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学者姓名：黄彦
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Abstract ：
The associative phase separation of charged biomacromolecules plays a key role in many biophysical events that take place in crowded intracellular environments. Such natural polyelectrolyte complexation and phase separation often occur at nonstoichiometric charge ratios with the incorporation of bioactive proteins, which is not studied as extensively as those complexations at stoichiometric ratios. In this work, we investigated how the addition of a crowding agent (polyethylene glycol, PEG) affected the complexation between chitosan (CS) and hyaluronic acid (HA), especially at nonstoichiometric ratios, and the encapsulation of enzyme (catalase, CAT) by the colloidal complexes. The crowded environment promoted colloidal phase separation at low charge ratios, forming complexes with increased colloidal and dissolution stability, which resulted in a smaller size and polydispersity (PDI). The binding isotherms revealed that the addition of PEG greatly enhanced the ion-pairing strength (with increased ion-pairing equilibrium constant K-a from 4.92 x 10(4) without PEG to 1.08 x 10(6) with 200 g/L PEG) and switched the coacervation from endothermic to exothermic, which explained the promoted complexation and phase separation. At the stoichiometric charge ratio, the enhanced CS-HA interaction in crowded media generated a more solid-like coacervate phase with a denser network, slower chain relaxation, and higher modulus. Moreover, both crowding and complex encapsulation enhanced the activity and catalytic efficiency of CAT, represented by a 2-fold increase in catalytic efficiency (K-cat/K-m) under 100 g/L PEG crowding and CS-HA complex encapsulation. This is likely due to the lower polarity in the microenvironment surrounding the enzyme molecules. By a systematic investigation of both nonstoichiometric and stoichiometric charge ratios under macromolecular crowding, this work provided new insights into the complexation between natural polyelectrolytes in a scenario closer to an intracellular environment.
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| GB/T 7714 | Ou, Xiatong , Tang, Ziyao , Ye, Yanqi et al. Macromolecular Crowding Effect on Chitosan-Hyaluronic Acid Complexation and the Activity of Encapsulated Catalase [J]. | BIOMACROMOLECULES , 2024 , 25 (6) : 3840-3849 . |
| MLA | Ou, Xiatong et al. "Macromolecular Crowding Effect on Chitosan-Hyaluronic Acid Complexation and the Activity of Encapsulated Catalase" . | BIOMACROMOLECULES 25 . 6 (2024) : 3840-3849 . |
| APA | Ou, Xiatong , Tang, Ziyao , Ye, Yanqi , Chen, Xiaochao , Huang, Yan . Macromolecular Crowding Effect on Chitosan-Hyaluronic Acid Complexation and the Activity of Encapsulated Catalase . | BIOMACROMOLECULES , 2024 , 25 (6) , 3840-3849 . |
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Due to the rapid reaction kinetics, the morphology of chitosan/tripolyphosphate nanoparticles was difficult to control. We mixed chitosan and tripolyphosphate through a multi-inlet vortex mixer at different mixing efficiency and characteristic mixing time (tau(mix)). Below a critical tau(mix), the aggregation of primary chitosan/TPP particles can be ceased. The corresponding aggregation time of primary particles (tau(agg)) was dependent on the ionic strength, the degree of deacetylation and molecular weight of chitosan. Moreover, the particle compactness was estimated from the hydrodynamic diameter and the turbidity using a model based on the Mie theory. Slow and nonhomogeneous mixing led to more compact nanoparticles, while rapid and homogeneous mixing pro-duced nanoparticles with a higher swelling ratio. Besides, the ionic strength and polymer concentration could affect the internal structure of nanoparticles. This study revealed the significance of mixing on the internal structure of chitosan/TPP nanoparticles, which could guide the preparation of other ionically-crosslinked polysaccharide colloids.
Keyword ：
Chitosan/tripolyphosphate nanoparticles Chitosan/tripolyphosphate nanoparticles Compactness Compactness Flash nano-complexation Flash nano-complexation Mixing kinetics Mixing kinetics
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| GB/T 7714 | Yuan, Yu , Gao, Jun , Zhai, Yuzhou et al. Mixing efficiency affects the morphology and compactness of chitosan/tripolyphosphate nanoparticles [J]. | CARBOHYDRATE POLYMERS , 2022 , 287 . |
| MLA | Yuan, Yu et al. "Mixing efficiency affects the morphology and compactness of chitosan/tripolyphosphate nanoparticles" . | CARBOHYDRATE POLYMERS 287 (2022) . |
| APA | Yuan, Yu , Gao, Jun , Zhai, Yuzhou , Li, Dongcui , Fu, Caili , Huang, Yan . Mixing efficiency affects the morphology and compactness of chitosan/tripolyphosphate nanoparticles . | CARBOHYDRATE POLYMERS , 2022 , 287 . |
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Achieving a high encapsulation efficiency and loading capacity of proteins in lecithin-based liposomes has always been a challenge. Here, we use Flash Nano-Precipitation (FNP) to produce liposomes and investigated the encapsulation of model protein (Bovine Serum Albumin, BSA). Through rapid turbulent mixing, we obtained liposomes with small size, low polydispersity, and good batch repeatability at a high production rate. We demonstrated that the bilayer of liposomes prepared solely using lecithin was defective, which led to the fusion, and increased size and polydispersity. When cholesterol was added to reach a lecithin-to-cholesterol molar ratio of 5:3, a compact bilayer formed to effectively inhibit liposome fusion. The encapsulation efficiency and loading capacity of BSA was as high as ti 68% and - 6% in lecithin-cholesterol liposome, respectively, far exceeding the values reported in the literature. Further study by Quartz Crystal Microbalance with Dissipation (QCM-D) revealed that the highly effective encapsulation was due to the rapid mutual adsorption between BSA and defective/curved lecithin double layers during the liposome formation. Such rapid mutual adsorption leads to the layer-by-layer assembly and formation of onion-like compact liposome structure as revealed by Cryo-TEM. This simple FNP method provides a scalable manufacturing approach for liposomes with efficient protein encapsulation. The revealed adsorption mechanism between protein and lecithin bilayers could also serve as a guide for similar studies.
Keyword ：
Bovine Serum Albumin Bovine Serum Albumin Dissipation Dissipation Flash Nano-Precipitation Flash Nano-Precipitation Liposome Liposome Quartz Crystal Microbalance with Quartz Crystal Microbalance with
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| GB/T 7714 | Zhan, Qiang-Wei , Gao, Jun , Li, Dongcui et al. High throughput onion-like liposome formation with efficient protein encapsulation under flash antisolvent mixing [J]. | JOURNAL OF COLLOID AND INTERFACE SCIENCE , 2022 , 618 : 185-195 . |
| MLA | Zhan, Qiang-Wei et al. "High throughput onion-like liposome formation with efficient protein encapsulation under flash antisolvent mixing" . | JOURNAL OF COLLOID AND INTERFACE SCIENCE 618 (2022) : 185-195 . |
| APA | Zhan, Qiang-Wei , Gao, Jun , Li, Dongcui , Huang, Yan . High throughput onion-like liposome formation with efficient protein encapsulation under flash antisolvent mixing . | JOURNAL OF COLLOID AND INTERFACE SCIENCE , 2022 , 618 , 185-195 . |
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The transition from soluble to colloidal polyelectrolyte complex normally occurs at a critical non-stoichiometric charge ratio. Here, it is demonstrated that the conventional batch mixing produces heterogeneous binding and complexation, which can easily mask this soluble-colloidal complex transition (sol-col transition) even for weakly binding polyelectrolytes like polyacrylic acid (PAA) and poly(diallyldimethylammonium chloride) (PDADMAC). When mixed efficiently using multi-inlet vortex mixer (MIVM), the sol-col transition occurs beyond a critical charge ratio (n-/n+) and the large colloidal complexes are formed through the aggregation of small primary complexes (as revealed by atomic force microscopy). Moreover, the sol-col transition occurs at a constant charge ratio below the overlapping concentration (c*) of the long host polyelectrolyte, but at lower charge ratios above c* due to chain entanglement. When adding NaCl to the solution, the sol-col transition charge ratio first decreases, then remained stable for a period, and finally increased and vanished at high ionic strength. When replacing NaCl with chaotropic salts, the sol-col transition occurs at lower charge ratios, while kosmotropes has little impact. The solvent quality and polymer hydrophobicity effects are also discussed. With the assistance of rapid mixing, this study provides a more reliable way of studying the sol-col transition of polyelectrolyte complexes.
Keyword ：
coacervate coacervate complexation complexation flash nanocomplexation flash nanocomplexation polyelectrolytes polyelectrolytes soluble complexes soluble complexes
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| GB/T 7714 | Gao, Jun , Zhan, Qiang-wei , Tang, Ziyao et al. The Critical Transition from Soluble Complexes to Colloidal Aggregates of Polyelectrolyte Complexes at Non-Stoichiometric Charge Ratios [J]. | MACROMOLECULAR RAPID COMMUNICATIONS , 2022 , 43 (7) . |
| MLA | Gao, Jun et al. "The Critical Transition from Soluble Complexes to Colloidal Aggregates of Polyelectrolyte Complexes at Non-Stoichiometric Charge Ratios" . | MACROMOLECULAR RAPID COMMUNICATIONS 43 . 7 (2022) . |
| APA | Gao, Jun , Zhan, Qiang-wei , Tang, Ziyao , Huang, Yan . The Critical Transition from Soluble Complexes to Colloidal Aggregates of Polyelectrolyte Complexes at Non-Stoichiometric Charge Ratios . | MACROMOLECULAR RAPID COMMUNICATIONS , 2022 , 43 (7) . |
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Insight is provided into the mechanism of peptide gelation, a self-assembled process of particular interest, due to its wide existence in natural events and broad applications in food and biomaterials field, but hard to control as minor alterations in the peptide sequence. Here, we design a family of pentapeptides and control their selfassembly behaviors, from micro- and nanoparticles to nanofibers and hydrogels. Furthermore, based on the thermodynamics, the gelation kinetics and the ionization status of terminal groups, the peptide assembly goes through five stages as varying the pH value and the assembly structures are highly dependent on the charging status of the terminal groups. The gelation rules of these peptides are further investigated. Besides, we also load hydrophobic functional molecule (curcumin) into different self-assembly nanostructures with high encapsulation efficiency and remarkable thermal and light protection on curcumin. These peptides assemblies with tunable structures, encapsulation ability and photothermal stabilization could become promising candidates for hydrophobic function factor delivery in food industry.
Keyword ：
Curcumin Curcumin Hydrogel Hydrogel Nanoparticle Nanoparticle Peptide Peptide Self-assembly Self-assembly
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| GB/T 7714 | Chen, Huimin , Zhang, Tianrui , Tian, Yongqi et al. Novel self-assembling peptide hydrogel with pH-tunable assembly microstructure, gel mechanics and the entrapment of curcumin [J]. | FOOD HYDROCOLLOIDS , 2022 , 124 . |
| MLA | Chen, Huimin et al. "Novel self-assembling peptide hydrogel with pH-tunable assembly microstructure, gel mechanics and the entrapment of curcumin" . | FOOD HYDROCOLLOIDS 124 (2022) . |
| APA | Chen, Huimin , Zhang, Tianrui , Tian, Yongqi , You, Lijun , Huang, Yan , Wang, Shaoyun . Novel self-assembling peptide hydrogel with pH-tunable assembly microstructure, gel mechanics and the entrapment of curcumin . | FOOD HYDROCOLLOIDS , 2022 , 124 . |
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Continuous and large-scale production of phospholipids stabilized emulsions and nanoparticles with controllable particle size and stability has always been a challenge. Here, we use flash nano-precipitation (FNP) to produce lecithin stabilized alpha-tocopheryl acetate (Vitamin E-acetate) particles at a production rate much higher than conventional batch mixing and thin-film hydration. The FNP produces particles with more homogeneous lecithin coverage comparing to conventional slow mixing. As determined by dynamic/electrophoretic light scattering, transmission electron microscope (TEM) and Quartz Crystal Microbalance with Dissipation (QCM-D), particles with low percent core are covered by thick multiple lecithin layers and aggregate easily with the coalescence of lecithin shell; particles with medium percent core content are covered with a thin layer of lecithin, which provides a high enough zeta-potential to stabilize the particle; for particles with percent core higher than 95%, the large spacing between lecithin molecules result in Ostwald ripening and aggregation. With a given composition, the particle size and stability could both be precisely predicted using the Smoluchowski's diffusion limited particle growth model and the Derjaguin-Landau, Verwey-Overbeek (DLVO) theory. This work demonstrates that the compositions affect the adsorption of phospholipid molecules at the particle surface, which further control particle size and stability.
Keyword ：
Flash nano-precipitation Flash nano-precipitation Lecithin Lecithin Nanoparticle Nanoparticle Quartz crystal microbalance with dissipation (QCM-D) Quartz crystal microbalance with dissipation (QCM-D)
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| GB/T 7714 | Zhan, Qiang-Wei , Huang, Yan . Continuous and large-scale fabrication of lecithin stabilized nanoparticles with predictable size and stability using flash nano-precipitation [J]. | LWT-FOOD SCIENCE AND TECHNOLOGY , 2021 , 139 . |
| MLA | Zhan, Qiang-Wei et al. "Continuous and large-scale fabrication of lecithin stabilized nanoparticles with predictable size and stability using flash nano-precipitation" . | LWT-FOOD SCIENCE AND TECHNOLOGY 139 (2021) . |
| APA | Zhan, Qiang-Wei , Huang, Yan . Continuous and large-scale fabrication of lecithin stabilized nanoparticles with predictable size and stability using flash nano-precipitation . | LWT-FOOD SCIENCE AND TECHNOLOGY , 2021 , 139 . |
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The infiltration of ions into hydrogel matrix could significantly affect the microstructure and macroscopic mechanics of the gels. Here, the Hofmeister effect of various salts on the whey protein isolate hydrogels with fine-stranded and particulate microstructures is investigated by soaking the preformed hydrogels in the sodium salts of different anions. The infiltration of kosmotropic anions yield stiffer hydrogels, whereas the chaotropic anions soften the hydrogels. The hydrogels with fine-stranded microstructures are more sensitive to the salts comparing to the particulate ones due to the microscopic phase transitions and enhanced hydrophobic interactions between polymer chains occurred in fine-stranded hydrogels. Besides, despite the significant difference in water binding ability of different salts, the water holding capacity of the salt-treated hydrogels was mainly determined by the gel stiffness instead of the salt types. Similar mechanical responses of BSA and egg white protein hydrogels to the Hofmeister series was also demonstrated, suggesting that the results shown here could potentially be generalized for other globular protein hydrogels.
Keyword ：
Hofmeister effect Hofmeister effect Mechanics Mechanics Microstructure Microstructure Protein hydrogel Protein hydrogel Water holding capacity Water holding capacity
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| GB/T 7714 | Lin, Junyan , Huang, Yan , Wang, Shaoyun . The Hofmeister effect on protein hydrogels with stranded and particulate microstructures [J]. | COLLOIDS AND SURFACES B-BIOINTERFACES , 2020 , 196 . |
| MLA | Lin, Junyan et al. "The Hofmeister effect on protein hydrogels with stranded and particulate microstructures" . | COLLOIDS AND SURFACES B-BIOINTERFACES 196 (2020) . |
| APA | Lin, Junyan , Huang, Yan , Wang, Shaoyun . The Hofmeister effect on protein hydrogels with stranded and particulate microstructures . | COLLOIDS AND SURFACES B-BIOINTERFACES , 2020 , 196 . |
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The interaction between polysaccharides and proteins has attracted great interests and the phase behavior and colloidal properties of complexes between chitosan, a positively charged polysaccharide, and proteins still need careful investigation. Here, we use chitosan/casein as model system and monitor their complex size, zeta-potential, light scattering intensity and phase behavior as functions of chitosan deacetylation degree, pH and ionic strength. Chitosan flocculates casein at low polysaccharide concentrations, while stabilizes casein at moderate to high concentrations. Such flocculation and stabilization ability are dependent on the linear charge density of chitosan, where high charge density chitosan saturates casein surface charge and stabilizes the complexes at lower polysaccharide concentration. The complexes are stable at acidic pH where chitosan is highly protonated and the addition of NaCl leads to the reduction in both size and zeta-potential and facilitates complex aggregation. The phase maps are constructed to provide guidelines for further studies on chitosan/casein and other chitosan/protein complexes.
Keyword ：
Casein Casein Chitosan Chitosan Complexation Complexation Phase behavior Phase behavior
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| GB/T 7714 | Ding, Lan , Huang, Yan , Cai, XiXi et al. Impact of pH, ionic strength and chitosan charge density on chitosan/casein complexation and phase behavior [J]. | CARBOHYDRATE POLYMERS , 2019 , 208 : 133-141 . |
| MLA | Ding, Lan et al. "Impact of pH, ionic strength and chitosan charge density on chitosan/casein complexation and phase behavior" . | CARBOHYDRATE POLYMERS 208 (2019) : 133-141 . |
| APA | Ding, Lan , Huang, Yan , Cai, XiXi , Wang, Shaoyun . Impact of pH, ionic strength and chitosan charge density on chitosan/casein complexation and phase behavior . | CARBOHYDRATE POLYMERS , 2019 , 208 , 133-141 . |
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The engineering of natural protein-based hydrogels with outstanding mechanics and functionalities is an eternal pursuit in biomaterials science. Soaking methods have recently been used to simply and efficiently tune the macroscopic mechanical properties of hydrogels consisting of natural polymers (proteins or polysaccharides). However, the high concentration of salts or organic solvent within the soaked hydrogels is harmful to cells. Once the salts were eliminated, however, these hydrogels experience mechanics attenuation and swelling, limiting their applications as biomaterials. Here we utilize dual cross-link networks to address these problems by preserving the physical interactions formed during the soaking treatment. As an example, a dual cross-link gelatin-chitosan hydrogel is prepared by a click reaction and hydrophobic interactions, which achieve an unusual combination of abundant water content (>87%), strong mechanics (ultimate strength ∼1.8 MPa), antiswelling properties (swelling ratio of 11.25% in PBS for 7 days), thermal stability, and biocompatibility. We expect that this strategy can be generalized for the development of tough, biocompatible, and environmentally stable protein-based hydrogels. © 2019 American Chemical Society.
Keyword ：
Biocompatibility Biocompatibility Hydrogels Hydrogels Hydrophobicity Hydrophobicity Mechanics Mechanics Proteins Proteins Salts Salts
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| GB/T 7714 | He, Qingyan , Huang, Da , Yang, Jianmin et al. Dual Cross-Link Networks to Preserve Physical Interactions Induced by Soaking Methods: Developing a Strong and Biocompatible Protein-Based Hydrogel [J]. | ACS Applied Bio Materials , 2019 , 2 (8) : 3352-3361 . |
| MLA | He, Qingyan et al. "Dual Cross-Link Networks to Preserve Physical Interactions Induced by Soaking Methods: Developing a Strong and Biocompatible Protein-Based Hydrogel" . | ACS Applied Bio Materials 2 . 8 (2019) : 3352-3361 . |
| APA | He, Qingyan , Huang, Da , Yang, Jianmin , Huang, Yan , Wang, Shaoyun . Dual Cross-Link Networks to Preserve Physical Interactions Induced by Soaking Methods: Developing a Strong and Biocompatible Protein-Based Hydrogel . | ACS Applied Bio Materials , 2019 , 2 (8) , 3352-3361 . |
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Mixing oppositely charged polyelectrolytes and multivalent counterion solutions at low concentrations leads to the formation of colloidal ionically crosslinked polyelectrolyte particles. Due to the rapid reaction kinetics, the complexation processes and the final product could vary significantly when changing the mixing efficiency, which was often overlooked in previous studies. To investigate the effect of mixing on the polyelectrolyte-based colloid formation, we use chitosan/tripolyphosphate mixtures as a model system and compare the particle formation under flash nano-complexation (FNC, representing rapid and efficient mixing) and conventional dropwise mixing. It turns out that the non-uniform mixing and rapid complex formation during conventional mixing lead to particle formation at a low tripolyphosphate : chitosan ratio, which could be avoided by FNC. When mixing using FNC, the particle formation started at a critical tripolyphosphate : glucosamine ratio, below which only soluble complexes exist, and such a critical ratio is independent of the chitosan molecular weight and charge density. Homogeneous mixing also leads to the formation of a large amount of small primary particles without further aggregation due to the rapid consumption of free crosslinking counterions. Such a strong dependency of ionically crosslinked polyelectrolyte colloid formation on the mixing efficiency was also demonstrated using other polyelectrolytes and counterions. Thus, the mixing efficiency could have a significant impact on the interpretation of the complexation process and the mechanisms and should be carefully discussed when studying ionically crosslinked polyelectrolyte colloids.
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| GB/T 7714 | Yuan, Yu , Huang, Yan . Ionically crosslinked polyelectrolyte nanoparticle formation mechanisms: the significance of mixing [J]. | SOFT MATTER , 2019 , 15 (48) : 9871-9880 . |
| MLA | Yuan, Yu et al. "Ionically crosslinked polyelectrolyte nanoparticle formation mechanisms: the significance of mixing" . | SOFT MATTER 15 . 48 (2019) : 9871-9880 . |
| APA | Yuan, Yu , Huang, Yan . Ionically crosslinked polyelectrolyte nanoparticle formation mechanisms: the significance of mixing . | SOFT MATTER , 2019 , 15 (48) , 9871-9880 . |
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