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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2022 · IF 9.965

In situ complex coacervation supported by self-coated polydopamine interlayer on uniform-sized essential oils droplet

Qirui Tian,Weiqing Zhou,Qiong Cai,Xiaoyun Pan,Guanghui Ma,Guoping Lian

Hypothesis Essential oils (EOs) are common additives in daily products by virtue of their olfactory, physicochemical, and biological characteristics . However, EOs are physicochemically unstable and susceptible to degradation or loss, leading to limited shelf life and inadequate efficacy. Herein we propose a new bi-layered encapsulation structure in combination with complex coacervation and self-coating of polydopamine (PDA) on membrane emulsified mono-dispersion of EOs droplets. Experiments A mono-dispersed EOs emulsion stabilized by nonionic surfactants was produced by membrane emulsification , wherein the EOs droplets were applied as soft templates to deposit a superficial PDA layer. Under alkaline conditions, gelatin (GE) was bound to the PDA layer and further applied as in situ coacervation sites for gum Arabic (GA). Structural identification and morphological observation proved the successful preparation of bi-layered EOs capsules. Findings Compared with traditional complex coacervation strategies, current novel bi-layered capsules showed significantly improved structural stability, thermal stability, providing better protection of EOs with sustained release properties. Moreover, the encapsulation efficiency and loading content were both proved higher for the bi-layered system. The first report on PDA-coating onto surfactants-absorbed macroemulsion droplets also provides an in-depth insight into applying PDA as versatile intermediate functional biomaterials.

研究领域: 食品科学 · 材料科学 · 化学工程
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FOOD RESEARCH INTERNATIONAL · 2023 · IF 8.1

pH-induced complex coacervation of fish gelatin and carboxylated chitosan: Phase behavior and structural properties

Chen Cheng,Zongcai Tu,Hui Wang

The aim of this study was to investigate the phase behavior and structural properties of fish gelatin complex coacervation with carboxylated chitosan as a function of pH by varying the amount of carboxylated chitosan added (0–0.25%, w/v) while keeping the fish gelatin concentration constant at 0.667% (w/v). Zeta potential indicated that electrostatic interaction drove the complex coalescence of fish gelatin and carboxylated chitosan to form soluble or insoluble complexes. The turbidity of the fish gelatin-carboxylated chitosan complex system was greatest at a carboxylated chitosan concentration of 0.2%. UV and fluorescence spectroscopy indicated that the carboxylated chitosan changed the tertiary conformation of fish gelatin. Circular dichroism showed that complexation of fish gelatin with carboxylated chitosan resulted in a shift from the α-helix to the β-sheet structure of fish gelatin. In particular, at pH 5, the fish gelatin complexed with carboxylated chitosan had a disordered structure. X-ray diffraction and scanning electron microscopy of the composite coacervates both investigated that electrostatic interaction between the two replaced molecular interaction within the carboxylated chitosan to form a new lamellar porous structure. These findings may in future enable the use of fish gelatin-carboxylated chitosan complex systems in the design of new food matrices.

CAS / MDL: 9012-76-4
研究领域: 食品科学 · 生物化学
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS · 2024 · IF 4.9

Bi-layered oil encapsulates formed by polydopamine-supported in situ complex coacervation: Investigation of structure formation and sustained release performance

Qirui Tian,Weiqing Zhou,Qiong Cai,Xiaoyun Pan,Guanghui Ma,Guoping Lian

In polydopamine (PDA)-supported in situ complex coacervation, PDA is pre-coated onto emulsion droplets, and further applied as an interlayer to support the interfacial immobilization of coacervates biopolymers. In the current research, the stepwise immobilization of gelatin (GE) and gum Arabic (GA) onto PDA layer is monitored to in-depth investigate the mechanism of PDA layer as coating material and functional substrates. GE and GA were applied as adsorbates, with different forms of PDA (spherical shell, planar solid, and nanoparticles) as substrates. Real-time observations of the binding steps were performed using quartz crystal monitor with dissipation (QCM-D) and isothermal titration calorimetry (ITC). Meanwhile, using PDA-supported coacervates as encapsulating material, sustained release of essential oil volatiles was also evaluated, either dispersed in detergent solution or freeze dried in open air. The anti-oxidation performance was determined by measuring the absorbance of lipid hydroperoxide using UV spectrophotometer. The results revealed that PDA enabled synergistic immobilization of biopolymers through chemical bonding and adhesive force during the processing of in situ complex coacervation, thus enhanced protection of core compounds with two-stage releasing kinetics and prevented hyperoxidation. Also, PDA-based colloids and substrates also exhibit controllable conformation characteristic, provide a promising prospect as versatile intermediate functional biomaterials for encapsulation.

研究领域: 材料科学 · 化学工程 · 食品科学 · 药学
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Polymers · 2021 ·Vol. 13 ·期 6 ·866 · IF 4.329

Sunscreen Enhancement of Octyl Methoxycinnamate Microcapsules by Using Two Biopolymers as Wall Materials

Chuntao Xu,Xuemin Zeng,Zujin Yang,Hongbing Ji

Octyl methoxycinnamate (OMC) is widely used as a chemical sunscreen in sunscreen cosmetics. However, its direct contact with the skin would bring certain risks, such as skin photosensitive reaction. How to improve the effect of skin photodamage protection has become a current research hotspot. Encapsulating ultraviolet (UV) filters into microcapsules is an interesting method to increase the photostability of filters. In this study, sodium caseinate (SC) and arabic gum (GA) are chosen as wall materials to prepare synergistic sunscreen microcapsules by complex coacervation technology. A series of experiments are conducted to investigate the effects of pH, wall material concentration, and wall/core ratio on the formation of OMC microcapsules. The morphology, composition, and stability of OMC microcapsules are characterized by scanning electron microscopy (SEM), Fourier transform infrared spectroscopy (FTIR), and thermogravimetric analysis (TGA). The OMC microcapsule is uniform in size distribution, smooth in surface morphology, and has good thermal stability. The results show that the ultraviolet absorption of the OMC microcapsules is better than that of the uncoated OMC for the ultraviolet-B (280–320 nm). Moreover, the OMC microcapsule released 40% in 12 h, while OMC released 65%, but the sun protection factor (SPF) of the OMC microcapsule sunscreen is 18.75% higher than that of OMC. This phenomenon may be attributed to the hydrophobic interaction between SC and OMC and the electrostatic interaction between SC and GA.Keywords:octyl methoxycinnamate;sunscreen;microcapsule;complex coacervation;synergistic effects

CAS / MDL: 83834-59-7 5466-77-3
研究领域: 生物学 · 材料科学 · 化妆品科学
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ACS Applied Polymer Materials · 2024 · IF 4.4

Heteropolysaccharide-Based Coacervate Microdroplets as Enzyme Carriers for Detection of Cholesterol

Cairong Qiao,Ling Qian,Qiang Peng,Wanqing Yue

We constructed heteropolysaccharide-based complex coacervate microdroplets using pectin and DEAE-dextran via electrostatic interactions. The coacervate microdroplets were stable from pH 3 to 12 and completely dissociated at a NaCl concentration of 160 mM. When cholesterol oxidase was distributed in the microdroplets, the enzyme activity of cholesterol oxidase did not decrease, and it was made more stable. Through spiked recovery experiments of cholesterol in serum and a comparison with the results of commercial assay kits, we successfully validated that the assay can be used for the detection of cholesterol in real samples.

CAS / MDL: 112-40-3 28752-68-3
研究领域: 生物化学 · 分析化学 · 材料科学
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2021 · IF 6.953

Microencapsulation of algae oil by complex coacervation of chitosan and modified starch: Characterization and oxidative stability

Hongyan Mu,Zhaoxia Song,Xin Wang,Deda Wang,Xiaoqing Zheng,Xiaodan Li

The formation of complex coacervation using chitosan and octenyl succinic anhydride modified starch (OSA starch) and microencapsulation of algae oil were investigated in this study. The zeta-potential, turbidity and coacervate yield were evaluated as a function of pH and the chitosan- OSA starch mass ratio. The highest coacervate yield was achieved at pH 6.0 with a chitosan to OSA starch ratio of 1:3 ( w/w ). Isothermal titration calorimetry (ITC) indicated favorable affinity (Ka = 1.51 × 10 5  M −1 ) between chitosan and OSA starch. The microcapsules yielded an encapsulation efficiency (EE) in the range of 42.8 ± 0.8%- 93.1 ± 1.2%, the loading capacity ranged between 30.4 ± 2.7% and 58.3 ± 1.3%. Fourier transform infrared spectroscopy (FT-IR) spectra and scanning electron microscopy (SEM) further confirmed the microencapsulation. In comparison with the bulk oil, the microencapsulated algae oil exhibited improved oxidative stability during storage.

CAS / MDL: 9012-76-4
研究领域: 食品科学 · 生物技术
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FOOD HYDROCOLLOIDS · 2021 · IF 9.147

Sodium chloride-programmed phase transition of β-conglycinin/lysozyme electrostatic complexes from amorphous precipitates to complex coacervates

Jiabao Zheng,Qing Gao,Ge Ge,Jihong Wu,Chuan-he Tang,Mouming Zhao,Weizheng Sun

The associative phase separation of biomacromolecules can produce both liquid-like coacervates or solid-like precipitates. In this study, we found that sodium chloride (NaCl) can programme the phase transition of β-conglycinin/lysozyme (β-CG/LYS) complexes. NaCl reduced the ζ-potential of both β-CG and LYS. Their complex coacervate was formed at pHs 6 and 7 with 5–80 mM NaCl and at pH 8 with 40–80 mM NaCl. Unlike the high critical salt concentration and entropy gain driving force of polyelectrolyte-based complex coacervation, 100 mM NaCl almost completely inhibited β-CG/LYS complexation, and the exothermic enthalpy change was the main driving force for β-CG/LYS complex formation. Confocal laser scanning microscopy with fluorescein isothiocyanate-labeled proteins demonstrated dynamic protein exchange in coacervate droplets, similar to that in polyelectrolyte-based complex coacervates.

CAS / MDL: 3326-32-7
研究领域: 食品科学 · 胶体化学 · 生物物理学
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Biomaterials Science · 2017 ·Vol. 5 ·期 8 ·1558-1566 · IF 4.21

Phosphatase-triggered cell-selective release of a Pt(IV)-backboned prodrug-like polymer for an improved therapeutic index

Shao-Lu Li,Yingqin Hou,Yali Hu,Jin Yu,Wei Wei,Hua Lu

We describe here the synthesis and cell-selective delivery of a cationic Pt(IV)-backboned prodrug-like polymer P(DSP-DAEP). P(DSP-DAEP) features excellent aqueous solubility, unusually high (44.5%) drug loading, can be rapidly reduced to release the active cisplatin, and is more potent than its small molecular Pt(IV) precursor DSP. P(DSP-DAEP) can be formulated with an oppositely charged methoxyl poly(ethylene glycol)-block-poly(L-phosphotyrosine) (mPEG-b-PpY) to afford a polyion micelle (Pt-PIC) by taking advantage of polyelectrolyte coacervation. Preliminary in vitro cellular uptake and cytotoxicity assays indicate that Pt-PIC exhibits receptor (surface alkaline phosphatase)-dependent uptake and cytotoxicity. Overall, our results suggest a new approach to the improved therapeutic index of platinum-based anticancer drugs via cell-selective delivery.

研究领域: 药物化学 · 肿瘤学 · 生物材料学
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS · 2010 · IF 1.988

Gelatin/carboxymethylcellulose/dioctyl sulfosuccinate sodium microcapsule by complex coacervation and its application for electrophoretic display

Runying Dai,Gang Wu,Weigang Li,Qiang Zhou,Xihua Li,Hongzheng Chen

We have described the microcapsules containing electrophoretic fluid as core material, prepared from gelatin, sodium carboxymethylcellulose (NaCMC) and dioctyl sulfosuccinate sodium (DSS) by complex coacervation method. The gelatin/NaCMC/DSS microcapsules are characterized by optical microscopy (OM), scanning electron microscopy (SEM), particle size analysis and thermogravimetric analysis (TGA). It is found that DSS plays an important role in the formation of the microcapsule wall and the concentration of DSS deeply affects the yield of microcapsules by enhancing the interaction between gelatin and NaCMC. The microcapsules prepared with DSS content of 0.6   mM show compact capsule wall which endows the capsules with good barrier property and high thermal stability. These microcapsules are applied successfully to prepare a 4-in. clock display panel controlled by single-chip microprocessor (SCM) operated at a low direct current (DC) voltage of 3   V, demonstrating that these microcapsules are potential for the applications in the area of electrophoretic displays.

研究领域: 材料科学 · 显示技术
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JOURNAL OF DRUG DELIVERY SCIENCE AND TECHNOLOGY · 2018 · IF 2.297

Roles of alcohol desolvating agents on the size control of bovine serum albumin nanoparticles in drug delivery system

Si Sun,Qian-Ru Xiao,Yang Wang,Yong Jiang

Nanoparticles made of bovine serum albumins (BSA) have shown great application value in medical field as drug carriers because of albumin's excellent biocompatibility. BSA nanoparticles are generally fabricated through coacervation process, which can be strongly affected by pH, temperature, dropping speed, and different desolvating agents, such as ethanol, acetone. However, the influence of different alcohols as desolvating agents on BSA nanoparticles has not been systematically clarified so far. Herein, ethanol, propyl alcohol and isopropyl alcohol were chosen as desolvating agents to produce BSA nanoparticles and the obtained nanoparticles were studied comprehensively in terms of their size, polydispersity, morphology, yield, spectroscopic property, encapsulation efficiency, and in vitro cell uptake. The results show that propyl alcohol and isopropyl alcohol had stronger coacervation ability to produce nanoparticles with larger sizes and higher yields, while it would be easier to control the size of the nanoparticles produced with ethanol. BSA nanoparticles produced with all of the three alcohols could be taken by MCF-7 cells, suggesting that they are suitable to be used as drug carriers. This work provides a good choice of alcohol derived desolvating agents for further studies on BSA nanoparticles and their potential applications in drug delivery systems.

CAS / MDL: 9048-46-8
研究领域: 纳米技术 · 药剂学 · 生物医学工程
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Advanced Science · 2025 · IF 14.1

Biomineralization-Inspired Membranization Toward Structural Enhancement of Coacervate Community

Chunyu Zhao,Xiaoliang Wang,Lianning Li,Hu Huang,Bingzhao Wu,Lei Zhang,Xin Huang

The design and assembly of protocell models that can mimic the features and functions of life present a significant research challenge with the potential for far-reaching impact. Inspired by the natural phenomenon of microbe-induced mineralization, a way is developed to induce the spontaneous formation of mineralized membrane on the surface of coacervate droplets utilizing Fe 3+ ions. In particular, the effect of Fe 3+ ions on the microstructure of droplets at the molecular level is dissected by combining theoretical and experimental approaches. The reversible formation process of membrane can be regulated by redox reactions involving Fe 2+ /Fe 3+ ions within the coacervate. The formation of mineralized membrane not only enhances the stability of the coacervate droplets and prevents aggregation and coalescence, but also allows the aggregation of adjacent droplets together. The membranized coacervate assemblages retain the inherent properties of biomolecule sequestration and enzyme catalysis, and also demonstrate excellent resistance to high temperatures and pressures as well as good stability for over 30 days. This study will offer a new platform for the assembly of coacervate-based life-like biomimetic systems, as well as enhance the understanding of the interactions underlying various biological phenomena at the molecular level.

研究领域: 生物化学 · 分子生物学 · 材料科学 · 生命起源研究
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FOOD HYDROCOLLOIDS · 2024 · IF 11

Fabrication and characterization of fish gelatin/soluble soybean polysaccharide edible blend films through complex coacervation

Yiwei Wang,Jie Liu,Yidan Ding,Xuejing Zheng,Yongchao Jiang,Keyong Tang

Complex coacervation of polysaccharides and proteins is a liquid-liquid phase separation that can occur when they are oppositely charged in aqueous solution. In the present work, soluble soybean polysaccharide (SSPS) and fish gelatin (FG) edible blend films were prepared through pH-induced complex coacervation. The optimal SSPS-to-FG mass ratio (1:3) and pH (5.0) conditions for complex coacervation was determined by measuring the maximum turbidity of SSPS/FG mixtures. The effect of SSPS-FG coacervates on microstructure and properties of SSPS/FG blend films were investigated. Results indicated that the film surface roughness and water contact angle were increased due to the presence of coacervates, while the water vapor permeability and Young's modulus were decreased. The SSPS/FG films containing coacervates had similar optical properties, tensile strength, heat seal ability and water sensitivity but improved thermal stability than the coacervate-free SSPS/FG films. When curcumin was incorporated into SSPS/FG films as an active ingredient, the complex coacervates effectively delayed the release of curcumin from the blend films into lipophilic food simulants. Thus, SSPS/FG blend films fabricated by complex coacervation could serve as potential substrates for developing active food packaging materials with satisfactory properties.

CAS / MDL: 64-19-7 56-81-5
研究领域: 食品科学 · 材料科学 · 化学工程
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