended to 90 days. CONCLUSION Through multi-angled research on the properties of the interfacial membrane, improvement of emulsion stability was due to the formation of viscoelastic interfacial film which resulted from the decrease of absorption rate between particles and interface. Using refined regulation to study the role of different sample preparation methods from a mechanistic perspective. Overall, this study has provided a reference for TA to regulate the surface properties and interface behavior of zein colloidal particles, enriched the understanding of colloidal interface assembly, and provided a theoretical basis for the quality control of interface-oriented food systems. This article is protected by copyright. All rights reserved.

HYPOTHESIS Gelatin is one of the most popular constituents of biodegradable/edible films. Because of its poor mechanical properties, it typically needs to be cross-linked. In this regard, the use of tannic acid has attracted significant interest. Whereas the biodegradability of gelatin is well established, little is known on how different crosslinking methods affect biodegradability. In most cases, the ionic strength at which protein films are grown has a drastic effect on their structure. Thus, it is expected that by controlling the ionic strength during the growth of cross-linked gelatin films it should be possible to tune the access to relevant cleavage sites by proteases and, therefore, their biodegradability. EXPERIMENTS Gelatin-tannic acid were grown at different ionic strengths by means of the layer-by-layer self-assembly method. The growth of these multilayers and their response to the presence of different proteases were monitored by means of Electrochemical Impedance Spectroscopy and Quartz Crystal Microbalance with Dissipation. FINDINGS Gelatin-tannic acid multilayers grown at low ionic strength exhibited a swollen structure that allowed easy access to their cleavage sites by proteases. Multilayers formed at physiological ionic strength exhibited a compacter structure, which limited their proteolytic degradation.

No abstract available

Despite their safety and widespread use, conventional protein antigen‐based subunit vaccines face significant challenges such as low immunogenicity, insufficient long‐term immunity, poor CD8+ T‐cell activation, and poor adaptation to viral variants. To address these issues, an infection‐mimicking gel (IM‐Gel) is developed that is designed to emulate the spatiotemporal dynamics of immune stimulation in acute viral infections through in situ supramolecular self‐assembly of nanoparticulate‐TLR7/8a (NP‐TLR7/8a) and an antigen with tannic acid (TA). Through collagen‐binding properties of TA, the IM‐Gel enables sustained delivery and enhanced retention of NP‐TLR7/8a and protein antigen in the lymph node subcapsular sinus of mice for over 7 days, prolonging the exposure of vaccine components in both B cell and T cell zones, leading to robust humoral and cellular responses. The IM‐Gel system with the influenza A antigen confers cross‐protection against multiple influenza subtypes (H1N1, H5N2, H3N2, H7N3, and H9N2) with long‐term immune responses. Combination of the IM‐Gel with the SARS‐CoV‐2 spike protein also elicits strong cross‐reactive antibody responses against multiple SARS‐CoV‐2 variants (Alpha, Beta, NY510+D614G, Gamma, Kappa, and Delta). The IM‐Gel, as a programmable immunomodulatory material, provides a vaccine design principle for the development of next‐generation universal vaccines that can elicit broad and durable protective immunity against emerging viruses.

Natural antimicrobial agents are both environmentally friendly and safe, and exhibit excellent biocompatibility. However, their instability and rapid release characteristics limit their application in food preservation packaging. In this study, a photothermal-responsive packaging film was developed by incorporating a Pickering emulsion of soy protein isolate-tannic acid-Fe3+(STF) nanoparticles stabilizing tea tree oil (TTO) into a chitosan (CS)/gelatin (Gel) matrix. The STF nanoparticles, synthesized via coordination-driven self-assembly, stabilized the Pickering emulsion and achieved an encapsulation efficiency of 84% for TTO. Under near-infrared (NIR) irradiation, STF nanoparticles transform light energy into thermal energy. On the one hand, the localized increase in temperature provides the film with a certain sterilizing effect. On the other hand, the film allows for the rapid, controlled release of tea tree oil as needed. Through the synergistic effect of localized thermal therapy and controlled release of essential oils, the film exhibits over 98% antibacterial activity against E. coli and S. aureus. Furthermore, the resultant film has outstanding mechanical strength, barrier properties, and antioxidant effects. Preservation experiments were ultimately carried out using strawberries and grapes as representative berries, and the results showed that the film can extend the shelf life by 3-8 days depending on the fruit type. These results demonstrate the application potential of this photothermal controlled-release film in the field of berry preservation.

The transfusion of donor red blood cells (RBCs) is seriously hampered by important drawbacks that include limited availability and portability, the requirement of being stored in refrigerated conditions, a short shelf life or the need for RBC group typing and crossmatching. Thus, hemoglobin (Hb)-based oxygen (O2) carriers (HBOCs) which make use of the main component of RBCs and the responsible protein for O2 transport, hold a lot of promise in modern transfusion and emergency medicine. Despite the great progress achieved, it is still difficult to create HBOCs with a high Hb content to attain the high O2 demands of our body. Herein a metal-phenolic self-assembly approach that can be conducted in water and in one step to prepare nanoparticles (NPs) fully made of Hb (Hb-NPs) is presented. In particular, by combining Hb with polyethylene glycol, tannic acid (TA) and manganese ions, spherical Hb-NPs with a uniform size around 350-525 nm are obtained. The functionality of the Hb-NPs is preserved as shown by their ability to bind and release O2 over multiple rounds. The binding mechanism of TA and Hb is thoroughly investigated by UV-vis absorption and fluorescence spectroscopy. The binding site number, apparent binding constant at two different temperatures and the corresponding thermodynamic parameters are identified. The results demonstrate that the TA-Hb interaction takes place through a static mechanism in a spontaneous process as shown by the decrease in Gibbs free energy. The associated increase in entropy suggests that the TA-Hb binding is dominated by hydrophobic interactions.

Flash NanoPrecipitation (FNP) is a rapid method for encapsulating hydrophobic materials in polymer nanoparticles with high loading capacity. Encapsulating biologics such as proteins remains a challenge due to their low hydrophobicity (logP < 6) and current methods require multiple processing steps. In this work, we report rapid, single-step protein encapsulation via FNP using bovine serum albumin (BSA) as a model protein. Nanoparticle formation involves complexation and precipitation of protein with tannic acid and stabilization with a cationic polyelectrolyte. Nanoparticle self-assembly is driven by hydrogen bonding and electrostatic interactions. Using this approach, high encapsulation efficiency (up to ~80%) of protein can be achieved. The resulting nanoparticles are stable at physiological pH and ionic strength. Overall, FNP is a rapid, efficient platform for encapsulating proteins for various applications.

Oxidative stress is associated with most traumatic or pathological bone defects, and seriously affects the effect of implantation. The construction of antioxidative and osteogenic coatings is of great significance to accelerate the bone regeneration of implants. In this study, baicalein (BAI), a nature flavonoid drug, was loaded in bovine serum albumin (BSA) by desolvent method to prepare BAI-BSA composite protein, and tannic acid (TA)/BAI-BSA coatings were further built via layer by layer self-assembly technology. BAI-BSA possesses good biocompatibility that showed no cytotoxicity to osteoblasts and erythrocytes, and helps to enhance the activity of alkaline phosphatase (ALP) and promote the formation of osteogenic mineralized calcium nodules. After assembled with TA, BAI-BSA coating significantly promoted cell adhesion and in vitro osteogenic mineralization of MC3T3-E1. Moreover, BAI drug loading improved the antioxidative function of BSA coatings effectively. The scavenging rates of (TA/BAI-BSA-10)4 for ABTS+• and DPPH• free radicals were 69.6 ± 16.1 % and 53.4 ± 2.4 %, respectively. At cellular level, the TA/BAI-BSA coating effectively inhibited the impact of oxidative stress on the oxidative damage of osteoblasts. The drug-loaded protein coatings possess both great antioxidative and osteogenic functions, which have important potential in the field of bone repair.

High intensity focused ultrasound (HIFU) is widely used in medical practice, including cancer therapy. Also this approach is promising for remote release of encapsulated drugs in various other biomedical applications where local treatment is needed. Our approach underpins the minimization of HIFU impact on possible degradation of biological tissues and expand the use of HIFU in the controlled release of encapsulated drugs. We demonstrated the efficient ultrasound-induced release of labeled protein (Cy7-BSA) from elaborated nanocomposite microcapsules in vitro an in vivo. The capsule fabrication was done using combination of recently developed freezing-induced loading (FIL) technique and Layer-by-Layer assembly (LbL) used for the preparation of complex multilayer BSA/tannic acid nanocomposite capsules sensitive to HIFU. These capsules contain NIR fluorescent Cy7-labeled BSA in the shell for tracking in vivo and the high concentration of labels inside the capsules resulted in self-quenching provides the real-time detection of the protein once it is released from the capsule. Ultrasound-induced release in vivo of Cy7-labeled BSA initially quenched by magnetite nanoparticles was confirmed by fluorescent tomography. The significant decrease of Cy7 fluorescence under HIFU treatment in vitro was found to be due to a generation of reactive oxygen species and fast dye oxidation. Our results demonstrate that adapted HIFU setup can be used for the directed release of encapsulated substances in vivo under tissue compatible NIR monitoring by fluorescent tomography.

Rice bran protein (RBP)-chitosan (CS) nanoparticles as a delivery system loaded with ε-polylysine (ε-PL) were successfully synthesized by thermal aggregation-induced self-assembly technique, and the physicochemical properties and antibacterial activity were comprehensively evaluated by various techniques. The results indicated that the preparation process parameters (RBP/CS mass ratios, ε-PL concentration, pH, time, and temperature) had a significant regulatory effect on the particle size, PDI, turbidity and encapsulation efficiency of R-C-ε-PL NPs. Meanwhile, the R-C-ε-PL NPs exhibited excellent thermal stability, hygroscopicity and storage stability. And ε-PL promoted the α-helix structure to a relatively stable β-sheet structure of R-C-ε-PL NPs with a more compact molecular structure through hydrophobic interactions, hydrogen bonding, and electrostatic forces. Furthermore, R-C-ε-PL showed better antioxidant and antibacterial activities for free DPPH and FRAP radicals as well as microorganisms than RBP-CS. Overall, the results revealed that R-C-ε-PL NPs was an effective delivery system of ε-PL, and provided theoretical references for application in food preservation.

This study developed PQSp wound dressing hydrogels (S0-S6) using polyvinyl alcohol (PVA), quaternary chitosan (QCS), and sodium alginate (SA) as the matrix, with the addition of coconut mesocarp polyphenol (P-CTP, 0.1 %, 0.5 %, and 1.0 %) and β-glycerophosphate disodium (GP, 1.0 %) through a freeze-thaw method. Compared to hydrogels without P-CTP and GP (S0), the tensile strength of S1-S6 increased from 0.08 MPa to 0.45 MPa, elongation at break improved from 200 % to 320 %, and the swelling ratio decreased from 186 % to 82 % due to the effects of P-CTP and GP, while maintaining water content above 80 %, ensuring a moist environment for wound healing. Their thermal stability was also improved. SEM, FTIR, and XPS results confirmed enhanced crosslinking within the multi-network of the hydrogels, attributed to the increased hydrogen bonding from GP and P-CTP, independent of chemical crosslinking. However, antioxidant and antibacterial activities were dose-dependent only on P-CTP, with S3 and S6 showing the best effects. CAM and chicken embryo assays confirmed the hydrogels' non-toxicity and biocompatibility. These findings suggest that PQSp hydrogels, with their excellent mechanical properties, bioactivity, and safety, hold great potential for advanced wound dressing applications and provide a reference for expanding the application range of P-CTP.

The use of facile methods to synthesize environmentally friendly and multifunctional hydrogel dressings is still a major challenge in development. Herein, Turkish gall extract (TGE) and carboxymethyl chitosan (CMCS) were combined and sprayed using a dual syringe to form a multifunctional TGE-CMCS hydrogel (TC gel) in one step through abundant hydrogen bonding between functional groups as a green approach. TC gel showed rapid gelation at 19.0 ± 2.9 s. Apart from the advantage of being able to adapt to different wound shapes, TC gel retained the antioxidant, antibacterial, hemostatic and anti-inflammatory properties of TGE. In vitro antibacterial experiments showed that TC-gel eliminated 98.27 ± 0.79 % of Staphylococcus aureus and 98.87 ± 1.08 % of Escherichia coli. Compared with TGE or CMCS alone, TC gel accelerates skin wound healing due to its three-dimensional network structure and continuous release of active components at the wound site, enhancing re-epithelialization, improving collagen deposition, and increasing angiogenesis. The wound healing rate of full-thickness skin defect rats treated with TC gel was 93.98 ± 0.63 % on the 10th day. These results suggest that TC gel combined with a facile and scalable manufacturing method is a promising multifunctional wound dressing for clinical wound management.

This study involved the fabrication of double-layer intelligent films using chitosan (CS), polyvinyl alcohol (PVA), grape skin anthocyanin (GSA), gellan gum (GG) and selenium nanoparticles (SeNPs). The CS/PVA/GSA layer functioned as the internal indicator layer, and the GG/SeNPs layer acted as the external layer for antioxidant and antimicrobial purposes. SEM, FTIR, XRD, and TGA results confirmed the successful fabrication of double-layer films as well as the presence of hydrogen bonding interaction between the two layers. The tensile strength of double-layer films (8.06 MPa-9.61 MPa) fallen between that of single-layer CS/PVA/GSA film (12.51 MPa) and GG/SeNPs film (1.50 MPa-7.67 MPa). The double-layer films demonstrated good UV-blocking abilities, as well as outstanding antioxidant (ABTS scavenging rate can be up to ~80 %) and antimicrobial properties. Compared with single-layer CS/PVA/GSA film, the double-layer film incorporated with 6.6 wt% SeNPs (CPG/GS2 film) possessed a more rapid and stronger response towards NH3/acetic acid as well as enhanced storage stability. Furthermore, the CPG/GS2 film can increase the shelf life of strawberries at 25 °C by 4 days, and its visible color change showed strong correlation with the weight loss rate (R2 = 0.99) and hardness (R2 = 0.98) of strawberries.

To address the persistent environmental burden of petroleum-based plastics and the intrinsic limitations of natural biopolymer films, this study developed an enhanced active packaging material (GC/BR composite film) via the strategic incorporation of self-assembled berberine-rhein nanoparticles (BR NPs) into a gelatin/chitosan (GC) hybrid matrix. Molecular dynamics simulations coupled with various spectroscopic analyses revealed that the co-assembly of BR NPs was primarily stabilized by robust π-π stacking, electrostatic interactions, and hydrogen bonding. The reinforcement effect of BR NPs is attributed to their uniform dispersion and interfacial interactions with the GC matrix, which facilitate efficient stress transfer. As a result, the composite film exhibits notable mechanical enhancements relative to the pure GC film: tensile strength increases by 62% and elongation at break by 88%, accompanied by an improved water vapor barrier. Notably, the GC/BR film retained the aggregation-induced emission characteristics of the photosensitizer, and exhibited effective photodynamic sterilization upon visible-light irradiation. In vitro antibacterial assays demonstrated 100% inactivation against Staphylococcus aureus and 99% against Escherichia coli within 20 min of visible-light irradiation. Real-food preservation trials using chicken breasts further validated the film's capacity to suppress microbial proliferation. Crucially, migration tests revealed a maximum BR NPs leachate concentration of 0.0032 mg/mL (60-fold lower than the highest concentration in hemolysis assays), suggesting a low migration risk and a favorable preliminary biosafety profile. This work provides a promising strategy for the rational design of robust, biodegradable active packaging materials with integrated photodynamic functionality.

Enzymatic browning in fresh-cut lettuce remains a critical challenge in the food industry, driving the search for effective natural preservatives. This study explores the innovative encapsulation of rambutan (Nephelium lappaceum L.) peel bioactive compounds with chitosan to enhance their stability and bioactivity. Among the various rambutan peel extracts (RPE) evaluated, the methanolic extract exhibited the highest DPPH scavenging activity (IC50: 2.28 ± 0.15 μg/mL), correlated with its total phenolic content. The ethanolic extract also demonstrated strong antioxidant activity (IC50: 3.26 ± 0.17 μg/mL) and was selected for further studies due to its balanced antioxidant performance and suitability as a food-grade solvent for potential commercial applications. Liquid chromatography-mass spectrometry (LC-MS) analysis identified Sanguiin H11 and ellagic acid as the key phenolic compounds. Notably, ellagic acid demonstrated strong molecular docking with polyphenol oxidase (PPO), showing a binding energy of -6.75 kcal/mol through specific hydrogen bonding through HIS296 interactions. The molecular docking results indicated that ellagic acid has a superior binding affinity compared to the reference inhibitor tropolone (-5.20 kcal/mol). The optimized chitosan encapsulation system (10:1 w/w RPE: chitosan ratio) produced uniform spherical microcapsules (3403 ± 8.79 nm) with excellent colloidal stability (zeta potential: 31.17 ± 0.83 mV) and high encapsulation efficiency (60.53 ± 0.48%). This formulation significantly enhanced both DPPH radical scavenging activity (6.99-fold increase) and green oak lettuce polyphenol oxidase (goPPO) inhibition (2.29-fold improvement) compared to the chitosan control group. This research demonstrated the successful conversion of agricultural waste into effective natural preservatives with PPO inhibitory and antioxidant activities, offering a promising solution for fresh-cut produce preservation.

Polymer nanoparticle-based drug carriers represent a new avenue for cancer therapy. In this work, we study the formation of chitosan/lignin (Chi/Lig) core–shell particles doped with samarium oxide nanoparticles as potential carriers for the hydrophobic anticancer drug curcumin. Electrostatic coassembly was responsible for the formation of Chi/Lig core–shell particles. The structural characterization suggested interactions between chitosan, lignin, and Sm2O3 through electrostatic interactions, such as hydrogen bonding. The incorporation of lignin into the chitosan matrix results in the formation of an amphiphilic core–shell structure, offering the potential for dual-drug-loading strategy studies, wherein one hydrophobic drug could reside in the lignin core while another hydrophilic drug occupies the chitosan shell. Additionally, the incorporation of lignin into the polymer systems not only contributes to a slower release of curcumin but also enables the design of pH-responsive drug carriers. Moreover, the strong red fluorescence observed in the samarium-containing composites suggests their potential for applications in bioimaging and in vitro assays, particularly with orally delivered microcarriers.

With increasing global environmental awareness and concerns about food safety, biodegradable active packaging has garnered widespread attention. In this study, the stability and bioactivity of tea polyphenol (TP) were enhanced through the preparation of TP-ferric nanoparticles (TP-Fe NPs) using metal-polyphenol ion coordination. Moreover, the introduction of Fe ions can further enhance the antibacterial effects of NPs. Using the hydrogen bonding between konjac glucomannan (KGM) and zein to enhance the hydrophobicity and mechanical properties of the film. By employing KGM and zein as the matrix, we incorporated TP-Fe NPs as active fillers to create multifunctional active packaging films. This study aimed to meet the needs of food safety and sustainable development goals. The resulting film exhibited excellent water resistance (water contact angle: 117.73°), mechanical strength (tensile strength: 21.82 MPa, elongation at break: 94.30 %), ultraviolet-shielding ability (>99 %), biodegradability (5 days in soil), and antioxidant (>85 %) and antibacterial (>99 %) properties. Moreover, the film significantly reduced strawberry decay and extended its shelf life by 10 days. These findings provide new insights into the application of nanomaterials in active packaging, highlighting their potential and advantages in food preservation.

Gelatin/chitosan nanoparticles loaded with carminic acid were adopted to construct and stabilize high internal phase Pickering emulsions for 3D/4D printing. Carminic acid was incorporated into gelatin/chitosan nanoparticles with excellent compatibility via interactions like hydrogen bonding and bridging flocculation. These gelatin/chitosan/carminic acid complex nanoparticles exhibited outstanding emulsifying ability, due to the fact that nanoparticle's amphiphilicity (hydrophilic-lipophilic balance) and interfacial wettability (contact angle) promoted its adsorption at the oil-water interface. The optimal high internal phase Pickering emulsion with proper-content carminic acid illustrated uniform droplets, excellent emulsion appearance, high viscosity, great thixotropy, high yield stress, high mechanical strength and outstanding thermal stability. The optimal emulsions also presented excellent 3D/4D printability with high shape maintainability, as well as potential usage in dysphagia diets. This study provides important implications for stabilizing emulsions with carminic acid-loaded nanoparticles and constructing creative, high-quality and functional food products via 3D/4D printing.

As a well-known plant flavanol, quercetin possesses a diverse range of biological properties. These include its ability to act as an antioxidant, reduce inflammation, and exhibit anticancer effects. Consequently, it finds extensive application in numerous models related to wound healing. However, the poor physicochemical characteristics of the molecule (which include low solubility, stability, and permeability) eventually reduce its bioavailability at the targeted sites. A variety of nano formulations with great therapeutic potential have been created in order to get around these obstacles on the way to successful therapy. The current investigation aims to examine the properties of nano- and micro-sized casein/chitosan gel polyelectrolyte complexes (PECs) with respect to their potential for quercetin loading and release. Four different types of hydrogel particles at pH 6 and different casein/chitosan charge ratios were synthesized; namely, 1:1, 2:1, 4:1, and 6:1 in excesses of casein. The attractive electrostatic interactions between the oppositely charged polyelectrolytes were proved by FT-IR spectroscopy. The process yield increased from 37.5% to 72.5% in excesses of casein. The gel particle’s size varied between 377 nm and 5.72 µm depending on the casein/chitosan stoichiometry. The morphology of the obtained gel polyelectrolyte complexes was found to be spherical, based on scanning electron microscopy and atomic force microscopy analysis. The quercetin loading efficiency was above 95% for all investigated hydrogel complexes. Investigation of the physical state of the loaded polyphenol by the differential scanning calorimetry and X-ray powdered diffraction technique suggested the occurrence of partial recrystallization phenomena. The quercetin release test was performed in phosphate buffer (pH 5.5) at 32 °C and permanent stirring at 50 rpm. A zero-order model was used to describe in the best way the release kinetics. The reported casein/chitosan complexes loaded with quercetin may find application in wound healing as a concomitant treatment.

No abstract available

No abstract available

Fermented dairy products (e.g., yogurt, kefir, and buttermilk) are significant in the dairy industry. They are less immunoreactive than the raw materials from which they are derived. The attractiveness of these products is based on their bioactivity and properties that induce immune or anti-inflammatory processes. In the search for new solutions, plant raw materials with beneficial effects have been combined to multiply their effects or obtain new properties. Polyphenols (e.g., flavonoids, phenolic acids, lignans, and stilbenes) are present in fruit and vegetables, but also in coffee, tea, or wine. They reduce the risk of chronic diseases, such as cancer, diabetes, or inflammation. Hence, it is becoming valuable to combine dairy proteins with polyphenols, of which epigallocatechin-3-gallate (EGCG) and chlorogenic acid (CGA) show a particular predisposition to bind to milk proteins (e.g., α-lactalbumin β-lactoglobulin, αs1-casein, and κ-casein). Reducing the allergenicity of milk proteins by combining them with polyphenols is an essential issue. As potential ‘metabolic prebiotics’, they also contribute to stimulating the growth of beneficial bacteria and inhibiting pathogenic bacteria in the human gastrointestinal tract. In silico methods, mainly docking, assess the new structures of conjugates and the consequences of the interactions that are formed between proteins and polyphenols, as well as to predict their action in the body.

Resveratrol (RES) is a functional polyphenol that suffers from low water solubility and poor bioavailability. A novel RES-loaded soy protein isolate-dipotassium glycyrrhizinate (SPI-DG) nanocomplex (RES@SPI-DG) was designed and evaluated in this study. RES@SPI-DG was prepared using a simple but novel self-assembly ultrasonic-assisted pH-driven method. The interactions between RES and SPI-DG were non-covalent bonds, including hydrophobic interactions, hydrogen bonds, and van der Waals interactions. RES@SPI-DG exhibited high encapsulation efficiency (97.60 ± 0.38 %) and loading capacity (8.74 ± 0.03 %) of RES with a uniform small size (68.39 ± 1.10 nm). RES in RES@SPI-DG was in an amorphous state and demonstrated a 24-h apparent solubility 482.53-fold higher than bare RES. RES@SPI-DG also showed strong in vitro antioxidant properties. The pH-responsive hydrogel character of SPI-DG makes it an effective intestine-targeted delivery system that could retard the release of RES in a simulated stomach and accelerate it in a simulated intestine. In animal experiments, the bioavailability of RES@SPI-DG was 5.17 times higher than that of bare RES, and the biodistribution was also significantly improved. RES@SPI-DG demonstrated a strong hepatoprotective effect against overdose acetaminophen-induced liver injury. The SPI-DG complex might be a promising nano-platform for enhancing the bioavailability and efficacy of hydrophobic polyphenols such as RES.

Phloretin (Phl) is a promising bioactive polyphenol but severely limited in practical applications due to its intrinsically low water solubility and chemical instability. Edible dock protein (EDP), an emerging plant protein with superior hydrophobicity and emulsification capacity, can form stable nanoemulsion with phloretin via protein-polyphenol noncovalent interactions, serving as an effective delivery vehicle. In this research, the influence of EDP concentration on the physicochemical characteristics, interfacial properties, and stabilization efficacy of EDP-Phl nanoemulsion was systematically explored. The optimized nanoemulsion at 0.3% EDP exhibited uniform droplet size (115.8 nm), suitable zeta potential (-28.5 mV), and low polydispersity index (0.193), corresponding to the highest encapsulation efficiency (92.4%) and loading capacity (12.45%). Confocal laser scanning microscopy confirmed regular spherical oil-in-water nanostructures. Saturation interfacial adsorption of EDP was achieved at 0.3% protein content, generating a compact and stable interfacial film. Simulated gastrointestinal digestion revealed that phloretin retention exceeded 86%, and its antioxidant activity was remarkably enhanced via EDP-based nanoencapsulation. At 0.3% EDP, the protein molecule formed a dense interfacial layer. The hydrophobic groups faced the oil phase, and the hydrophilic groups faced the aqueous phase. This structure improved the interfacial stability. These findings elucidated the stabilization mechanism driven by protein-polyphenol interactions and supported the application of EDP nanoemulsion as food-grade delivery systems for hydrophobic bioactives.

Abstract An oil-in-water (O/W) emulsion stabilized by a protein-based nanocomplex was developed for the co-delivery of quercetin (Q) and perilla oil. Several nanocomplexes, synthesized by exploiting noncovalent interactions between black bean protein (BBP) and Q, were evaluated using fluorescence and Fourier-transform infrared (FTIR) spectroscopies. Thermodynamic analysis (ΔH > 0, ΔS > 0) indicated that the interactions between BBP and Q were mainly hydrophobic in nature, and FTIR spectroscopy suggested that the BBP-Q complexes, particularly BBP-Q3 (BBP:Q = 10:1, v/v), contained several α-helix structures and many β-sheet secondary structures. Compared with the emulsion stabilized by BBP alone, the BBP-Q3-nanocomplex-stabilized O/W emulsion featured a smaller particle size (278.7 nm), lower viscosity, better emulsifying properties, and significantly reduced Q and perilla oil release during gastrointestinal digestion. These findings indicate that BBP-Q nanocomplexes can act as effective O/W stabilizers for the co-encapsulation of polyphenols and oils in emulsions.

Abstract Decellularization is a promising technique to produce natural scaffolds for tissue engineering applications. However, non-crosslinked natural scaffolds disfavor application in cardiovascular surgery due to poor biomechanics and rapid degradation. Herein, we proposed a green strategy to crosslink and functionalize acellular scaffolds via the self-assembly of copper@tea polyphenol nanoparticles (Cu@TP NPs), and the resultant nanocomposite acellular scaffolds were named as Cu@TP-dBPs. The crosslinking degree, biomechanics, denaturation temperature and resistance to enzymatic degradation of Cu@TP-dBPs were comparable to those of glutaraldehyde crosslinked decellularized bovine pericardias (Glut-dBPs). Furthermore, Cu@TP-dBPs were biocompatible and had abilities to inhibit bacterial growth and promote the formation of capillary-like networks. Subcutaneous implantation models demonstrated that Cu@TP-dBPs were free of calcification and allowed for host cell infiltration at Day 21. Cardiac patch graft models confirmed that Cu@TP-dBP patches showed improved ingrowth of functional blood vessels and remodeling of extracellular matrix at Day 60. These results suggested that Cu@TP-dBPs not only had comparable biomechanics and biostability to Glut-dBPs, but also had several advantages over Glut-dBPs in terms of anticalcification, remodeling and integration capabilities. Particularly, they were functional patches possessing antibacterial and proangiogenic activities. These material properties and biological functions made Cu@TP-dBPs a promising functional acellular patch for cardiovascular applications.

No abstract available

Natural polymeric hydrogels are expected to serve as potential structural biomaterials, but, most of them are usually soft and fragile. Herein, a polyphenol-mediated self-assembly (PMS) strategy was developed to significantly enhance the chitin hydrogel strength and toughness at the same time, which is distinctive from the rigid-soft double-network energy-dissipation approaches. A polyphenol (tannic acid, TA as a model compound) was introduced to compete with the chitin chains self-assembly for simultaneously forming the weak chitin-TA and strong chitin-chitin networks. High-density noncovalent crosslinking involving hydrogen bonding and ionic and hydrophobic interactions endowed the PMS hydrogels with a high modulus and strength. The relatively weaker chitin-TA crosslinking acted as the sacrificial bonds to dissipate the energy, leading to the high toughness. The mechanical properties of the PMS chitin hydrogels depended on the TA concentration and ethanol aqueous coagulation, which mainly contributed to the hydrophobic and hydrophilic interactions formation, respectively. The fully naturally robust chitin-TA hydrogels exhibited considerable antibacterial properties, stomach acid solubility, and excellent biocompatibility and degradability, enabling their potential in food, biomedical, and sustainable applications.

In this study, novel tea polyphenolic-copper hybrid nanoflowers were assembled with tea polyphenol palmitate oligomers generated simply through air oxidation. It was revealed that the growth of tea polyphenolic-based hybrid nanoflowers was notably faster than protein-based ones, presumably owing to rigid polyphenolic molecular architecture and the resultant different growth mechanism. The structures and composition investigation by FT-IR, X-ray, and SEM-EDS unveiled that the whole framework of the nanoflowers was composed of complexes of tea polyphenolic oligomers and copper phosphate crystals. The tea polyphenolic hybrid nanoflowers demonstrated high loading capacity of curcumin due to flower-like porous structure and hydrophobic pockets furnished by lipophilic side chains. The nanoflowers exhibited remarkable protection capacity for carried curcumin from UV irradiation and thermal treatment. Controlled release of the nanoflowers could be readily achieved by adjustment of pH condition. Owing to high assembly efficiency, biocompatibility, and natural abundance, tea polyphenols are intriguing organic components to generate nanoflowers.

Industrial dye pollution poses a significant ecological threat, yet conventional catalytic remediation faces challenges such as catalyst aggregation and the high cost of synthetic supports. Herein, interconnected multicompartment zein porous microspheres (ZPP) were synthesized via salt crystal-induced antisolvent self-assembly to construct a green core-satellite enzyme-photocatalytic platform (ZTFTPS). ZPP exhibits excellent mass transfer and adsorption performance, with its saturated dye adsorption capacity far exceeding that of nonporous solid zein. Glucose oxidase (GOX) was encapsulated in ZPP cavities and stabilized by Fe3+-tannic acid metal-polyphenol network (MPN) coating, which acts as a selective nanofiltration gate to suppress enzyme leakage while allowing substrate transport. With Fe3+ bridging, rutile-phase titanium dioxide nanoparticles were hierarchically assembled on ZPP as satellite units to form integrated ZTFTPS. The platform integrates adsorption enrichment, in-situ H2O2 generation and photocatalytic oxidation, and locally produced H2O2 significantly enhances catalytic activity. Under optimized conditions, ZTFTPS achieves a malachite green (MG) degradation efficiency of 92.14% within 180 min, and its apparent rate constant is 217% higher than that of the unassembled physical mixture. After five consecutive cycles, the system still maintains a degradation efficiency of approximately 71.36%. Moreover, ZTFTPS effectively reduces the aquatic toxicity of dye wastewater, demonstrating outstanding biocompatibility and environmental safety. Overall, this work provides a green, scalable strategy for designing efficient porous bioreactors for organic dye wastewater treatment.

Function-inspired design of natural building blocks enables engineering nanostructured particles for tailored applications. Here, a facile coordination-driven assembly of natural polyphenols was proposed for incorporating hydrophobic citrus-derived nobiletin (NOB) into the nanoparticles (NPs) via a one-pot method in aqueous solutions. The obtained NPs provide high NOB encapsulation efficiency with small, but uniform size (≈250 nm). Moreover, they possessed prolonged colloidal stability and excellent biocompatibility and achieved robust therapeutic efficacy in alleviating ulcerative colitis (UC), in comparison with free NOB. Mechanistically, the desirable NPs maximized the inherent anti-inflammatory and antioxidant activities of natural building blocks, enabling effective attenuation of intestinal inflammation and oxidative stress, thus contributing to the restoration of the intestinal mucosal barrier and immune homeostasis. Overall, this work proposes a promising self-assembly strategy to improve the bioavailability and therapeutic potential of natural flavonoids for the treatment of UC, and ultimately offering potential benefits for patients suffering from it.